GCB Bioenergy - 2018 - Schmidt - Pyrogenic Carbon Capture and Storage

Received: 27 March 2018
| Accepted: 4 August 2018
DOI: 10.1111/gcbb.12553
RESEARCH REVIEW
Pyrogenic carbon capture and storage
Hans‐Peter Schmidt1 | Andrés Anca‐Couce2 | Nikolas Hagemann1,3 |

Constanze Werner4 | Dieter Gerten4,5 | Wolfgang Lucht4,5 | Claudia Kammann6
1
Ithaka Institute, Hamburg, Germany
2
Abstract
Institute of Thermal Engineering, Graz
University of Technology, Graz, Austria The growth of biomass is considered the most efficient method currently available
3
Environmental Analytics, Agroscope, to extract carbon dioxide from the atmosphere. However, biomass carbon is easily
Zurich, Switzerland degraded by microorganisms releasing it in the form of greenhouse gases back to the
4
Potsdam Institute for Climate Impact atmosphere. If biomass is pyrolyzed, the organic carbon is converted into solid (bio-
Research (PIK), Research Domain I:
Earth System Analysis, Potsdam, char), liquid (bio‐oil), and gaseous (permanent pyrogas) carbonaceous products.
Germany During the last decade, biochar has been discussed as a promising option to improve
5
Humboldt‐Universität zu Berlin, soil fertility and sequester carbon, although the carbon efficiency of the thermal con-
Geography Department, Berlin, Germany
6
version of biomass into biochar is in the range of 30%–50% only. So far, the liquid
Department of Applied Ecology,
Hochschule Geisenheim University,
and gaseous pyrolysis products were mainly considered for combustion, though they
Geisenheim, Germany can equally be processed into recalcitrant forms suitable for carbon sequestration. In
this review, we show that pyrolytic carbon capture and storage (PyCCS) can aspire
Correspondence
Hans‐Peter Schmidt, Ithaka Institute, for carbon sequestration efficiencies of >70%, which is shown to be an important
Hamburg, Germany. threshold to allow PyCCS to become a relevant negative emission technology. Pro-
Email: [email protected]
longed residence times of pyrogenic carbon can be generated (a) within the terres-
Funding information trial biosphere including the agricultural use of biochar; (b) within advanced bio‐
Bundesministerium für Bildung und based materials as long as they are not oxidized (biochar, bio‐oil); and (c) within
Forschung, Grant/Award Number:
suitable geological deposits (bio‐oil and CO2 from permanent pyrogas oxidation).
01LS1620A, 01LS1620B
While pathway (c) would need major carbon taxes or similar governmental incen-
tives to become a realistic option, pathways (a) and (b) create added economic value
and could at least partly be implemented without other financial incentives. Pyroly-
sis technology is already well established, biochar sequestration and bio‐oil seques-
tration in soils, respectively biomaterials, do not present ecological hazards, and
global scale‐up appears feasible within a time frame of 10–30 years. Thus, PyCCS
could evolve into a decisive tool for global carbon governance, serving climate
change mitigation and the sustainable development goals simultaneously.
KEYWORDS
biochar, bio‐oil, carbon sequestration, climate mitigation, permanent pyrogas, pyrolysis, tCDR
1 | INTRODUCTION accumulation in the terrestrial system has to return to an

equilibrium by 2050 at the latest (Obersteiner et al., 2018;
To keep global warming in the range that has sustained
Rockström et al., 2016, 2009 ). To achieve this, greenhouse
civilization during the past millennia, the carbon balance
gas (GHG) emissions need to be reduced by at least 90%
between emissions to the atmosphere and carbon
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© 2018 John Wiley & Sons Ltd
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574
| SCHMIDT ET AL.
with the world economy becoming climate neutral by 2050 However, the capacity of soils to accumulate organic carbon
(Rogelj et al., 2015, Bertram et al., 2015; Sanderson, is likely limited (Barré et al., 2017; Minasny, Arrouays,
O’Neill, & Tebaldi, 2016; Schleussner et al., 2016). How- et al., 2017) and requires large amounts of nitrogen (van
ever, even if the most ambitious scenarios of global GHG Groenigen et al., 2017). Maintaining increased soil organic
emission reductions were implemented within this time matter (SOM) stocks will depend on agronomic methods and
frame, the additional need for large‐scale atmospheric car- may further be hampered by the effects of climate change
bon dioxide removal (CDR) to prevent overshooting the (Sierra, Trumbore, Davidson, Vicca, & Janssens, 2015). The
1.5°C temperature threshold remains (Boysen, Lucht, MRT of SOM is 50–80 years at maximum (Schmidt et al.,
Schellnhuber, et al., 2016; Hansen et al., 2017; Smith 2011; Wang & Chang, 2001). Thus, increasing SOM is
et al., 2015). Thus, most recent scenarios from integrated clearly an important CDR with extensive ecological cobene-
assessment models (IAMs) include the large‐scale deploy- fits; however, its long‐term potential may not be sufficient as
ment of so‐called negative emissions technologies (NETs) sole CDR technology (Boysen, Lucht, Schellnhuber, et al.,
to achieve CDR (Fuss et al., 2014; Hansen et al., 2017; 2016; Smith et al., 2015; Soussana et al., 2017; van Groeni-
Riahi et al., 2015; Rogelj et al., 2015; Rogelj, McCollum, gen et al., 2017). Moreover, the conversion of plant residues
Reisinger, Meinshausen, & Riahi, 2013; Van Vuuren et al., (shoots, roots, and root‐derived C) into SOM has low C‐effi-
2013). Technical solutions to extract CO2 from the atmo- ciencies of 10%–15% (Bolinder, Angers, Giroux, & Laver-
sphere like direct air capture (Kumar et al., 2015; Sanz‐ dière, 1999) not considering SOM saturation (Six & Jastrow,
Pérez, Murdock, Didas, & Jones, 2016), enhanced weather- 2002). A complementary way forward to extend the MRT of
ing (Koeve, Keller, & Oschlies, 2017; Moosdorf, Renforth, biogenic C in the terrestrial system and to increase C‐effi-
& Hartmann, 2014), and artificial ocean alkalinization ciencies is the pyrolytic treatment of biomass with subse-
(Montserrat et al., 2017) are promising geoengineering quent sequestration in the bio‐, geo‐, and anthroposphere.
approaches, although they are, to different degrees, either In pyrolysis processes, shredded biomass is heated under
not yet mature or available at the needed scale, or the risk oxygen‐deficient atmospheres to temperatures between 350
of large‐scale implementation may still be considered too and 900°C (EBC, 2012) converting the biomass into a solid
high (Hansen et al., 2017). An increase in terrestrial and (biochar), a liquid (bio‐oil), and a permanent pyrogas frac-
marine biomass production, combined where possible with tion. In most current pyrolysis systems, the pyrolysis liquids
the sequestration of a significant part of its accumulated and gases are combusted for the production of thermal and
carbon, is therefore considered a CDR strategy that may be electric energy releasing the carbon as GHG back to the
implemented most rapidly, and with the lowest risk of atmosphere. While this is often considered as carbon neutral,
other geological and ecological processes (Hansen et al., that is “green energy” because it is made from biomass, it
2017; Rockström et al., 2017; Smith et al., 2015). can only sequester the biochar carbon but not the carbon
Beside afforestation, bioenergy production with carbon from the gaseous and liquid phases which is more than half
capture and storage (BECCS) is the only NET included in of the initial biomass carbon. To optimize the carbon
the mitigation scenarios of the Intergovernmental Panel on sequestration potential, the following review is focused on
Climate Change's (IPCC) Fifth Assessment Report (Allen the material use of all pyrogenic carbon species (i.e. solid,
et al., 2014). The BECCS scenario anticipates that biomass liquid, gaseous), and to reduce the combustion of pyrolytic
combustion could become a major pathway for clean products to a minimum. We specifically investigate the con-
energy production and that capturing the emitted CO2 ditions and capacity of pyrogenic carbon capture and storage
would become a complementary technology. Besides the (PyCCS) as a complete negative emission system, quantify-
known and unknown risks of fossilizing CO2 and its high ing the C‐sequestration potential of all three pyrolysis prod-
costs (>150 USD/t CO2 (Klein et al., 2014; Smith et al., ucts including their use as bio‐based materials and
2015), BECCS is increasingly being recognized for poten- agronomic amendments, but also for geologic carbon stor-
tially harming ecosystem services and the integrity of the age. We review literature on biochar, bio‐oil, and pyrolysis
biosphere with its extended implementation (Boysen, systems for the required properties of pyrolytic products and
Lucht, Gerten, & Heck, 2016; Burns & Nicholson, 2017; summarize production conditions optimized for material use
Heck, Gerten, Lucht, & Popp, 2018). and C sequestration. We then compare PyCCS with BECCS
Alternatively, CDR could be achieved through increased in terms of carbon and nutrient efficiency, costs, environ-
net primary productivity (NPP) of the biosphere, combined mental risks, and time frame for technology implementation.
with the extension of the mean residence time (MRT) of the
biogenic carbon (i.e. net C sequestration) (Erb et al., 2017;
Smith et al., 2015). Increasing soil organic matter is one way
2 | PYROLYSIS TECHNOLOGY
forward to extend MRTs (Lal, 2011; Minasny, Malone, Pyrolysis is the thermal conversion of carbonaceous materi-
et al., 2017; Zomer, Bossio, Sommer, & Verchot, 2017). als (e.g. biomass) in a low oxygen atmosphere. During
SCHMIDT ET AL. | 575
pyrolysis, biomass evolves into biochar (solid product) and natural fires (Cheng, Lehmann, & Engelhard, 2008; Santín
releases volatiles, the so‐called pyrolytic gas or pyrogas. et al., 2017), or by (c) archeological evidence (Braadbaart,
Cooled to ambient temperature, pyrogases mostly condense Poole, & Brussel, 2009; Criscuoli et al., 2014).
into a liquid, the bio‐oil. The remaining gas is called per- The MRT of biochar is strongly related to its H/Corg
manent pyrogas referring to the volatiles of the pyrolysis ratio (which depends mainly on the pyrolysis temperature)
gas that do not condense at ambient temperature. The qual- and to the environmental conditions of its storage (Braad-
ity and properties of the three products and their yield frac- baart et al., 2009; Camps‐Arbestain, Amonette, Singh,
tion depend on the feedstock and its properties (e.g. woody Wang, & Schmidt, 2015). In a meta‐analysis of 111 experi-
vs. herbaceous biomass, soft‐ vs. hard‐wood, moisture con- ments on biochar persistence, Lehmann et al. (2015) esti-
tent, particle size) and on the pyrolysis process conditions. mated that biochars with a H/Corg ratio of <0.4 have, when
These include heating rate, highest treatment temperature applied to soil, a MRT of >1,000 years, corresponding to
(HTT), residence time of the solid, residence time of the half‐life (T½) times of ~700 years. Similar estimates were
volatiles as determined by the gas flow rate in the pyrolysis obtained in a review by Zimmerman and Gao (2013).
reactor, direction of gas flow and pyrogas pressure, residual Another meta‐analysis by Wang, Xiong, and Kuzyakov
oxygen contact, and for biochar also quenching/activation (2016) based on 24 studies with stable (13C) and radioac-
procedures (Boateng, Garcia‐Perez, Masek, Brown, & tive (14C) carbon isotopes found MRTs of 556 years inde-
Campo, 2015; Hagemann et al., 2018; Weber & Quicker, pendent of the H/Corg ratio. However, the soil environment
2018). seems to play a dominant role in PyC persistence. While
The solid pyrolysis product, biochar, is a highly porous the majority of field and laboratory studies reveal centen-
material consisting mainly of polyaromatic hydrocarbons nial MRTs of >100 years (Lehmann et al., 2015; Rasse
and inorganic species originally contained in the biomass. et al., 2017), some studies show that under certain soil
Bio‐oil is a dark brown, oil‐like liquid composed of water (biota) conditions, biochar can be degraded biologically
and more than 100 oxygenated condensable hydrocarbon with much shorter MRTs (de la Rosa, Miller, & Knicker,
species including acetic acid, methanol, aldehydes, ketones, 2018; de la Rosa, Rosado, Paneque, Miller, & Knicker,
phenols, oligomeric sugars, and water‐insoluble lignin‐ 2018). In their recent assessment of the worlds’ stocks of
derived compounds (Sanna, Li, Linforth, Smart, & a, PyC, Reisser et al. (2016) found that soil PyC stocks aver-
Andrésen JM, 2011). The remaining permanent pyrogas age 13.7% (i.e. 200 Pg C globally) of the overall soil
includes CO, CO2, CH4, H2, and CxHy; it is highly inflam- organic carbon stocks down to 2 m depth. Soil clay content
mable. To date, a multitude of different pyrolysis technolo- and pH were the variables with the strongest predictive
gies exists that are usually optimized for one of the value for high PyC contents in soils. However, native, fire‐
products, for example fast or flash pyrolysis for bio‐oil, derived PyC in soils is chemically different to biochar pro-
slow pyrolysis for biochar, or gasification for pyrolytic duced from the same feedstock; the chemical characteristics
gases. of biochar produced from the same material point toward
greater stability of the latter (Santín et al., 2017).
Once mixed into soil, PyC particles shatter into micro‐
3 | BIOCHAR CARBON
and nanoparticles (Zimmerman & Gao, 2013). This is
PERSISTENCE
mainly a physical process, that is the chemical structure
During the last decade, biochar was increasingly discussed and the amount of carbon stored remain unchanged (Spo-
as a tool for carbon sequestration in soil (Fowles, 2007; kas, et al., 2014). Fine particles can be transported verti-
Laird, 2008; Lehmann, Gaunt, & Rondon, 2006; Matovic, cally to deeper soil horizons, groundwater, or horizontally
2011; Woolf, Amonette, Street‐Perrott, Lehmann, & into adjacent soils or waterbodies where it may be pro-
Joseph, 2010; Woolf, Lehmann, & Lee, 2016). It is the tected against degradation. In fact, deep soil horizons are
most resistant form of organic carbon in soils as well as in the most important compartments for sequestration of soil
lake and ocean sediments (Cotrufo et al., 2016; Lehmann organic carbon on timescales of decades to centuries (Lor-
et al., 2015; Reisser, Purves, Schmidt, & Abiven, 2016; enz & Lal, 2014). Over longer timescales, groundwater and
Zimmerman & Gao, 2013). In the absence of very long‐ sediments may be more relevant sequestration compart-
term (1,000 years) field experiments in various environments due to micronized biochar–carbon species being
ments and climatic zones, the MRT can only be approxi- even better preserved there from microbial and chemical
mated by (a) short‐term (<10 years) experimental data, degradation (Zimmerman & Gao, 2013). Micron‐sized and
combined with mathematical decay models and temperature nanofractured PyC may ultimately reach the ocean (Foer-
normalization (Kuzyakov, Bogomolova, & Glaser, 2014; eid, Lehmann, & Major, 2011; Hockaday, Grannas, Kim,
Lehmann et al., 2015), by (b) bottom‐up assessments of & Hatcher, 2007; Jaffe et al., 2013; Major, Lehmann, Ron-
fire frequencies and pyrogenic carbon (PyC) leftovers from don, & Goodale, 2010). In the ocean floor sediments, PyC
576
| SCHMIDT ET AL.
MRTs of >6,000 years were calculated (Coppola, Ziolk- substrate additive (Jaiswal, Elad, Cytryn, Graber, & Fren-
owski, Masiello, & Druffel, 2014). However, to the best of kel, 2018; Kern et al., 2017). When applied to soil, biochar
our knowledge, no published study experimentally proved can, but does not always, improve parameters like soil
and quantified the transfer of PyC from topsoil applications nutrient retention, water retention, soil pH, cation exchange
to waterbodies and sediments (Maestrini et al., 2014). capacity, or microbial activity, with effects strongly
Often, a proportion of an applied biochar are just missing depending on both soil and biochar characteristics (Atkin-
after several years without having left the soil system as son, Fitzgerald, & Hipps, 2010; Cornelissen et al., 2013;
CO2 efflux (e.g. Major et al., 2010). Lehmann et al., 2011) and plant species grown on it (e.g.
Based on the available data, it is hard to provide a Guereña et al., 2015; Schmidt, Pandit, Cornelissen, &
globally valid leakage rate of biochar applied to soil after Kammann, 2017). In the longer term, for example with
80 years. Biochars produced at pyrolysis temperatures repeated additions of biochar organic blends, biochar will
>400°C show MRTs, based on extrapolations from degra- modify the original soil chemical and physical properties
dation assessments of at least three years, that range from and cause bulk density decreases, improved water infiltra-
201 years (Singh, Cowie, & Smernik, 2012) to 4,419 years tion, and increased stocks of water or plant‐available nutri-
(Lehmann et al., 2015; Zimmerman & Gao, 2013), depend- ents. Such modifications are frequent in PyC‐rich
ing on the models, degradation methods, and biochar char- anthropogenic dark earth soils worldwide (Glaser & Birk,
acteristics. Under a conservative estimation and 2012; Solomon et al., 2016) or at old charcoal‐making
considering a double‐exponential decay model (Lehmann (kiln) places (Borchard et al., 2014; Criscuoli et al., 2014).
et al., 2015; Zimmerman & Gao, 2013), we assume aver- Biochar can have contrasting effects on nonpyrogenic
age C‐leakage rates for the first 100 years after soil appli- soil organic carbon stocks (Wang et al., 2016). As shown
cation (BC+100) between 10% at molar H/Corg ratios below in some studies, biochar soil application may enhance the
0.4% and 20% above. However, caution is recommended accumulation of plant‐derived carbon entering the soil (lit-
as some soils, for example with low SOC and frequent ter, root exudates) and thus increase the content of soil
harvest‐residue fires or frequent frost–thaw cycles, may organic carbon beyond the addition of biochar's PyC
turn out to be less suitable for biochar carbon sequestration (Amendola et al., 2017; Bruun, Petersen, Hansen, Holm, &
causing lower MRTs (Rosa, Rosado, et al., 2018). While Hauggaard‐Nielsen, 2014; Ventura et al., 2014; Weng
more research about mechanisms of PyC degradation and et al., 2017). In some cases, however, decomposition of
the fate of the degradation products are clearly needed, already present nonpyrogenic soil organic carbon was
three meta‐analyses and all studies on biochar persistence accelerated (Wardle, Nilsson, & Zackrisson, 2008; Whit-
in soil (based on >120 experiments) confirm that biochars man & Lehmann, 2015). Thus, biochar can have positive
are much more recalcitrant than their precursor materials or negative priming effects; particularly, the interaction
and natural SOM and that MRTs exceed the centennial with plant roots is not well understood (Cross & Sohi,
scale. 2011; Wang et al., 2016). To trace C flows, C sources
must be traced by stable isotopes to three CO2–C sources:
plant‐derived C, soil organic matter‐derived C, and bio-
4 | BIOCHAR USES AND FURTHER
char‐derived C. Due to the complexity of such experiments,
CLIMATE‐RELEVANT EFFECTS
the number of published studies is still low.
Biochar can not only be used as soil amendment but also Several meta‐analyses of biochar field trials indicate
in multiple ways for industrial products like construction average yield increases of 10%–20% following amendments
materials (Gupta & Kua, 2017), for wastewater treatment of more than 5 t/ha of pure, not‐nutrient‐enriched biochar
(Mohan, Sarswat, Ok, & Pittman, 2014), and for electron- (Crane‐Droesch, Abiven, Jeffery, & Torn, 2013; Jeffery,
ics (Gu et al., 2014). In all of these products, PyC can Abalos, Spokas, & Verheijen, 2015). While yield increases
serve as a C‐sink, as long as the product is not thermally (with pure biochar use) are low or absent in temperate
degraded and oxidized during use, recycling, or disposal. soils, biochar application increased yields in tropical and
When biochar is not used as a soil amendment but, for subtropical soils by 25% on average, according to the latest
example, as a composite building material or stored in a extensive meta‐analysis (Jeffery et al., 2017). The increase
long‐term deep soil repositories, it can likely be protected also enhances accumulated C from the atmosphere by the
more efficiently from microbial and chemical degradation same percentage; if the same practice is maintained over
to reach MRTs comparable to those of PyC in sediments decades, the sustained increase in NPP increases the terres-
(Coppola & Druffel, 2016). trial carbon pool by the corresponding amount. Such a “re-
To date, biochar is mainly used as a soil amendment, as turn of investment” of biochar use, that is the increase in
animal feed ingredient, for manure treatment in agriculture non‐PyC SOC and NPP, may be as important for PyCCS
(Schmidt & Shackley, 2016) or as a compost or planting as the PyC sequestration by the biochar itself.
However, the use of large amounts of pure biochar may alcohols), and small amounts of solid particles including
not become the final pathway of soil application in the char, ash, or sand (Bayerbach & Meier, 2009; Oasmaa
future. Biochar may serve as raw material for different et al., 2016, 2015 ).
agricultural (fertilizer) products rather than being a final Bio‐oil can be also obtained from slow pyrolysis pro-
amendment product in itself. For example, biochar made cesses over the whole pyrolysis temperature range (350–
from invasive weed and harvest residues improved fertilizer 900°C) and from all types of biomass feedstocks (Sanna
efficiencies and boosted yields in fertile soils in Nepal by et al., 2011). Thus, pyrolysis optimized for biochar produc-
on average 100% when used as a nutrient carrier at low tion still yields bio‐oil, though at considerably lower
dosages (<1–2 t/ha) (Schmidt et al., 2017). Moreover, bio- amounts and with some distinct differences in composition.
char can be used as a tool to further reduce agronomic At a given temperature, slow pyrolysis bio‐oil has similar
GHG emissions (Kammann et al., 2017) as it has been elemental composition on a dry basis, although with the
shown to reduce methane emissions in saturated soils, for following differences:
example in rice agriculture (Han et al., 2016; Jeffery, Ver-
heijen, Kammann, & Abalos, 2016), or N2O emissions The water content is increased, which leads to enhanced
from fertilized soils by 40%–50% on average (meta‐studies: phase separation.
Cayuela et al., 2014; Schirrmann et al., 2017). The sugar content is significantly reduced due to sec-
ondary reactions (Anca‐Couce, Mehrabian, Scharler, &
5 | BIO‐OIL, THE LIQUID PRODUCT Obernberger, 2014; Branca, Giudicianni, & Blasi, 2003).
OF PYROLYSIS The pyrolytic lignin yield is reduced.
The production of benzene, toluene, and xylene isomers
While biochar is well established as a means of carbon (BTX) and polycyclic aromatic hydrocarbons (PAH) is
sequestration (Brassard, Godbout, & Raghavan, 2016), bio‐ enhanced to significant values, which can be a concern
oil was not yet discussed as such. Bio‐oil, also known for some applications due to their toxicity (Fagernäs,
under the names pyrolysis liquids, pyroligneous acid, or Kuoppala, & Simell, 2012; Milhé et al., 2013).
(more historically) wood vinegar, is a very complex liquid
mixture composed of hundreds of different oxygenated
6 | BIO‐OIL USES AND ITS
hydrocarbons and water. It is an obligate by‐product of all
SEQUESTRATION
kinds of pyrolysis. When bio‐oil is the main intended
pyrolysis product, optimal production parameters are fast Bio‐oil can be employed for heat and power generation in
(<1 s) pyrolysis at 500°C (Xie, Xu, Fang, Luo, & Ma, gas turbines or furnaces and, after an upgrading, as biofuel
2013). for internal combustion engines (Elliott, 2007; Fagernäs,
Fast pyrolysis, bio‐oil is typically viscous but free‐flow- Kuoppala, Tiilikkala, & Oasmaa, 2012; Kauffman, Dumor-
ing and dense (~1.2 kg/L), has usually a dark brown color, tier, Hayes, Brown, & Laird, 2014). Here, however, we do
is acidic (pH ~2.5), and has a low net calorific value (NCV not consider the purpose of energetic use which is of
<20 MJ/kg) due to the high oxygen content and moisture course possible but would release the carbon back to the
(Mohan, Pittman, & Steele, 2006; Oasmaa, Beld, Saari, atmosphere. We rather consider applications and uses that
Elliott, & Solantausta, 2015). It is a micro‐emulsion, in maintain the bio‐oil's carbon sequestered. Instead of com-
which pyrolytic lignin and other water‐insoluble organic busting the nonsolid by‐products of biomass pyrolysis as
compounds are dispersed. Pyrogenic organic compounds suggested by Woolf et al. (2016), the bio‐oil could be
dissolved in the aqueous phase serve as emulsifiers, though either used in a biorefinery approach (Table 1) or seques-
it has a strong tendency for phase separation. A decanted tered in geological repositories as discussed below.
heavy oil phase at the bottom, rich in nonpolar compounds Before the advent of fossil fuel extraction in the early
(mainly pyrolytic lignin), can be distinguished from an 20th century, main raw materials for the chemical industry
upper aqueous phase rich in polar compounds (light were produced by wood distillation, which is a historical
organic compounds and heavy sugars) (Oasmaa, Fonts, name for pyrolytic bio‐oil production. Besides tar and pitch
Pelaez‐Samaniego, Garcia‐Perez, & Garcia‐Perez, 2016). for building ships and roads, basic chemicals like naph-
Additionally, a distinctive upper layer rich in extractives thalene, anthracene, aniline, phenol, benzene, methanol,
(mainly waxes, fatty acids, phenolics) may form. acidic acid, and acetone were produced with pyrolysis sys-
A typical composition of bio‐oil made from woody bio- tems for the nascent chemical industry (Aftalion, 2001).
mass by fast pyrolysis at 500°C includes, in mass percent- Until 1950, methanol was still mainly produced through
age, 25% water, 20% pyrolytic lignin, 55% of organic wood pyrolysis, though by then the much cheaper and
water‐soluble compounds (around 30% of sugars produced more homogeneous fossil oils replaced the biomass materi-
from cellulose and hemicellulose and 20% of carbonyls and als as important resource for the chemical industry (Soltes
578
| SCHMIDT ET AL.
T A B L E 1 Suggested and tested uses of bio‐oil‐based products carbon storage deposits, as those materials would end their
Bio‐oil‐based material life cycle in other construction works or landfills.
product and use References Those applications could be realized already within years,
Bioplastics Crombie and Mašek (2014) that is short to mid term.
More challenging is the use of bio‐oil as raw material
Asphalt amendment Raman et al. (2015)
for bioplastics and other types of composite materials
Amendment for Czernik and Bridgwater (2004) and Xie
(Crombie & Mašek, 2014), which will need advanced
building materials et al. (2013)
chemical engineering. Depending on the life cycle of the
Wood preservative Czernik and Bridgwater (2004) and
plastic materials, carbon fibers and carbon composites, the
Tiilikkala, Fagernäs, and Tiilikkala (2010)
persistence of the carbon in the terrestrial system would
Biocide and crop Tiilikkala et al. (2010) vary between short, mid, and long term. With the increas-
protection
ing public and political pressure on recycling plastic mate-
Feed additive Yamauchi, Ruttanavut, and Takenoyama rials (instead of waste combustion and landfill dumping),
(2010), Cai, Jiang, and He (2011) and
the carbon contained in the advanced biomaterials could be
Chu et al. (2013)
stored for much longer timescales in the terrestrial system,
Plant growth Ratanapisit, Apiraksakul, Rerngnarong,
so that the material use and recycling would become a
enhancer Chungsiriporn, and Bunyakarn (2009),
long‐term carbon sink.
Tiilikkala et al. (2010) and Hagner,
Penttinen, Tiilikkala, and Setälä (2013) Research and development in regard to biorefinery of
bio‐oil is, although based on a long history, currently only
at the beginning though, from the theory, it is rather clear
that bio‐oil could well become a decisive raw material for
& Elder, 2017). Currently, 10% of annually produced fossil the chemical industry once the production of fossil fuels
oils are used as raw material by the chemical industry would be banned. Further possible fields of bio‐oil applica-
(Keim, 2014). If humanity succeeds in limiting mean glo- tion include agronomy, animal husbandry, pharmaceutical
bal warming to 1.5°C or 2°C as specified in the Paris industry, or wood preservation (Table 1). However, those
Agreement (Schleussner et al., 2016, Rockström et al., latter applications would have a rather short carbon storage
2017), carbon emissions will have to be reduced by 90% capacity.
until 2050. Emission reduction of this order can only be As long as the chemicals or materials using bio‐oil car-
achieved with rapid and complete phasing‐out fossil fuels bon are not combusted or otherwise oxidized, the carbon
within the next 30 years (Rogelj et al., 2015, Bertram remains sequestered, augmenting the terrestrial carbon pool.
et al., 2015; Sanderson et al., 2016; Schleussner et al., With advanced end‐of‐life product management, the carbon
2016). This, however, implicates that the 440 million tons of these bio‐oil based products could be recycled or
of fossil oil (OECD, 2018) that are currently extracted and sequestered in protected deposits at the end of its lifetime,
used as raw material for the chemical industry would have then still serving as a C‐sink.
to be replaced by biomass‐derived raw chemicals, that is
bio‐oil, cellulose, starch, lactic acid monomers.
7 | GEOLOGICAL STORAGE OF
Most chemical products that are currently produced
BIO‐OIL
from fossil fuels can as well be produced from bio‐oils in a
biorefinery approach (see Table 1) though today (until CO2 Compared to fossil crude oil, bio‐oil is characterized by a
emissions are properly taxed) at higher costs. higher moisture and oxygen content, lower viscosity, and
The most pertinent industrial C‐storing use of bio‐oil is lower caloric value. However, both liquids are similar in
certainly its blending to asphalt binder for road construc- regard to pumping, transportation, and storage (Czernik &
tion. Raman, Hainin, Hassan, and Ani (2015) have shown Bridgwater, 2004; Gueudré et al., 2017; Staš, Chudoba,
that the addition of 5%–20% of bio‐oil to the asphalt mix- Kubicka, Blazek, & Pospíšil, 2017). It can be assumed that
ture improves asphalt quality like stiffness and durability. the environmental toxicity of fossil crude and bio‐oil is
If 10% bio‐oil by weight were added as binder additives similar (Fermoso, Pizarro, Coronado, & Serrano, 2017;
and/or aggregates to 1.8 billion tons of asphalt poured each Louwes et al., 2017; Varma & Mondal, 2017; Zhang,
year, 180 million tons of carbonized material would be Chang, Wang, & Xu, 2007) though direct comparisons and
entombed annually. With a carbon content of 55%, the ecotoxicological assessments were not yet done. It is clear
amount of sequestered C in asphalt could be 100 million that both should not be applied to soil. However, bio‐oil
tons per year. Bio‐oil could further be added to concrete carbon could, as crude oil was for millions of years, be
and other building materials (Czernik & Bridgwater, 2004; sequestered for the long term (>1,000 years) when pumped
Xie et al., 2013), which would also become long‐term into depleted fossil oil deposits (Werner, Schmidt, Gerten,
Lucht, & Kammann, 2018). Those deposits would have the condense at lower temperatures (Oasmaa et al., 2016). The
advantage that they are typically deeper than 1,000 m composition of each phase can be controlled by the temper-
below the surface, that is deep below the groundwater zone ature in the fractional condensation when cooling down the
(Philp, 1985). They would thus be protected from oxygen pyrolysis volatiles or by stepwise distillation of biomass
and microbial degradation. Any risk of leaching would be (i.e. recovering volatiles when heating the biomass at 250,
avoided. The bio‐oil carbon could thus, in theory, be 350, 400°C). It would thus be possible to recover first
sequestered without any apparent environmental risk while those parts of the pyrolytic oil that are, already today, eco-
being protected from decomposition. The geological integ- nomically valuable for bio‐based chemical materials (C
rity of the sequestration deposits was demonstrated by the sequestration in economically valuable products) and to
ability to hold fossil oil for millions of years without leak- sequester the remaining fractions in geological deposits.
age. Risks of volatilization to the atmosphere, except for While the aqueous phase of the oil is well pumpable
the transportation to the final geological deposit, could be but has a low pH (<3), the heavy tar fraction is not well
assumed to be minimal considering that bio‐oil has a poor pumpable but has a more neutral pH, which would facili-
volatility compared to fossil oil (Czernik & Bridgwater, tate the intermediate storage of that fraction. The following
2004). bio‐oil properties should further be considered when plan-
The carbon density of bio‐oil (590–750 kg C/m3 ning for transport and storage:
(Neves, Thunman, Matos, Tarelho, & Gómez‐Barea, 2011))
is slightly lower than that of fossil oil (800 kg C/m3 (Czer- Bio‐oils are incapable of sustaining combustion and can
nik & Bridgwater, 2004)) though more than three times be classified as nonflammable liquids (Oasmaa et al.,
higher than that of liquefied CO2 (135–220 kg C/m3 2012).
(IPCC, 2005)), which is proposed to be used for BECCS. Bio‐oil is slightly corrosive, and toxicity increases from
Geologic sequestration of bio‐oil would therefore take less fast to slow pyrolysis bio‐oils, which is associated with
volume than CO2–CCS. Moreover, it would avoid most of a higher concentration of PAHs (Blin, 2005).
the known and unknown short‐ and long‐term risks associ- Bio‐oil has a high viscosity, commonly in the order of
ated with geological storage of CO2 (CO2 leakage, alter- tens of centistokes, and the viscosity increases during
ation of groundwater chemistry, seismic activity, etc. storage (Mohan et al., 2006).
(Vaughan & Gough, 2016; Burns & Nicholson, 2017)). In Short‐term storage should be conducted in the type of
Werner et al. (2018), the carbon leakage during transporta- containers recommended for fast pyrolysis oil (Oasmaa
tion of the bio‐oil to the final repository and the millennial et al., 2016), which are composed of corrosion‐resistant
underground storage was assumed to be 2% over 80 years steel and materials such as AISI 304, AISI 316, polyte-
for the geological bio‐oil storage pathway. trafluoroethylene (PTFE), high‐density polyethylene
Today, the geological storage of bio‐oil can only be (HDPE), and polyvinyl chloride (PVC).
considered a thought experiment. It certainly seems coun-
terintuitive to replenish fossil oil reservoirs with bio‐oil, It can be expected that dedicated research and engineer-
when today's fossil oil extraction continues unabated at ing could solve the mentioned storage and displacement
4.4 Gt per year (OECD, 2018). However, it might become issues. However, more research is clearly needed, espe-
one of the options of last resort when, as it appears today, cially for value‐generating and cascading uses of bio‐oil for
the phasing out of fossil fuels will be delayed by one or C‐sequestering and its environmentally safe long‐term stor-
more decades. To return atmospheric CO2 concentrations age.
to a save level, humanity might be soon forced (Rockström
et al., 2016) not only to stop fossil fuel extraction but also
8 | OXIDATIVE USE AND
to reverse the direction of liquid‐C movement to geological
SEQUESTRATION OF THE GASEOUS
stores using the same pipelines. In the meantime, bio‐oil
CARBON (CO 2 –CCS)
may reduce the dependency on fossil fuels by being used
as energy carrier or raw material for the chemical industry. Depending on the process parameters, the carbon contained
The bio‐oil can either be stored as one mixed liquid in the permanent pyrogas accounts for 15%–45% of the
substance or it can be stored in different fractions, which total carbon of the initial biomass (Table 2). To ensure a
are obtained either by phase separation or by fractional high C‐sequestration efficiency of PyCCS, the gaseous car-
condensation. Fractional condensation of bio‐oil would be bon should be included in the sequestration scenarios (Fig-
controlled by a liquid–vapor equilibrium separating the ure 1). Usually, the gas is combusted to produce thermal
heavy tars (polar and nonpolar, including pyrolytic lignin energy to drive the pyrolytic process (Crombie & Mašek,
and heavy sugars) which condense at higher temperatures 2014) or to produce electricity. However, in conventional
and an aqueous phase with light organic molecules which combustion where air is used as oxidizing agent, the flue
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T A B L E 2 Pyrolysis product properties for five PyCCS scenarios

Slow pyrolysis Slow pyrolysis Slow pyrolysis Slow pyrolysis Fast pyrolysis
Units 400°C 500°C 650°C 800°C 500°C
Ash content % d.b. 1 1 1 1 1
Initial moisture % w.b. 25 25 25 25 5
Char yield % w.b. 26.1 22.4 17.9 14.4 20.0
C char % 74.6 79.8 83.8 85.4 78.6
H char % 3.4 2.5 1.6 1.0 2.5
O char % 19.1 14.4 10.4 8.4 14.1
Ash char % 2.9 3.3 4.2 5.2 4.8
H/C ratio – 0.54 0.38 0.23 0.14 0.38
Liquids yield % w.b. 52.8 56.1 54.3 49.2 61.2
C liquids % d.b. 56.3 56.3 59.9 63.6 56.3
H liquids % d.b. 6.1 6.1 6.4 6.7 6.1
O liquids % d.b. 37.6 37.6 33.6 29.7 37.6
Moisture liquids % w.b. 66.4 62.4 64.5 71.2 28.9
Permanent gas % w.b. 21.1 21.4 27.7 36.5 18.9
yield
C gases % 37.1 35.1 38.6 44.0 37.5
H gases % 7.1 7.4 6.9 6.5 6.5
O gases % 55.8 57.5 54.5 49.5 56.0
LCV biomass MJ/kg 13.4 13.4 13.4 13.4 17.7
w.b.
LCV char MJ/kg 27.2 28.7 29.7 29.8 28.3
LCV liquids MJ/kg 5.6 6.6 6.8 5.6 14.7
w.b.
LCV gases MJ/kg 13.9 13.4 14.5 16.4 13.5
3
C‐density of char kg/m 239 298 235
3
C‐density of kg/m 672 590 734
liquids
C in char % 52.1 48.0 40.3 32.9 33.2
C in liquids % 26.8 31.9 31.0 24.1 51.9
C in gases % 21.0 20.2 28.7 43.0 15.0
Leakage BC+100 % 20 10 10 10 10
CSE without CO2 % 70 74 67 53 81
CSE % 88 94 94 94 95
Note. BC+100: biochar carbon that remains after 100 years after soil amendment; CSE without CO2: CSE of the PyCCS pathway with biochar and bio‐oil seques-
tration only; CSE: total carbon sequestration efficiency of the complete PyCCS pathway; d.b.: based on dry matter; LCV: low caloric value; w.b.: based on wet mat-
ter; PyCCS: pyrolytic carbon capture and storage.
Biomass feedstock for all considered scenarios is woody biomass. The correlations are derived from pyrolysis process parameters, and they are based on the assump-
tions and formula presented in the SI.
gas contains beside CO2 and H2O more than 50% N2. small‐scale production units (e.g. one unit per farm or vil-
Separating the flue gas from the N2 to obtain pure CO2 for lage), this may exclude CO2–CCS from gas combustion. A
CCS purposes would be a complex and expensive process recent alternative that could well be set up in small‐scale
increasing the cost of CO2–CCS heavily. It would therefore devices is chemical‐looping combustion (CLC). In CLC, a
only be economically viable in large‐scale industrial solid oxygen carrier is used for combustion instead of air
devices (Reynolds, Ebner, & Ritter, 2006). As one impor- (Adanez, Abad, Garcia‐Labiano, Gayan, & Diego, 2012).
tant advantage of PyCCS is the option for decentralized, The oxygen carrier, most often based on nickel, iron, or
F I G U R E 1 General pyrolytic carbon capture and storage scheme for pyrolytic treatment of biomass, the pathways of solid, liquid, and
gaseous products, their use and sequestration scenarios, the respective C‐leakage rates, and the circular effect on carbon farming systems and
sustainable biomass production
manganese oxides, is moved through the permanent pyro- Following Kemper (2015) and Vaughan and Gough
gas stream in a countercurrent process where the metal‐ (2016) and assuming that captured CO2 is harder to contain
bound oxygen reacts with the gas. Once the oxygen carri- than bio‐oil and biochar, we assume leakage rates of 5%
ers are reduced, they are conveyed out of the combustion over 80 years for the geological CO2 storage.
reactor into another reactor where they get reoxidized with
air before being reused. This chemical looping can be
9 | MINERAL NUTRIENT
repeated for countless cycles without losing its efficiency
BALANCES
(Adanez et al., 2012). The reaction products of permanent
pyrogas CLC are nearly pure CO2 and water, which can Biomass contains a wealth of elements beyond CHO.
easily be separated by condensation. The CO2 could by Although present only in lower concentrations, they are of
then be treated as in conventional CO2–CCS scenarios high relevance due to their role as plant macro‐ and
(Zakkour, Kemper, & Dixon, 2014). micronutrients. After harvest, essential nutrients bound in
Alternatively, the gases could also be treated with a biomass should be returned to biomass‐producing agroe-
chemical‐looping reforming (CLR) process that results in cosystems. Otherwise, soil fertility deteriorates over time
CO2 and H2 as reaction products (Adanez et al., 2012; de (Hänsch & Mendel, 2009; Ingerslev, Skov, Sevel, & Ped-
Diego et al., 2008). While the resulting H2 will be a car- ersen, 2011). Already today, the mineral depletion of
bon‐neutral energy carrier, the pure CO2 could be pro- agronomically used soils is a point of concern, affecting
cessed for geological sequestration. As this process would global food security (Jones et al., 2013). This would be
not generate the heat needed for pyrolysis, the required further accelerated when biomass is extracted without
energy input needs to be generated from renewable electric- returning the minerals it contains to the soil. The latter is
ity (i.e. E‐pyrolysis). This approach should be investigated the case in BECCS scenarios where biomass is combusted
as a new option for power to gas. to produce energy, and the resulting ashes cannot or can
CLC and CLR are considered as the most promising only partially be returned back to soils due to heavy
alternative to reduce the costs of CO2 capture (Kerr, 2005) metal, PAH, and dioxin contamination (Ingerslev et al.,
and are fitting technical opportunities to increase the C‐ 2011) or to toxic ash transformation reactions during com-
transformation efficiency of the PyCCS technology. How- bustion (Boström et al., 2012). On the other hand, return-
ever, CLC and CLR in combination with pyrolysis are not ing the ashes and minerals to the soil with the biochar
yet widely tested or mature technologies. Hence, they need will likely deliver a “mineral weathering” CCS contribu-
further development and up‐scaling before being imple- tion to CDR, which would need to be further explored
mented at larger scales. and quantified.
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Nitrogen is an important nutrient of plants, and its avail- the atmosphere) and products with a long‐term C‐stability.
ability is often limiting for plant growth. In biomass, it is As biochar is the pyrolytic carbon product that can be
mainly present in the form of proteins. The main primary sequestered at the lowest costs and with large cobenefits,
pyrolysis product of proteins at temperatures around 500°C high biochar yields are targeted. As the sequestration of the
is amides, which are present in the bio‐oil. Nitrogen is fur- carbon from the permanent pyrogases is the most expensive
ther retained to a lower extent in the biochar but also and technically challenging C‐sequestration pathway, the
released in small amounts as NH3 and HCN with the gas gas production should be minimized. While pyrolysis is
phase (Nussbaumer, 2003). At higher temperatures, tars often optimized for the production of one product and the
crack, reducing the N‐content in the bio‐oil and enhance other two products are considered either a waste or a barely
the production of NH3 and HCN in the permanent pyrogas. valued coproduct, in PyCCS scenarios all three pyrolysis
NH3 and HCN are precursors of nitrogen oxides (NOx), products have to be used to optimize the transformation of
which can form during combustion of the volatiles depend- the biomass carbon into pyrogenic forms for long‐term C
ing on the combustion technology employed (Vermeulen, sequestration. Overall, an optimum between production
Block, & Vandecasteele, 2012). However, using a proper costs, robustness of the process, product distribution, qual-
combustion approach, harmful emissions can be minimized ity and product value, sequestration potential (half‐life in
(Nussbaumer, 2003) to near zero (i.e. N2 release), in accor- the terrestrial system), and the recycling of biomass
dance with the clean air regulations that are in place in extracted nutrients should be achieved (Appendix S1).
industrialized countries such as Germany. The distribution and characteristics of the solid, liquid,
Several elements such as Ca, Si, Mg, Al, Fe, or Ti are and gaseous pyrolysis products depend mainly on the
almost entirely retained in the solid fraction due to their pyrolysis temperature, particle size, residence time of the
nonvolatile nature. At pyrolysis temperatures of up to pyrolysis volatiles in the kiln, pressure, and feedstock com-
700°C, alkali metals (K and Na) are mainly retained in the position (Anca‐Couce, 2016). Slow pyrolysis at low tem-
char, but they are partially released to the gas phase above peratures (350–450°C) has the highest solid yield, though
700°C (van Lith, Jensen, Frandsen, & Glarborg, 2008). the carbon stability of the biochar is rather low, as is the
Most of the chlorine and a considerable proportion of sul- quality of the bio‐oil (Camps‐Arbestain et al., 2015; Fager-
fur are released to the gas phase at temperatures above näs, Kuoppala, & Simell, 2012). At a given pyrolysis tem-
400°C where it can be easily scrubbed off (Van Lith, Jen- perature, the biochar yield can further be increased with
sen, Frandsen, & Glarborg, 2008). Cl and S‐bearing slow heating rates, higher residence time of the volatiles,
organic compounds are further present in the bio‐oil. How- larger particle size of the feedstock, and higher pressure
ever, the sulfur and chlorine content of bio‐oil made from (Anca‐Couce, 2016).
woody biomass are lower than 100 ppm (Oasmaa et al., At higher pyrolysis temperatures (700–850°C), the per-
2015), which is considerably lower than the sulfur content manent pyrogas yield is significantly increased; conse-
in crude oil. quently, lower biochar and bio‐oil yields will be obtained
Thus, most of the biomass nutrients are retained in the (Anca‐Couce, Sommersacher, & Scharler, 2017; Sadaka &
biochar when slow pyrolysis technology is used at tempera- Boateng, 2009; Tripathi, Sahu, & Ganesan, 2016). The
tures below 700°C. The bio‐oil is mainly composed of car- resulting biochar contains graphite‐like carbon (instead of
bon, hydrogen, and oxygen, with a minor content of amorphous carbon), which increases its recalcitrance, for
nitrogen, still smaller amounts of sulfur and chlorine, and example in soil (Budai et al., 2014; Keiluweit, Nico, John-
only traces (in the ppm range) of all other elements (Oas- son, & Kleber, 2010). At these high temperatures, the pyro-
maa et al., 2015). The nutrient concentrations in biochar lytic liquids show a higher carbon content and higher
and bio‐oil mainly depend on the initial biomass composi- aromaticity and contain a large spectrum of typical tertiary
tion with woody feedstock having lower and annual harvest tars (Anca‐Couce, 2016). Tertiary tars are molecules free of
residues have much higher mineral contents, particularly oxygen, which can be stable at high temperatures having a
graminoid species (e.g. switchgrass, miscanthus, or crop single aromatic ring (BTX) or several rings (PAH). Also,
residue of rice, wheat, maize, or others) with their compa- high‐temperature pyrolysis oils have a high content of phe-
rably high silicon content. nols. Therefore, high concentrations of BTX/PAH and phe-
nols might pose an environmental concern for certain bio‐
oil use scenarios (e.g. when used in asphalt or for plant
10 | CARBON BALANCES AND
protection), but not when sequestered geologically.
OPTIMIZED PYROLYSIS
Fast pyrolysis is less suited for the purpose of carbon
PARAMETERS FOR PYCCS
sequestration because the overall energy expenditure is
The overarching aim of PyCCS is to enable low‐cost high high due to the necessary drying and milling of the feed-
C‐transformation rates (i.e. minimum losses of carbon to stock and very high heating rates (>500°C/s) (Lédé &
Authier, 2015). Moreover, the fast pyrolysis biochar yield after the oxidation of these gases is captured and stored,
and quality are rather low (Brewer et al., 2012). the overall carbon efficiency can still be high.
To provide an example for the selection of optimal To pyrolyze biomass, the feedstock has to be harvested,
PyCCS parameters, we expose in Table 2 the results of an transported, chipped, or milled. All these processes are cur-
exemplary calculation of carbon yields, distribution, and rently executed by fossil fuel‐driven machinery though it
composition for four slow and one fast pyrolysis scenarios could equally be powered by carbon‐neutral electricity.
as a function of the pyrolysis temperature according to Except for the proposed concept of E‐pyrolysis for CLR,
Neves et al. (2011). Their comprehensive literature review pyrolysis itself has low electric consumption and the neces-
of pyrolysis experiments includes data from more than 60 sary thermal energy is provided by the permanent pyrogas
biomass samples with different reactor configurations and oxidation (Crombie & Mašek, 2014). The postpyrolysis
temperatures between 350 and 1,000°C. processing of the products like quenching and milling of
Modifying pyrolysis conditions determine yield and biochar or the pumping of bio‐oil to geological storages
quality of biochar, bio‐oil, and permanent pyrogas. Summa- can be done electrically. The application of biochar to soil
rizing the above considerations, we suggest the following necessitates land management machinery, although the car-
general guidelines to optimize the pyrolysis process condi- bon footprint of an estimated one liter of diesel per ton of
tions for PyCCS scenarios: biochar is negligible and could in the near future be exe-
cuted by electric tractors (Lünenbürger, 2012; Tubiello
Produce a low portion of permanent pyrogas and high et al., 2013). Liquefaction and pumping of CO2 after CLC
portion of biochar and bio‐oil (avoid temperatures or CLR are equally a process that could be powered by
>700°C); carbon‐neutral electricity (Kerr, 2005). The carbon footprint
Maximize the biochar yield compared to bio‐oil, using for the production and maintenance of the machinery dedi-
rather slow than fast pyrolysis, as it is easier and less cated to the preparation, pyrolysis, and postproduction pro-
cost‐intensive to sequester biochar, in soils or materials, cesses is compared to the amount of treated carbon
than bio‐oil; negligible, although detailed calculations are missing in the
Achieve low H/C ratios of <0.4 and thus a high recalci- literature. Based on these assumptions, we do not include
trance of biochar by using pyrolysis temperatures not further C‐expenditures beside the C‐leakages of the applied
lower than 450°C. PyCCS products as considered in the chapters above
(10%–20%, 2%, and 5% over 80 years for soil‐applied bio-
Based on these guidelines, we suggest using slow pyrol- char, geological bio‐oil storage, and geological CO2‐stor-
ysis with a highest treatment temperature between 500 and age, respectively).
650°C for PyCCS‐based CDR. In this temperature range, a
compromise between high biochar yield and its recalci-
11 | IMPLEMENTATION
trance is achieved for a large spectrum of diverse biomass
POTENTIAL AND ADVANTAGES OF
feedstocks (Brassard et al., 2016; Weber & Quicker, 2018).
PYCCS IN COMPARISON WITH
At these temperatures, the gas yield is low, and only few
BECCS
minerals end up in the bio‐oil. When the resulting biochar
is applied to soil, either directly or via cascading use in Biochar is suggested as a material for long‐term carbon
animal husbandry or prior material use (Schmidt, 2012), sequestration since the late 1990 s (Ogawa, 1991; Okimori,
most of the minerals (but only reduced portions of nitro- Ogawa, & Takahashi, 2003). However, burning pyrolysis
gen) can be recycled within the biosphere. liquids and gases and sequestering only the biochar result
However, the suggested temperature range does not in C‐sequestration efficiencies that are too low for making
exclude the application of higher or lower pyrolysis tem- it a competitive NET (Werner et al., 2018). This is espe-
peratures in individual cases. Depending on the economic cially the case when biochar is produced at higher tempera-
scenarios and intended uses of the pyrolysis products, the tures (>500°C), which is necessary to produce a
production parameters can and sometimes should be recalcitrant product well suited for most material uses.
adapted, for example, lower temperatures are recommended In earlier studies, the potential of PyCCS was calculated
to produce biochar for peat replacement (Kern et al., 2017) for harvest residues under the assumption that only the bio-
or for soilless media to enhance plant growth and/or dis- char is sequestered (Smith, 2016; Woolf et al., 2010, 2016
ease suppression (Jaiswal et al., 2018). Higher temperatures ). Compared to the current practice of burning or decompo-
are necessary to produce activated biochar for remediation sition of these residues, pyrolysis would clearly be an
of contaminated soils or for electric capacitors (Frack- improvement, even if only 40% of the biomass‐C is eventu-
owiak, 2007; Hagemann et al., 2018). The latter pyrolysis ally sequestered. However, the calculated NET potential of
conditions will increase the yield of gas, but if the CO2 0.7 Gt Ceq/year (Smith, 2016) would, even when doubled
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| SCHMIDT ET AL.
under a complete PyCCS‐scenario, not be sufficient to ful- recycled back to the soil, maintaining the soil fertility in
fill current climate change mitigation targets (Fajardy & the long term. Thanks to the yield increasing value of bio-
Mac Dowell, 2017; Smith et al., 2015). Specific new and char and the added value of bio‐oil and biochar, once a
complementary global biomass production would thus be market can be established for its material use, the C‐se-
needed. When biomass production is undertaken for the questration costs of PyCCS may be expected to be signifi-
purpose of NET, the carbon sequestration efficiency is the cantly lower than for BECCS. However, for the moment
crucial factor that determines the size of the land area this can only be assumed as it is not yet possible to pro-
needed for biomass production (Werner et al., 2018). vide a comprehensive cost‐benefit assessment based on
Increasing the carbon sequestration efficiency of a technol- peer‐reviewed literature.
ogy will thus decrease the land requirements substantially The expected 25% yield increases in tropical and sub-
(Beringer, Lucht, & Schaphoff, 2011; Boysen, Lucht, Ger- tropical climates (Jeffery et al., 2017) following the amend-
ten, et al., 2016). ment of biochar to soil would lead to a higher production
The current benchmark for BECCS‐based NETs is a C‐ of biomass and thus to more positive feedstock toward
sequestration efficiency (CSE) of 90% (Klein et al., 2014), PyCCS. Consequentially, the 70%–80% C‐sequestration
which can theoretically be attained, but only at high eco- efficiency of the biochar and bio‐oil PyCCS pathway could
nomic costs and environmental risks (Fajardy & Mac Dow- effectively rise to >90%. Moreover, biochar application
ell, 2017; Smith et al., 2015). PyCCS systems can equally could reduce agricultural non‐CO2 GHG emissions (Kam-
theoretically attain CSEs of ~90% when the sequestration mann et al., 2017) and most likely increase nonbiochar soil
of CO2–CCS is included and more realistically 70%–80% organic matter (Tian et al., 2016; Weng et al., 2017). Con-
(Table 2) when only biochar and bio‐oil are sequestered. sidering all these secondary climate mitigation effects of
Using the latter pathway avoids the high costs, environ- PyCCS, the high C‐sequestration efficiencies would trans-
mental risks, and societal challenges of geological CO2 late into an even higher climate mitigation potential.
storage. The technology for PyCCS is ready to be imple- Another major argument for pursuing PyCCS instead of
mented across small‐to‐industrial scales: Networks of small BECCS is the fact that the supposed massive switch from
production units could be installed avoiding the constraints fossil fuel energy production to bioenergy production
of using massive industrial power plants only (Schmidt & (170 EJ/year (Smith et al., 2015)) is economically unlikely
Shackley, 2016). Rather than establishing vast industrial at a large scale. Solar and wind energy production costs
biomass plantations with their monoculture drawbacks, are expected to decrease to <0.03 USD/kWh (Kumar Sahu,
their trade‐offs with food production, and other SDGs or 2015), whereas prices for bioelectricity production without
their environmental side effects (Boysen, Lucht, Schellnhu- CCS range from 0.06 USD with waste materials as feed-
ber, et al., 2016), a network of smaller scale PyCCS sys- stock to >0.12 USD for low‐cost feedstock and can go up
tems would allow to establish biomass as a desired and to 0.30 USD when pelletized biomass has to be purchased
cultivated coproduct of agriculture, for example in agro- (International Renewable Energy Agency, 2012). Although
forestry, silvopasture, and perennial coppicing types of the transformation of biomass into heat for, for example,
agricultures (i.e. carbon farming approaches, (Toensmeier, district heating systems in temperate climates may remain
2016)). However, the logistics of such farm‐based PyCCS economically viable at current prices of 0.02–0.04 USD/
systems producing biochar for local soil applications while kWh, the global need for heating is rather small compared
delivering the bio‐oil to centralized processing facilities are to the global electricity demand, particularly in tropical cli-
challenging especially in tropical and subtropical countries mates. Considering further that biomass will have to
with poor infrastructure and low degree of economic orga- become the principal source of chemicals for C‐based
nization. materials when decarbonization (i.e. the reduction in
If PyCCS generates sustainable tCDR that are paid for anthropogenic carbon emissions) eventually leads to phas-
by society (i.e. negative carbon taxes), economic incentives ing out of fossil carbon (Honary & Singh, 2010), prices for
could be provided for farmers to optimize their land man- biomass feedstock and thus for bioenergy will increase
agement with combined crop and biomass production. rather than decrease in the future. Hence, the long‐term
Thanks to the plant growth‐enhancing properties of bio- economic viability of biomass‐based electricity production
char‐based fertilization, the same food and feed crop pro- becomes increasingly unlikely, even if carbon‐offset pay-
ductivity per cultivation area could be maintained, while ments would finance the extra costs for CCS. If the pro-
the focus on additional biomass production could increase duction of thermal energy from biomass remains an
the NPP of agricultural land and thus the terrestrial carbon important factor for the future energy mix, at least in tem-
accumulation. With biochar being applied back to agricul- perate climates, the bio‐oil and permanent pyrogas of
tural soils, preferentially nutrient‐loaded after cascading use PyCCS systems hold an interesting potential as flexible
(Schmidt et al., 2017), most of the nutrients would be energy carrier to produce heat on demand in the cold
season while it could be sequestered in the warm season or could increasingly replace fossil oil during the expected
when market prices for heat are low. Biomass pyrolysis phasing out of fossil fuels. Given the current economic and
could also produce fuel, especially methane and hydrogen, political situation, it seems extremely unlikely that, anytime
to replace fossil fuel though the carbon sequestration effi- soon, global governance may decide to set the incentives
ciency of the system would be lowered. to pump bio‐oil into geological storages. However, it may
Pyrolytic carbon capture and storage is mainly designed become an option of last resort if the combustion of fossil
to produce biomaterials that have multiple industrial and fuels will not be reduced quickly enough within the next
agronomic uses besides sequestering carbon. This does, 30 years. In the meantime, a mix of PyCCS and BECCS,
however, not exclude that in some scenarios biofuels may where pyrogas is used for methane and hydrogen fuel pro-
remain for a more or less long transitional period a valu- duction, and where biochar is applied to soil or used in
able coproduct of PyCCS. While all pyrolytic products biomaterials, could evolve into a way forward to early
already have an industrial value with a current market adoption of scalable, SDG‐supporting CDR technologies.
price, the large‐scale adaptation of the technology will cer-
tainly depend on the price that the global community is
willing to pay per sequestered ton of carbon. The current ACKNOWLEDGEMENTS
price paid by the market for biochar (300–600 Eur/t (Sch- This study was conducted within the BMBF‐funded project
midt & Shackley, 2016)) and bio‐oil (150–400 Eur/t (Ali- BioCAP‐CCS, grants no. 01LS1620A and 01LS1620B.
baba, 2018)) exceeds by far its energetic value, which is
about 135 and 33 Eur, respectively (based on a caloric
value of 29 GJ/t = 8.1 MWh/t for biochar and 6.8 GJ/ ORCID
t = 1.9 MWh/t for bio‐oil; an average price of 60 Eur/
Hans‐Peter Schmidt http://orcid.org/0000-0001-8275-
MWh electricity (Kost et al., 2013); the average energy
7506
efficiency of 32% for coal‐fired power plants with CCS
(Goto, Yogo, & Higashii, 2013); and a 10% for investment
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Received: 27 March 2018

| Accepted: 4 August 2018

Pyrogenic carbon capture and storage

Hans‐Peter Schmidt1 | Andrés Anca‐Couce2 | Nikolas Hagemann1,3 |

1 | INTRODUCTION accumulation in the terrestrial system has to return to an

GCB Bioenergy. 2019;11:573–591. wileyonlinelibrary.com/journal/gcbb | 573

T A B L E 2 Pyrolysis product properties for five PyCCS scenarios

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