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| Verfasst von: | Kim, Han Ung |
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| | Kim, Jichan |
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| | Lee, Hong-Shik |
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| | Wulandari, Sabrinna |
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| | Murali, Vishnu |
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| | Kim, Jaehoon |
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| | Park, Young-Kwon |
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| | Ha, Jeong-Myeong |
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| | Jae, Jungho |
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| Titel: | Highly efficient hydrolysis of cellulose to sugars using supercritical CO2 as a green acid catalyst and solvent |
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| Verlag: | Elsevier B.V |
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| Jahr: | 2024 |
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| Inhalt: | •The co-use of supercritical CO2 and carbon results in the significant synergy in cellulose hydrolysis.•Supercritical CO2 and water form a Pickering emulsion, enhancing the cellulose-carbon contact.•The initial cellulose hydrolysis rate increases up to 3 × at the emulsion interface.•The in-situ formed carbonic acid (pH ∼ 3.1) helps to hydrolyze oligosaccharides to glucose.•The promoting role of supercritical CO2 in cellulose hydrolysis is more profound in the mix-milled cellulose.
Rapid depolymerization of cellulose into processable monomers (e.g., sugars) using solid acid catalysts is an important step for cost-effective biofuel and biochemical production, but has not yet been achieved due to the limited contact between solid cellulose and solid catalysts. Herein, the unique roles of supercritical CO2 (i.e., scCO2) as an in-situ acid catalyst and reaction solvent in achieving the ultra-fast full solid catalytic hydrolysis of cellulose are disclosed for the first time. When the ball-milling pretreated cellulose was hydrolyzed using oxidized carbon catalysts at 150 °C and 100–300 bar-CO2, the hydrolysis kinetics remarkably increased by 3× for conversion and 5× for glucose, resulting in ∼90% conversion and ∼85% total sugar selectivity at 20 min. The hydrolysis rate obtained with scCO2 here was higher than conventional ones with toxic and unrecyclable homogeneous catalysts (e.g., HCl) under harsh reaction conditions (i.e., 180–220 °C and pH of 1–2). A comprehensive reaction engineering study (e.g., temperature, CO2 pressure, stirring speed, catalyst acid properties) combined with the estimation of the solution pH by the CO2 phase equilibrium model and the in-situ and ex-situ monitoring of the phase behavior of the H2O/scCO2 solution were conducted to quantify the activity promotion by scCO2 and understand the acid-solvent roles of scCO2 toward the enhanced hydrolysis of cellulose. Specifically, the formation of the Pickering emulsions at the interface between scCO2 and water and their impact on the enhancement of the cellulose-carbon contact were proposed and verified in detail. |
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| ISSN: | 1385-8947 |
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| Titel Quelle: | Chemical engineering journal (Lausanne, Switzerland : 1996) |
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| Jahr Quelle: | 2024 |
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| Band/Heft Quelle: | 493, S. 152336 |
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| DOI: | doi:10.1016/j.cej.2024.152336 |
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| URL: | http://www.ub.uni-heidelberg.de/cgi-bin/edok?dok=https%3A%2F%2Ffanyv88.com%3A443%2Fhttps%2Fdx.doi.org%2F10.1016%2Fj.cej.2024.152336 |
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| | DOI: https://doi.org/10.1016/j.cej.2024.152336 |
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| Sprache: | English |
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| Sach-SW: | Cellulose |
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| | Glucose |
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| | Hydrolysis |
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| | Pickering emulsions |
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| | Supercritical CO2 |
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| Verknüpfungen: | → Sammelwerk |
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