Zheng Remote-Controlled Droplet Chains-Based

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This is the peer reviewed version of the following article: Zheng, H., Wu, H., Yi, Z., Song, Y., Xu, W., Yan, X., Zhou, X., Wang, S., Wang, Z., Remote-Controlled Droplet
Chains-Based Electricity Generators. Adv. Energy Mater. 2023, 13, 2203825, which has been published in final form at https://doi.org/10.1002/aenm.202203825. This
article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced,
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Remote-controlled droplet chains-based electricity generators

Abstract

Harnessing ambient renewable mechanical energies for achieving carbon-neutrality generally demands

the rational design of materials and architectures which are favorable for both energy collection and

conversion simultaneously. However, the direct coupling of energy collection and conversion modules

leads to many unwanted problems such as material wearing, spatial constraint for large-scale integration,

and low energy conversion efficiency. Herein, we develop a remote-controlled energy harvesting strategy

that cleverly harnesses the unique advantage of diffusive, long-range air flow within confined capillary

channel, imparting to separate the energy collection unit, made of elastic cavity that directly transforms

external mechanical motion to pneumatic motion, from the conversion units, made of encapsulated droplet

chains that serve to translate their recurring motion within the capillary channel into electrical output.

Particularly, distinct from single-drain electrode design for electricity generation from fresh droplets in

the open space, we design two drain electrodes to collect and release electrostatically induced charges

from recurring droplets in the confined channel, respectively, thereby eliminating the unwanted charge

accumulation on recurring droplets and leading to efficient output performance. The integration of

multiple electricity generation units with such a two-drain electrode architecture with a single energy

collector improves the design resilience and relaxes the spatial limitation.

Introduction

Addressing energy and climate challenges requires the comprehensive exploitation of carbon-neutral

energy sources1-5 . Although abundant renewable and carbon-free energies are contained in our living

surroundings, such as water waves6-10 , rain droplets11-19 , wind20,21 , and biomechanical motions22,23 , their

intrinsic limitations of low frequency and irregularity impede the efficient translation of their energies into

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electricity via the conventional electromagnetic-based approach24 . As we enter the era of the Internet of

Things, harnessing these omnipresent mechanical energies has become increasingly essential for the

perspective of powering the worldwide distributed small electronics. To this end, various new techniques

have been developed in recent years for harnessing these ambient mechanical energies, including

triboelectric nanogenerators (TENGs)25-29, piezoelectric generators (PEGs)30,31 , and droplet-based

electricity generators (DEG)18,32 .

These emerging energy conversion techniques generally rely on the coupling in energy collection

and the subsequent conversion, directly translating the external input into electricity through various

mechanisms33-41 . For example, the external impact on a TENG or a PEG device triggers the material

deformation at the area underneath the impact, which leads to on-site electricity generation via

electrostatic induction or piezoelectric effects. Similarly, for a DEG device with transistor-like architecture

including source, drain, and gate terminals42 , the droplet impact induces the charge reformulation in the

modules beneath the impact area, and thereby directly translating droplet kinetic energy into electricity

(as shown in Fig. 1a). Although these techniques are all capable of converting small mechanical energies

into electricity, their common weakness of the utility of on-site energy conversion strategies leads to

several essential bottlenecks. On the one hand, the severe impact on the whole device would easily cause

material wearing and devices’ functional degradation. On the other hand, the coupled energy collection

and conversion constructions impose significant challenges in achieving high space utilization for the

large-scale integrated device and high energy harvesting efficiency, impeding the development of real

applications.

Here we propose a remote-controlled droplet chains-based electricity generator (RC-DEG) by

separating the coupled energy collection and electricity generation modules into different domains. An

elastic cavity is utilized as an energy collector to convert the external mechanical motion into pneumatic

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motion, which subsequently triggers the recurring movements of the encapsulated droplet chains in the

slippery tubes located at the electricity generation domain. The separated energy collection and conversion

strategy cleverly harnesses the unique advantage of diffusive, long-range air flow to eliminate the direct

contact-induced material wearing, relax the spatial constraints for large-scale integration, and more

importantly, endow the building of one energy collector with multiple electricity generation units for

generating multiplied electricity output upon one trigger. Particularly, distinct from previous droplet

electricity generation with single-drain electrode design limited to fresh droplets in the open space, we

design two drain electrodes to efficiently collect and release electrostatically induced charges from

recurring droplets in the confined channel, respectively, thereby eliminating the unwanted charge

accumulation on recurring droplets and leading to considerable output performance. Our strategy skillfully

expands the high-efficient droplet electricity generation from open-space to confined space and from the

fresh droplets to recurring droplet, which are significant for broadening its range of applications.

Additionally, with demonstrating the applications of RC-DEG for biomechanical energy harvesting, we

anticipate that a broad range of technologies and applications towards renewable energies will be

developed based on our proposed droplet chains-based electricity generation strategy.

Results and discussion

Fig. 1b shows the schematic drawing of our RC-DEG, in which the normally coupled energy

collection and electricity generation modules are separated to allow for the energy harvesting in remote

control manner. First, we choose the air as a unique transmission medium based on its diffusive and long-

range features to allow for the translation of the external input into the moving motion of water through

the entire RC-DEG by simply applying a mechanical force toward a rubber cavity (Fig. S1). To minimize

the water viscous energy dissipation and maximize collective power generation, we choose the capillary

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tube (FEP) with a very slippery property and high surface charge density as the core element of electricity

generation module, which serves as both the dielectric layer and carrier for liquid transport. To further

ensure efficient electricity generation, two-drain electrode design is used to efficiently collect and release

electrostatically induced charges from recurring droplets in the confined channel, respectively. Besides

imparting the preferred performances within one unit, separating the energy collection and conversion

modules also endows the three-dimensional integration of multiple electricity generation units (Fig. S2),

all of which can be actuated by a common input that resolves the spatial restriction encountered in

conventional design.

The main body of the electricity generation module of our RC-DEG is constructed based on capillary

tubes made of FEP material with a favored slipperiness, hydrophobicity, and strong charge affinity (each

unit tube with a length of 20 cm and inner diameter of 4 mm). Two polished aluminum rings are placed at

both sides of the unit tube, and a sheet electrode is wrapped half of the tube from outside (Fig. 1b). After

the fabrication, we then fill water into half of the unit tube and use an air pipe to connect the rubber cavity

and the FEP tubes so that the force-induced air pressure is endowed to be translated from the energy

collection domain to the electricity generation domain to drive the movements of the droplets. The spacing

between each droplet is ~ 10 cm (equaling half the length of the FEP tube unit), which can be tailored by

controlling the volume of water injected into each unit. Each unit tube is carefully fabricated to connect

with the adjacent unit with a U-type connecting tube to form the airflow channel for transmitting the air

pressure changes. The schematic and the as-fabricated RC-DEG arrays are shown in Fig. 1b and 1c.

Fig. 1d shows that the measured voltage, current, and charge outputs from a single-unit RC-DEG are

370 V, 0.7 mA, and 65 nC, respectively. The instantaneous high peaks in voltage and current outputs

appear when the moving water droplet contacts the two aluminum ring electrodes (Movie S1), in which

water droplet behaves like a gate in analogy to a field-effect transistor (Table S1), whereas two ring

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electrodes and the sheet electrode can be regarded as drains and source, respectively. Therefore, the contact

between the water and the drain leads to the formation of a closed-loop circuit which allows for the flowing

of charges between the source and the drain. Corresponding to the pressing and releasing of the rubber

cavity, a single-unit RC-DEG is capable of lighting up 100 LEDs twice (Movie S2). Moreover, the RC-

DEG device integrating eight electricity generation units can light up 800 LEDs by simply pressing on the

cavity (Fig. 1c and Movie S3). The power generation can be further amplified by mounting up more units

and leveraging on the precision manufacturing and mass production.

To demonstrate the advantage of our design, we also fabricate two control samples containing

identical structure, size, and materials but different number of drain electrodes (Fig. 2a and S3). Under the

same experimental conditions, the charge output from the RC-DEG featuring two- drain electrodes is four-

fold higher than those of control samples. More pronouncedly, both the voltage and current outputs of the

RC-DEG are around two orders of magnitude larger than those of the control devices (Fig. 2b-d),

suggesting that the adoption of two-drain electrodes design is essential to the pronounced output.

To understand the underlying mechanism responsible for the enhanced output rendered by the two-

drain electrode design, we further examine the mapping between transport dynamics of the water droplet

and the corresponding charge transfer. Notably, the flow direction of charges between the source and drain

is closely governed by the moving direction of water droplet (Fig. 3b and Movie S1). Moreover, this flow

characteristic of the charge performs good stability during 3600 cycles (Fig. S4). Meanwhile, we also

observe that the emergence of two electric current peaks originates from contacting of the gating water

with the drain electrodes (Fig. 3c). Fundamentally, the two-drain design endows the RC-DEG with the

capacity of efficiently collect and release the electrostatically induced charges, respectively, thereby

eliminating the unwanted charge accumulation and leading to better output performance than two control

groups (Fig. S5).

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In detail, four characteristic time points (t0 , t1 , t2 , and t3 ) and four corresponding stages (t0 -t1 , t1 -t2 , t2 -

t3 , and t3 - t0 ) are defined to describe the charge transfer process during one cycle of droplet movement

(Fig. 3d). Among, t0 denotes the initial time when the water droplet is at the left side of the unit and

conductively connects with the drain-I. In the first stage (t0 -t1 ), the water droplet starts to move to the

right direction yet maintaining conductive connection with the drain-I when pressure balance inside the

tube is broken by pressing the cavity located at the leftmost of the device. From the circuit perspective, a

closed-loop circuit between the drain-I, source and the FEP is established. With the water droplet

movement, electrostatically-induced positive charges on the source gradually transfer to the drain-I. The

process terminates when the water droplet detaches from the left drain-I at the time t1 . Then, moving to

the second stage (t1 -t2 ), the charge transfer process stops because the loop circuit is open. When the water

droplet connects with the right drain-II at t2 , the open-loop circuit is switched on again, accompanied by

the quick transfer of positive charges from the source to drain-II and hence a high current peak. Meanwhile,

the charge transfer process moves to the third stage (t2 -t3 ). The charge transfer process terminates when

the water droplet is oppositely driven to detach with the left drain-II quickly under negative pressure

induced by the released cavity. This quick detachment results in the accumulation of electrostatically-

induced charges in the water droplet. Next, an opposite high current peak is formed at t3 when the water

droplet connects with the drain-I again. In the final stage (t3 - t0 ), the accumulated charges fully transfer

from the connected drain-I to the source electrode. This process stops when the water droplet moves back

to the original location. The recurring droplet also recovers its original status in electrical property. To

furtherly understand the underlying mechanism of the whole charge transfer process, we develop a

theoretical model based on the transport dynamics of the recurring droplet (Fig. S6) and the electrostatic

induction (Supporting information note 1, Table S2, Fig. S7). The charge output obtained by the theoretical

model has a good agreement with the experimental results (Fig. S8).

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Understanding the basic charge transfer process enables us to investigate the parameter influencing

the performance of the RC-DEG devices. Fig. 4a shows that the measured peak current output is reversely

proportional to the load resistance, and the maximum current and the power is around 0.7 mA and 80 mW,

respectively. Note that the electrical output can be enhanced further by increasing the unit length (Fig. S9).

As shown in Fig. 4b, the charge, voltage, and current outputs of the RC-DEG become larger as we increase

the unit length (Fig. S10). In addition to the unit length, we also determine the optimal driven frequency

for energy generation (Fig. S11). Varying the driven frequency ranging from 0.25 Hz to1.5 Hz, we achieve

the maximum performance of the RC-DEG at ~ 1 Hz probably owing to the best stability of surface charge

and the water dynamics (Fig. 4c). Fig. 4d and Fig. S12 shows the time-dependent variation of the voltage

for the RC-DEG connecting to capacitors of 4.7 μF, 10 μF, 22 μF, and 47 μF, in which a maximum voltage

of 10.5 V can be obtained within 500 s charging (The left figure of Fig. 4d). We also quantitatively

demonstrate the capacitor charging performance of the integrated RC-DEG (The right figure of Fig. 4d).

A capacitor of 47 μF can be charged to 0.8V, 1.5 V, and 7.0V in 10 min by the RC-DEG containing 1, 2

and 10 units, respectively, at a frequency of 1Hz, exhibiting a linearly proportional relationship between

the output voltage and the unit number. For practical applications, the synergy of the integration and

indirect-control capability of our RC-DEG endows assembling of a large amount of the arrayed RC-DEG

devices. This multi-unit integration strategy also has the capacity to broaden the output voltage bandwidth

in parallel connection (Fig. S13).

The RC-DEG can also serve as a generic toolkit for energy harvesting in various application scenarios

(Fig. 5a). During the COVID-19 outbreak, wearing face masks has been recommended as an important

public measure for control and prevention of spread of SARS-CoV-2 variants. However, reducing the face

mask leak and ensuring the continuous monitoring of mask status, especially for children, still present a

great technological challenge. Here, we develop a self-powered mask wearing status monitoring system

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based on our presented RC-DEG, which can be embed with the face mask and enables a high-efficient

conversion of the gas pressure fluctuation energy generated by the respiration in the confined space

between the face and the face mask (Fig. 5b). The monitoring system can generate synchronously a blink

reminder on the liquid crystal display screen with the respiration, if the face mask is worn properly (Movie

S4). On the contrary, the monitoring system will stop working due to the insufficient power supply when

the face mask is worn improperly. Additionally, we also demonstrate the RC-DEG’s energy harvesting

capability in shoe energy harvesting (Fig. 5c). We assemble an integrated RC-DEG with a rubber cap as

an energy collector and three electricity generation units into an insole to collect the walking energy. One

single-stepping motion on the integrated RC-DEG can light up 63 LEDs in total twice (Fig. 5d): once for

droplet moving first forwards and another for backwards, as shown in Movie S5.

Conclusion

In this work, we propose a generic energy harvesting strategy that indirectly converts the ambient

mechanical energies into electricity with high efficiency by cleverly using the two-drain transistor-like

architecture and separating energy collection and conversion into different modules. In contrast to

previous direct electricity generation approaches, the proposed new RC-DEG circumvents many

drawbacks including violent external impact, unwanted charge accumulation, the alignment between the

energy source and the energy collection unit, and the spatial constraint for scalable integration. Particularly,

the two-drain architecture efficiently collect and release electrostatically induced charges from recurring

droplets in the confined channel, respectively, thereby eliminating the unwanted charge accumulation on

recurring droplets and leading to current and voltage outputs two orders of magnitude higher than

conventional designs. In coupling with the design of two-drain transistor-like architecture, separating the

energy collection and conversion units endows the multiplexed electricity generation based on a single

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energy collector. We envision that the droplet chains-based electricity generation strategy points a new

direction for efficient ambient renewable energy harvesting for multi-scenario applications.

Methods

RC-DEG fabrication. The RC-DEG comprises an elastic cavity and an FEP (Fluorinated ethylene

propylene) tube with an inner diameter of 4mm and an outer diameter of 5mm connected with the cavity.

The FEP tube can be divided into several tube units with several tube units. For a typical unit with a length

of 20 cm, we first cut the FEP tube into three sections with lengths of 5cm, 5cm and 10 cm, respectively.

Then we connected these three tube elements via connectors, and at their junctions, we assembled in the

Al rings with an inner diameter of 4mm as the drain electrode. The inner surfaces of the Al rings were

polished to be very smooth and perfectly fitted the inner wall of the FEP tube, which enables the free

movements of the water inside the tube. Copper tape (or copper-based cloth) with 10 cm length was

wrapped outside the tube at one side of the unit as the source electrode. Electric wires were used to connect

the drain electrodes and the source electrodes.

Microfluidic-based RC-DEG fabrication. A template of the microfluidic chip was first prepared by 3D

printing technology. Then, a certain volume of mixed liquid of polydimethylsiloxane and curing agent

(ration 10:1) was poured into the template and vacuumed for 1 h to remove internal gas. After curing for

30 minutes at 80°C, we peeled off the PDMS sample from the template and bonded it with a PDMS film.

To construct the electrodes, ten metal needles were embedded in the microchannel as drain electrodes,

five conductive Cu tapes of 2 mm×8 mm were assembled onto the PDMS film as external electrodes.

Several electric wires were used to connect the drain electrodes and the source electrodes.

Characterization and electrical measurement. The water movement in the RC-DEG was recorded by a

high-speed camera (Photron FASTCAM SA4) at a typical recording speed of 6000 fps. The voltage output

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of RWT-TENG was measured using an oscilloscope (Rohde & Schwarz RTE1024) equipped with a high-

impedance (10 MΩ) probe. The current and the transferred charges were measured using the oscilloscope

coupled with a low-noise current preamplifier (Stanford Research System Model SR570) and a Faraday

cup connected with a nanocoulomb meter (MONROE Model 284), respectively.

Data availability. The data that support the findings of this study are available from the corresponding

authors on reasonable request.

Acknowledgements: We acknowledge the financial support from Research Grants Council of Hong Kong

(No. C1006-20WF, No. 11213320), Tencent Foundation through the XPLORER PRIZE, Innovation and

Technology Council (No. 9440248), National Natural Science Foundation of China (Grant Nos. 51975502

and 21621001), Science and Technology Planning Project of Guangdong Province (No.

2021A0505110002), Innovation Technology Fund(GHP/092/20GD), and the 111 Project (B17020).

Author contributions: Z.W. supervised the research. H.Z., H.W., Y.S. and Z.Y. conducted the experiment

and data analysis. Z.Y., H.Z., Y.S. and W.X. built the model. All authors participated in the discussion of

the experimental design. Z.W., H.Z., H.W. Z.Y. and S.W. wrote the paper. All authors commented on the

paper.

Competing interests: The authors declare that they have no competing interests.

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Figure captions

Fig. 1. Design of the RC-DEG. a. Schematic diagram of the conventional direct-mode electricity

generators. b. Schematic diagram of the RC-DEG. Eight individual electricity generation units are

connected in series and driven by an energy collector. Insert: schematic diagrams of an individual RC-

DEG consisting of an FEP tube, water gate, two drain electrodes and a source electrode. c. 800 commercial

LEDs are lighted up together powered by one RC-DEG device equipped with eight electricity generation

units. Scale bar: 5 cm. d. The voltage and current outputs of a single-unit RC-DEG operating at the
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frequency of 1.0 Hz.

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Fig. 2. The design of “drain” electrode of RC-DEG. a. Schematic of RC-DEG with two drain electrodes,

the control devices with single electrode and without electrode. b-d. Comparison of the voltage, current

and charge outputs from a single-unit RC-DEG and two control groups (operation frequency: 1.0 Hz).

16
Fig. 3. Working mechanism of the RC-DEG. a. The optical photo of an individual RC-DEG. Scale bar:

1 cm. b. Time-dependent variation of the transferred charge between the source electrode and two drain

electrodes during one cycle, indicating that the charge transfer has superior reversibility. c. Time-resolved

17
current variation corresponding to the charge transfer. d. Schematic drawing of RC-DEG working

mechanism. Four stages (t0 -t1 , t1 -t2 , t2 -t3 , and t3 - t0 ) segmented by four characteristic time points (t0 , t1 , t2,

and t3 ) are defined to describe the charge transfer process during one cycle movement of the water droplet.

In the first stage (t0 -t1 ), the charge transfer process starts from the initial time t0 , when the water droplet

is at the left side of the unit and connects with the drain-I, and terminates at the time t1 when the water

droplet detaches from the drain-I. The electrostatically-induced positive charges on the source gradually

transfer to the drain with the droplet movement through an established closed-loop circuit between the

drain electrode I, source and the FEP. Then, moving to the second stage (t1 -t2 ), the charge transfer process

stops because the loop circuit is open. When the water droplet connects with the right drain-II at t2 , the

loop circuit is closed again, which accompanies by the quick transfer of electrostatically induced charges.

Meanwhile, the charge transfer process moves to the third stage (t2 -t3 ). The charge transfer process

terminates at the time when the water droplet to detach from the right drain-II, resulting in charge

accumulation in the droplet, and recovers at the time t3 when the droplet moves to the left direction and

contact with the drain-I. In the final stage (t3 -t0 ), the accumulated charges gradually transfer from the

drain-I to the source electrode and will stop when the water droplet moves back to the original location.

The pictures below each schematic are optical photographs at the corresponding moment.

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Fig. 4. Performance of the RC-DEG. a. Generated current and power of the single-unit RC-DEG

depending on load resistance. The voltage, current and charge outputs of the single-unit RC-DEGs with

b. varying the unit lengths and c. the operation frequency. d. Capacitor charging performance of single-

unit RC-DEG aiming at the different capacitors with distinctive capacity and the RC-DEG with one, two

and ten electricity generation units.

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Fig. 5. Applications of the RC-DEG. a. The schematic diagram of the potential application scenarios of

our RC-DEG. b. The status that a person wears a face mask properly and improperly. c. A wearable shoe’s

sole RC-DEG and the output voltage performance, Scale bar: 5 cm. d. Simultaneously lighting up 63

LEDs by using this wearable shoe’s sole RC-DEG.

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