A study on the electrochemical disinfection with H202 generated at the gas diffusion electrode （GDE） from active carbon/poly- tetrafluoroethylene was performed in a non-membrane cell. The effects of Pt load and the ...A study on the electrochemical disinfection with H202 generated at the gas diffusion electrode （GDE） from active carbon/poly- tetrafluoroethylene was performed in a non-membrane cell. The effects of Pt load and the pore-forming agent content in GDE, and operating conditions were investigated. The experimental results showed that nearly all bacterial cultures inoculated in the secondary effluent from wastewater treatment plant could be inactivated within 30 min at a current density of 10 mA/cm^2. The disinfection improved with increasing Pt load. Addition of the pore-forming agent NH4HCO3 improved the disinfection, while a drop in the pH value resulted in a rapid rise of germicidal efficacy and the disinfection time was shortened with increasing oxygen flow rate. Adsorption was proved to be ineffective in destroying bacteria, while germicidal efficacy increased with current density. The acceleration rate was different, it initially increased with current density. Then decreased, and finally reached a maximum at a current density of 6.7 mA/cm^2. The disinfection also improved with decreasing total bacterial count. The germicidal efficacy in the cathode compartment was approximately the same as in the anode compartment, indicating that the contribution of direct oxidation and the indirect treatment of bacterial cultures by hydroxyl radical was similar to the oxidative indirect effect of the generated H2O2.展开更多
Gas diffusion electrodes are applied to the coupled reaction of water electrolysis and electrocatalytic benzene hydrogenation. The effects of the preparation conditions of electrodes, electrolyte acidity, the concent...Gas diffusion electrodes are applied to the coupled reaction of water electrolysis and electrocatalytic benzene hydrogenation. The effects of the preparation conditions of electrodes, electrolyte acidity, the concentration of benzene and water vapor, and the flow rate of N2 are investigated by evaluating the efficiency of the current. Furthermore, the optimal operational conditions have been ascertained. The results of our experiment show that gas diffusion electrodes have good performance when the content of PTFE is 10% (wt) and that of Nafion is 0.75mg/cm2. The optimal operational conditions are as follows: The temperature of electrolysis is 70℃, acidity 0.5mol/L, the concentration of benzene 26%, the concentration of vapor 10%, the flow rate of N2 80mL/min-240mL/min. The efficiency of the current can reach 35% under optimal operational conditions. Then, a conclusion can be drawn that gas diffusion electrodes can improve the rate of the coupled reaction effectively.展开更多
α-MnO_(2) is a promising,inexpensive,and readily producible catalyst for the oxygen reduction reaction(ORR)in alkaline media,but its application is limited by low electronic conductivity.In this study,we enhance the ...α-MnO_(2) is a promising,inexpensive,and readily producible catalyst for the oxygen reduction reaction(ORR)in alkaline media,but its application is limited by low electronic conductivity.In this study,we enhance the performance ofα-MnO_(2) electrodes by systematically varying theα-MnO_(2)-to-Vulcan ratio within the catalyst layer.Electrodes are evaluated in a gas diffusion electrode(GDE)half-cell,where an optimized catalyst layer composition leads to significantly improved ORR performance.By finetuning both theα-MnO_(2)-to-Vulcan ratio and theα-MnO_(2) loading,the electrode outperforms a commercial MnO_(2)-based electrode and approaches the performance of the Pt/C benchmark.The improvement is attributed to the presence of a three-dimensional(3D)Vulcan network electronically connecting catalytically activeα-MnO_(2) sites with the substrate.Additionally,the optimized electrodes are employed in a prototype Al-O_(2) flow cell.Under constant oxygen flow,power densities exceed 250 mW cm^(-2),which is significantly higher than that of conventional Al-air batteries.Electrochemical impedance spectroscopy combined with distribution of relaxation times(DRT)analysis enables the separation of anode and cathode charge transfer impedances without the need for an additional reference electrode.The analysis reveals that the anode contributes more than twice as much impedance as the cathode,highlighting the need for further anode optimization.This work demonstrates a transferable approach for catalyst layer screening under technically relevant conditions in the GDE half-cell.Subsequent measurements in an Al-O_(2) flow cell validate the approach.The methodology is widely applicable to the development of advanced electrodes for a variety of metal-air battery technologies.展开更多
Aqueous hydrogen(H_(2))gas batteries with unmatched lifespan are ideal for grid-scale energy storage,yet their deployment remains limited by the lack of low-cost,efficient,and durable hydrogen electrodes.Here,we repor...Aqueous hydrogen(H_(2))gas batteries with unmatched lifespan are ideal for grid-scale energy storage,yet their deployment remains limited by the lack of low-cost,efficient,and durable hydrogen electrodes.Here,we report a high-throughput and durable gas diffusion electrode(GDE)based on a simply preparable carbon-coated nickel(Ni@C)catalyst and the design of H_(2) diffusion channels.By optimizing the carbon layer structure,a balance between the intrinsic activity and stability of the catalyst can be achieved.This Ni@C catalyst exhibits a hydrogen oxidation reaction(HOR)activity of 44 A g^(-1) as well as remarkable hydrogen evolution reaction(HER)performance.Experimental results and theoretical calculations confirm the electronic interaction between the carbon shell and Ni.In combination with a hydrophobic design,a robust and durable Ni@C-GDE has been fabricated.This electrode achieves a low HOR polarization of only 91 mV at 30 mA cm^(-2),outperforming Pt/C-GDE(154 mV),and operates stably over 4500cycles(3200 h)for HOR/HER reversing.Enabled by this electrode,a 10 Ah Ni-H_(2) battery with an energy density of 156.3 Wh kg^(-1) and cost of 62.2$kWh^(-1) is demonstrated.This work offers a viable strategy for practical and scalable hydrogen gas batteries.展开更多
The global production of organic wastes and heavy metals(HMs)poses significant environmental risks,along with considerable carbon emissions from waste decomposition.This highlights the significance of synergistic mana...The global production of organic wastes and heavy metals(HMs)poses significant environmental risks,along with considerable carbon emissions from waste decomposition.This highlights the significance of synergistic management of both wastes and CO_(2),which is a vital strategy for mitigating environmental pollution and climate change.Herein,we employed waste protein from wastewater produced during soybean peptide(SP)processing as a carbon matrix to anchor HMs Ni from electroplating wastewater.This mixture was electrospun into a gas diffusion electrode(GDE).This unique GDE design eliminates the need for a separate gas diffusion layer(GDL)and simplifies catalyst production.This versatile GDE consists of nanofibers with uniformly dispersed Ni single atom catalysts(SACs)on the fiber surface.Therefore,boasts a porous structure that facilitates CO_(2)diffusion and storage.The homogeneous distribution of Ni SACs within the GDE fosters high activity in the electrochemical conversion of CO_(2)to CO.At 50 mA/cm^(2)and 2.5 V cell voltage,Ni SACs achieved an excellent Faradaic efficiency of 81%-98%in a membrane electrode assembly(MEA).This technique holds a promise in achieving the collaborative management of carbon mitigation and wastes recovery.展开更多
A Pb loaded gas diffusion electrode was fabricated and used for the electroreduction of CO2 to formic acid. The Pb/C catalyst was prepared by isometric impregnation. The crystal structure and morphology of the Pb/C ca...A Pb loaded gas diffusion electrode was fabricated and used for the electroreduction of CO2 to formic acid. The Pb/C catalyst was prepared by isometric impregnation. The crystal structure and morphology of the Pb/C catalyst were characterized by X-ray diffraction （XRD） and transmission electron microscope （TEM）. The preparation conditions of the gas diffusion electrode were optimized by adjusting the amounts of polytetrafluoroethylene （PTFE） in the gas diffusion layer and acetylene black in the catalytic layer. The electrochemical performance of the as-prepared gas diffusion electrode was studied by chronoamperometry and cyclic voltammetry. The optimized gas diffusion electrode showed good catalytic performance for the electroreduction of CO2. The current efficiency of formic acid after 1 h of operation reached a maximum of 22% at -2.0 V versus saturated calomel electrode （SCE）.展开更多
Membrane electrode assembly(MEA)is widely considered to be the most promising type of electrolyzer for the practical application of electrochemical CO_(2) reduction reaction(CO_(2)RR).In MEAs,a square-shaped cross-sec...Membrane electrode assembly(MEA)is widely considered to be the most promising type of electrolyzer for the practical application of electrochemical CO_(2) reduction reaction(CO_(2)RR).In MEAs,a square-shaped cross-section in the flow channel is normally adopted,the configuration optimization of which could potentially enhance the performance of the electrolyzer.This paper describes the numerical simulation study on the impact of the flow-channel cross-section shapes in the MEA electrolyzer for CO_(2)RR.The results show that wide flow channels with low heights are beneficial to the CO_(2)RR by providing a uniform flow field of CO_(2),especially at high current densities.Moreover,the larger the electrolyzer,the more significant the effect is.This study provides a theoretical basis for the design of high-performance MEA electrolyzers for CO_(2)RR.展开更多
The electrocatalytic C-N coupling reaction involving carbon dioxide(CO_(2))and nitrogenous small molecules has recently emerged as a subject of considerable interest within the field of urea synthesis.This approach ha...The electrocatalytic C-N coupling reaction involving carbon dioxide(CO_(2))and nitrogenous small molecules has recently emerged as a subject of considerable interest within the field of urea synthesis.This approach has the potential to facilitate the clean,sustainable production of urea,thereby contributing to the attainment of carbon neutrality and the advancement of artificial nitrogen cycling.Nevertheless,electrocatalytic urea synthesis still faces significant challenges due to the difficulty of balancing the co-activation of carbon and nitrogen sources and the subsequent catalytic C-N coupling of in situ-generated species,as well as competing reactions.To overcome these challenges,there is a growing emphasis on the research of gas diffusion electrodes(GDEs)and the design of electrode materials.This article provides a comprehensive review of the C-N coupling mechanisms,the classification of catalysts,the electrocatalyst design and optimization strategies,and the fundamental functions and importance of GDEs in electrocatalytic C-N coupling reactions.It also provides insights and perspectives on the major challenges and future research directions for GDEs and electrocatalysts in electrocatalytic urea synthesis.展开更多
The gas diffusion electrode(GDE)is widely employed in various electrocatalytic reactions,such as CO_(2) reduction,hydrogen/oxygen evolution,and oxygen reduction.However,the structural complexity of GDE makes a number ...The gas diffusion electrode(GDE)is widely employed in various electrocatalytic reactions,such as CO_(2) reduction,hydrogen/oxygen evolution,and oxygen reduction.However,the structural complexity of GDE makes a number of factors other than the intrinsic activity of catalysts relevant to the reaction performance,including the catalyst layer(CL)structure,feed flow rate,and pressure balance between liquid and gas feeds[1].展开更多
The industrial adoption of microbial electrosynthesis(MES)is hindered by high overpotentials deriving from low electrolyte conductivity and inefficient cell designs.In this study,a mixed microbial consortium originati...The industrial adoption of microbial electrosynthesis(MES)is hindered by high overpotentials deriving from low electrolyte conductivity and inefficient cell designs.In this study,a mixed microbial consortium originating from an anaerobic digester operated under saline conditions(∼13 g L^(−1)NaCl)was adapted for acetate production from bicarbonate in galvanostatic(0.25 mA cm^(−2))H-type cells at 5,10,15,or 20 g L^(−1)NaCl concentration.The acetogenic communities were successfully enriched only at 5 and 10 g L^(−1)NaCl,revealing an inhibitory threshold of about 6 g L^(−1)Na^(+).The enriched planktonic communities were then used as inoculum for 3D printed,three-chamber cells equipped with a gas diffusion biocathode.The cells were fed with CO_(2)gas and operated galvanostatically(0.25 or 1.00 mA cm^(−2)).The highest production rate of 55.4 g m^(−2) d^(−1)(0.89 g L^(−1)d^(−1)),with 82.4%Coulombic efficiency,was obtained at 5 g L^(−1)NaCl concentration and 1 mA cm^(−2)applied current,achieving an average acetate production of 44.7 kg MWh−1.Scanning electron microscopy and 16S rRNA sequencing analysis confirmed the formation of a cathodic biofilm dominated by Acetobacterium sp.Finally,three 3D printed cells were hydraulically connected in series to simulate an MES stack,achieving three-fold production rates than with the single cell at 0.25 mA cm^(−2).This confirms that three-chamber MES cells are an efficient and scalable technology for CO_(2)bio-electro recycling to acetate and that moderate saline conditions(5 g L^(−1)NaCl)can help reduce their power demand while preserving the activity of acetogens.展开更多
The global concerns of energy crisis and climate change,primarily caused by carbon dioxide(CO_(2)),are of utmost importance.Recently,the electrocatalytic CO_(2) reduction reaction(CO_(2)RR) to high value-added multi-c...The global concerns of energy crisis and climate change,primarily caused by carbon dioxide(CO_(2)),are of utmost importance.Recently,the electrocatalytic CO_(2) reduction reaction(CO_(2)RR) to high value-added multi-carbon(C_(2+)) products driven by renewable electricity has emerged as a highly promising solution to alleviate energy shortages and achieve carbon neutrality.Among these C_(2+) products,ethylene(C_(2)H_(4))holds particular importance in the petrochemical industry.Accordingly,this review aims to establish a connection between the fundamentals of electrocatalytic CO_(2) reduction reaction to ethylene(CO_(2)RRto-C_(2)H_(4)) in laboratory-scale research(lab) and its potential applications in industrial-level fabrication(fab).The review begins by summarizing the fundamental aspects,including the design strategies of high-performance Cu-based electrocatalysts and advanced electrolyzer devices.Subsequently,innovative and value-added techniques are presented to address the inherent challenges encountered during the implementations of CO_(2)RR-to-C_(2)H_(4) in industrial scenarios.Additionally,case studies of the technoeconomic analysis of the CO_(2)RR-to-C_(2)H_(4) process are discussed,taking into factors such as costeffectiveness,scalability,and market potential.The review concludes by outlining the perspectives and challenges associated with scaling up the CO_(2)RR-to-C_(2)H_(4) process.The insights presented in this review are expected to make a valuable contribution in advancing the CO_(2)RR-to-C_(2)H_(4) process from lab to fab.展开更多
CO_(2) electroreduction(CO_(2) ER)to high value-added chemicals is considered as a promising technology to achieve sustainable carbon neutralization.By virtue of the progressive research in recent years aiming at desi...CO_(2) electroreduction(CO_(2) ER)to high value-added chemicals is considered as a promising technology to achieve sustainable carbon neutralization.By virtue of the progressive research in recent years aiming at design and understanding of catalytic materials and electrolyte systems,the CO_(2) ER performance(such as current density,selectivity,stability,CO_(2) conversion,etc.)has been continually increased.Unfortunately,there has been relatively little attention paid to the large-scale CO 2 electrolyzers,which stand just as one obstacle,alongside series-parallel integration,challenging the practical application of this infant technology.In this review,the latest progress on the structures of low-temperature CO_(2) electrolyzers and scale-up studies was systematically overviewed.The influence of the CO_(2) electrolyzer configurations,such as the flow channel design,gas diffusion electrode(GDE)and ion exchange membrane(IEM),on the CO_(2) ER performance was further discussed.The review could provide inspiration for the design of large-scale CO_(2) electrolyzers so as to accelerate the industrial application of CO_(2) ER technology.展开更多
Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to i...Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to its low solubility in aqueous electrolytes.Herein,we propose phosphorus-activated Cu electrocatalysts to generate electron-deficient Cu sites on the catalyst surface to promote the adsorption of N_(2) molecules.The eNRR system is further modified using a gas diffusion electrode(GDE) coated with polytetrafluoroethylene(PTFE) to form an effective three-phase boundary of liquid water-gas N_(2)-solid catalyst to facilitate easy access of N_(2) to the catalytic sites.As a result,the new catalyst in the flow-type cell records a Faradaic efficiency of 13.15% and an NH_(3) production rate of 7.69 μg h^(-1) cm^(-2) at-0.2 V_(RHE),which represent 3.56 and 59.2 times increases from those obtained with a pristine Cu electrode in a typical electrolytic cell.This work represents a successful demonstration of dual modification strategies;catalyst modification and N_(2) supplying system engineering,and the results would provide a useful platform for further developments of electrocatalysts and reaction systems.展开更多
The use of gas diffusion electrode(GDE)based flow cell can realize industrial-scale CO_(2) reduction reactions(CO_(2)RRs).Controlling local CO_(2) and CO intermediate diffusion plays a key role in CO_(2)RR toward mult...The use of gas diffusion electrode(GDE)based flow cell can realize industrial-scale CO_(2) reduction reactions(CO_(2)RRs).Controlling local CO_(2) and CO intermediate diffusion plays a key role in CO_(2)RR toward multi-carbon(C_(2+))products.In this work,local CO_(2) and CO intermediate diffusion through the catalyst layer(CL)was investigated for improving CO_(2)RR toward C_(2+)products.The gas permeability tests and finite element simulation results indicated CL can balance the CO_(2) gas diffusion and residence time of the CO intermediate,leading to a sufficient CO concentration with a suitable CO_(2)/H_(2)O supply for high C_(2+)products.As a result,an excellent selectivity of C_(2+)products~79%at a high current density of 400 mA·cm^(-2) could be obtained on the optimal 500 nm Cu CL(Cu500).This work provides a new insight into the optimization of CO_(2)/H_(2)O supply and local CO concentration by controlling CL for C_(2+)products in CO_(2)RR flow cell.展开更多
The solar energy-driven electrochemical CO_(2)reduction to value-added fuels or chemicals is considered as an attractive path to store renewable energy in the form of chemical energy to close the carbon cycle.However,...The solar energy-driven electrochemical CO_(2)reduction to value-added fuels or chemicals is considered as an attractive path to store renewable energy in the form of chemical energy to close the carbon cycle.However,CO_(2)reduction suffers from a number of challenges including slow reaction rates,low selectivity,and low energy conversion efficiency.Recently,innovative strategies have been developed to mitigate this challenges.Especially the development of flow cell reactors with a gas diffusion electrode,ionic liquid electrolytes,and new electrocatalysts have dramatically improved the reaction rates and selectivity to desired products.In this perspective,we highlight the key recent developments and challenges in PVpowered electrochemical CO_(2)reduction and propose effective strategies to improve the reaction kinetics,to minimize the electrical energy losses,and to tune the selectivity of the catalysts for desired products,and then suggest future direction of research and development.展开更多
Electrochemical reduction of CO_(2)(CO_(2)RR)coupled with renewable electrical energy is an attractive way of upgrading CO_(2)to value-added chemicals and closing the carbon cycle.However,CO_(2)RR electrocatalysts sti...Electrochemical reduction of CO_(2)(CO_(2)RR)coupled with renewable electrical energy is an attractive way of upgrading CO_(2)to value-added chemicals and closing the carbon cycle.However,CO_(2)RR electrocatalysts still suffer from high overpotential,and the complex reaction pathways of CO_(2)RR often lead to mixed products.Early research focuses on tuning the binding of reaction intermediates on electrocatalysts,and recent efforts have revealed that the design of electrolysis reactors is equally important for efficient and selective CO_(2)RR.In this review,we present an overview of recent advances and challenges toward achieving high activity and high selectivity in CO_(2)RR at ambient conditions,with a particular focus on the progress of CO_(2)RR electrocatalyst engineering and reactor design.Our discussion begins with three types of electrocatalysts for CO_(2)RR(noble metalbased,none-noble metal-based,and metal-free electrocatalysts),and then we examine systems-level strategies toward engineering specific components of the electrolyzer,including gas diffusion electrodes,electrolytes,and polymer electrolyte membranes.We close with future perspectives on catalyst development,in-situ/operando characterization,and electrolyzer performance evaluation in CO_(2)RR studies.展开更多
Electrochemical CO_(2)reduction reaction(CO_(2)RR)is a promising technique to address the excess CO_(2)emissions for closing the global carbon cycle.However,challenges remain to break the trade-off between high Farada...Electrochemical CO_(2)reduction reaction(CO_(2)RR)is a promising technique to address the excess CO_(2)emissions for closing the global carbon cycle.However,challenges remain to break the trade-off between high Faradaic efficiencies and high current densities.Herein,we synthesize Ag nano-foams(Ag NFs)featuring sufficient gas channels by a facile wet-chemical method.It is revealed that the gaseous products can be rapidly released from Ag NFs with the presence of nanochannels,profiting from the exposure of active sites and their further access to CO_(2).COMSOL simulation verifies the uniform distribution of low-pressure drop and thus promotes local mass transfer within the catalyst layers.Benefiting from the improved transport features,the Ag NFs achieve excellent CO Faradaic efficiencies(FE_(CO)>90.9%)in a wide potential window(-0.5VRHE--1.2V_(RHE)),together with a high partial current density of 365.7 mA cm^(-2)at-1.2VRHE.This study provides insights into the rational regulation of gas and electrons within electrocatalysts for efficient CO_(2)-to-gas conversion.展开更多
Decentralized solutions for the low-cost and sustainable treatment of large-scale natural water bodies contaminated with organic pollutants are urgently needed.This study introduces a self-powered clean boat using a p...Decentralized solutions for the low-cost and sustainable treatment of large-scale natural water bodies contaminated with organic pollutants are urgently needed.This study introduces a self-powered clean boat using a photovoltaic(PV)-driven electrochemical Fenton system,featuring a gas diffusion electrode(GDE)and a quasi-solid hydrogel electrolyte.This setup enables in-situ oxygen reduction in low-conductivity lake water,achieving a high H_(2)O_(2)production rate of 290±10 mg L^(-1)h^(-1).The hydrogel,containing Fe^(2+)/Fe^(3+)pairs,enriches ion concentration,enhances conductivity,and triggers the Fenton reaction to convert H_(2)O_(2)into·OH radicals for efficient antibiotic degradation.The boat achieved a 99.4%removal rate for tetracycline(TC)at 1 mg L^(-1)in contaminated water within 3 h,demonstrating over 98%removal efficiency for other common antibiotics.This system integrates clean energy use,H_(2)O_(2)production,Fenton reaction activation,and pollutant degradation,addressing the limitations of conventional electrochemical methods in low-conductivity waters.It offers a sustainable solution for decentralized water treatment in pilot-scale experiments with low unique energy consumption(0.43 kWh mg^(-1))by solar energy.展开更多
The demand for converting CO_(2)into fuels or chemicals is on the rise to achieve a carbon-efficient circular economy.Biohybrid CO_(2)electrolysis shows potential for increasing production rates and diversifying produ...The demand for converting CO_(2)into fuels or chemicals is on the rise to achieve a carbon-efficient circular economy.Biohybrid CO_(2)electrolysis shows potential for increasing production rates and diversifying product spectra by combining electrocatalysts and microbial catalysts.However,it is important to note that utilizing a shared catholyte for biohybrid CO_(2)electrolysis has not demonstrated significant performance improvements to date.In this study,we developed a biohybrid CO_(2)electrolysis system utilizing a solid electrolyte operating in an external mode.The produced formic acid was extracted and used as an intermediate for microbial conversion.Impressively,the solid-electrolyte CO_(2)electrolysers obtained a remarkable total Faradic efficiency of 81.4%for formic acid production.In-situ mechanism studies unveiled metallic tin as the probable real active site,prompting further exploration of strategies to boost the activity and stability of electrocatalysts.In the bioconversion step,we achieved a noteworthy 8-day duration for generating bioelectricity,nearly 100%electron recovery for biomethane production,and 90.8%for acetate generation.Additionally,when ethanol was co-fed,a C_(6)specificity of 41.1%was observed for the generation of medium-chain fatty acids(MCFAs).This study presents groundbreaking experimental data that demonstrates the numerous advantages of utilizing hybrid systems as advanced synthesis techniques.展开更多
Electrochemical CO_(2)reduction reaction(CO_(2)RR)on gas diffusion electrodes(GDEs)offers a promising route for carbon-neutral fuel production at commercially relevant current densities(J>200 mA cm^(-2))[1,2].Howev...Electrochemical CO_(2)reduction reaction(CO_(2)RR)on gas diffusion electrodes(GDEs)offers a promising route for carbon-neutral fuel production at commercially relevant current densities(J>200 mA cm^(-2))[1,2].However,under high-rate operation,GDE performance deteriorates due to mass transport limitations[3,4].First,local CO_(2)depletion near the catalyst surface intensifies the competing hydrogen evolution reaction(HER),diminishing the selectivity[5].展开更多
基金supported by the National Natural Science Foundation of China (No.20777053)
文摘A study on the electrochemical disinfection with H202 generated at the gas diffusion electrode （GDE） from active carbon/poly- tetrafluoroethylene was performed in a non-membrane cell. The effects of Pt load and the pore-forming agent content in GDE, and operating conditions were investigated. The experimental results showed that nearly all bacterial cultures inoculated in the secondary effluent from wastewater treatment plant could be inactivated within 30 min at a current density of 10 mA/cm^2. The disinfection improved with increasing Pt load. Addition of the pore-forming agent NH4HCO3 improved the disinfection, while a drop in the pH value resulted in a rapid rise of germicidal efficacy and the disinfection time was shortened with increasing oxygen flow rate. Adsorption was proved to be ineffective in destroying bacteria, while germicidal efficacy increased with current density. The acceleration rate was different, it initially increased with current density. Then decreased, and finally reached a maximum at a current density of 6.7 mA/cm^2. The disinfection also improved with decreasing total bacterial count. The germicidal efficacy in the cathode compartment was approximately the same as in the anode compartment, indicating that the contribution of direct oxidation and the indirect treatment of bacterial cultures by hydroxyl radical was similar to the oxidative indirect effect of the generated H2O2.
文摘Gas diffusion electrodes are applied to the coupled reaction of water electrolysis and electrocatalytic benzene hydrogenation. The effects of the preparation conditions of electrodes, electrolyte acidity, the concentration of benzene and water vapor, and the flow rate of N2 are investigated by evaluating the efficiency of the current. Furthermore, the optimal operational conditions have been ascertained. The results of our experiment show that gas diffusion electrodes have good performance when the content of PTFE is 10% (wt) and that of Nafion is 0.75mg/cm2. The optimal operational conditions are as follows: The temperature of electrolysis is 70℃, acidity 0.5mol/L, the concentration of benzene 26%, the concentration of vapor 10%, the flow rate of N2 80mL/min-240mL/min. The efficiency of the current can reach 35% under optimal operational conditions. Then, a conclusion can be drawn that gas diffusion electrodes can improve the rate of the coupled reaction effectively.
基金part of the ALU-STORE project(Aluminum Metal as Energy Carrier for Seasonal Energy Storage)funded by the KIT Future Fieldsthe research performed at CELEST(Center for Electrochemical Energy Storage Ulm-Karlsruhe)+1 种基金funding from the German Federal Ministry of Research,Technology and Space(BMFTR)in the Nano Mat Futur program(03XP0423)basic funding from the Helmholtz Association。
文摘α-MnO_(2) is a promising,inexpensive,and readily producible catalyst for the oxygen reduction reaction(ORR)in alkaline media,but its application is limited by low electronic conductivity.In this study,we enhance the performance ofα-MnO_(2) electrodes by systematically varying theα-MnO_(2)-to-Vulcan ratio within the catalyst layer.Electrodes are evaluated in a gas diffusion electrode(GDE)half-cell,where an optimized catalyst layer composition leads to significantly improved ORR performance.By finetuning both theα-MnO_(2)-to-Vulcan ratio and theα-MnO_(2) loading,the electrode outperforms a commercial MnO_(2)-based electrode and approaches the performance of the Pt/C benchmark.The improvement is attributed to the presence of a three-dimensional(3D)Vulcan network electronically connecting catalytically activeα-MnO_(2) sites with the substrate.Additionally,the optimized electrodes are employed in a prototype Al-O_(2) flow cell.Under constant oxygen flow,power densities exceed 250 mW cm^(-2),which is significantly higher than that of conventional Al-air batteries.Electrochemical impedance spectroscopy combined with distribution of relaxation times(DRT)analysis enables the separation of anode and cathode charge transfer impedances without the need for an additional reference electrode.The analysis reveals that the anode contributes more than twice as much impedance as the cathode,highlighting the need for further anode optimization.This work demonstrates a transferable approach for catalyst layer screening under technically relevant conditions in the GDE half-cell.Subsequent measurements in an Al-O_(2) flow cell validate the approach.The methodology is widely applicable to the development of advanced electrodes for a variety of metal-air battery technologies.
基金financially supported by the“National Natural Science Foundation of China”(No.22279082)the“Natural Science Foundation of Sichuan”(2025YFHZ0056)。
文摘Aqueous hydrogen(H_(2))gas batteries with unmatched lifespan are ideal for grid-scale energy storage,yet their deployment remains limited by the lack of low-cost,efficient,and durable hydrogen electrodes.Here,we report a high-throughput and durable gas diffusion electrode(GDE)based on a simply preparable carbon-coated nickel(Ni@C)catalyst and the design of H_(2) diffusion channels.By optimizing the carbon layer structure,a balance between the intrinsic activity and stability of the catalyst can be achieved.This Ni@C catalyst exhibits a hydrogen oxidation reaction(HOR)activity of 44 A g^(-1) as well as remarkable hydrogen evolution reaction(HER)performance.Experimental results and theoretical calculations confirm the electronic interaction between the carbon shell and Ni.In combination with a hydrophobic design,a robust and durable Ni@C-GDE has been fabricated.This electrode achieves a low HOR polarization of only 91 mV at 30 mA cm^(-2),outperforming Pt/C-GDE(154 mV),and operates stably over 4500cycles(3200 h)for HOR/HER reversing.Enabled by this electrode,a 10 Ah Ni-H_(2) battery with an energy density of 156.3 Wh kg^(-1) and cost of 62.2$kWh^(-1) is demonstrated.This work offers a viable strategy for practical and scalable hydrogen gas batteries.
基金supported by the National Natural Science Foundation of China(No.22176046)the Science Fund for Creative Research Groups of the National Natural Science Foundation of China(No.52321005)+1 种基金the Shenzhen Science and Technology Program(Nos.KQTD20190929172630447,JCYJ20210324124209025,and GXWD20220811173949005)the Natural Science Foundation of Guangdong Province(No.2022A1515012016).
文摘The global production of organic wastes and heavy metals(HMs)poses significant environmental risks,along with considerable carbon emissions from waste decomposition.This highlights the significance of synergistic management of both wastes and CO_(2),which is a vital strategy for mitigating environmental pollution and climate change.Herein,we employed waste protein from wastewater produced during soybean peptide(SP)processing as a carbon matrix to anchor HMs Ni from electroplating wastewater.This mixture was electrospun into a gas diffusion electrode(GDE).This unique GDE design eliminates the need for a separate gas diffusion layer(GDL)and simplifies catalyst production.This versatile GDE consists of nanofibers with uniformly dispersed Ni single atom catalysts(SACs)on the fiber surface.Therefore,boasts a porous structure that facilitates CO_(2)diffusion and storage.The homogeneous distribution of Ni SACs within the GDE fosters high activity in the electrochemical conversion of CO_(2)to CO.At 50 mA/cm^(2)and 2.5 V cell voltage,Ni SACs achieved an excellent Faradaic efficiency of 81%-98%in a membrane electrode assembly(MEA).This technique holds a promise in achieving the collaborative management of carbon mitigation and wastes recovery.
文摘A Pb loaded gas diffusion electrode was fabricated and used for the electroreduction of CO2 to formic acid. The Pb/C catalyst was prepared by isometric impregnation. The crystal structure and morphology of the Pb/C catalyst were characterized by X-ray diffraction （XRD） and transmission electron microscope （TEM）. The preparation conditions of the gas diffusion electrode were optimized by adjusting the amounts of polytetrafluoroethylene （PTFE） in the gas diffusion layer and acetylene black in the catalytic layer. The electrochemical performance of the as-prepared gas diffusion electrode was studied by chronoamperometry and cyclic voltammetry. The optimized gas diffusion electrode showed good catalytic performance for the electroreduction of CO2. The current efficiency of formic acid after 1 h of operation reached a maximum of 22% at -2.0 V versus saturated calomel electrode （SCE）.
基金the National Key R&D Program of China(No.2021YFA1501503)the National Natural Science Foundation of China(Nos.22250008,22121004,22108197)+3 种基金the Haihe Laboratory of Sustainable Chemical Transformations(No.CYZC202107)the Natural Science Foundation of Tianjin City(No.21JCZXJC00060)the Program of Introducing Talents of Discipline to Universities(No.BP0618007)the Xplorer Prize for financial support。
文摘Membrane electrode assembly(MEA)is widely considered to be the most promising type of electrolyzer for the practical application of electrochemical CO_(2) reduction reaction(CO_(2)RR).In MEAs,a square-shaped cross-section in the flow channel is normally adopted,the configuration optimization of which could potentially enhance the performance of the electrolyzer.This paper describes the numerical simulation study on the impact of the flow-channel cross-section shapes in the MEA electrolyzer for CO_(2)RR.The results show that wide flow channels with low heights are beneficial to the CO_(2)RR by providing a uniform flow field of CO_(2),especially at high current densities.Moreover,the larger the electrolyzer,the more significant the effect is.This study provides a theoretical basis for the design of high-performance MEA electrolyzers for CO_(2)RR.
基金Natural Science Foundation of China(52404332,22178394)the ScienceTechnology Innovation Program of Hunan Province(2022RC3048)the Postdoctoral Fellowship Program of CPSF(GZB20240860)for financial support.
文摘The electrocatalytic C-N coupling reaction involving carbon dioxide(CO_(2))and nitrogenous small molecules has recently emerged as a subject of considerable interest within the field of urea synthesis.This approach has the potential to facilitate the clean,sustainable production of urea,thereby contributing to the attainment of carbon neutrality and the advancement of artificial nitrogen cycling.Nevertheless,electrocatalytic urea synthesis still faces significant challenges due to the difficulty of balancing the co-activation of carbon and nitrogen sources and the subsequent catalytic C-N coupling of in situ-generated species,as well as competing reactions.To overcome these challenges,there is a growing emphasis on the research of gas diffusion electrodes(GDEs)and the design of electrode materials.This article provides a comprehensive review of the C-N coupling mechanisms,the classification of catalysts,the electrocatalyst design and optimization strategies,and the fundamental functions and importance of GDEs in electrocatalytic C-N coupling reactions.It also provides insights and perspectives on the major challenges and future research directions for GDEs and electrocatalysts in electrocatalytic urea synthesis.
文摘The gas diffusion electrode(GDE)is widely employed in various electrocatalytic reactions,such as CO_(2) reduction,hydrogen/oxygen evolution,and oxygen reduction.However,the structural complexity of GDE makes a number of factors other than the intrinsic activity of catalysts relevant to the reaction performance,including the catalyst layer(CL)structure,feed flow rate,and pressure balance between liquid and gas feeds[1].
基金This work was performed on the framework of the Science Foundation Ireland(SFI)Pathfinder Award on“Hybrid Bio-Solar Reactors for wastewater treatment and CO_(2)recycling”(award nr.19/FIP/ZE/7572 PF)PD is supported by the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement,project ATMESPHERE,No 101029266.SP is a Serra Hunter Fellow(UdG-AG-575)+4 种基金acknowledges the funding from the ICREA Academia award.LEQUIA has been recognised as a consolidated research group by the Catalan Government(2021-SGR-01352)UZI is supported by EPSRC(EP/P029329/1 and EP/V030515/1)VOF is supported by the Enterprise Ireland Technology Centres Programme(TC/2014/0016)Science Foundation Ireland(14/IA/2371,19/FFP/6746 and 16/RC/3889)DP acknowledges the support of the VIVALDI project that has received funding from the European Union's Horizon 2020 research and innovation program under grant agreement 101000441.
文摘The industrial adoption of microbial electrosynthesis(MES)is hindered by high overpotentials deriving from low electrolyte conductivity and inefficient cell designs.In this study,a mixed microbial consortium originating from an anaerobic digester operated under saline conditions(∼13 g L^(−1)NaCl)was adapted for acetate production from bicarbonate in galvanostatic(0.25 mA cm^(−2))H-type cells at 5,10,15,or 20 g L^(−1)NaCl concentration.The acetogenic communities were successfully enriched only at 5 and 10 g L^(−1)NaCl,revealing an inhibitory threshold of about 6 g L^(−1)Na^(+).The enriched planktonic communities were then used as inoculum for 3D printed,three-chamber cells equipped with a gas diffusion biocathode.The cells were fed with CO_(2)gas and operated galvanostatically(0.25 or 1.00 mA cm^(−2)).The highest production rate of 55.4 g m^(−2) d^(−1)(0.89 g L^(−1)d^(−1)),with 82.4%Coulombic efficiency,was obtained at 5 g L^(−1)NaCl concentration and 1 mA cm^(−2)applied current,achieving an average acetate production of 44.7 kg MWh−1.Scanning electron microscopy and 16S rRNA sequencing analysis confirmed the formation of a cathodic biofilm dominated by Acetobacterium sp.Finally,three 3D printed cells were hydraulically connected in series to simulate an MES stack,achieving three-fold production rates than with the single cell at 0.25 mA cm^(−2).This confirms that three-chamber MES cells are an efficient and scalable technology for CO_(2)bio-electro recycling to acetate and that moderate saline conditions(5 g L^(−1)NaCl)can help reduce their power demand while preserving the activity of acetogens.
基金supported by Zhejiang Provincial Department of Science and Technology under its Provincial Key Laboratory Program(2020E10018)the financial support from Fundamental Research Funds for the Central Universities(2022LHJH01-03,2022ZFJH04,2022QZJH14)+5 种基金Pioneer R&D Program of Zhejiang Province(2022C03040)the financial aid from National Natural Science Foundation of China(22005266)Zhejiang Provincial Natural Science Foundation(LR21E020003)Fundamental Research Funds for the Central Universities(2021FZZX001-09)supported by the Royal Academy of Engineering under the Chairs in Emerging Technologies scheme(CiET2021_17)University of Nottingham Ningbo China for providing a full PhD scholarship。
文摘The global concerns of energy crisis and climate change,primarily caused by carbon dioxide(CO_(2)),are of utmost importance.Recently,the electrocatalytic CO_(2) reduction reaction(CO_(2)RR) to high value-added multi-carbon(C_(2+)) products driven by renewable electricity has emerged as a highly promising solution to alleviate energy shortages and achieve carbon neutrality.Among these C_(2+) products,ethylene(C_(2)H_(4))holds particular importance in the petrochemical industry.Accordingly,this review aims to establish a connection between the fundamentals of electrocatalytic CO_(2) reduction reaction to ethylene(CO_(2)RRto-C_(2)H_(4)) in laboratory-scale research(lab) and its potential applications in industrial-level fabrication(fab).The review begins by summarizing the fundamental aspects,including the design strategies of high-performance Cu-based electrocatalysts and advanced electrolyzer devices.Subsequently,innovative and value-added techniques are presented to address the inherent challenges encountered during the implementations of CO_(2)RR-to-C_(2)H_(4) in industrial scenarios.Additionally,case studies of the technoeconomic analysis of the CO_(2)RR-to-C_(2)H_(4) process are discussed,taking into factors such as costeffectiveness,scalability,and market potential.The review concludes by outlining the perspectives and challenges associated with scaling up the CO_(2)RR-to-C_(2)H_(4) process.The insights presented in this review are expected to make a valuable contribution in advancing the CO_(2)RR-to-C_(2)H_(4) process from lab to fab.
基金supported by National Key R&D Program of China(2020YFA0710200)the National Natural Science Foundation of China(21838010,22122814)+2 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciences(2018064)State Key Laboratory of Multiphase complex systems,Institute of Process Engineering,Chinese Academy of Sciences(No.MPCS-2022-A-03)Innovation Academy for Green Manufacture Institute,Chinese Academy of Science(IAGM2020C14).
文摘CO_(2) electroreduction(CO_(2) ER)to high value-added chemicals is considered as a promising technology to achieve sustainable carbon neutralization.By virtue of the progressive research in recent years aiming at design and understanding of catalytic materials and electrolyte systems,the CO_(2) ER performance(such as current density,selectivity,stability,CO_(2) conversion,etc.)has been continually increased.Unfortunately,there has been relatively little attention paid to the large-scale CO 2 electrolyzers,which stand just as one obstacle,alongside series-parallel integration,challenging the practical application of this infant technology.In this review,the latest progress on the structures of low-temperature CO_(2) electrolyzers and scale-up studies was systematically overviewed.The influence of the CO_(2) electrolyzer configurations,such as the flow channel design,gas diffusion electrode(GDE)and ion exchange membrane(IEM),on the CO_(2) ER performance was further discussed.The review could provide inspiration for the design of large-scale CO_(2) electrolyzers so as to accelerate the industrial application of CO_(2) ER technology.
基金supported by the Climate Change Response Project (NRF-2019M1A2A2065612)the Brainlink Project (NRF2022H1D3A3A01081140)+3 种基金the NRF-2021R1A4A3027878 and the No. RS-2023-00212273 funded by the Ministry of Science and ICT of Korea via National Research Foundationresearch funds from Hanhwa Solutions Chemicals (1.220029.01)UNIST (1.190013.01)supported by the Institute for Basic Science (IBS-R019-D1)。
文摘Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to its low solubility in aqueous electrolytes.Herein,we propose phosphorus-activated Cu electrocatalysts to generate electron-deficient Cu sites on the catalyst surface to promote the adsorption of N_(2) molecules.The eNRR system is further modified using a gas diffusion electrode(GDE) coated with polytetrafluoroethylene(PTFE) to form an effective three-phase boundary of liquid water-gas N_(2)-solid catalyst to facilitate easy access of N_(2) to the catalytic sites.As a result,the new catalyst in the flow-type cell records a Faradaic efficiency of 13.15% and an NH_(3) production rate of 7.69 μg h^(-1) cm^(-2) at-0.2 V_(RHE),which represent 3.56 and 59.2 times increases from those obtained with a pristine Cu electrode in a typical electrolytic cell.This work represents a successful demonstration of dual modification strategies;catalyst modification and N_(2) supplying system engineering,and the results would provide a useful platform for further developments of electrocatalysts and reaction systems.
基金The authors gratefully thank the National Natural Science Foundation of China(No.22002189)Central South University Research Programme of Advanced Interdisciplinary Studies(No.2023QYJC012)+1 种基金Central South University Innovation-Driven Research Program(No.2023CXQD042)the Fundamental Research Funds for the Central Universities of Central South University(No.2023ZZTS0962).
文摘The use of gas diffusion electrode(GDE)based flow cell can realize industrial-scale CO_(2) reduction reactions(CO_(2)RRs).Controlling local CO_(2) and CO intermediate diffusion plays a key role in CO_(2)RR toward multi-carbon(C_(2+))products.In this work,local CO_(2) and CO intermediate diffusion through the catalyst layer(CL)was investigated for improving CO_(2)RR toward C_(2+)products.The gas permeability tests and finite element simulation results indicated CL can balance the CO_(2) gas diffusion and residence time of the CO intermediate,leading to a sufficient CO concentration with a suitable CO_(2)/H_(2)O supply for high C_(2+)products.As a result,an excellent selectivity of C_(2+)products~79%at a high current density of 400 mA·cm^(-2) could be obtained on the optimal 500 nm Cu CL(Cu500).This work provides a new insight into the optimization of CO_(2)/H_(2)O supply and local CO concentration by controlling CL for C_(2+)products in CO_(2)RR flow cell.
基金supported by the Climate Change Response Project(NRF-2019M1A2A2065612)the Basic Science Grant(NRF2019R1A4A1029237)+2 种基金the Korea-China Key Joint Research Program(2017K2A9A2A11070341)funded by the Ministry of Science and ICT,and by the 2019 Research Fund(1.190013.01)of UNISTsupport from‘‘Carbon to X Project”(Project No.2020M3H7A1098231)through the National Research Foundation(NRF)funded by the Ministry of Science and ICT,Republic of Korea。
文摘The solar energy-driven electrochemical CO_(2)reduction to value-added fuels or chemicals is considered as an attractive path to store renewable energy in the form of chemical energy to close the carbon cycle.However,CO_(2)reduction suffers from a number of challenges including slow reaction rates,low selectivity,and low energy conversion efficiency.Recently,innovative strategies have been developed to mitigate this challenges.Especially the development of flow cell reactors with a gas diffusion electrode,ionic liquid electrolytes,and new electrocatalysts have dramatically improved the reaction rates and selectivity to desired products.In this perspective,we highlight the key recent developments and challenges in PVpowered electrochemical CO_(2)reduction and propose effective strategies to improve the reaction kinetics,to minimize the electrical energy losses,and to tune the selectivity of the catalysts for desired products,and then suggest future direction of research and development.
基金We acknowledge the support from the National Natural Science Foundation of China(21991153,21991150).
文摘Electrochemical reduction of CO_(2)(CO_(2)RR)coupled with renewable electrical energy is an attractive way of upgrading CO_(2)to value-added chemicals and closing the carbon cycle.However,CO_(2)RR electrocatalysts still suffer from high overpotential,and the complex reaction pathways of CO_(2)RR often lead to mixed products.Early research focuses on tuning the binding of reaction intermediates on electrocatalysts,and recent efforts have revealed that the design of electrolysis reactors is equally important for efficient and selective CO_(2)RR.In this review,we present an overview of recent advances and challenges toward achieving high activity and high selectivity in CO_(2)RR at ambient conditions,with a particular focus on the progress of CO_(2)RR electrocatalyst engineering and reactor design.Our discussion begins with three types of electrocatalysts for CO_(2)RR(noble metalbased,none-noble metal-based,and metal-free electrocatalysts),and then we examine systems-level strategies toward engineering specific components of the electrolyzer,including gas diffusion electrodes,electrolytes,and polymer electrolyte membranes.We close with future perspectives on catalyst development,in-situ/operando characterization,and electrolyzer performance evaluation in CO_(2)RR studies.
基金supported by the National Natural Science Foundation of China(22479048,22109044,22178099)the Natural Science Foundation of Shanghai+2 种基金China(22ZR1418500)the Start-up Funds from the East China University of Science and Technologythe Fundamental Research Funds for the Central Universities。
文摘Electrochemical CO_(2)reduction reaction(CO_(2)RR)is a promising technique to address the excess CO_(2)emissions for closing the global carbon cycle.However,challenges remain to break the trade-off between high Faradaic efficiencies and high current densities.Herein,we synthesize Ag nano-foams(Ag NFs)featuring sufficient gas channels by a facile wet-chemical method.It is revealed that the gaseous products can be rapidly released from Ag NFs with the presence of nanochannels,profiting from the exposure of active sites and their further access to CO_(2).COMSOL simulation verifies the uniform distribution of low-pressure drop and thus promotes local mass transfer within the catalyst layers.Benefiting from the improved transport features,the Ag NFs achieve excellent CO Faradaic efficiencies(FE_(CO)>90.9%)in a wide potential window(-0.5VRHE--1.2V_(RHE)),together with a high partial current density of 365.7 mA cm^(-2)at-1.2VRHE.This study provides insights into the rational regulation of gas and electrons within electrocatalysts for efficient CO_(2)-to-gas conversion.
基金supported by the National Key Research and Develop- ment Program of China ( 2021YFA1202500 )National Natural Science Foundation of China ( 21777045 )+3 种基金Guangdong Provincial Key Labora- tory of Soil and Groundwater Pollution Control ( 2023B1212060002 )Stable Support Plan Program of Shenzhen Natural Science Foundation ( 20231122110855002 )High level of special funds ( G03034K001 ) from SUSTechShenzhen Science and Technology Innovation Commit- tee ( KCXST20221021111208018 , JCYJ20241202125900002 ).
文摘Decentralized solutions for the low-cost and sustainable treatment of large-scale natural water bodies contaminated with organic pollutants are urgently needed.This study introduces a self-powered clean boat using a photovoltaic(PV)-driven electrochemical Fenton system,featuring a gas diffusion electrode(GDE)and a quasi-solid hydrogel electrolyte.This setup enables in-situ oxygen reduction in low-conductivity lake water,achieving a high H_(2)O_(2)production rate of 290±10 mg L^(-1)h^(-1).The hydrogel,containing Fe^(2+)/Fe^(3+)pairs,enriches ion concentration,enhances conductivity,and triggers the Fenton reaction to convert H_(2)O_(2)into·OH radicals for efficient antibiotic degradation.The boat achieved a 99.4%removal rate for tetracycline(TC)at 1 mg L^(-1)in contaminated water within 3 h,demonstrating over 98%removal efficiency for other common antibiotics.This system integrates clean energy use,H_(2)O_(2)production,Fenton reaction activation,and pollutant degradation,addressing the limitations of conventional electrochemical methods in low-conductivity waters.It offers a sustainable solution for decentralized water treatment in pilot-scale experiments with low unique energy consumption(0.43 kWh mg^(-1))by solar energy.
基金supported by the National Natural Science Foundation of China(52370033,31970106)CAS Key Laboratory of Environmental and Applied Microbiology&Environmental Microbiology Key Laboratory of Sichuan Province,Chengdu Institute of Biology,Chinese Academy of Sciences(KLCAS-2023-1).
文摘The demand for converting CO_(2)into fuels or chemicals is on the rise to achieve a carbon-efficient circular economy.Biohybrid CO_(2)electrolysis shows potential for increasing production rates and diversifying product spectra by combining electrocatalysts and microbial catalysts.However,it is important to note that utilizing a shared catholyte for biohybrid CO_(2)electrolysis has not demonstrated significant performance improvements to date.In this study,we developed a biohybrid CO_(2)electrolysis system utilizing a solid electrolyte operating in an external mode.The produced formic acid was extracted and used as an intermediate for microbial conversion.Impressively,the solid-electrolyte CO_(2)electrolysers obtained a remarkable total Faradic efficiency of 81.4%for formic acid production.In-situ mechanism studies unveiled metallic tin as the probable real active site,prompting further exploration of strategies to boost the activity and stability of electrocatalysts.In the bioconversion step,we achieved a noteworthy 8-day duration for generating bioelectricity,nearly 100%electron recovery for biomethane production,and 90.8%for acetate generation.Additionally,when ethanol was co-fed,a C_(6)specificity of 41.1%was observed for the generation of medium-chain fatty acids(MCFAs).This study presents groundbreaking experimental data that demonstrates the numerous advantages of utilizing hybrid systems as advanced synthesis techniques.
基金supported by the Natural Science Foundation of China(22178394,22376222,and 52404332)the Science and Technology Innovation Program of Hunan Province(2022RC3048 and 2023RC1012)+1 种基金Central South University Research Program of Advanced Interdisciplinary Studies(2023QYJC012)the Postdoctoral Fellowship Program of CPSF(GZB20240860)for financial support。
文摘Electrochemical CO_(2)reduction reaction(CO_(2)RR)on gas diffusion electrodes(GDEs)offers a promising route for carbon-neutral fuel production at commercially relevant current densities(J>200 mA cm^(-2))[1,2].However,under high-rate operation,GDE performance deteriorates due to mass transport limitations[3,4].First,local CO_(2)depletion near the catalyst surface intensifies the competing hydrogen evolution reaction(HER),diminishing the selectivity[5].
