This work investigates the transient performance and stability of CO_(2)/H_(2)O co-electrolysis in an air-free environment using a flat-tube solid oxide electrolysis cell(SOEC)stack.The results showed that the transie...This work investigates the transient performance and stability of CO_(2)/H_(2)O co-electrolysis in an air-free environment using a flat-tube solid oxide electrolysis cell(SOEC)stack.The results showed that the transient behavior of the stack with and without blowing gas into the air electrode is almost the same.With a current density of 0.67 A·cm^(-2)@750℃,the stack operated for over 200 h under co-electrolysis conditions without air blowing,and the voltage drop rate of the stack was approximately 0.203%/100 hours.Microstructure analysis revealed a significant loss of nickel particles and an apparent for-mation of an insulating phase strontium chromate(SrCrO4)on the surface of the current collection layer of the air electrode,which are identified as key factors contributing to the performance degradation of the stack.This study provides a reference for development of efficient fuel preparation technology based on SOEC stack in airless environments.展开更多
The performance of the fuel electrode in a solid oxide electrolysis cell(SOEC)is crucial to facilitating fuel gas electrolysis and is the key determinant of overall electrolysis efficiency.Nevertheless,the commerciali...The performance of the fuel electrode in a solid oxide electrolysis cell(SOEC)is crucial to facilitating fuel gas electrolysis and is the key determinant of overall electrolysis efficiency.Nevertheless,the commercialization of integrated CO_(2)-H_(2)O electrolysis in SOEC remains constrained by suboptimal catalytic efficiency and long-term stability limitations inherent to conventional fuel electrode architec-tures.A novel high-entropy Sr_(2)FeTi_(0.2)Cr_(0.2)Mn_(0.2)Mo_(0.2)Co_(0.2)O_(6−δ)(SFTCMMC)was proposed as a prospective electrode material of co-elec-trolysis in this work.The physicochemical properties and electrochemical performance in the co-electrolysis reaction were investigated.Full cell is capable of electrolyzing H_(2)O and CO_(2)effectively with an applied voltage.The effects of temperature,H_(2)O and CO_(2)concentra-tions,and applied voltage on the electrochemical performance of Sc_(0.18)Zr_(0.82)O_(2−δ)(SSZ)-electrolyte supported SOEC were investigated by varying the operating conditions.The SOEC obtains a favorable electrolysis current density of 1.47 A·cm^(−2)under co-electrolysis condi-tion at 850℃ with 1.5 V.Furthermore,the cell maintains stable performance for 150 h at 1.3 V,and throughout this period,no carbon de-position is detected.The promising findings suggest that the high-entropy SFTCMMC perovskite is a viable fuel electrode candidate for efficient H_(2)O/CO_(2)co-electrolysis.展开更多
Co-electrolysis of CO2and H2O using high-temperature solid oxide electrolysis cells(SOECs) into valuable chemicals has attracted great attentions recently due to the high conversion and energy efficiency,which provide...Co-electrolysis of CO2and H2O using high-temperature solid oxide electrolysis cells(SOECs) into valuable chemicals has attracted great attentions recently due to the high conversion and energy efficiency,which provides opportunities of reducing CO2emission, mitigating global warming and storing intermittent renewable energies. A single SOEC typically consists of an ion conducting electrolyte, an anode and a cathode where the co-electrolysis reaction takes place. The high operating temperature and difficult activated carbon-oxygen double-bond of CO2put forward strict requirements for SOEC cathode. Great efforts are being devoted to develop suitable cathode materials with high catalytic activity and excellent long-term stability for CO2/H2O electro-reduction. The so far cathode material development is the key point of this review and alternative strategies of high-performance cathode material preparation is proposed. Understanding the mechanism of CO2/H2O electro-reduction is beneficial to highly active cathode design and optimization. Thus the possible reaction mechanism is also discussed. Especially, a method in combination with electrochemical impedance spectroscopy(EIS) measurement, distribution functions of relaxation times(DRT) calculation, complex nonlinear least square(CNLS) fitting and operando ambient pressure X-ray photoelectron spectroscopy(APXPS) characterization is introduced to correctly disclose the reaction mechanism of CO2/H2O co-electrolysis. Finally, different reaction modes of the CO2/H2O coelectrolysis in SOECs are summarized to offer new strategies to enhance the CO2conversion. Otherwise,developing SOECs operating at 300-600 °C can integrate the electrochemical reduction and the Fischer-Tropsch reaction to convert the CO2/H2O into more valuable chemicals, which will be a new research direction in the future.展开更多
A solid oxide electrolysis cell(SOEC) is an environmental-friendly device which can convert electric energy into chemical energy with high efficiency. In this paper,the progress on structure and operational principle ...A solid oxide electrolysis cell(SOEC) is an environmental-friendly device which can convert electric energy into chemical energy with high efficiency. In this paper,the progress on structure and operational principle of an SOEC for co-electrolyzing H2O and CO2to generate syngas was reviewed. The recent development of high temperature H2O/CO2co-electrolysis from solid oxide single electrolysis cell was introduced. Also investigated was H2O/CO2co-electrolysis research using hydrogen electrode-supported nickel(Ni)-yttria-stabilized zirconia(YSZ)/YSZ/Sr-doped LaMnO3(LSM)-YSZ cells in our group. With 50 % H2O,15.6 % H2and 34.4 % CO2inlet gas to Ni- YSZ electrode,polarization curves(I- U curves) and electrochemical impedance spectra(EIS) were measured at 800 ℃ and 900 ℃. Long-term durability of electrolysis was carried out with the same inlet gas at 900 ℃ and 0.2 A/cm2. In addition,the improvement of structure and development of novel materials for increasing the electrolysis efficiency of SOECs were put forward as well.展开更多
In the context of carbon neutrality,conversion of CO_(2)into CO is an effective way for negative carbon emission.Electrochemical reduction is a novel developed pathway,among which,solid oxide co-electrolysis technolog...In the context of carbon neutrality,conversion of CO_(2)into CO is an effective way for negative carbon emission.Electrochemical reduction is a novel developed pathway,among which,solid oxide co-electrolysis technology is promising for its high efficiency and low electricity demand.Researches concerning the large-size cell and stack of application level are important.This review,targeting at the not yet fully understood reaction mechanism and the most concerning issue of durability,details the reported factors playing important roles in the reaction mechanism and durability of co-electrolysis.It is found that the operating conditions such as inlet mixtures and applied current significantly affect the reaction mechanism of co-electrolysis and the experiments on button cells can not reflect the real reaction mechanism on industrial-size cells.Besides,the durability test of large-size single cells and stacks at high current with high conversion rate and the potential of solid oxide co-electrolysis combing with intermittent renewable energy are also reviewed and demonstrated.Finally,an outlook for future exploration is also offered.展开更多
Current major electrocatalytic reactions,such as hydrogen evolution reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction,focus on single-target chemical production,which suffers from strong compe...Current major electrocatalytic reactions,such as hydrogen evolution reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction,focus on single-target chemical production,which suffers from strong competitive reactions at the same electrodes and/or high energy barrier reactions at the counterpart electrodes.The co-electrolysis of more than one kind,typically two kinds,of chemical precursors in one electrolytic system is therefore a highly attractive strategy for both energy input reduction and concurrent production of double value-added chemicals.Exciting progress has been achieved in this area recently,and a timely review on this specific topic will be highly desired.In this review,the reported co-electrolysis systems are classified into four categories:(1)agent sacrificing at one electrode promoting electrochemical precursor conversion at the other;(2)parallel electrochemical precursor conversions,i.e.,electrosyntheses,simultaneously at both sides;(3)electrochemical conversions of two precursors at both sides into one/the same product;(4)double/multiple electrochemical conversions at one side.The current challenges and future opportunities of co-electrolysis toward high value-added products are discussed at the end.展开更多
The rising level of CO_(2) concentration in the atmosphere poses major threats to the global climate and environment.Various technologies have been developed to mitigate its negative effects through nonconversion and ...The rising level of CO_(2) concentration in the atmosphere poses major threats to the global climate and environment.Various technologies have been developed to mitigate its negative effects through nonconversion and conversion routes.Particularly,solid oxide electrolysis cells(SOECs),as a promising technology with the highest energy efficiency,have garnered considerable attention for their effectiveness to electrochemically convert CO_(2) into high-value fuels.However,the insufficient catalytic activity,poor longterm stability,and high costs have significantly hindered the industrial-scale application of SOECs.To this end,substantial efforts,with an emphasis on the smart design of targeting electrode materials for specific applications have been devoted to advancing the electrosynthesis of high-value fuels from CO_(2) in various SOECs,but there still lacks a critical and comprehensive review in-depth discussing the fundamentals,and summarizing the latest advances in various applications and electrode materials for electrochemically converting CO_(2) to high-value fuels in SOECs.This review thus aims to fill this gap by focusing on the fundamentals(i.e.,SOEC working principles,thermodynamics,kinetics and representative evaluation parameters),specific applications(i.e.,pure CO_(2) electrolysis,CO_(2)-H_(2)O co-electrolysis,fuel-assisted CO_(2) conversion),and material selection criteria(i.e.,cathodic materials for CO_(2) conversion,and anodic materials for fuel-assisted CO_(2) conversion).In addition,the challenges that this technology is currently facing,and our perspectives on electrochemical CO_(2) conversion in SOECs are proposed to guide the smart design of high-performance electrocatalysts and future industrial-scale application of SOECs for electrosynthesizing high-value fuels from CO_(2).展开更多
Developing energy-efficient nitrite-to-ammonia(NO_(2)RR)conversion technologies while simultaneously enabling the electrochemical upcycling of waste polyethylene terephthalate(PET)plastics into highvalue-added chemica...Developing energy-efficient nitrite-to-ammonia(NO_(2)RR)conversion technologies while simultaneously enabling the electrochemical upcycling of waste polyethylene terephthalate(PET)plastics into highvalue-added chemicals is of great significance.Herein,an atomic oxygen vacancy(V_(o))engineering is developed to optimize the catalytic performance of V_(o2)-Co(OH)F nanoarray towards the NO_(2)RR and PET-derived ethylene glycol oxidation reaction(EGOR).The optimal V_(o2)-Co(OH)F achieves an ultralow operating potential of -0.03 V vs.RHE at -100 mA cm^(-2)and a remarkable NH_(3)Faradaic efficiency(FE)of 98.4% at -0.2 V vs.RHE for NO_(2)RR,and a high formate FE of 98.03% for EGOR.Operando spectroscopic analysis and theoretical calculations revealed that oxygen vacancies play a crucial role in optimizing the electronic structure of V_(o2)-Co(OH)F,modulating the adsorption free energies of key reaction intermediates,and lowering the reaction energy barrier,thereby enhancing its overall catalytic performance.Remarkably,the V_(o2)-Co(OH)F-based NO_(2)RR||EGOR electrolyzer realized high NH_(3)and formate yield rates of 33.9 and 44.9 mg h^(-1)cm^(-2)at 1.7 V,respectively,while demonstrating outstanding long-term stability over 100 h.This work provides valuable insights into the rational design of advanced electrocatalysts for co-electrolysis systems.展开更多
The inefficiency of water splitting is mainly due to the sluggish anodic water oxidation reaction. Replacing water oxidation with thermodynamically more favorable selective methanol oxidation reaction and developing r...The inefficiency of water splitting is mainly due to the sluggish anodic water oxidation reaction. Replacing water oxidation with thermodynamically more favorable selective methanol oxidation reaction and developing robust bifunctional electrocatalysts are of great significance. Herein, a hierarchical heteronanostructure with Ni–Co layered double hydroxide(LDH) ultrathin nanosheets coated on cobalt phosphide nanosheets arrays(CoxP@NiCo-LDH) are fabricated and used for co-electrolysis of methanol/water to co-produce value-added formate and hydrogen with saving energy. Benefiting from the fast charge transfer introduced by phosphide nanoarrays, the synergy in nanosheets catalysts with hetero-interface,CoxP@NiCo-LDH/Ni foam(NF) exhibits superior electrocatalytic performance(10 mA cm-2@ 1.24 V and-0.10 V for methanol selective oxidation and hydrogen evolution reaction, respectively). Furthermore,CoxP@NiCo-LDH/NF-based symmetric two-electrode electrolyzer drives a current density of 10 m A cm-2 with a low cell voltage of only 1.43 V and the Faradaic efficiency towards the generation of formate and H2 are close to 100% in the tested range of current density(from 40 to 200 m A cm-2). This work highlights the positive effect of hetero-interaction in the design of more efficient eletrocatalysts and might guide the way towards facile upgrading of alcohols and energy-saving electrolytic H2 co-generation.展开更多
The overall energy efficiency(EE)is critical for commercializing promising electrochemical technologies,such as the carbon dioxide reduction reaction(CO_(2)RR).Despite the rapid development of advanced catalysts and r...The overall energy efficiency(EE)is critical for commercializing promising electrochemical technologies,such as the carbon dioxide reduction reaction(CO_(2)RR).Despite the rapid development of advanced catalysts and reactors for CO_(2)RR,its commercial potential is still hindered by the sluggish oxygen evolution reaction(OER),which causes high cell voltages and low EEs.Herein,we developed a NiOOH@Ni_(3)S_(2)catalyst on the surface of nickel foam(NF)via an electrochemical surface reconstruction strategy.We observed that the oxidation of glycerol(GLY)to formate(FA)is more thermodynamically favorable than the OER on the developed NiOOH@Ni_(3)S_(2)/NF catalysts.The Ni^(2+)/Ni^(3+)redox couples within the NiOOH@Ni_(3)S_(2)heterojunction enhance the charge transfer kinetics between the active sites and adsorbed reaction intermediates,facilitating the highly selective and active generation of FA from GLY oxidation reaction(GOR),with a remarkable Faradaic efficiency(FE)of 94%achieved at 100 mA·cm^(−2).Comprehensive mechanistic studies identified that the reaction pathway towards FA generation starts from glyceraldehyde intermediates,and glycolate was considered as the key species.Moreover,benefiting from the efficient conversion of CO_(2)to FA on bismuth nanosheets,the GOR//CO_(2)RR paired electrolysis system realizes a remarkable overall FE of ca.190%for FA co-production at 160 mA·cm^(−2)(cathodic FE:91.25%and anodic FE:98.70%).This proceeds at a cell voltage of ca.2.32 V,which is ca.0.85 V lower than that of OER-assisted CO_(2)RR system at the same current density.This work provides new insights for co-upgrading CO_(2)and biomass to value-added chemicals.展开更多
Electrochemical urea synthesis from CO_(2)and NO(EUCN)offers a promising route for sustainable urea production,whereas it still suffers from low C-N coupling efficiency and poor selectivity.Herein,atomically dispersed...Electrochemical urea synthesis from CO_(2)and NO(EUCN)offers a promising route for sustainable urea production,whereas it still suffers from low C-N coupling efficiency and poor selectivity.Herein,atomically dispersed p-block Bi catalyst is explored for highly active and selective EUCN.Theoretical calculations and in situ spectroscopic analyses reveal a unique*CO-mediated C-N coupling mechanism,where isolated Bi sites facilitate CO_(2)reduction for*CO formation and enrichment,while*CO-enriched microenvironment boosts subsequent C-N coupling of*CO and*NO to*CONO,a critical C-N intermediate for urea generation,while simultaneously suppressing the competing side reactions.Notably,by pairing cathodic EUCN with anodic glycerol oxidation in a membrane electrode assembly electrolyzer,we achieve a record-high performance with urea yield rate of 86.5 mmol·h^(-1)·g^(-1)and Faradaic efficiency of 52.1%,as well as the outstanding stability for over 200 h electrolysis.展开更多
The co-electrolysis of CO_(2)and H_(2)O through solid oxide electrolysis cells(SOECs),powered by renewable energy sources,offers a promising pathway to achieving carbon neutrality in the chemical industry.However,the ...The co-electrolysis of CO_(2)and H_(2)O through solid oxide electrolysis cells(SOECs),powered by renewable energy sources,offers a promising pathway to achieving carbon neutrality in the chemical industry.However,the inherent intermittency of renewable energy generation,such as wind power,leads to unstable power input for electrolysis.This variability induces significant thermal stress in SOECs,potentially causing cracks or even system failure.To address this challenge,a hybrid deep learning architecture(HDLA)was developed to control the temperature gradient of SOECs.The architecture combines a convolutional neural network(CNN)and a long short-term memory(LSTM)model for wind power prediction,a multi-physics model for temperature gradient simulation,and a linear neural network regression model to simulate the temperature distribution in SOECs.Training and verification are conducted using 16 datasets from an industrial wind farm.The results demonstrate that the application of HDLA successfully reduce the temperature gradient of SOECs from±20℃ to±5℃.Additionally,the potential wind power utilization achieved near-complete wind power utilization,increasing from 18%to 99%.This real-time control strategy,which optimizes flow regulation,effectively mitigates thermal stress,thereby extending the lifespan of SOECs and ensuring continuous carbon reduction,efficient conversion,and utilization.展开更多
Solid oxide electrolysis cell(SOEC)is a promising water electrolysis technology that produces hydrogen or syngas through water electrolysis or water and carbon dioxide co-electrolysis.Green hydrogen or syngas can be p...Solid oxide electrolysis cell(SOEC)is a promising water electrolysis technology that produces hydrogen or syngas through water electrolysis or water and carbon dioxide co-electrolysis.Green hydrogen or syngas can be produced by SOEC with renewable energy.Thus,SOEC has attracted continuous attention in recent years for the urgency of developing environmentally friendly energy sources and achieving carbon neutrality.Focusing on 1276 related articles retrieved from the Web of Science(WoS)database,the historical development of SOECs are depicted from 1983 to 2023 in this paper.The co-occurrence networks of the countries,source journals,and author keywords are generated.Moreover,three main clusters showing different content of the SOEC research are identified and analyzed.Furthermore,the scientometric analysis and the content of the high-cited articles of the research of different topics of SOECs:fuel electrode,air electrode,electrolyte,co-electrolysis,proton-conducting SOECs,and the modeling of SOECs are also presented.The results show that co-electrolysis and proton-conducting SOECs are two popular directions in the study of SOECs.This paper provides a straightforward reference for researchers interested in the field of SOEC research,helping them navigate the landscape of this area of study,locate potential partners,secure funding,discover influential scholars,identify leading countries,and access key research publications.展开更多
基金co-supported by the National Key R&D Program of China(No.2022YFB4002203)Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(No.LBMHY24B060003)Ningbo Key R&D Project(No.2023Z155).
文摘This work investigates the transient performance and stability of CO_(2)/H_(2)O co-electrolysis in an air-free environment using a flat-tube solid oxide electrolysis cell(SOEC)stack.The results showed that the transient behavior of the stack with and without blowing gas into the air electrode is almost the same.With a current density of 0.67 A·cm^(-2)@750℃,the stack operated for over 200 h under co-electrolysis conditions without air blowing,and the voltage drop rate of the stack was approximately 0.203%/100 hours.Microstructure analysis revealed a significant loss of nickel particles and an apparent for-mation of an insulating phase strontium chromate(SrCrO4)on the surface of the current collection layer of the air electrode,which are identified as key factors contributing to the performance degradation of the stack.This study provides a reference for development of efficient fuel preparation technology based on SOEC stack in airless environments.
基金supported by the National Natural Science Foundation of China(No.52472270)the Basic Research Program of Jiangsu(No.BK20243049)the Fundamental Research Funds for the Central Universities(No.2023KYJD1010).
文摘The performance of the fuel electrode in a solid oxide electrolysis cell(SOEC)is crucial to facilitating fuel gas electrolysis and is the key determinant of overall electrolysis efficiency.Nevertheless,the commercialization of integrated CO_(2)-H_(2)O electrolysis in SOEC remains constrained by suboptimal catalytic efficiency and long-term stability limitations inherent to conventional fuel electrode architec-tures.A novel high-entropy Sr_(2)FeTi_(0.2)Cr_(0.2)Mn_(0.2)Mo_(0.2)Co_(0.2)O_(6−δ)(SFTCMMC)was proposed as a prospective electrode material of co-elec-trolysis in this work.The physicochemical properties and electrochemical performance in the co-electrolysis reaction were investigated.Full cell is capable of electrolyzing H_(2)O and CO_(2)effectively with an applied voltage.The effects of temperature,H_(2)O and CO_(2)concentra-tions,and applied voltage on the electrochemical performance of Sc_(0.18)Zr_(0.82)O_(2−δ)(SSZ)-electrolyte supported SOEC were investigated by varying the operating conditions.The SOEC obtains a favorable electrolysis current density of 1.47 A·cm^(−2)under co-electrolysis condi-tion at 850℃ with 1.5 V.Furthermore,the cell maintains stable performance for 150 h at 1.3 V,and throughout this period,no carbon de-position is detected.The promising findings suggest that the high-entropy SFTCMMC perovskite is a viable fuel electrode candidate for efficient H_(2)O/CO_(2)co-electrolysis.
基金financial support from the Ministry of Science and Technology of China (Grants 2016YFB0600901 and 2013CB933100)the National Natural Science Foundation of China (Grants 21573222 and 91545202)+2 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB17020200)China Postdoctoral Science Foundation (NO. 2016M600220)the financial support from CAS Youth Innovation Promotion
文摘Co-electrolysis of CO2and H2O using high-temperature solid oxide electrolysis cells(SOECs) into valuable chemicals has attracted great attentions recently due to the high conversion and energy efficiency,which provides opportunities of reducing CO2emission, mitigating global warming and storing intermittent renewable energies. A single SOEC typically consists of an ion conducting electrolyte, an anode and a cathode where the co-electrolysis reaction takes place. The high operating temperature and difficult activated carbon-oxygen double-bond of CO2put forward strict requirements for SOEC cathode. Great efforts are being devoted to develop suitable cathode materials with high catalytic activity and excellent long-term stability for CO2/H2O electro-reduction. The so far cathode material development is the key point of this review and alternative strategies of high-performance cathode material preparation is proposed. Understanding the mechanism of CO2/H2O electro-reduction is beneficial to highly active cathode design and optimization. Thus the possible reaction mechanism is also discussed. Especially, a method in combination with electrochemical impedance spectroscopy(EIS) measurement, distribution functions of relaxation times(DRT) calculation, complex nonlinear least square(CNLS) fitting and operando ambient pressure X-ray photoelectron spectroscopy(APXPS) characterization is introduced to correctly disclose the reaction mechanism of CO2/H2O co-electrolysis. Finally, different reaction modes of the CO2/H2O coelectrolysis in SOECs are summarized to offer new strategies to enhance the CO2conversion. Otherwise,developing SOECs operating at 300-600 °C can integrate the electrochemical reduction and the Fischer-Tropsch reaction to convert the CO2/H2O into more valuable chemicals, which will be a new research direction in the future.
文摘A solid oxide electrolysis cell(SOEC) is an environmental-friendly device which can convert electric energy into chemical energy with high efficiency. In this paper,the progress on structure and operational principle of an SOEC for co-electrolyzing H2O and CO2to generate syngas was reviewed. The recent development of high temperature H2O/CO2co-electrolysis from solid oxide single electrolysis cell was introduced. Also investigated was H2O/CO2co-electrolysis research using hydrogen electrode-supported nickel(Ni)-yttria-stabilized zirconia(YSZ)/YSZ/Sr-doped LaMnO3(LSM)-YSZ cells in our group. With 50 % H2O,15.6 % H2and 34.4 % CO2inlet gas to Ni- YSZ electrode,polarization curves(I- U curves) and electrochemical impedance spectra(EIS) were measured at 800 ℃ and 900 ℃. Long-term durability of electrolysis was carried out with the same inlet gas at 900 ℃ and 0.2 A/cm2. In addition,the improvement of structure and development of novel materials for increasing the electrolysis efficiency of SOECs were put forward as well.
基金supported by the National Natural Science Foundation of China(No.5201101243)Project of State Key Laboratory of Power System and Generation Equipment(No.SKLD22M06)the Institute for Guo Qiang(No.2020GQG1003).
文摘In the context of carbon neutrality,conversion of CO_(2)into CO is an effective way for negative carbon emission.Electrochemical reduction is a novel developed pathway,among which,solid oxide co-electrolysis technology is promising for its high efficiency and low electricity demand.Researches concerning the large-size cell and stack of application level are important.This review,targeting at the not yet fully understood reaction mechanism and the most concerning issue of durability,details the reported factors playing important roles in the reaction mechanism and durability of co-electrolysis.It is found that the operating conditions such as inlet mixtures and applied current significantly affect the reaction mechanism of co-electrolysis and the experiments on button cells can not reflect the real reaction mechanism on industrial-size cells.Besides,the durability test of large-size single cells and stacks at high current with high conversion rate and the potential of solid oxide co-electrolysis combing with intermittent renewable energy are also reviewed and demonstrated.Finally,an outlook for future exploration is also offered.
基金supported by the Natural Science Foundation of Shanghai(21ZR1418700)China Postdoctoral Science Foundation funded project(2020T130193)the Fundamental Research Funds for the Central Universities.
文摘Current major electrocatalytic reactions,such as hydrogen evolution reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction,focus on single-target chemical production,which suffers from strong competitive reactions at the same electrodes and/or high energy barrier reactions at the counterpart electrodes.The co-electrolysis of more than one kind,typically two kinds,of chemical precursors in one electrolytic system is therefore a highly attractive strategy for both energy input reduction and concurrent production of double value-added chemicals.Exciting progress has been achieved in this area recently,and a timely review on this specific topic will be highly desired.In this review,the reported co-electrolysis systems are classified into four categories:(1)agent sacrificing at one electrode promoting electrochemical precursor conversion at the other;(2)parallel electrochemical precursor conversions,i.e.,electrosyntheses,simultaneously at both sides;(3)electrochemical conversions of two precursors at both sides into one/the same product;(4)double/multiple electrochemical conversions at one side.The current challenges and future opportunities of co-electrolysis toward high value-added products are discussed at the end.
基金supported by the Pilot Group Program of the Research Fund for International Senior Scientists(No.22350710789)the National Natural Science Foundation of China(NSFC,No.22109182)+2 种基金the Natural Science Foundation of Hunan Province,China(No.2022JJ30684)the Start-up Funding of Central South University(No.206030104)supported in part by the High-Performance Computing Center of Central South University。
文摘The rising level of CO_(2) concentration in the atmosphere poses major threats to the global climate and environment.Various technologies have been developed to mitigate its negative effects through nonconversion and conversion routes.Particularly,solid oxide electrolysis cells(SOECs),as a promising technology with the highest energy efficiency,have garnered considerable attention for their effectiveness to electrochemically convert CO_(2) into high-value fuels.However,the insufficient catalytic activity,poor longterm stability,and high costs have significantly hindered the industrial-scale application of SOECs.To this end,substantial efforts,with an emphasis on the smart design of targeting electrode materials for specific applications have been devoted to advancing the electrosynthesis of high-value fuels from CO_(2) in various SOECs,but there still lacks a critical and comprehensive review in-depth discussing the fundamentals,and summarizing the latest advances in various applications and electrode materials for electrochemically converting CO_(2) to high-value fuels in SOECs.This review thus aims to fill this gap by focusing on the fundamentals(i.e.,SOEC working principles,thermodynamics,kinetics and representative evaluation parameters),specific applications(i.e.,pure CO_(2) electrolysis,CO_(2)-H_(2)O co-electrolysis,fuel-assisted CO_(2) conversion),and material selection criteria(i.e.,cathodic materials for CO_(2) conversion,and anodic materials for fuel-assisted CO_(2) conversion).In addition,the challenges that this technology is currently facing,and our perspectives on electrochemical CO_(2) conversion in SOECs are proposed to guide the smart design of high-performance electrocatalysts and future industrial-scale application of SOECs for electrosynthesizing high-value fuels from CO_(2).
基金financially supported by the National Natural Science Foundation of China(22205205)the Fundamental Research Funds of Zhejiang Sci-Tech University(ZSTU,25262157Y)the staff of beamline BL11B and BL13SSW at Shanghai Synchrotron Radiation Facility for experimental support。
文摘Developing energy-efficient nitrite-to-ammonia(NO_(2)RR)conversion technologies while simultaneously enabling the electrochemical upcycling of waste polyethylene terephthalate(PET)plastics into highvalue-added chemicals is of great significance.Herein,an atomic oxygen vacancy(V_(o))engineering is developed to optimize the catalytic performance of V_(o2)-Co(OH)F nanoarray towards the NO_(2)RR and PET-derived ethylene glycol oxidation reaction(EGOR).The optimal V_(o2)-Co(OH)F achieves an ultralow operating potential of -0.03 V vs.RHE at -100 mA cm^(-2)and a remarkable NH_(3)Faradaic efficiency(FE)of 98.4% at -0.2 V vs.RHE for NO_(2)RR,and a high formate FE of 98.03% for EGOR.Operando spectroscopic analysis and theoretical calculations revealed that oxygen vacancies play a crucial role in optimizing the electronic structure of V_(o2)-Co(OH)F,modulating the adsorption free energies of key reaction intermediates,and lowering the reaction energy barrier,thereby enhancing its overall catalytic performance.Remarkably,the V_(o2)-Co(OH)F-based NO_(2)RR||EGOR electrolyzer realized high NH_(3)and formate yield rates of 33.9 and 44.9 mg h^(-1)cm^(-2)at 1.7 V,respectively,while demonstrating outstanding long-term stability over 100 h.This work provides valuable insights into the rational design of advanced electrocatalysts for co-electrolysis systems.
基金financially supported by the National Natural Science Foundation of China(Nos.21975163 and 21905181)。
文摘The inefficiency of water splitting is mainly due to the sluggish anodic water oxidation reaction. Replacing water oxidation with thermodynamically more favorable selective methanol oxidation reaction and developing robust bifunctional electrocatalysts are of great significance. Herein, a hierarchical heteronanostructure with Ni–Co layered double hydroxide(LDH) ultrathin nanosheets coated on cobalt phosphide nanosheets arrays(CoxP@NiCo-LDH) are fabricated and used for co-electrolysis of methanol/water to co-produce value-added formate and hydrogen with saving energy. Benefiting from the fast charge transfer introduced by phosphide nanoarrays, the synergy in nanosheets catalysts with hetero-interface,CoxP@NiCo-LDH/Ni foam(NF) exhibits superior electrocatalytic performance(10 mA cm-2@ 1.24 V and-0.10 V for methanol selective oxidation and hydrogen evolution reaction, respectively). Furthermore,CoxP@NiCo-LDH/NF-based symmetric two-electrode electrolyzer drives a current density of 10 m A cm-2 with a low cell voltage of only 1.43 V and the Faradaic efficiency towards the generation of formate and H2 are close to 100% in the tested range of current density(from 40 to 200 m A cm-2). This work highlights the positive effect of hetero-interaction in the design of more efficient eletrocatalysts and might guide the way towards facile upgrading of alcohols and energy-saving electrolytic H2 co-generation.
基金supported by the National Natural Science Foundation of China(Nos.22105133,22275205,and 52273269)Natural Science Foundation of Sichuan Province of China(No.2022NSFSC0617)+3 种基金Sichuan Science and Technology Program(No.2023YFH0027)Central Guidance for Local Science and Technology Development Fund Projects(No.2024ZYD0099)China Scholarship Council,Science and Technology Project of the State Administration for Market Regulation(No.2022MK111)Fundamental Research Funds for the Central Universities(No.1082204112I96).
文摘The overall energy efficiency(EE)is critical for commercializing promising electrochemical technologies,such as the carbon dioxide reduction reaction(CO_(2)RR).Despite the rapid development of advanced catalysts and reactors for CO_(2)RR,its commercial potential is still hindered by the sluggish oxygen evolution reaction(OER),which causes high cell voltages and low EEs.Herein,we developed a NiOOH@Ni_(3)S_(2)catalyst on the surface of nickel foam(NF)via an electrochemical surface reconstruction strategy.We observed that the oxidation of glycerol(GLY)to formate(FA)is more thermodynamically favorable than the OER on the developed NiOOH@Ni_(3)S_(2)/NF catalysts.The Ni^(2+)/Ni^(3+)redox couples within the NiOOH@Ni_(3)S_(2)heterojunction enhance the charge transfer kinetics between the active sites and adsorbed reaction intermediates,facilitating the highly selective and active generation of FA from GLY oxidation reaction(GOR),with a remarkable Faradaic efficiency(FE)of 94%achieved at 100 mA·cm^(−2).Comprehensive mechanistic studies identified that the reaction pathway towards FA generation starts from glyceraldehyde intermediates,and glycolate was considered as the key species.Moreover,benefiting from the efficient conversion of CO_(2)to FA on bismuth nanosheets,the GOR//CO_(2)RR paired electrolysis system realizes a remarkable overall FE of ca.190%for FA co-production at 160 mA·cm^(−2)(cathodic FE:91.25%and anodic FE:98.70%).This proceeds at a cell voltage of ca.2.32 V,which is ca.0.85 V lower than that of OER-assisted CO_(2)RR system at the same current density.This work provides new insights for co-upgrading CO_(2)and biomass to value-added chemicals.
基金supported by the National Natural Science Foundation of China(No.52561042)Gansu Province Key Talent Project(2025RCXM008).
文摘Electrochemical urea synthesis from CO_(2)and NO(EUCN)offers a promising route for sustainable urea production,whereas it still suffers from low C-N coupling efficiency and poor selectivity.Herein,atomically dispersed p-block Bi catalyst is explored for highly active and selective EUCN.Theoretical calculations and in situ spectroscopic analyses reveal a unique*CO-mediated C-N coupling mechanism,where isolated Bi sites facilitate CO_(2)reduction for*CO formation and enrichment,while*CO-enriched microenvironment boosts subsequent C-N coupling of*CO and*NO to*CONO,a critical C-N intermediate for urea generation,while simultaneously suppressing the competing side reactions.Notably,by pairing cathodic EUCN with anodic glycerol oxidation in a membrane electrode assembly electrolyzer,we achieve a record-high performance with urea yield rate of 86.5 mmol·h^(-1)·g^(-1)and Faradaic efficiency of 52.1%,as well as the outstanding stability for over 200 h electrolysis.
基金The authors would like to acknowledge the financial support from the National Key Research and Development Program of China(No.2022YFB4500500)the National Natural Science Foundation of China(No.22250710676).
文摘The co-electrolysis of CO_(2)and H_(2)O through solid oxide electrolysis cells(SOECs),powered by renewable energy sources,offers a promising pathway to achieving carbon neutrality in the chemical industry.However,the inherent intermittency of renewable energy generation,such as wind power,leads to unstable power input for electrolysis.This variability induces significant thermal stress in SOECs,potentially causing cracks or even system failure.To address this challenge,a hybrid deep learning architecture(HDLA)was developed to control the temperature gradient of SOECs.The architecture combines a convolutional neural network(CNN)and a long short-term memory(LSTM)model for wind power prediction,a multi-physics model for temperature gradient simulation,and a linear neural network regression model to simulate the temperature distribution in SOECs.Training and verification are conducted using 16 datasets from an industrial wind farm.The results demonstrate that the application of HDLA successfully reduce the temperature gradient of SOECs from±20℃ to±5℃.Additionally,the potential wind power utilization achieved near-complete wind power utilization,increasing from 18%to 99%.This real-time control strategy,which optimizes flow regulation,effectively mitigates thermal stress,thereby extending the lifespan of SOECs and ensuring continuous carbon reduction,efficient conversion,and utilization.
基金supported by the National Natural Science Foundation of China(Grant Nos.52102226 and 11932005)the Department of Education of Guangdong Province,China(Grant Nos.2021KCXTD006 and 2021KQNCX272)+1 种基金the Science,Technology and Innovation Commission of Shenzhen Municipality,China(Grant Nos.GJHZ20220913143009017,JCYJ20210324120404013,and GXWD20220811165757005)the Development and Reform Commission of Shenzhen Municipality,China(Grant No.XMHT20220103004).
文摘Solid oxide electrolysis cell(SOEC)is a promising water electrolysis technology that produces hydrogen or syngas through water electrolysis or water and carbon dioxide co-electrolysis.Green hydrogen or syngas can be produced by SOEC with renewable energy.Thus,SOEC has attracted continuous attention in recent years for the urgency of developing environmentally friendly energy sources and achieving carbon neutrality.Focusing on 1276 related articles retrieved from the Web of Science(WoS)database,the historical development of SOECs are depicted from 1983 to 2023 in this paper.The co-occurrence networks of the countries,source journals,and author keywords are generated.Moreover,three main clusters showing different content of the SOEC research are identified and analyzed.Furthermore,the scientometric analysis and the content of the high-cited articles of the research of different topics of SOECs:fuel electrode,air electrode,electrolyte,co-electrolysis,proton-conducting SOECs,and the modeling of SOECs are also presented.The results show that co-electrolysis and proton-conducting SOECs are two popular directions in the study of SOECs.This paper provides a straightforward reference for researchers interested in the field of SOEC research,helping them navigate the landscape of this area of study,locate potential partners,secure funding,discover influential scholars,identify leading countries,and access key research publications.
