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
Solid oxide electrolysis cells(SOECs)provide a promising way for converting renewable energy into chemical fuels.Traditionally,NiO/CGO(nickel-gadolinium doped ceria)cermet has shown its excellent properties in ionic a...Solid oxide electrolysis cells(SOECs)provide a promising way for converting renewable energy into chemical fuels.Traditionally,NiO/CGO(nickel-gadolinium doped ceria)cermet has shown its excellent properties in ionic and electronic conductivity under reducing conditions.Herein,we developed a novel 1D NiO/CGO cathode through a cerium metal-organic framework(MOF)derived process.The cathode’s 1D nanostructure integrated with a microchannel scaffold facilitates enhanced mass transport,providing vertically aligned pathways for CO_(2)and H_(2)O diffusion.Additionally,the 1D framework increases the number of interfacial sites and reduces ion diffusion distances,thereby simplifying electron/ion transport.Consequently,this advanced cathode achieved a significant breakthrough in SOEC performance,maintaining efficient CO_(2)and H_(2)O electrolysis at an extraordinary current density of 1.41 A/cm^(2)at 1.5 V and excellent stability over 24 h at 850℃.The enhanced performance of this newly developed cathode not only achieves a remarkable 100%improvement compared to those of NiO/CGO cathodes with varying geometrical configurations but also surpasses those of commercial NiO/CGO catalysts by an outstanding 40%when tested under identical conditions.The development of the 1D NiO/CGO enhances the efficiency and durability of ceramic cathodes for CO_(2)and H_(2)O co-electrolysis in SOECs and improves the scalability and effectiveness of SOECs in renewable energy applications.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
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
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
Gold, as the common current collector in solid oxide electrolysis cell(SOEC), is traditionally considered to be inert for oxygen evolution reaction at the anode of SOEC. Herein, gold nanoparticles were loaded onto con...Gold, as the common current collector in solid oxide electrolysis cell(SOEC), is traditionally considered to be inert for oxygen evolution reaction at the anode of SOEC. Herein, gold nanoparticles were loaded onto conventional strontium doped lanthanum manganite-yttria stabilized zirconia(LSM-YSZ) anode, which evidently improved the performance of oxygen evolution reaction at 800 °C. The current densities at 1.2 V and 1.4 V increased by 60.0% and 46.9%, respectively, after loading gold nanoparticles onto the LSM-YSZ anode. Physicochemical characterizations and electrochemical measurements suggested that the improved SOEC performance was attributed to the accelerated electron transfer of elementary process in anodic polarization reaction and the newly generated triple phase boundaries in gold nanoparticles-loaded LSMYSZ anode.展开更多
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.
基金supported by the National Natural Science Foundation of China(Nos.22275121,21931005,22105122,52272265)the National Key R&D Program of China(No.2023YFA1506300)+1 种基金the Shanghai Municipal Science and Technology Major Project of China,the Open Foundation Commission of Shaoxing Research Institute of Renewable Energy and Molecular Engineering,China(No.JDSX2022038)the Project of Jiangxi Academy of Sciences,China(No.2023YSTZX01).
文摘Solid oxide electrolysis cells(SOECs)provide a promising way for converting renewable energy into chemical fuels.Traditionally,NiO/CGO(nickel-gadolinium doped ceria)cermet has shown its excellent properties in ionic and electronic conductivity under reducing conditions.Herein,we developed a novel 1D NiO/CGO cathode through a cerium metal-organic framework(MOF)derived process.The cathode’s 1D nanostructure integrated with a microchannel scaffold facilitates enhanced mass transport,providing vertically aligned pathways for CO_(2)and H_(2)O diffusion.Additionally,the 1D framework increases the number of interfacial sites and reduces ion diffusion distances,thereby simplifying electron/ion transport.Consequently,this advanced cathode achieved a significant breakthrough in SOEC performance,maintaining efficient CO_(2)and H_(2)O electrolysis at an extraordinary current density of 1.41 A/cm^(2)at 1.5 V and excellent stability over 24 h at 850℃.The enhanced performance of this newly developed cathode not only achieves a remarkable 100%improvement compared to those of NiO/CGO cathodes with varying geometrical configurations but also surpasses those of commercial NiO/CGO catalysts by an outstanding 40%when tested under identical conditions.The development of the 1D NiO/CGO enhances the efficiency and durability of ceramic cathodes for CO_(2)and H_(2)O co-electrolysis in SOECs and improves the scalability and effectiveness of SOECs in renewable energy applications.
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financial supports from Singapore Ministry of Education Academic Research Fund Tier 2(Grant No.MOE-T2EP10220-0005)Academic Research Fund Tier 1(Grant No.RG104/18)。
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financial support from the National Key R&D Program of China (Grant 2017YFA0700102)the National Natural Science Foundation of China (Grants 21573222 and 91545202)+4 种基金Dalian National Laboratory for Clean Energy (DNL180404)Dalian Institute of Chemical Physics (Grant DICP DMTO201702)Dalian Outstanding Young Scientist Foundation (Grant 2017RJ03)the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant no. XDB17020200)the financial support from CAS Youth Innovation Promotion (Grant no. 2015145)
文摘Gold, as the common current collector in solid oxide electrolysis cell(SOEC), is traditionally considered to be inert for oxygen evolution reaction at the anode of SOEC. Herein, gold nanoparticles were loaded onto conventional strontium doped lanthanum manganite-yttria stabilized zirconia(LSM-YSZ) anode, which evidently improved the performance of oxygen evolution reaction at 800 °C. The current densities at 1.2 V and 1.4 V increased by 60.0% and 46.9%, respectively, after loading gold nanoparticles onto the LSM-YSZ anode. Physicochemical characterizations and electrochemical measurements suggested that the improved SOEC performance was attributed to the accelerated electron transfer of elementary process in anodic polarization reaction and the newly generated triple phase boundaries in gold nanoparticles-loaded LSMYSZ anode.
