1.Introduction Controlled combustion is perhaps the oldest human invention,providing food,warmth,protection,and power over millennia.In the last century,for example,it has enabled the United Kingdom to cut its agricul...1.Introduction Controlled combustion is perhaps the oldest human invention,providing food,warmth,protection,and power over millennia.In the last century,for example,it has enabled the United Kingdom to cut its agricultural labor force to near 1% of the population,replacing the horse and muscle power that dominated the 19th and earlier centuries[1].展开更多
The development of renewable and affordable energy is crucial for building a sustainable society. In this context, establishing a sustainable infrastructure for renewable energy requires the integration of energy stor...The development of renewable and affordable energy is crucial for building a sustainable society. In this context, establishing a sustainable infrastructure for renewable energy requires the integration of energy storage, specifically use of renewable hydrogen. The hydrogen evolution reaction (HER) of electrochemical water splitting is a promising method for producing green hydrogen. Recently, two-dimensional nanomaterials have shown great promise in promoting the HER in terms of both fundamental research and practical applications due to their high specific surface areas and tunable electronic properties. Among them, molybdenum disulfide (MoS2), a non-noble metal catalyst, has emerged as a promising alternative to replace expensive platinum-based catalysts for the HER because MoS_(2)has a high inherent activity, low cost, and abundant reserves. At present, greatly improved activity and stability are urgently needed for MoS_(2)to enable wide deployment of water electrolysis devices. In this regard, efficient strategies for precisely modifying MoS_(2)are of interest. Herein, the progress made with MoS_(2)as an HER catalyst is reviewed, with a focus on modification strategies, including phase engineering, morphology design, defect engineering, heteroatom doping, and heterostructure construction. It is believed that these strategies will be helpful in designing and developing high-performance and low-cost MoS2-based catalysts by lowering the charge transfer barrier, increasing the active site density, and optimizing the surface hydrophilicity. In addition, the challenges of MoS_(2)electrocatalysts and perspectives for future research and development of these catalysts are discussed.展开更多
Protonic solid oxide electrolysis cells(P-SOECs)operating at intermediate temperatures,which have low costs,low environmental impact,and high theoretical electrolysis efficiency,are considered promising next-generatio...Protonic solid oxide electrolysis cells(P-SOECs)operating at intermediate temperatures,which have low costs,low environmental impact,and high theoretical electrolysis efficiency,are considered promising next-generation energy conversion devices for green hydrogen production.However,the developments and applications of P-SOECs are restricted by numerous material-and interface-related issues,including carrier mismatch between the anode and electrolyte,current leakage in the electrolyte,poor interfacial contact,and chemical stability.Over the past few decades,considerable attempts have been made to address these issues by improving the properties of P-SOECs.This review comprehensively explores the recent advances in the mechanisms governing steam electrolysis in P-SOECs,optimization strategies,specially designed components,electrochemical performance,and durability.In particular,given that the lack of suitable anode materials has significantly impeded P-SOEC development,the relationships between the transferred carriers and the cell performance,reaction models,and surface decoration approaches are meticulously probed.Finally,the challenges hindering P-SOEC development are discussed and recommendations for future research directions,including theoretical calculations and simulations,structural modification approaches,and large-scale single-cell fabrication,are proposed to stimulate research on P-SOECs and thereby realize efficient electricity-to-hydrogen conversion.展开更多
Layered double hydroxides(LDHs)with decent oxygen evolution reaction(OER)activity have been extensively studied in the fields of energy storage and conversion.However,their poor conductivity,ease of agglomeration,and ...Layered double hydroxides(LDHs)with decent oxygen evolution reaction(OER)activity have been extensively studied in the fields of energy storage and conversion.However,their poor conductivity,ease of agglomeration,and low intrinsic activity limit their practical application.To date,improvement of the intrinsic activity and stability of NiFe-LDHs through the introduction of heteroatoms or its combination with other conductive substrates to enhance their water-splitting performance has drawn increasing attention.In this study,vertically interlaced ternary phosphatised nickel/iron hybrids grown on the surface of titanium carbide flakes(NiFe P/MXene)were successfully synthesised through a hydrothermal reaction and phosphating calcination process.The optimised NiFe P/MXene exhibited a low overpotential of 286 m V at 10 m A cm^(-2) and a Tafel slope of 35 m V dec^(-1) for the OER,which exceeded the performance of several existing NiFe-based catalysts.NiFe P/MXene was further used as a water-splitting anode in an alkaline electrolyte,exhibiting a cell voltage of only 1.61 V to achieve a current density of 10 m A cm^(-2).Density functional theory(DFT)calculations revealed that the combination of MXene acting as a conductive substrate and the phosphating process can effectively tune the electronic structure and density of the electrocatalyst surface to promote the energy level of the d-band centre,resulting in an enhanced OER performance.This study provides a valuable guideline for designing high-performance MXenesupported NiFe-based OER catalysts.展开更多
Typically,rational interfacial engineering can effectively modify the adsorption energy of active hydrogen molecules to improve water splitting efficiency.NiFe layered double hydroxide(NiFe LDH)composite,an efficient ...Typically,rational interfacial engineering can effectively modify the adsorption energy of active hydrogen molecules to improve water splitting efficiency.NiFe layered double hydroxide(NiFe LDH)composite,an efficient oxygen evolution reaction(OER)catalyst,suffers from slow hydrogen evolution reaction(HER)kinetics,restricting its application for overall water splitting.Herein,we construct the hierarchical MoS_(2)/NiFe LDH nanosheets with a heterogeneous interface used for HER and OER.Benefiting the hierarchical heterogeneous interface optimized hydrogen Gibbs free energy,tens of exposed active sites,rapid mass-and charge-transfer processes,the MoS_(2)/NiFe LDH displays a highly efficient synergistic electrocatalytic effect.The MoS_(2)/NiFe LDH electrode in 1 mol/L KOH exhibits excellent HER activity,only 98 mV overpotential at 10 mA/cm^(2).Significantly,when it assembled as anode and cathode for overall water splitting,only 1.61 V cell voltage was required to achieve 10 mA/cm^(2)with excellent durability(50 h).展开更多
Hydrogen,especially the“green hydrogen”based on water electrolysis,is of great importance to build a sustainable society due to its high-energy-density,zero-carbon-emission features,and wide-range applications.Today...Hydrogen,especially the“green hydrogen”based on water electrolysis,is of great importance to build a sustainable society due to its high-energy-density,zero-carbon-emission features,and wide-range applications.Today's water electrolysis is usually carried out in either low-temperature(<100℃),e.g.,alkaline electrolyzer,or high-temperature(>700℃)applications,e.g.,solid oxide electrolyzer.However,the low-temperature devices usually suffer from high applied voltages(usually>1.5 V@0.01 A cm^(-2))and high cost;meanwhile,the high-temperature ones have an unsatisfied lifetime partially due to the incompatibility among components.Reasonably,an intermediate-temperature device,namely,proton ceramic cell(PCC),has been recently proposed.The widely-used air electrode for PCC is based on double O^(2-)/e^(-)conductor or composited O^(2-)/e^(-)-H^(+)conductor,limiting the accessible reaction region.Herein,we designed a single-phase La_(0.8)Sr_(0.2)Co_(1-x)Mn_(x)O_(3-δ)(LSCM)with triple H^(+)/O^(2-)/e^(-)conductivity as the air electrode for PCCs.Specifically,the La_(0.8)Sr_(0.2)Co_(0.8)Mn_(0.2)O_(3-δ)(LSCM8282)incorporates 5.8%proton carriers in molar fraction at 400℃,indicating superior proton conducting ability.Impressively,a high current density of 1580 mA cm^(-2) for hydrogen production(water electrolysis)is achieved at 1.3 V and 650℃,surpassing most low-and high-temperature devices reported so far.Meanwhile,such a PCC can also be operated under a reversible fuel cell mode,with a peak power density of 521 mW cm^(-2) at 650℃.By correlating the electrochemical performances with the hydrated proton concentration of single-phase triple conducting air electrodes in this work and our previous work,a principle for rational design of high-performance PCCs is proposed.展开更多
文摘1.Introduction Controlled combustion is perhaps the oldest human invention,providing food,warmth,protection,and power over millennia.In the last century,for example,it has enabled the United Kingdom to cut its agricultural labor force to near 1% of the population,replacing the horse and muscle power that dominated the 19th and earlier centuries[1].
基金the Outstanding Youth Project of Guangdong Provincial Natural Science Foundation,China(Grant No.2022B1515020020)the National Natural Science Foundation of China(Grant No.2225071013)+2 种基金the Guangdong Basic and Applied Basic Research Foundation,China(No.2022B1515120079)the Funding by Science and Technology Projects in Guangzhou,China(No.202206050003)the Guangdong Engineering Technology Research Center for Hydrogen Energy and Fuel Cells,China.
文摘The development of renewable and affordable energy is crucial for building a sustainable society. In this context, establishing a sustainable infrastructure for renewable energy requires the integration of energy storage, specifically use of renewable hydrogen. The hydrogen evolution reaction (HER) of electrochemical water splitting is a promising method for producing green hydrogen. Recently, two-dimensional nanomaterials have shown great promise in promoting the HER in terms of both fundamental research and practical applications due to their high specific surface areas and tunable electronic properties. Among them, molybdenum disulfide (MoS2), a non-noble metal catalyst, has emerged as a promising alternative to replace expensive platinum-based catalysts for the HER because MoS_(2)has a high inherent activity, low cost, and abundant reserves. At present, greatly improved activity and stability are urgently needed for MoS_(2)to enable wide deployment of water electrolysis devices. In this regard, efficient strategies for precisely modifying MoS_(2)are of interest. Herein, the progress made with MoS_(2)as an HER catalyst is reviewed, with a focus on modification strategies, including phase engineering, morphology design, defect engineering, heteroatom doping, and heterostructure construction. It is believed that these strategies will be helpful in designing and developing high-performance and low-cost MoS2-based catalysts by lowering the charge transfer barrier, increasing the active site density, and optimizing the surface hydrophilicity. In addition, the challenges of MoS_(2)electrocatalysts and perspectives for future research and development of these catalysts are discussed.
基金Huangpu Hydrogen Energy Innovation Center at Guangzhou UniversityLaboratory of Electronic Materials Chemistry at Hokkaido University+1 种基金Basic and Applied Basic Research Foundation of Guangdong Province,Grant/Award Number:2022A1515110470Guangdong Engineering Technology Research Center for Hydrogen Energy and Fuel Cells。
文摘Protonic solid oxide electrolysis cells(P-SOECs)operating at intermediate temperatures,which have low costs,low environmental impact,and high theoretical electrolysis efficiency,are considered promising next-generation energy conversion devices for green hydrogen production.However,the developments and applications of P-SOECs are restricted by numerous material-and interface-related issues,including carrier mismatch between the anode and electrolyte,current leakage in the electrolyte,poor interfacial contact,and chemical stability.Over the past few decades,considerable attempts have been made to address these issues by improving the properties of P-SOECs.This review comprehensively explores the recent advances in the mechanisms governing steam electrolysis in P-SOECs,optimization strategies,specially designed components,electrochemical performance,and durability.In particular,given that the lack of suitable anode materials has significantly impeded P-SOEC development,the relationships between the transferred carriers and the cell performance,reaction models,and surface decoration approaches are meticulously probed.Finally,the challenges hindering P-SOEC development are discussed and recommendations for future research directions,including theoretical calculations and simulations,structural modification approaches,and large-scale single-cell fabrication,are proposed to stimulate research on P-SOECs and thereby realize efficient electricity-to-hydrogen conversion.
基金supported by the National Natural Science Foundation of China(21875048)the Outstanding Youth Project of Guangdong Natural Science Foundation(2020B1515020028)+1 种基金the Yangcheng Scholars Research Project of Guangzhou(201831820)the Science and Technology Research Project of Guangzhou(202002010007)。
文摘Layered double hydroxides(LDHs)with decent oxygen evolution reaction(OER)activity have been extensively studied in the fields of energy storage and conversion.However,their poor conductivity,ease of agglomeration,and low intrinsic activity limit their practical application.To date,improvement of the intrinsic activity and stability of NiFe-LDHs through the introduction of heteroatoms or its combination with other conductive substrates to enhance their water-splitting performance has drawn increasing attention.In this study,vertically interlaced ternary phosphatised nickel/iron hybrids grown on the surface of titanium carbide flakes(NiFe P/MXene)were successfully synthesised through a hydrothermal reaction and phosphating calcination process.The optimised NiFe P/MXene exhibited a low overpotential of 286 m V at 10 m A cm^(-2) and a Tafel slope of 35 m V dec^(-1) for the OER,which exceeded the performance of several existing NiFe-based catalysts.NiFe P/MXene was further used as a water-splitting anode in an alkaline electrolyte,exhibiting a cell voltage of only 1.61 V to achieve a current density of 10 m A cm^(-2).Density functional theory(DFT)calculations revealed that the combination of MXene acting as a conductive substrate and the phosphating process can effectively tune the electronic structure and density of the electrocatalyst surface to promote the energy level of the d-band centre,resulting in an enhanced OER performance.This study provides a valuable guideline for designing high-performance MXenesupported NiFe-based OER catalysts.
基金financially supported by National Natural Science Foundation of China(Nos.21875048 and 21905063)Outstanding Youth Project of Guangdong Natural Science Foundation(No.2020B1515020028)+1 种基金Guangdong Natural Science Foundation(No.2021A1515010066)Science and Technology Research Project of Guangzhou(Nos.201904010052 and 202002010007)。
文摘Typically,rational interfacial engineering can effectively modify the adsorption energy of active hydrogen molecules to improve water splitting efficiency.NiFe layered double hydroxide(NiFe LDH)composite,an efficient oxygen evolution reaction(OER)catalyst,suffers from slow hydrogen evolution reaction(HER)kinetics,restricting its application for overall water splitting.Herein,we construct the hierarchical MoS_(2)/NiFe LDH nanosheets with a heterogeneous interface used for HER and OER.Benefiting the hierarchical heterogeneous interface optimized hydrogen Gibbs free energy,tens of exposed active sites,rapid mass-and charge-transfer processes,the MoS_(2)/NiFe LDH displays a highly efficient synergistic electrocatalytic effect.The MoS_(2)/NiFe LDH electrode in 1 mol/L KOH exhibits excellent HER activity,only 98 mV overpotential at 10 mA/cm^(2).Significantly,when it assembled as anode and cathode for overall water splitting,only 1.61 V cell voltage was required to achieve 10 mA/cm^(2)with excellent durability(50 h).
基金This research was supported by Guangdong Postdoctoral Research Project(62104380),Guangdong Natural Science Funds for Distinguished Young Scholar.
文摘Hydrogen,especially the“green hydrogen”based on water electrolysis,is of great importance to build a sustainable society due to its high-energy-density,zero-carbon-emission features,and wide-range applications.Today's water electrolysis is usually carried out in either low-temperature(<100℃),e.g.,alkaline electrolyzer,or high-temperature(>700℃)applications,e.g.,solid oxide electrolyzer.However,the low-temperature devices usually suffer from high applied voltages(usually>1.5 V@0.01 A cm^(-2))and high cost;meanwhile,the high-temperature ones have an unsatisfied lifetime partially due to the incompatibility among components.Reasonably,an intermediate-temperature device,namely,proton ceramic cell(PCC),has been recently proposed.The widely-used air electrode for PCC is based on double O^(2-)/e^(-)conductor or composited O^(2-)/e^(-)-H^(+)conductor,limiting the accessible reaction region.Herein,we designed a single-phase La_(0.8)Sr_(0.2)Co_(1-x)Mn_(x)O_(3-δ)(LSCM)with triple H^(+)/O^(2-)/e^(-)conductivity as the air electrode for PCCs.Specifically,the La_(0.8)Sr_(0.2)Co_(0.8)Mn_(0.2)O_(3-δ)(LSCM8282)incorporates 5.8%proton carriers in molar fraction at 400℃,indicating superior proton conducting ability.Impressively,a high current density of 1580 mA cm^(-2) for hydrogen production(water electrolysis)is achieved at 1.3 V and 650℃,surpassing most low-and high-temperature devices reported so far.Meanwhile,such a PCC can also be operated under a reversible fuel cell mode,with a peak power density of 521 mW cm^(-2) at 650℃.By correlating the electrochemical performances with the hydrated proton concentration of single-phase triple conducting air electrodes in this work and our previous work,a principle for rational design of high-performance PCCs is proposed.