Hydrogen is a promising candidate for clean and sustainable energy resources to substitute fossil fuels to mitigate global environmental issues.Electrochemical hydrogen production has been regarded as a viable and pro...Hydrogen is a promising candidate for clean and sustainable energy resources to substitute fossil fuels to mitigate global environmental issues.Electrochemical hydrogen production has been regarded as a viable and promising strategy.The overall water splitting is currently the predominant electrochemical hydrogen production method,which could be driven by renewable energy to achieve sustainable production.However,the current challenges are the intrinsically sluggish and energy-intensive oxygen evolution reduction(OER)at the anode and the expensive noble metal-based catalysts for overall water splitting,which limit the practical applications.Extensive efforts have been made to develop bifunctional non-noble metal-based electrocatalysts to boost hydrogen production efficiency and lower the cost.Meanwhile,alternative oxidation reactions with faster kinetics and less energy requirement than OER are being explored as the anodic reaction to couple with the hydrogen evolution reaction for energy-saving hydrogen production.In this review,the non-noble metal-based bifunctional electrocatalysts for overall water splitting,as well as other novel energy-saving hydrogen productions have been introduced and summarized.Current challenges and outlooks are commented on at the end of the article.展开更多
Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can impr...Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can improve the energy conversion efficiency.Since iron corrodes easily and even self-corrodes to form magnetic iron oxide species and generate corrosion currents,a novel strategy to integrate the hydrogen evolution reaction(HER)with waste Fe upgrading reaction(FUR)is proposed and demonstrated for energy-efficient hydrogen production in neutral media.The heterostructured MoSe_(2)/MoO_(2) grown on carbon cloth(MSM/CC)shows superior HER performance to that of commercial Pt/C at high current densities.By replacing conventional OER with FUR,the potential required to afford the anodic current density of 10 m A cm^(-2)decreases by 95%.The HER/FUR overall reaction shows an ultralow voltage of 0.68 V for 10 m A cm^(-2)with a power equivalent of 2.69 k Wh per m^(3)H_(2).Additionally,the Fe species formed at the anode extract the Rhodamine B(Rh B)pollutant by flocculation and also produce nanosized magnetic powder and beneficiated Rh B for value-adding applications.This work demonstrates both energy-saving hydrogen production and pollutant recycling without carbon emission by a single system and reveals a new direction to integrate hydrogen production with environmental recovery to achieve carbon neutrality.展开更多
Seawater electrolysis could address the water scarcity issue and realize the grid-scale production of carbon-neutral hydrogen,while facing the challenge of high energy consumption and chloride corrosion.Thermodynamica...Seawater electrolysis could address the water scarcity issue and realize the grid-scale production of carbon-neutral hydrogen,while facing the challenge of high energy consumption and chloride corrosion.Thermodynamically more favorable hydrazine oxidation reaction(HzOR)assisted water electrolysis is efficiency for energy-saving and chlorine-free hydrogen production.Herein,the MoNi alloys supported on MoO_(2) nanorods with enlarged hollow diameter on Ni foam(MoNi@NF)are synthesized,which is constructed by limiting the outward diffusion of Ni via annealing and thermal reduction of NiMoO_(4) nanorods.When coupling HzOR and hydrogen evolution reaction(HER)by employing MoNi@NF as both anode and cathode in two-electrode seawater system,a low cell voltage of 0.54 V is required to achieve 1,000 mA·cm^(−2) and with long-term durability for 100 h to keep above 100 mA·cm^(−2) and nearly 100%Faradaic efficiency.It can save 2.94 W·h to generate per liter H_(2) relative to alkaline seawater electrolysis with 37%lower energy equivalent input.展开更多
Electrocatalytic water splitting is a viable technique for generating hydrogen but is precluded from the sluggish kinetics of oxygen evolution reactions(OER).Small molecule oxidation reactions with lower working poten...Electrocatalytic water splitting is a viable technique for generating hydrogen but is precluded from the sluggish kinetics of oxygen evolution reactions(OER).Small molecule oxidation reactions with lower working potentials,such as methanol oxidation reactions,are good alternatives to OER with faster kinetics.However,the typically employed Ni-based electrocatalysts have poor activity and stability.Herein,a novel three-dimensional(3D)-networking Modoped Ni(OH)_(2) with ultralow Ni-Ni coordination is synthesized,which exhibits a high MOR activity of 100 mA cm^(−2) at 1.39 V,delivering 28 mV dec^(−1) for the Tafel slope.Meanwhile,hydrogen evolution with value-added formate co-generation is boosted with a current density of more than 500 mA cm^(−2) at a cell voltage of 2.00 V for 50 h,showing excellent stability in an industrial alkaline concentration(6 M KOH).Mechanistic studies based on density functional the-ory and X-ray absorption spectroscopy showed that the improved performance is mainly attributed to the ultralow Ni-Ni coordination,3D-networking structures and Mo dopants,which improve the catalytic activity,increase the active site density and strengthen the Ni(OH)_(2)3D-networking structures,respectively.This study paves a new way for designing electrocatalysts with enhanced activity and durability for industrial energy-saving hydrogen production.展开更多
基金financially supported by the National Key R&D Program of China (No. 2021YFA1501101)the National Natural Science Foundation of China (No. NSFC 21771156)the NSFC/RGC Joint Research Scheme Project (N_Poly U502/ 21)
文摘Hydrogen is a promising candidate for clean and sustainable energy resources to substitute fossil fuels to mitigate global environmental issues.Electrochemical hydrogen production has been regarded as a viable and promising strategy.The overall water splitting is currently the predominant electrochemical hydrogen production method,which could be driven by renewable energy to achieve sustainable production.However,the current challenges are the intrinsically sluggish and energy-intensive oxygen evolution reduction(OER)at the anode and the expensive noble metal-based catalysts for overall water splitting,which limit the practical applications.Extensive efforts have been made to develop bifunctional non-noble metal-based electrocatalysts to boost hydrogen production efficiency and lower the cost.Meanwhile,alternative oxidation reactions with faster kinetics and less energy requirement than OER are being explored as the anodic reaction to couple with the hydrogen evolution reaction for energy-saving hydrogen production.In this review,the non-noble metal-based bifunctional electrocatalysts for overall water splitting,as well as other novel energy-saving hydrogen productions have been introduced and summarized.Current challenges and outlooks are commented on at the end of the article.
基金financially supported by the Key Research and Development Program of Hubei Province (2021BAA208)the National Natural Science Foundation of China (52002294,51974208 and U2003130)+3 种基金the Young Top-notch Talent Cultivation Program of Hubei ProvinceKnowledge Innovation Program of Wuhan-Shuguang Project (2022010801020364)the City University of Hong Kong Strategic Research Grant (SRG) (7005505)the City University of Hong Kong Donation Research Grant (DONRMG 9229021)。
文摘Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can improve the energy conversion efficiency.Since iron corrodes easily and even self-corrodes to form magnetic iron oxide species and generate corrosion currents,a novel strategy to integrate the hydrogen evolution reaction(HER)with waste Fe upgrading reaction(FUR)is proposed and demonstrated for energy-efficient hydrogen production in neutral media.The heterostructured MoSe_(2)/MoO_(2) grown on carbon cloth(MSM/CC)shows superior HER performance to that of commercial Pt/C at high current densities.By replacing conventional OER with FUR,the potential required to afford the anodic current density of 10 m A cm^(-2)decreases by 95%.The HER/FUR overall reaction shows an ultralow voltage of 0.68 V for 10 m A cm^(-2)with a power equivalent of 2.69 k Wh per m^(3)H_(2).Additionally,the Fe species formed at the anode extract the Rhodamine B(Rh B)pollutant by flocculation and also produce nanosized magnetic powder and beneficiated Rh B for value-adding applications.This work demonstrates both energy-saving hydrogen production and pollutant recycling without carbon emission by a single system and reveals a new direction to integrate hydrogen production with environmental recovery to achieve carbon neutrality.
基金supported by the National Natural Science Foundation of China(Nos.51772162 and 52072197)the Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14)+3 种基金the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2019KJC004)the Major Scientific and Technological Innovation Project(No.2019JZZY020405)the Major Basic Research Program of Natural Science Foundation of Shandong Province(No.ZR2020ZD09)the Taishan Scholar Young Talent Program(No.tsqn201909114).
文摘Seawater electrolysis could address the water scarcity issue and realize the grid-scale production of carbon-neutral hydrogen,while facing the challenge of high energy consumption and chloride corrosion.Thermodynamically more favorable hydrazine oxidation reaction(HzOR)assisted water electrolysis is efficiency for energy-saving and chlorine-free hydrogen production.Herein,the MoNi alloys supported on MoO_(2) nanorods with enlarged hollow diameter on Ni foam(MoNi@NF)are synthesized,which is constructed by limiting the outward diffusion of Ni via annealing and thermal reduction of NiMoO_(4) nanorods.When coupling HzOR and hydrogen evolution reaction(HER)by employing MoNi@NF as both anode and cathode in two-electrode seawater system,a low cell voltage of 0.54 V is required to achieve 1,000 mA·cm^(−2) and with long-term durability for 100 h to keep above 100 mA·cm^(−2) and nearly 100%Faradaic efficiency.It can save 2.94 W·h to generate per liter H_(2) relative to alkaline seawater electrolysis with 37%lower energy equivalent input.
基金We gratefully thank the financial support from the National Natural Science Foundation of China(22272108,21975163 and 22003041)Shenzhen Science and Technology Program(No.KQTD20190929173914967,JCYJ20200109110416441)the Senior Talent Research Start-up Fund of Shenzhen University(000263 and 000265).
文摘Electrocatalytic water splitting is a viable technique for generating hydrogen but is precluded from the sluggish kinetics of oxygen evolution reactions(OER).Small molecule oxidation reactions with lower working potentials,such as methanol oxidation reactions,are good alternatives to OER with faster kinetics.However,the typically employed Ni-based electrocatalysts have poor activity and stability.Herein,a novel three-dimensional(3D)-networking Modoped Ni(OH)_(2) with ultralow Ni-Ni coordination is synthesized,which exhibits a high MOR activity of 100 mA cm^(−2) at 1.39 V,delivering 28 mV dec^(−1) for the Tafel slope.Meanwhile,hydrogen evolution with value-added formate co-generation is boosted with a current density of more than 500 mA cm^(−2) at a cell voltage of 2.00 V for 50 h,showing excellent stability in an industrial alkaline concentration(6 M KOH).Mechanistic studies based on density functional the-ory and X-ray absorption spectroscopy showed that the improved performance is mainly attributed to the ultralow Ni-Ni coordination,3D-networking structures and Mo dopants,which improve the catalytic activity,increase the active site density and strengthen the Ni(OH)_(2)3D-networking structures,respectively.This study paves a new way for designing electrocatalysts with enhanced activity and durability for industrial energy-saving hydrogen production.
