Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting el...Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting electrolyzers.Herein,a cost‐effective and ecofriendly strategy is reported to fabricate coral‐like FeNi(OH)x/Ni as a bifunctional electrocatalyst for overall water splitting in alkaline media.With the assistance of mild corrosion of Ni by Fe(NO3)3,in situ generated FeNi(OH)x nanosheets are intimately attached on metallic coral‐like Ni.Integration of these nanosheets with the electrodeposited coral‐like Ni skeleton and the supermacroporous Ni foam substrate forms a binder‐free hierarchical electrode,which is beneficial for exposing catalytic active sites,accelerating mass transport,and facilitating the release of gaseous species.In 1.0 mol L^-1 KOH solution,a symmetric electrolyzer constructed with FeNi(OH)x/Ni as both the anode and the cathode exhibits an excellent activity with an applied potential difference of 1.52 V at 10 mA cm^-2,which is superior to that of an asymmetric electrolyzer constructed with the state‐of‐the‐art RuO2‐PtC couple(applied potential difference of 1.55 V at 10 mA cm^-2).This work contributes a facile and reliable strategy for manufacturing affordable,practical,and promising water‐splitting devices.展开更多
The catalytic/electrocatalytic performance of platinum(Pt)nanostructures highly relates to their morphology.Herein,we propose a facile self-template pyrolysis strategy at high temperature to synthesize one-dimensional...The catalytic/electrocatalytic performance of platinum(Pt)nanostructures highly relates to their morphology.Herein,we propose a facile self-template pyrolysis strategy at high temperature to synthesize one-dimensionally holey Pt nanotubes(Pt-hNTs)using Pt^(Ⅱ)-dimethylglyoxime complex(Pt^(Ⅱ)-DMG)nanorods as the reaction precursor.The coordination capability of DMG results in the generation of Pt^(Ⅱ)-DMG nanorods,whereas the reducibility of DMG at high temperature leads to the reduction of Pt^(Ⅱ)species in Pt^(Ⅱ)-DMG nanorods.During the reaction process,the inside-out Ostwald ripening phenomenon leads to the hollow morphology of Pt-hNTs.Benefiting from the physical characteristics of hollow and holey structure,Pt-hNTs with clean surface show superior electroactivity and durability for catalyzing ethanol electrooxidation as well as hydrogen evolution reaction in alkaline media.Under optimized experimental conditions,the constructed symmetric Pt-hNTs||Pt-hNTs ethanol electrolyzer only requires an electrolysis voltage of 0.40 V to achieve the electrochemical hydrogen production,demonstrating a highly energy saving strategy relative to traditional water electrolysis.展开更多
Development of highly active electrocatalysts for oxygen evolution reaction(OER)is one of the critical issues for water splitting,and most reported catalysts operate at overpotentials above 190 mV.Here we present a mu...Development of highly active electrocatalysts for oxygen evolution reaction(OER)is one of the critical issues for water splitting,and most reported catalysts operate at overpotentials above 190 mV.Here we present a multiphase nickel iron sulfide(MPS)hybrid electrode with a hierarchical structure of iron doped NiS and Ni3S2,possessing a benchmark OER activity in alkaline media with a potential as low as 1.33 V(vs.reversible hydrogen electrode)to drive an OER current density of 10 mA cm^-2.The Fe doped NiS,combined with highly conductive disulfide phase on porous Ni foam,is believed to be responsible for the ultrahigh activity.Furthermore,density functional theory simulation reveals that partially oxidized sulfur sites in Fe doped NiS could dramatically lower the energy barrier for the rate-determining elementary reaction,thus contributing to the active oxygen evolution.展开更多
Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion e...Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion efficiency.Herein we report a strategy of boosting H_(2)production at low voltages by replacing OER with a bioelectrochemical cascade reaction at a triphase bioanode.In the presence of oxygen,oxidase enzymes can convert biomass into valuable products,and concurrently generate H_(2)O_(2) that can be further electrooxidized at the bioanode.Benefiting from the efficient oxidase kinetics at an oxygen-rich triphase bioanode and the more favorable thermodynamics of H_(2)O_(2)oxidation than that of OER,the cell voltage and energy consumption are reduced by~0.70 V and~36%,respectively,relative to regular water electrolysis.This leads to an efficient H_(2)production at the cathode and valuable product generation at the bioanode.Integration of a bioelectrochemical cascade into the water splitting process provides an energy-efficient and promising pathway for achieving a renewable fuel.展开更多
文摘Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting electrolyzers.Herein,a cost‐effective and ecofriendly strategy is reported to fabricate coral‐like FeNi(OH)x/Ni as a bifunctional electrocatalyst for overall water splitting in alkaline media.With the assistance of mild corrosion of Ni by Fe(NO3)3,in situ generated FeNi(OH)x nanosheets are intimately attached on metallic coral‐like Ni.Integration of these nanosheets with the electrodeposited coral‐like Ni skeleton and the supermacroporous Ni foam substrate forms a binder‐free hierarchical electrode,which is beneficial for exposing catalytic active sites,accelerating mass transport,and facilitating the release of gaseous species.In 1.0 mol L^-1 KOH solution,a symmetric electrolyzer constructed with FeNi(OH)x/Ni as both the anode and the cathode exhibits an excellent activity with an applied potential difference of 1.52 V at 10 mA cm^-2,which is superior to that of an asymmetric electrolyzer constructed with the state‐of‐the‐art RuO2‐PtC couple(applied potential difference of 1.55 V at 10 mA cm^-2).This work contributes a facile and reliable strategy for manufacturing affordable,practical,and promising water‐splitting devices.
基金supported by the Natural Science Foundation of Hainan Province(2019RC007)Key Research and Development Project of Hainan Province(ZDYF2020037)+5 种基金the National Natural Science Foundation of China(21875133 and 51873100)Natural Science Foundation of Shaanxi Province(2020JZ-23)Fundamental Research Funds for the Central Universities(GK202101005,GK201901002,2019TS007,2021CBLZ004,and 2020CSLZ012)the Innovation Team Project for Graduate Students at Shaanxi Normal University(TD2020048Y)Open Foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials at Guangxi University(2021GXYSOF02)the 111 Project(B14041)。
文摘The catalytic/electrocatalytic performance of platinum(Pt)nanostructures highly relates to their morphology.Herein,we propose a facile self-template pyrolysis strategy at high temperature to synthesize one-dimensionally holey Pt nanotubes(Pt-hNTs)using Pt^(Ⅱ)-dimethylglyoxime complex(Pt^(Ⅱ)-DMG)nanorods as the reaction precursor.The coordination capability of DMG results in the generation of Pt^(Ⅱ)-DMG nanorods,whereas the reducibility of DMG at high temperature leads to the reduction of Pt^(Ⅱ)species in Pt^(Ⅱ)-DMG nanorods.During the reaction process,the inside-out Ostwald ripening phenomenon leads to the hollow morphology of Pt-hNTs.Benefiting from the physical characteristics of hollow and holey structure,Pt-hNTs with clean surface show superior electroactivity and durability for catalyzing ethanol electrooxidation as well as hydrogen evolution reaction in alkaline media.Under optimized experimental conditions,the constructed symmetric Pt-hNTs||Pt-hNTs ethanol electrolyzer only requires an electrolysis voltage of 0.40 V to achieve the electrochemical hydrogen production,demonstrating a highly energy saving strategy relative to traditional water electrolysis.
基金supported by the National Natural Science Foundation of Chinathe National Key Research and Development Project (2018YFB1502401)+4 种基金the Royal Society and Newton Fund through Newton Advanced Fellowship award (NAF\R1\191294)the Program for Changjiang Scholars and Innovative Research Team in the Universitythe Fundamental Research Funds for the Central Universitiesthe Longterm Subsidy Mechanism from the Ministry of Finance and the Ministry of Education of Chinathe financial support from China Scholarships Council (CSC)
文摘Development of highly active electrocatalysts for oxygen evolution reaction(OER)is one of the critical issues for water splitting,and most reported catalysts operate at overpotentials above 190 mV.Here we present a multiphase nickel iron sulfide(MPS)hybrid electrode with a hierarchical structure of iron doped NiS and Ni3S2,possessing a benchmark OER activity in alkaline media with a potential as low as 1.33 V(vs.reversible hydrogen electrode)to drive an OER current density of 10 mA cm^-2.The Fe doped NiS,combined with highly conductive disulfide phase on porous Ni foam,is believed to be responsible for the ultrahigh activity.Furthermore,density functional theory simulation reveals that partially oxidized sulfur sites in Fe doped NiS could dramatically lower the energy barrier for the rate-determining elementary reaction,thus contributing to the active oxygen evolution.
基金supported by the National Key R&D Program of China(2019YFA0709200)the National Natural Science Foundation of China(21988102,51772198 and 21975171)。
文摘Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion efficiency.Herein we report a strategy of boosting H_(2)production at low voltages by replacing OER with a bioelectrochemical cascade reaction at a triphase bioanode.In the presence of oxygen,oxidase enzymes can convert biomass into valuable products,and concurrently generate H_(2)O_(2) that can be further electrooxidized at the bioanode.Benefiting from the efficient oxidase kinetics at an oxygen-rich triphase bioanode and the more favorable thermodynamics of H_(2)O_(2)oxidation than that of OER,the cell voltage and energy consumption are reduced by~0.70 V and~36%,respectively,relative to regular water electrolysis.This leads to an efficient H_(2)production at the cathode and valuable product generation at the bioanode.Integration of a bioelectrochemical cascade into the water splitting process provides an energy-efficient and promising pathway for achieving a renewable fuel.