Currently,seawater electrolysis is an effective technology for the large-scale production of green hydrogen,but the issues of poisoning active sites and catalyst corrosion caused by chloride ions in seawater urgently ...Currently,seawater electrolysis is an effective technology for the large-scale production of green hydrogen,but the issues of poisoning active sites and catalyst corrosion caused by chloride ions in seawater urgently need to be addressed.This paper reports a non-precious metal cobalt sulfide with sulfur vacancies(v-Co_(9)S_(8))catalyst,where the presence of sulfur vacancies can accelerate the formation of metal hydroxyl oxides and induce the generation of high-valent Co,enabling v-Co_(9)S_(8) to exhibit long-term stability and excellent oxygen evolution reaction(OER)activity in seawater electrolysis.At the same time,the high-valent Co acts as a Lewis acid,providing stronger OH^(−) adsorption and Cl^(−) repulsion capabilities during the seawater OER process.Therefore,v-Co_(9)S_(8) catalyst achieves an overpotential of only 420 mV at 1000 mA·cm^(−2) in alkaline seawater.At the same time,the assembled alkaline seawater anion exchange membrane(AEM)electrolyzer operates stably for over 130 h under the condition of 500 mA·cm^(−2).This work reports a mechanism where anion vacancy-induced metal sulfide reconstruction forms high-valent metals,which is expected to provide effective guidance for the development of seawater electrocatalysts.展开更多
The development of efficient oxygen reduction reaction(ORR)electrocatalysts that utilize seawater as an electrolyte is crucial for harnessing marine resources and advancing the application of zinc-air batteries(ZABs)....The development of efficient oxygen reduction reaction(ORR)electrocatalysts that utilize seawater as an electrolyte is crucial for harnessing marine resources and advancing the application of zinc-air batteries(ZABs).Here,Er_(2)O_(3-)Pt electrocatalysts enriched oxygen vacancies were constructed by a one-step microwave method.Theoretical calculations indicate that the unique 4f orbitals of Er,in conjunction with the Pt 5d and O 2p orbitals,allow the 4f electrons to demonstrate a degree of mobility.This behavior provides flexible electronic states and optimizes the binding strength of oxygen intermediates in the ORR.In addition,quasi in-situ characterization has proven that the addition of Er and the mediation of the oxygen vacancies have enriched the electrons at Pt,effectively reducing the adsorption of Cl-and preventing the poisoning of the active site of Pt.As a result,Er_(2)O_(3-)Pt with half-wave potentials(E_(1/2))of 0.85 and 0.67 V in alkaline seawater and pure seawater,respectively,was used as a cathodic catalyst in alkaline seawater-based ZABs to obtain a maximum power density of 184.6 mW·cm^(-2)and remarkable stability in pure seawater.展开更多
Direct seawater electrolysis technology shows great potential,but chloride ions corrode the electrodes and cause competitive reactions,which limits its application.In recent years,metal phosphides with excellent intri...Direct seawater electrolysis technology shows great potential,but chloride ions corrode the electrodes and cause competitive reactions,which limits its application.In recent years,metal phosphides with excellent intrinsic catalytic activity have attracted much attention as electrocatalysts for the seawater splitting process,especially as efficient oxygen evolution reaction(OER)catalysts.This paper reviews the preparation methods for phosphide-based catalysts,the mechanism involved and related parameters for the OER.Innovative strategies for designing effective anode electrocatalysts to address the challenges are summarized.Furthermore,we outline a general strategy for enhancing the activity,selectivity,and stability of metal phosphides for the OER in seawater.Finally,future prospects for the development of metal phosphide catalysts are proposed and discussed.展开更多
Hydrogen produced by water electrolysis is considered an ideal,safe,and clean energy source.However,the high cost of noble metal-based electrocatalysts and the high overpotential of non-noble metals for the hydrogen e...Hydrogen produced by water electrolysis is considered an ideal,safe,and clean energy source.However,the high cost of noble metal-based electrocatalysts and the high overpotential of non-noble metals for the hydrogen evolution reaction(HER)are key bottlenecks limiting the practical application of water splitting technology.To tackle this challenge,extensive efforts have been made to explore strategies for improving the HER activity.This paper systematically reviews the critical roles of nonmetallic doping in enhancing HER catalyst performance,including electronic structure adjustment,active site regulation,and the generation of synergistic effects.Subsequently,we categorized the reported nonmetal-atom-doped HER catalysts by composition and introduced the mechanisms behind their high performance and long-term stability.In addition,this review also provides a comprehensive summary of the synthesis strategies and characterization techniques associated with non-metallic doping,aiming to offer practical guidance for future research and catalyst development in this field.Finally,this review discusses the development of non-metal-doped electrocatalysts,the key challenges in industrial water electrolysis,and the promising application of artificial intelligence(AI)in accelerating catalyst design and system optimization.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52072197,52174283,and 22301156)the Natural Science Foundation of Shandong Province(No.ZR2024QB012)+1 种基金the Qingdao Natural Science Foundation(No.24-4-4-zrjj-16-jch)Shandong Province“Double-Hundred Talent Plan”(No.WST2020003).
文摘Currently,seawater electrolysis is an effective technology for the large-scale production of green hydrogen,but the issues of poisoning active sites and catalyst corrosion caused by chloride ions in seawater urgently need to be addressed.This paper reports a non-precious metal cobalt sulfide with sulfur vacancies(v-Co_(9)S_(8))catalyst,where the presence of sulfur vacancies can accelerate the formation of metal hydroxyl oxides and induce the generation of high-valent Co,enabling v-Co_(9)S_(8) to exhibit long-term stability and excellent oxygen evolution reaction(OER)activity in seawater electrolysis.At the same time,the high-valent Co acts as a Lewis acid,providing stronger OH^(−) adsorption and Cl^(−) repulsion capabilities during the seawater OER process.Therefore,v-Co_(9)S_(8) catalyst achieves an overpotential of only 420 mV at 1000 mA·cm^(−2) in alkaline seawater.At the same time,the assembled alkaline seawater anion exchange membrane(AEM)electrolyzer operates stably for over 130 h under the condition of 500 mA·cm^(−2).This work reports a mechanism where anion vacancy-induced metal sulfide reconstruction forms high-valent metals,which is expected to provide effective guidance for the development of seawater electrocatalysts.
基金the National Natural Science Foundation of China(Nos.52072197,52174283,22301156)Key R.&D.,the Natural Science Foundation of Shandong Province(No.ZR2024QB012)+1 种基金the Qingdao Natural Science Foundation(24-4-4-zrjj-16-jch)Shandong Province“Double-Hundred Talent Plan”(No.WST2020003).
文摘The development of efficient oxygen reduction reaction(ORR)electrocatalysts that utilize seawater as an electrolyte is crucial for harnessing marine resources and advancing the application of zinc-air batteries(ZABs).Here,Er_(2)O_(3-)Pt electrocatalysts enriched oxygen vacancies were constructed by a one-step microwave method.Theoretical calculations indicate that the unique 4f orbitals of Er,in conjunction with the Pt 5d and O 2p orbitals,allow the 4f electrons to demonstrate a degree of mobility.This behavior provides flexible electronic states and optimizes the binding strength of oxygen intermediates in the ORR.In addition,quasi in-situ characterization has proven that the addition of Er and the mediation of the oxygen vacancies have enriched the electrons at Pt,effectively reducing the adsorption of Cl-and preventing the poisoning of the active site of Pt.As a result,Er_(2)O_(3-)Pt with half-wave potentials(E_(1/2))of 0.85 and 0.67 V in alkaline seawater and pure seawater,respectively,was used as a cathodic catalyst in alkaline seawater-based ZABs to obtain a maximum power density of 184.6 mW·cm^(-2)and remarkable stability in pure seawater.
基金financially supported by the National Natural Science Foundation of China(52072197,52174283,and 22301156)the Qingdao Natural Science Foundation(24-4-4-zrjj-16-jch)+4 种基金the Natural Science Foundation of Shandong Province(ZR2021QE165)the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(2019KJC004)the Major Scientific and Technological Innovation Project(2019JZZY020405)the Shandong Province“Double-Hundred Talent Plan”(WST2020003)the Taishan Scholar Young Talent Program(tsqn201909114).
文摘Direct seawater electrolysis technology shows great potential,but chloride ions corrode the electrodes and cause competitive reactions,which limits its application.In recent years,metal phosphides with excellent intrinsic catalytic activity have attracted much attention as electrocatalysts for the seawater splitting process,especially as efficient oxygen evolution reaction(OER)catalysts.This paper reviews the preparation methods for phosphide-based catalysts,the mechanism involved and related parameters for the OER.Innovative strategies for designing effective anode electrocatalysts to address the challenges are summarized.Furthermore,we outline a general strategy for enhancing the activity,selectivity,and stability of metal phosphides for the OER in seawater.Finally,future prospects for the development of metal phosphide catalysts are proposed and discussed.
基金financially supported by the National Natural Science Foundation of China(52072197,52174283,and 22301156)the Natural Science Foundation of Shandong Province(ZR2021QE165)+1 种基金the Qingdao Natural Science Foundation(24-4-4-zrjj-16-jch)the Shandong Province“Double-Hundred Talent Plan”(WST2020003).
文摘Hydrogen produced by water electrolysis is considered an ideal,safe,and clean energy source.However,the high cost of noble metal-based electrocatalysts and the high overpotential of non-noble metals for the hydrogen evolution reaction(HER)are key bottlenecks limiting the practical application of water splitting technology.To tackle this challenge,extensive efforts have been made to explore strategies for improving the HER activity.This paper systematically reviews the critical roles of nonmetallic doping in enhancing HER catalyst performance,including electronic structure adjustment,active site regulation,and the generation of synergistic effects.Subsequently,we categorized the reported nonmetal-atom-doped HER catalysts by composition and introduced the mechanisms behind their high performance and long-term stability.In addition,this review also provides a comprehensive summary of the synthesis strategies and characterization techniques associated with non-metallic doping,aiming to offer practical guidance for future research and catalyst development in this field.Finally,this review discusses the development of non-metal-doped electrocatalysts,the key challenges in industrial water electrolysis,and the promising application of artificial intelligence(AI)in accelerating catalyst design and system optimization.
