There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to i...There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of electrodes.The Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 V.The results provide insights into the ioncatalyzed effects boosting OER performance.展开更多
Electrocatalytic water splitting is crucial to renewable and clean hydrogen generation.Achieving high efficiency and stability in hydrogen generation by freshwater/seawater electrolysis at a high current density(HCD)u...Electrocatalytic water splitting is crucial to renewable and clean hydrogen generation.Achieving high efficiency and stability in hydrogen generation by freshwater/seawater electrolysis at a high current density(HCD)using low-cost electrode materials is of utmost importance for the future hydrogen economy.However,conventional freshwater/seawater electrolysis suffers from low current density due to inefficient electrocatalysts and competitive reactions of the chlorine evolution reaction(ClER),consequently hampering its industrial adoption.Advanced surface and interface engineering techniques are essential for the development of efficient and long-lasting electrodes for freshwater and seawater electrolysis at HCD.In the review,we begin by discussing the fundamental aspects of freshwater/seawater splitting,focusing on recent advancements and strategies to increase the efficiency at HCD.We then comprehensively discuss the rational design strategies for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)at HCD together with the associated fundamental electrode reactions by considering the thermodynamic and kinetic aspects of the catalytic efficiency,selectivity,and corrosion resistance.It is followed by a discussion of some existing issues and limitations of HCD freshwater/seawater splitting and viable solutions.Finally,the issues facing the field and possible future research directions for efficient large-scale industrial water splitting are discussed.展开更多
基金financially supported by the 2022 Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province(STKJ202209077 and STKJ202209083)the Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme 2019(GDUPS2019)the City University of Hong Kong Strategic Research Grant(SRG)(7005505)。
文摘There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of electrodes.The Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 V.The results provide insights into the ioncatalyzed effects boosting OER performance.
基金support from the National Natural Science Foundation of China(grant no.U2004210)the Basic Research Program of Shenzhen Municipal Science and Technology Innovation Committee(grant nos.JCYJ20210324141613032 and JCYJ202308073003128)+4 种基金the Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province(grant nos.STKJ202209083 and STKJ202209077)Guangdong Basic and Applied Basic Research Foundation(grant no.2022A1515240007)Jieyang Science and Technology Project(grant no.skjcx039)City University of Hong Kong Strategic Research Grant(grant no.SRG 7005505)City University of Hong Kong Donation Research Grant(grant no.DON-RMG 9229021).
文摘Electrocatalytic water splitting is crucial to renewable and clean hydrogen generation.Achieving high efficiency and stability in hydrogen generation by freshwater/seawater electrolysis at a high current density(HCD)using low-cost electrode materials is of utmost importance for the future hydrogen economy.However,conventional freshwater/seawater electrolysis suffers from low current density due to inefficient electrocatalysts and competitive reactions of the chlorine evolution reaction(ClER),consequently hampering its industrial adoption.Advanced surface and interface engineering techniques are essential for the development of efficient and long-lasting electrodes for freshwater and seawater electrolysis at HCD.In the review,we begin by discussing the fundamental aspects of freshwater/seawater splitting,focusing on recent advancements and strategies to increase the efficiency at HCD.We then comprehensively discuss the rational design strategies for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)at HCD together with the associated fundamental electrode reactions by considering the thermodynamic and kinetic aspects of the catalytic efficiency,selectivity,and corrosion resistance.It is followed by a discussion of some existing issues and limitations of HCD freshwater/seawater splitting and viable solutions.Finally,the issues facing the field and possible future research directions for efficient large-scale industrial water splitting are discussed.
