Electrocatalytic hydrogenation(ECH)of organics using water as hydrogen donors has been regarded as a green organic reduction technique to replace traditional chemical reactions that use sacrificial chemicals.The devel...Electrocatalytic hydrogenation(ECH)of organics using water as hydrogen donors has been regarded as a green organic reduction technique to replace traditional chemical reactions that use sacrificial chemicals.The development of ECH process provides potential applications in the production of value-added chemicals owing to its low energy consumption,low pollution,high safety,and superior sustainability.However,its application is limited by the low conversion rate and poor selectivity toward desired products.The efficiency of ECH can be improved by rational design of electrocatalysts.This review covers several representative electrocatalytic systems(aldehydes,ketones,phenolic organics,alkynes,and organonitrogen compounds)and summarizes different ECH mechanisms,followed by thorough discussion on the modification strategies of electrocatalysts that are currently adopted to enhance the catalytic performance.Finally,in view of the current challenges for ECH,we discuss possible future directions in the field,aiming to provide guidance to the catalyst design toward highly efficient ECH reactions over different organic feedstocks.展开更多
In contrast to alkaline water electrolysis,acidic water electrolysis remains an elusive goal due to the lack of earth-abundant,efficient,and acid-stable water oxidation electrocatalysts.Here,we show that materials wit...In contrast to alkaline water electrolysis,acidic water electrolysis remains an elusive goal due to the lack of earth-abundant,efficient,and acid-stable water oxidation electrocatalysts.Here,we show that materials with intrinsically poor electrocatalytic activity can be turned into active electrocatalysts that drive the acidic oxygen evolution reaction(OER)effectively.This development is achieved through ultrafast plasma sputtering,which introduces abundant oxygen vacancies that reconstruct the surface electronic structures,and thus,regulated the surface interactions of electrocatalysts and the OER intermediates.Using tungsten oxide(WO_(3))as an example,we present a broad spectrum of theoretical and experimental characterizations that show an improved energetics of OER originating from surface oxygen vacancies and resulting in a significantly boosted OER performance,compared with pristine WO_(3).Our result suggests the efficacy of using defect chemistry to modify electronic properties and hence to improve the OER performance of known materials with poor activity,providing a new direction for the discovery of acid-stable OER catalysts.展开更多
基金supported by the Fundamental Research Funds for the Central Universities in China(No.20720210010)National Natural Science Foundation of China(No.22001081)+2 种基金the Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM,Grant No.:HRTP-[2022]-7)Xiamen University.Qiu Jiang acknowledges the China Postdoctoral Science Foundation funded project(2022M710601)the University of Electronic Science and Technology of China for startup funding(Y030212059003039).
文摘Electrocatalytic hydrogenation(ECH)of organics using water as hydrogen donors has been regarded as a green organic reduction technique to replace traditional chemical reactions that use sacrificial chemicals.The development of ECH process provides potential applications in the production of value-added chemicals owing to its low energy consumption,low pollution,high safety,and superior sustainability.However,its application is limited by the low conversion rate and poor selectivity toward desired products.The efficiency of ECH can be improved by rational design of electrocatalysts.This review covers several representative electrocatalytic systems(aldehydes,ketones,phenolic organics,alkynes,and organonitrogen compounds)and summarizes different ECH mechanisms,followed by thorough discussion on the modification strategies of electrocatalysts that are currently adopted to enhance the catalytic performance.Finally,in view of the current challenges for ECH,we discuss possible future directions in the field,aiming to provide guidance to the catalyst design toward highly efficient ECH reactions over different organic feedstocks.
基金supported by the King Abdullah University of Science and Technology(KAUST)。
文摘In contrast to alkaline water electrolysis,acidic water electrolysis remains an elusive goal due to the lack of earth-abundant,efficient,and acid-stable water oxidation electrocatalysts.Here,we show that materials with intrinsically poor electrocatalytic activity can be turned into active electrocatalysts that drive the acidic oxygen evolution reaction(OER)effectively.This development is achieved through ultrafast plasma sputtering,which introduces abundant oxygen vacancies that reconstruct the surface electronic structures,and thus,regulated the surface interactions of electrocatalysts and the OER intermediates.Using tungsten oxide(WO_(3))as an example,we present a broad spectrum of theoretical and experimental characterizations that show an improved energetics of OER originating from surface oxygen vacancies and resulting in a significantly boosted OER performance,compared with pristine WO_(3).Our result suggests the efficacy of using defect chemistry to modify electronic properties and hence to improve the OER performance of known materials with poor activity,providing a new direction for the discovery of acid-stable OER catalysts.