Oxygen defects play a critical role in the electrocatalytic oxygen evolution reaction(OER).Therefore,in-depth understanding the structure-activity-mechanism relationship of these defects is the key to design efficient...Oxygen defects play a critical role in the electrocatalytic oxygen evolution reaction(OER).Therefore,in-depth understanding the structure-activity-mechanism relationship of these defects is the key to design efficient OER electrocatalysts.This relationship needs to be understood dynamically due to the potential for irreversible phase transitions during OER.Consequently,significant efforts have been devoted to study the dynamic evolution of oxygen defects to shed light on the OER mechanism.This review critically examines and analyzes the dynamic processes occurring at oxygen defect sites during OER,including defect formation and defect evolution mechanisms,along with the advanced characterization techniques needed to understand these processes.This review aims to provide a comprehensive understanding of high-efficiency electrocatalysts,with a particular emphasis on the importance of in situ monitoring the dynamic evolution of oxygen defects,providing a new perspective towards efficient OER electrocatalyst design.展开更多
In recent times there has been a great deal of interest in the conversion of carbon dioxide into more useful chemical compounds.On the other hand,the translation of these developments in electrochemical reduction of c...In recent times there has been a great deal of interest in the conversion of carbon dioxide into more useful chemical compounds.On the other hand,the translation of these developments in electrochemical reduction of carbon dioxide from the laboratory bench to practical scale remains an underexplored topic.Here we examine some of the major challenges,demonstrating some promising strategies towards such scale-up,including increased electrode area and stacking of electrode pairs in different configurations.We observed that increasing the electrode area from 1 to 10 cm^(2) led to only a 4%drop in current density,with similarly small penalties realised when stacking sub-cells together.展开更多
Photosensitized heterogeneous CO_(2) reduction(PHCR)has emerged as a promising means to convert CO_(2) into valuable chemicals,however,challenged by the relatively low carbonaceous product selectivity caused by the co...Photosensitized heterogeneous CO_(2) reduction(PHCR)has emerged as a promising means to convert CO_(2) into valuable chemicals,however,challenged by the relatively low carbonaceous product selectivity caused by the competing hydrogen evolution reaction(HER).Here,we report a PHCR system that couples Ru(bpy)32+photosensitizer with{001}faceted LiCoO_(2) nanosheets photocatalyst to simultaneously yield 21.2 and 722μmol·g^(-1)·h^(-1) of CO,and 4.42 and 108μmol·g^(-1)·h^(-1) of CH4 under the visible light and the simulated sunlight irradiations,respectively,with completely suppressed HER.The experimental and theoretical studies reveal that the favored CO_(2) adsorption on the exposed Li sites on{001}faceted LiCoO_(2) surface is responsible for the completely suppressed HER.展开更多
基金supported by the Ministry of Science and Technology(MOST)of China through the Key Project of Research&Development(2021YFF0500502)。
文摘Oxygen defects play a critical role in the electrocatalytic oxygen evolution reaction(OER).Therefore,in-depth understanding the structure-activity-mechanism relationship of these defects is the key to design efficient OER electrocatalysts.This relationship needs to be understood dynamically due to the potential for irreversible phase transitions during OER.Consequently,significant efforts have been devoted to study the dynamic evolution of oxygen defects to shed light on the OER mechanism.This review critically examines and analyzes the dynamic processes occurring at oxygen defect sites during OER,including defect formation and defect evolution mechanisms,along with the advanced characterization techniques needed to understand these processes.This review aims to provide a comprehensive understanding of high-efficiency electrocatalysts,with a particular emphasis on the importance of in situ monitoring the dynamic evolution of oxygen defects,providing a new perspective towards efficient OER electrocatalyst design.
基金Funding from the Australian Research Council Centre of Excellence Scheme(Project Number CE 140100012)is gratefully acknowledged.
文摘In recent times there has been a great deal of interest in the conversion of carbon dioxide into more useful chemical compounds.On the other hand,the translation of these developments in electrochemical reduction of carbon dioxide from the laboratory bench to practical scale remains an underexplored topic.Here we examine some of the major challenges,demonstrating some promising strategies towards such scale-up,including increased electrode area and stacking of electrode pairs in different configurations.We observed that increasing the electrode area from 1 to 10 cm^(2) led to only a 4%drop in current density,with similarly small penalties realised when stacking sub-cells together.
基金supported by Australian Research Council Discovery Projects(Nos.DP170104834 and DP200100965)。
文摘Photosensitized heterogeneous CO_(2) reduction(PHCR)has emerged as a promising means to convert CO_(2) into valuable chemicals,however,challenged by the relatively low carbonaceous product selectivity caused by the competing hydrogen evolution reaction(HER).Here,we report a PHCR system that couples Ru(bpy)32+photosensitizer with{001}faceted LiCoO_(2) nanosheets photocatalyst to simultaneously yield 21.2 and 722μmol·g^(-1)·h^(-1) of CO,and 4.42 and 108μmol·g^(-1)·h^(-1) of CH4 under the visible light and the simulated sunlight irradiations,respectively,with completely suppressed HER.The experimental and theoretical studies reveal that the favored CO_(2) adsorption on the exposed Li sites on{001}faceted LiCoO_(2) surface is responsible for the completely suppressed HER.
