Electrochemical carbon dioxide reduction(CO_(2)RR)has been generally regarded as green technologies that can convert renewable energy such as sunlight and wind into fuels and valuable chemicals.However,the large‐scal...Electrochemical carbon dioxide reduction(CO_(2)RR)has been generally regarded as green technologies that can convert renewable energy such as sunlight and wind into fuels and valuable chemicals.However,the large‐scale implementation of CO_(2)RR is severely hindered by the lack of high‐performance CO_(2)RR electrocatalysts.Heterogeneous molecular catalysts and metal‐organic framework with well‐defined structure and high tunability of the metal centers and ligands show great promise for CO_(2)RR in terms of both fundamental understanding and practical application.Here,structural and interfacial engineering of these well‐defined metal‐organic ensembles is summarized.This review starts from the fundamental electrochemistry of CO_(2)RR and its evaluation criteria,and then moves to the heterogeneous molecular catalysts and metal‐organic framework with emphasis on the engineering of metal centers and ligands,their interaction with supports,as well as in situ reconstruction of metal‐organic ensembles.Summary and outlook are present in the end,with the hope to inspire and provoke more genuine thinking on the design and fabrication of efficient CO_(2)RR electrocatalysts.展开更多
Oxygen evolution reaction(OER)plays a key role in the electrochemical conversion and storage processes,but the sluggish kinetics of OER strongly impedes its large-scale applications.We herein reported the in situ grow...Oxygen evolution reaction(OER)plays a key role in the electrochemical conversion and storage processes,but the sluggish kinetics of OER strongly impedes its large-scale applications.We herein reported the in situ growth of Fe-benzenedicarboxylate(Fe-BDC)on Co(OH)_(2) nanoplates[Fe-BDC/Co(OH)_(2)]that showed remarkably enhanced OER activity than the pristine Co(OH)_(2).The incorporation of Fe species could enhance the intrinsic OER activity of Co and BDC could increase the electrochemically active surface area(ECSA),thus resulting in dramatically enhanced OER activity.In situ Raman spectroscopy characterization disclosed that Fe-CoOOH reconstructed from Fe-BDC/Co(OH)_(2) was the real active site for OER.This work highlights the significance of rational tailoring of the nanostructure and electronic structure of Co(OH)_(2) and provides more opportunities for its widespread applications.展开更多
文摘Electrochemical carbon dioxide reduction(CO_(2)RR)has been generally regarded as green technologies that can convert renewable energy such as sunlight and wind into fuels and valuable chemicals.However,the large‐scale implementation of CO_(2)RR is severely hindered by the lack of high‐performance CO_(2)RR electrocatalysts.Heterogeneous molecular catalysts and metal‐organic framework with well‐defined structure and high tunability of the metal centers and ligands show great promise for CO_(2)RR in terms of both fundamental understanding and practical application.Here,structural and interfacial engineering of these well‐defined metal‐organic ensembles is summarized.This review starts from the fundamental electrochemistry of CO_(2)RR and its evaluation criteria,and then moves to the heterogeneous molecular catalysts and metal‐organic framework with emphasis on the engineering of metal centers and ligands,their interaction with supports,as well as in situ reconstruction of metal‐organic ensembles.Summary and outlook are present in the end,with the hope to inspire and provoke more genuine thinking on the design and fabrication of efficient CO_(2)RR electrocatalysts.
基金National Key R&D Program of China(No.2020YFB1505703)National Natural Science Foundation of China(Nos.22072101,22075193)+3 种基金Natural Science Foundation of Jiangsu Province,China(Nos.BK20211306,BK20220483)Fund of the Key Technology Initiative of Suzhou Municipal Science and Technology Bureau,China(No.SYG201934)Six Talent Peaks Project in Jiangsu Province,China(No.TD-XCL-006)Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutions,China.
文摘Oxygen evolution reaction(OER)plays a key role in the electrochemical conversion and storage processes,but the sluggish kinetics of OER strongly impedes its large-scale applications.We herein reported the in situ growth of Fe-benzenedicarboxylate(Fe-BDC)on Co(OH)_(2) nanoplates[Fe-BDC/Co(OH)_(2)]that showed remarkably enhanced OER activity than the pristine Co(OH)_(2).The incorporation of Fe species could enhance the intrinsic OER activity of Co and BDC could increase the electrochemically active surface area(ECSA),thus resulting in dramatically enhanced OER activity.In situ Raman spectroscopy characterization disclosed that Fe-CoOOH reconstructed from Fe-BDC/Co(OH)_(2) was the real active site for OER.This work highlights the significance of rational tailoring of the nanostructure and electronic structure of Co(OH)_(2) and provides more opportunities for its widespread applications.
