期刊
SCIENCE ADVANCES
卷 7, 期 13, 页码 -出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.abf3989
关键词
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资金
- National Research Foundation (NRF), Prime Minister's Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) program
- academic research fund AcRF tier 1, Ministry of Education, Singapore [M4012076 RG118/18]
Heterogeneous molecular catalysts based on transition metal complexes are increasingly being studied for their potential use in electrochemical energy conversion. This review discusses how tuning the first and second coordination spheres of these complexes can optimize their activities and serve as models for studying the impact of structural variations on activity. Structural tuning, such as adjusting ligated atoms and appending adjacent metal centers or pendant groups, can result in different geometric and electronic configurations of the complexes, ultimately leading to improved activity through stability adjustments and redox behaviors.
Heterogeneous molecular catalysts based on transition metal complexes have received increasing attention for their potential application in electrochemical energy conversion. The structural tuning of first and second coordination spheres of complexes provides versatile strategies for optimizing the activities of heterogeneous molecular catalysts and appropriate model systems for investigating the mechanism of structural variations on the activity. In this review, we first discuss the variation of first spheres by tuning ligated atoms; afterward, the structural tuning of second spheres by appending adjacent metal centers, pendant groups, electron withdrawing/donating, and conjugating moieties on the ligands is elaborated. Overall, these structural tuning resulted in different impacts on the geometric and electronic configurations of complexes, and the improved activity is achieved through tuning the stability of chemisorbed reactants and the redox behaviors of immobilized complexes.
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