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Journal Article
Review
Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction.
ACS Nano 2024 March 29
With the increasingly serious greenhouse effect, the electrochemical carbon dioxide reduction reaction (CO2 RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, the performance of CO2 RR can hardly meet expectations because of the diverse intermediates and complicated reaction processes, necessitating the exploitation of highly efficient catalysts. In recent years, with advanced characterization technologies and theoretical simulations, the exploration of catalytic mechanisms has gradually deepened into the electronic structure of catalysts and their interactions with intermediates, which serve as a bridge to facilitate the deeper comprehension of structure-performance relationships. Transition metal-based catalysts (TMCs), extensively applied in electrochemical CO2 RR, demonstrate substantial potential for further electronic structure modulation, given their abundance of d electrons. Herein, we discuss the representative feasible strategies to modulate the electronic structure of catalysts, including doping, vacancy, alloying, heterostructure, strain, and phase engineering. These approaches profoundly alter the inherent properties of TMCs and their interaction with intermediates, thereby greatly affecting the reaction rate and pathway of CO2 RR. It is believed that the rational electronic structure design and modulation can fundamentally provide viable directions and strategies for the development of advanced catalysts toward efficient electrochemical conversion of CO2 and many other small molecules.
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