Promoted CO2 photoreduction toward HCOOH generation through a nucleophilic effect in Co/Mg synergistic catalysis.

Autor: Luyao Wang, Siqi You, Yaru Gong, Jianxia Gu, Jiangwei Zhang, Guogang Shan, Bo Zhu, Weiting Yang, Chunyi Sun, Xinlong Wang, Zhongmin Su
Předmět:
Zdroj: Green Chemistry; 9/7/2024, Vol. 26 Issue 17, p9415-9422, 8p
Abstrakt: The photoreduction of carbon dioxide (CO2) into valuable energy is one of the most promising strategies to overcome the current global climate crisis. The synergistic catalysis of bimetallic metal--organic frameworks (MOFs) has shown considerable potential for the photocatalytic reduction of CO2. However, how to design an efficient catalytic active center is still a thorny problem. Herein, a bimetallic MOF, CoMg- TCPP, was successfully prepared via a post-synthetic exchange method. Under visible light, CoMg-TCPP can be an efficient catalyst for CO2 reduction with yields of gas product (CO) and liquid product (HCOOH) of up to 14.34 mmol g-1 h-1 and 0.94 mmol g-1 h-1, respectively. Notably, the synergistic effect between the bimetals in CoMg-TCPP generated formic acid with an yield more than twice that generated by the monometallic counterpart Co-TCPP. Theoretical calculations show that the introduction of the second metal regulates the electronic structure of intermediates, which reduces the formation energy barrier of Co--O--COH intermediates and significantly promotes the formation of Co--HCOOH, thus obtaining efficient HCOOH generation performance. Moreover, the addition of Mg to Co-TCPP enhances the nucleophilicity of the Co center and makes it more inclined to interact with O--COH groups. This work provides further insights into the mechanisms of CO2 photocatalytic reduction based on a bimetal-- organic framework. [ABSTRACT FROM AUTHOR]
Databáze: Complementary Index