Photocatalytic CO2 reduction using La-Ni bimetallic sites within a covalent organic framework

Min Zhou, Zhiqing Wang, Aohan Mei, Zifan Yang, Wen Chen, Siyong Ou, Shengyao Wang (), Keqiang Chen (), Peter Reiss (), Kun Qi, Jingyuan Ma and Yueli Liu ()
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Min Zhou: Wuhan University of Technology
Zhiqing Wang: Wuhan University of Technology
Aohan Mei: Wuhan University of Technology
Zifan Yang: Wuhan University of Technology
Wen Chen: Wuhan University of Technology
Siyong Ou: Wuhan University of Technology
Shengyao Wang: Huazhong Agricultural University
Keqiang Chen: Wuhan University of Technology
Peter Reiss: Univ. Grenoble-Alpes, CEA, CNRS, IRIG/SyMMES, STEP
Kun Qi: Université Montpellier, ENSCM, CNRS
Jingyuan Ma: Chinese Academy of Sciences
Yueli Liu: Wuhan University of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract The precise construction of photocatalysts with diatomic sites that simultaneously foster light absorption and catalytic activity is a formidable challenge, as both processes follow distinct pathways. Herein, an electrostatically driven self-assembly approach is used, where phenanthroline is used to synthesize bifunctional LaNi sites within covalent organic framework. The La and Ni site acts as optically and catalytically active center for photocarriers generation and highly selective CO2-to-CO reduction, respectively. Theory calculations and in-situ characterization reveal the directional charge transfer between La-Ni double-atomic sites, leading to decreased reaction energy barriers of *COOH intermediate and enhanced CO2-to-CO conversion. As a result, without any additional photosensitizers, a 15.2 times enhancement of the CO2 reduction rate (605.8 μmol·g−1·h−1) over that of a benchmark covalent organic framework colloid (39.9 μmol·g−1·h−1) and improved CO selectivity (98.2%) are achieved. This work presents a potential strategy for integrating optically and catalytically active centers to enhance photocatalytic CO2 reduction.

Date: 2023
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DOI: 10.1038/s41467-023-37545-2

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