Selective CO2 reduction to CH3OH over atomic dual-metal sites embedded in a metal-organic framework with high-energy radiation

Changjiang Hu, Zhiwen Jiang, Qunyan Wu, Shuiyan Cao, Qiuhao Li, Chong Chen, Liyong Yuan, Yunlong Wang, Wenyun Yang, Jinbo Yang, Jing Peng, Weiqun Shi, Maolin Zhai (), Mehran Mostafavi () and Jun Ma ()
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Changjiang Hu: Nanjing University of Aeronautics and Astronautics
Zhiwen Jiang: Nanjing University of Aeronautics and Astronautics
Qunyan Wu: Chinese Academy of Sciences
Shuiyan Cao: College of Physics, Nanjing University of Aeronautics and Astronautics
Qiuhao Li: Nanjing University of Aeronautics and Astronautics
Chong Chen: Nanjing University of Aeronautics and Astronautics
Liyong Yuan: Chinese Academy of Sciences
Yunlong Wang: Nanjing University of Aeronautics and Astronautics
Wenyun Yang: Peking University
Jinbo Yang: Peking University
Jing Peng: Peking University
Weiqun Shi: Chinese Academy of Sciences
Maolin Zhai: Peking University
Mehran Mostafavi: UMR8000 CNRS/Université Paris-Saclay
Jun Ma: Nanjing University of Aeronautics and Astronautics

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract The efficient use of renewable X/γ-rays or accelerated electrons for chemical transformation of CO2 and water to fuels holds promise for a carbon-neutral economy; however, such processes are challenging to implement and require the assistance of catalysts capable of sensitizing secondary electron scattering and providing active metal sites to bind intermediates. Here we show atomic Cu-Ni dual-metal sites embedded in a metal-organic framework enable efficient and selective CH3OH production (~98%) over multiple irradiated cycles. The usage of practical electron-beam irradiation (200 keV; 40 kGy min−1) with a cost-effective hydroxyl radical scavenger promotes CH3OH production rate to 0.27 mmol g−1 min−1. Moreover, time-resolved experiments with calculations reveal the direct generation of CO2•‒ radical anions via aqueous electrons attachment occurred on nanosecond timescale, and cascade hydrogenation steps. Our study highlights a radiolytic route to produce CH3OH with CO2 feedstock and introduces a desirable atomic structure to improve performance.

Date: 2023
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DOI: 10.1038/s41467-023-40418-3

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