期刊
ACS APPLIED MATERIALS & INTERFACES
卷 10, 期 43, 页码 36866-36872出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b10394
关键词
single-atom catalyst; boron monolayer; one-pot; CO2 capture and activation; CO2 reduction
资金
- National Key R&D Program of China [2017YFA0204800]
- National Natural Science Funds of China [21525311, 21773027]
- Jiangsu 333 project [BRA2016353]
- China Scholarship Council (CSC) [201706090115]
- Fundamental Research Funds for the Central Universities
- Australian Research Council [DP170103598]
- Australian Government
- Government of Western Australia
- Postgraduate Research & Practice Innovation Program of Jiangsu Province in China [KYCX17_0044]
Lowering the concentration of CO2 in atmosphere is a global concern but yet remains one of the most challenging processes in chemistry. Herein, we report a rational design of single atom catalyst (SAC), namely, vanadium atom supported on newly synthesized beta(12) boron monolayer (V-1/beta(12)-BM), for one-pot CO2 capture, activation, and efficient conversion into methanol. Our first principles computations reveal that strong interaction ensures V-1/beta(12)-BM can capture CO2 at ambient and elevated temperatures. Substantial charge transfer between V-1/beta(12)-BM and CO2 triggers the activation of CO2 into anionic CO2-, which can be efficiently hydrogenated into CH3OH with an ultralow limiting potential of 0.54 V and a rather low rate-determining barrier of 1.04 eV. Moreover, the adsorption of H2O molecules can make the reaction intermediates closer to the hydrogen source by the steric hindrance, which plays a key role in lowering the reaction barrier. Our findings present the first SAC for one-pot CO2 capture, activation, and conversion, which may open a new avenue for recycling CO2.
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