Discovery of single-atom alloy catalysts for CO2-to-methanol reaction by density functional theory calculations

Li, Meng; Hua, Bin; Wang, Lu-Cun; Zhou, Zheng; Stowers, Kara J.; Ding, Dong

doi:10.1016/j.cattod.2020.04.059

Title: Discovery of single-atom alloy catalysts for CO₂-to-methanol reaction by density functional theory calculations

Journal Article · Thu May 07 04:00:00 UTC 2020 · Catalysis Today

DOI: https://doi.org/10.1016/j.cattod.2020.04.059 · OSTI ID:1897469

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^[2]; Stowers, Kara J. ^[3];

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Idaho National Lab. (INL), Idaho Falls, ID (United States)
Idaho National Lab. (INL), Idaho Falls, ID (United States); Brigham Young Univ., Provo, UT (United States)
Brigham Young Univ., Provo, UT (United States)

The transformations of CO₂ molecules into valuable products are of increasing interest due to the negative impact of anthropogenic CO₂ emissions on global warming. The CO₂-to-methanol hydrogenation is an economically profitable reaction of carbon fixation, but it still steps away from widespread industrialization because of the lack of efficient and selective catalysts. Recently, single-atom alloy (SAA) catalysts have been developed to work remarkably in CO₂ hydrogenation reactions. Doping isolated single atoms into metallic catalyst can dramatically alter the catalytic performance of the host. Here, we have performed a screening discovery on Ru and 6 RuX (X = Fe, Co, Ni, Cu, Ir and Pt) SAAs using density functional theory (DFT) computations. We considered 13 possible elementary reactions in 4 possible reaction pathways on Ru and all RuX surfaces. In the computed mechanisms, we found that the formation of *H₂COOH and *HCOO intermediates plays a critical role in determining catalysts’ activities. Doping Co and Pt isolated single atoms into Ru surface can thermodynamically and kinetically facilitate these intermediates formation processes, eventually promoting the production of methanol. The combination of weak binding and enhanced charge redistribution on RuCo and RuPt surfaces give them improved catalytic activities over pure Ru. This work will ultimately facilitate the discovery and development of SAAs for CO₂ to methanol, serving as guidance to experiments and theoreticians alike.

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Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 1897469

Report Number(s):: INL/JOU-20-57655-Rev000

Journal Information:: Catalysis Today, Journal Name: Catalysis Today Vol. 388-389; ISSN 0920-5861

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
36 MATERIALS SCIENCE
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Title: Discovery of single-atom alloy catalysts for CO2-to-methanol reaction by density functional theory calculations

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Title: Discovery of single-atom alloy catalysts for CO₂-to-methanol reaction by density functional theory calculations