Bioinspired Metal–Organic Framework Catalysts for Selective Methane Oxidation to Methanol

Baek, Jayeon; Rungtaweevoranit, Bunyarat; Pei, Xiaokun; Park, Myeongkee; Fakra, Sirine C.; Liu, Yi-Sheng; Matheu, Roc; Alshmimri, Sultan A.; Alshehri, Saeed; Trickett, Christopher A.; Somorjai, Gabor A.; Yaghi, Omar M.

doi:10.1021/jacs.8b11525

Title: Bioinspired Metal–Organic Framework Catalysts for Selective Methane Oxidation to Methanol

Journal Article · 09 December 2018 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.8b11525 · OSTI ID:1656485

^[1]; Rungtaweevoranit, Bunyarat ^[2]; Pei, Xiaokun ^[1];

^[3]; Fakra, Sirine C. ^[4]; Liu, Yi-Sheng ^[4];

^[1]; Alshmimri, Sultan A. ^[5]; Alshehri, Saeed ^[5]; Trickett, Christopher A. ^[1];

^[6];

^[1]

Kavli Energy NanoScience Institute, Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States). Berkeley Global Science Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Kavli Energy NanoScience Institute, Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States). Berkeley Global Science Inst.
Dong-A Univ., Busan (South Korea)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
King Abdulaziz City for Science and Technology, Riyadh (Saudi Arabia)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

Particulate methane monooxygenase (pMMO) is an enzyme that oxidizes methane to methanol with high activity and selectivity. Limited success has been achieved in incorporating biologically relevant ligands for the formation of such active site in a synthetic system. In this work, we report the design and synthesis of metal-organic framework (MOF) catalysts inspired by pMMO for selective methane oxidation to methanol. Furthermore, my judicious selection of a framework with appropriate topology and chemical functionality, MOF-808 was used to postsynthetically install ligands bearing imidazole units for subsequent metalation with Cu(I) in the presence of dioxygen. The catalysts show high selectivity for methane oxidation to methanol under isothermal conditions at 150 °C. Combined spectroscopies and density functional theory calculations suggest bis(μ-oxo) dicopper species as probable active site of the catalysts.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Institutes of Health (NIH); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1656485

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 51 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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