Highly Efficient and Selective Methanol Production from Paraformaldehyde and Water at Room Temperature

Wang, Lin; Ertem, Mehmed Z.; Murata, Kazuhisa; Muckerman, James T.; Fujita, Etsuko; Himeda, Yuichiro

doi:10.1021/acscatal.8b00321

Title: Highly Efficient and Selective Methanol Production from Paraformaldehyde and Water at Room Temperature

Journal Article · 30 April 2018 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.8b00321 · OSTI ID:1460702

Wang, Lin ^[1]; Ertem, Mehmed Z. ^[2]; Murata, Kazuhisa ^[1]; Muckerman, James T. ^[2];

^[2];

^[1]

National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan). Research Inst. of Energy Frontier. Dept. of Energy and Environment
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division

In this paper, an efficient catalytic system using a water-soluble iridium complex, Cp*IrL(OH₂)²⁺ (Cp* = pentamethylcyclopentadienyl, L = 2,2',6,6'-tetrahydroxy-4,4'-bipyrimidine), was developed for highly selective methanol production at room temperature (initial turnover frequency of 4120 h^–1) with a very high yield (93%). This catalytic system features paraformaldehyde as the sole carbon and hydride source, leading to a record turnover number of 18200 at 25 °C. A step-by-step mechanism has been proposed for the catalytic conversion of paraformaldehyde to methanol on the basis of density functional theory (DFT) calculations. Finally, the proposed pathway holds the potential capacity to extend the scope of indirect routes for methanol production from CO₂.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States); National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)

Sponsoring Organization:: ENEOS Hydrogen Trust Fund (Japan); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1460702

Report Number(s):: BNL-207839-2018-JAAM

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 6 Vol. 8; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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homogeneous catalysis
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transformation of paraformaldehyde

Title: Highly Efficient and Selective Methanol Production from Paraformaldehyde and Water at Room Temperature

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