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

Abstract

In this paper, an efficient catalytic system using a water-soluble iridium complex, Cp*IrL(OH 2) 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 CO 2.

Authors:
 [1];  [2];  [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan). Research Inst. of Energy Frontier. Dept. of Energy and Environment
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); ENEOS Hydrogen Trust Fund (Japan)
OSTI Identifier:
1460702
Report Number(s):
BNL-207839-2018-JAAM
Journal ID: ISSN 2155-5435
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 8; Journal Issue: 6; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; homogeneous catalysis; iridium complexes; methanol production; proton-responsive ligand; transformation of paraformaldehyde

Citation Formats

Wang, Lin, Ertem, Mehmed Z., Murata, Kazuhisa, Muckerman, James T., Fujita, Etsuko, and Himeda, Yuichiro. Highly Efficient and Selective Methanol Production from Paraformaldehyde and Water at Room Temperature. United States: N. p., 2018. Web. doi:10.1021/acscatal.8b00321.
Wang, Lin, Ertem, Mehmed Z., Murata, Kazuhisa, Muckerman, James T., Fujita, Etsuko, & Himeda, Yuichiro. Highly Efficient and Selective Methanol Production from Paraformaldehyde and Water at Room Temperature. United States. doi:10.1021/acscatal.8b00321.
Wang, Lin, Ertem, Mehmed Z., Murata, Kazuhisa, Muckerman, James T., Fujita, Etsuko, and Himeda, Yuichiro. Tue . "Highly Efficient and Selective Methanol Production from Paraformaldehyde and Water at Room Temperature". United States. doi:10.1021/acscatal.8b00321. https://www.osti.gov/servlets/purl/1460702.
@article{osti_1460702,
title = {Highly Efficient and Selective Methanol Production from Paraformaldehyde and Water at Room Temperature},
author = {Wang, Lin and Ertem, Mehmed Z. and Murata, Kazuhisa and Muckerman, James T. and Fujita, Etsuko and Himeda, Yuichiro},
abstractNote = {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.},
doi = {10.1021/acscatal.8b00321},
journal = {ACS Catalysis},
number = 6,
volume = 8,
place = {United States},
year = {2018},
month = {5}
}

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Works referencing / citing this record:

Metallo-supramolecular assembly of protic pincer-type complexes: encapsulation of dinitrogen and carbon disulfide into a multiproton-responsive diruthenium cage
journal, January 2019

  • Toda, Tatsuro; Suzuki, Satoshi; Kuwata, Shigeki
  • Chemical Communications, Vol. 55, Issue 8
  • DOI: 10.1039/c8cc08384c

Metallo-supramolecular assembly of protic pincer-type complexes: encapsulation of dinitrogen and carbon disulfide into a multiproton-responsive diruthenium cage
journal, January 2019

  • Toda, Tatsuro; Suzuki, Satoshi; Kuwata, Shigeki
  • Chemical Communications, Vol. 55, Issue 8
  • DOI: 10.1039/c8cc08384c