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Title: Additive-Free Ruthenium-Catalyzed Hydrogen Production from Aqueous Formaldehyde with High Efficiency and Selectivity

Abstract

In this study, an efficient water-soluble ruthenium complex was developed for selective hydrogen production from aqueous formaldehyde under mild conditions with a high yield (~95%). Hydrogen production by this catalytic system proceeds without using any additives or organic solvents, leading to a high turnover frequency (8300 h –1) and a record turnover number of 24 000. Additionally, based on mechanistic experiments and density functional theory (DFT) calculations, a step-by-step mechanism has been proposed for the catalytic cycle.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [1];  [3];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. National Institute of Advanced Industrial Science and Technology (Japan). Research Institute of Energy Frontier, Department of Energy and Environment
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  3. Baruch College, CUNY, New York, NY (United States). Department of Natural Sciences
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1473638
Report Number(s):
BNL-209075-2018-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: 9; 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; dehydrogenation; formaldehyde; H2 production; homogeneous catalysis; ruthenium complex

Citation Formats

Wang, Lin, Ertem, Mehmed Z., Kanega, Ryoichi, Murata, Kazuhisa, Szalda, David J., Muckerman, James T., Fujita, Etsuko, and Himeda, Yuichiro. Additive-Free Ruthenium-Catalyzed Hydrogen Production from Aqueous Formaldehyde with High Efficiency and Selectivity. United States: N. p., 2018. Web. doi:10.1021/acscatal.8b02088.
Wang, Lin, Ertem, Mehmed Z., Kanega, Ryoichi, Murata, Kazuhisa, Szalda, David J., Muckerman, James T., Fujita, Etsuko, & Himeda, Yuichiro. Additive-Free Ruthenium-Catalyzed Hydrogen Production from Aqueous Formaldehyde with High Efficiency and Selectivity. United States. doi:10.1021/acscatal.8b02088.
Wang, Lin, Ertem, Mehmed Z., Kanega, Ryoichi, Murata, Kazuhisa, Szalda, David J., Muckerman, James T., Fujita, Etsuko, and Himeda, Yuichiro. Thu . "Additive-Free Ruthenium-Catalyzed Hydrogen Production from Aqueous Formaldehyde with High Efficiency and Selectivity". United States. doi:10.1021/acscatal.8b02088. https://www.osti.gov/servlets/purl/1473638.
@article{osti_1473638,
title = {Additive-Free Ruthenium-Catalyzed Hydrogen Production from Aqueous Formaldehyde with High Efficiency and Selectivity},
author = {Wang, Lin and Ertem, Mehmed Z. and Kanega, Ryoichi and Murata, Kazuhisa and Szalda, David J. and Muckerman, James T. and Fujita, Etsuko and Himeda, Yuichiro},
abstractNote = {In this study, an efficient water-soluble ruthenium complex was developed for selective hydrogen production from aqueous formaldehyde under mild conditions with a high yield (~95%). Hydrogen production by this catalytic system proceeds without using any additives or organic solvents, leading to a high turnover frequency (8300 h–1) and a record turnover number of 24 000. Additionally, based on mechanistic experiments and density functional theory (DFT) calculations, a step-by-step mechanism has been proposed for the catalytic cycle.},
doi = {10.1021/acscatal.8b02088},
journal = {ACS Catalysis},
number = 9,
volume = 8,
place = {United States},
year = {2018},
month = {8}
}

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