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Title: Catalytic coproduction of methanol and glycol in one pot from epoxide, CO2, and H2

Abstract

An atom (100%) and energy-efficient approach to coproduce two commodity chemicals, methanol and glycol, has been demonstrated for the first time using H2, CO2, and epoxide as feeds. A basic medium used for CO2 capture, polyethyleneimine (PEI600), is shown to facilitate the formation of a key reaction intermediate, cyclic carbonates. Upon hydrogenation of cyclic carbonates in the presence of a homogenous Ru-PNP catalyst, a 1 : 1 mixture of methanol and glycol is produced. This approach has been demonstrated in one pot by adding all the required reactants directly or stepwise. The stepwise addition of reactants resulted in good yields (>95% for PG and 84% for methanol) and selectivity of products.

Authors:
ORCiD logo [1]; ORCiD logo [2]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1734647
Report Number(s):
PNNL-SA-153614
Journal ID: ISSN 2046-2069
Grant/Contract Number:  
AC05-76RL01830; FWP-67038
Resource Type:
Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 10; Journal Issue: 69; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kothandaraman, Jotheeswari, and Heldebrant, David J. Catalytic coproduction of methanol and glycol in one pot from epoxide, CO2, and H2. United States: N. p., 2020. Web. https://doi.org/10.1039/d0ra09459e.
Kothandaraman, Jotheeswari, & Heldebrant, David J. Catalytic coproduction of methanol and glycol in one pot from epoxide, CO2, and H2. United States. https://doi.org/10.1039/d0ra09459e
Kothandaraman, Jotheeswari, and Heldebrant, David J. Tue . "Catalytic coproduction of methanol and glycol in one pot from epoxide, CO2, and H2". United States. https://doi.org/10.1039/d0ra09459e. https://www.osti.gov/servlets/purl/1734647.
@article{osti_1734647,
title = {Catalytic coproduction of methanol and glycol in one pot from epoxide, CO2, and H2},
author = {Kothandaraman, Jotheeswari and Heldebrant, David J.},
abstractNote = {An atom (100%) and energy-efficient approach to coproduce two commodity chemicals, methanol and glycol, has been demonstrated for the first time using H2, CO2, and epoxide as feeds. A basic medium used for CO2 capture, polyethyleneimine (PEI600), is shown to facilitate the formation of a key reaction intermediate, cyclic carbonates. Upon hydrogenation of cyclic carbonates in the presence of a homogenous Ru-PNP catalyst, a 1 : 1 mixture of methanol and glycol is produced. This approach has been demonstrated in one pot by adding all the required reactants directly or stepwise. The stepwise addition of reactants resulted in good yields (>95% for PG and 84% for methanol) and selectivity of products.},
doi = {10.1039/d0ra09459e},
journal = {RSC Advances},
number = 69,
volume = 10,
place = {United States},
year = {2020},
month = {11}
}

Journal Article:
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