TY - JOUR
T1 - Performance enhancing additives for reusable ruthenium-triphos catalysts in the reduction of CO2to dimethoxymethane
AU - Konrath, Robert
AU - Sekine, Kohei
AU - Jevtovikj, Ivana
AU - Paciello, Rocco A.
AU - Hashmi, A. Stephen K.
AU - Schaub, Thomas
N1 - Funding Information:
The authors are grateful to funding by the German Federal Ministry of Education and Research (BMBF) within the funding initiative ‘CO2Plus – Stoffliche Nutzung von CO2 zur Verbreiterung der Rohstoffbasis’. CaRLa (Catalysis Research Laboratory) is co-financed by the Heidelberg University and BASF SE.
Publisher Copyright:
© The Royal Society of Chemistry.
Copyright:
Copyright 2020 Elsevier B.V., All rights reserved.
PY - 2020/10/7
Y1 - 2020/10/7
N2 - The direct access to dimethoxymethane (DMM) from CO2/H2 in MeOH is an attractive approach, but more active, selective, and robust catalyst systems are still desirable for an application of this system. Herein, we present the performance enhancing effect of additives on ruthenium-triphos catalyst systems for CO2 hydrogenation to DMM. In the presence of PPh3, functioning as both additional ligand and precursor for Lewis-acidic phosphonium salts, increased turnover numbers for DMM are achieved. Moreover, PPh3 significantly diminishes catalyst degradation via carbonylation to cationic [RuH(CO)2(triphos)]OTf, which remains an active species in the synthesis of DMM. Catalyst recycling over up to five runs with minimal loss in catalyst performance underlines the robustness of the system. Both, the recyclability of the system and the suppression of catalyst deactivation pathways encourage for application in sustainable continuous processes. This journal is
AB - The direct access to dimethoxymethane (DMM) from CO2/H2 in MeOH is an attractive approach, but more active, selective, and robust catalyst systems are still desirable for an application of this system. Herein, we present the performance enhancing effect of additives on ruthenium-triphos catalyst systems for CO2 hydrogenation to DMM. In the presence of PPh3, functioning as both additional ligand and precursor for Lewis-acidic phosphonium salts, increased turnover numbers for DMM are achieved. Moreover, PPh3 significantly diminishes catalyst degradation via carbonylation to cationic [RuH(CO)2(triphos)]OTf, which remains an active species in the synthesis of DMM. Catalyst recycling over up to five runs with minimal loss in catalyst performance underlines the robustness of the system. Both, the recyclability of the system and the suppression of catalyst deactivation pathways encourage for application in sustainable continuous processes. This journal is
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U2 - 10.1039/d0gc02528c
DO - 10.1039/d0gc02528c
M3 - Article
AN - SCOPUS:85095956886
VL - 22
SP - 6464
EP - 6470
JO - Green Chemistry
JF - Green Chemistry
SN - 1463-9262
IS - 19
ER -