Design Strategy toward Recyclable and Highly Efficient Heterogeneous Catalysts for the Hydrogenation of CO2 to Formate

Authors
Gunasekar, Gunniya HariyanandamShin, JeongcheolJung, Kwang-DeogPark, KiyoungYoon, Sungho
Issue Date
2018-05
Publisher
AMER CHEMICAL SOC
Citation
ACS CATALYSIS, v.8, no.5, pp.4346 - 4353
Abstract
One bottleneck in the realization of CO2 conversion into value-added compounds is the lack of catalysts with both excellent activity and recyclability. Herein, a catalyst is designed for the hydrogenation of CO2 to formate to boost up these features by considering the leaching pathway of previously reported heterogenized catalyst; the design strategy incorporates oxyanionic ligand(s) in the coordination sphere to provide a pathway for both preventing the deleterious interactions and assisting the heterolysis of H-2. The tailored heterogenized catalyst, [bpy-CTF-Ru(acac)(2)]Cl, demonstrated excellent recyclability over consecutive runs with a highest turnover frequency of 22 700 h(-1), and produced a highest formate concentration of 1.8 M in 3 h. This work is significant in elucidating new principles for the development of industrially viable hydrogenation catalysts.
Keywords
EFFECTIVE CORE POTENTIALS; COVALENT ORGANIC FRAMEWORKS; IR-III COMPLEXES; CARBON-DIOXIDE; FORMIC-ACID; MOLECULAR CALCULATIONS; HOMOGENEOUS HYDROGENATION; AMBIENT-TEMPERATURE; IRIDIUM COMPLEX; GRAPHENE OXIDE; EFFECTIVE CORE POTENTIALS; COVALENT ORGANIC FRAMEWORKS; IR-III COMPLEXES; CARBON-DIOXIDE; FORMIC-ACID; MOLECULAR CALCULATIONS; HOMOGENEOUS HYDROGENATION; AMBIENT-TEMPERATURE; IRIDIUM COMPLEX; GRAPHENE OXIDE; design of hydrogenation catalyst; heterogenized CO2 hydrogenation catalyst; oxyanionic ligated Ru complex; covalent triazine framework; formic acid production
ISSN
2155-5435
URI
https://pubs.kist.re.kr/handle/201004/121438
DOI
10.1021/acscatal.8b00392
Appears in Collections:
KIST Article > 2018
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