Journal
ACS CATALYSIS
Volume 9, Issue 11, Pages 10253-10259Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b03449
Keywords
CO2 hydrogenation; methanol synthesis; solid solution catalyst; dual active sites; H-2 heterolytic dissociation
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Funding
- National Key R&D Program of China [2017YFB0702800]
- Transformational Technologies for Clean Energy and Demonstration [XDA21090202]
- National Natural Science Foundation of China [21802139]
- Project of Key Research Plan of Ningxia [2019BDE03003]
- Youth Innovation Promotion Association CAS [2019183]
- NWO veni grant [016.Veni.172.034]
- NWO-surfsara
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Hydrogenation of CO2 to methanol utilizing the hydrogen from renewable energy sources offers a promising way to reduce CO2 emissions through the CO2 utilization as a carbon source. However, it is a challenge to convert CO2 to methanol with high activity and high methanol selectivity. Herein, we report a class of metal-oxide solid-solution catalysts: MaZrOx (M-a = Cd, Ga), which show a methanol selectivity up to 80% with the CO2 single pass conversion reaching 4.3%-12.4% under the reaction conditions of H-2/CO2 = 3/1, 24 000 h(-1), 5 MPa. Structural and electronic characterizations combined with denisty functional theory calculations suggest that the M-a and Zr components in MaZrOx (M-a = Cd, Ga) solid-solution catalysts show a strong synergetic effect, which enhances the H-2 heterolytic dissociation and results in high activity and high methanol selectivity. The solid-solution catalyst with dual metal oxide components offers an approach for the selective hydrogenation of CO2 to chemicals.
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