The lattice oxygen determines the methanol selectivity in CO2 hydrogenation over ZnZrOx catalysts

Mao, Xiaoying; Zhang, Yaping; Xu, Yun; Zhou, Yu; Zhuang, Ke; Shen, Kai; Ding, Shipeng

doi:10.1039/d3cy01471a

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“…It is necessary to develop efficient catalysts for the hydrogenation of CO 2 to methanol with simultaneously high methanol productivity and long-term stability. Encouragingly, several Cu-free metal oxide-based catalysts such as ZnZrO x (ZZO) solid solution, , In 2 O 3 − , In 2 O 3 /ZrO 2 , , MnO x /m-Co 3 O 4 , and MaZrO x (Ma = Cd, Ga) solid solutions have been identified as new classes of catalysts for CO 2 hydrogenation to methanol, which display a higher methanol selectivity, excellent resistance to sintering, and sulfur. In addition, they can be easily coupled with zeolites to directly realize the conversion of CO 2 to C 2+ products. − Among them, the ZZO solid solution is a promising catalyst for CO 2 hydrogenation to methanol, showing high catalytic stability with a CO 2 single-pass conversion of more than 10% .…”

Section: Introductionmentioning

confidence: 99%

Indium-Promoted ZnZrO_x Solid Solution Catalyst for CO₂ Hydrogenation to Methanol

Zhou,

Wei,

Zhang

et al. 2024

Ind. Eng. Chem. Res.

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Methanol synthesis is one of the most important and industrially viable approaches to carbon dioxide (CO 2 ) utilization. Both the ZnZrO x (ZZO) solid solution catalyst and the In 2 O 3 catalyst have garnered extensive attention for their high methanol selectivity and excellent resistance to sintering and sulfur in CO 2 hydrogenation. Herein, a ZZO solid solution with a large surface area is selected as the carrier, and the supported In 2 O 3 strongly interacts with the ZZO to boost the generation of more oxygen vacancies on the ZZO surface that catalyzes methanol production. On incorporating an appropriate amount of In 2 O 3 (In 2.5 wt %) onto the ZZO catalyst, In 2.5 /ZZO exhibits markedly enhanced methanol production with a CO 2 conversion rate of 13.5% and a methanol space-time yield of 0.749 g g cat −1 h −1 at 330 °C, 5 MPa, and 24,000 mL g cat −1 h −1 . In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) reveals that the incorporated indium species facilitate hydrogen activation to increase the availability of surface hydrogen. The surface hydrogen is transferred to the active sites due to hydrogen spillover, facilitating the formation of HCOO* intermediates and boosting the hydrogenation of CO 2 to methanol. Theoretical analysis allows the rationalization of the observed improvement in the catalytic performance of the In 2.5 /ZZO catalyst. In 2.5 /ZZO showed excellent stability for up to 200 h on stream, demonstrating its potential as a practical catalyst for the hydrogenation of CO 2 to methanol.

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Section: Introductionmentioning

confidence: 99%

Indium-Promoted ZnZrO_x Solid Solution Catalyst for CO₂ Hydrogenation to Methanol

Zhou,

Wei,

Zhang

et al. 2024

Ind. Eng. Chem. Res.

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The lattice oxygen determines the methanol selectivity in CO₂ hydrogenation over ZnZrO_x catalysts

Abstract: In the reaction of carbon dioxide hydrogenation to methanol, CO2 was adsorbed and activated on the oxygen vacancies neighboring Zr species, while the rate-limiting step H2 activation occurred in the Zn–O sites.

Cited by 1 publication

References 50 publications

Indium-Promoted ZnZrO_x Solid Solution Catalyst for CO₂ Hydrogenation to Methanol

Indium-Promoted ZnZrO_x Solid Solution Catalyst for CO₂ Hydrogenation to Methanol

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The lattice oxygen determines the methanol selectivity in CO2 hydrogenation over ZnZrOx catalysts

Abstract: In the reaction of carbon dioxide hydrogenation to methanol, CO2 was adsorbed and activated on the oxygen vacancies neighboring Zr species, while the rate-limiting step H2 activation occurred in the Zn–O sites.

Cited by 1 publication

References 50 publications

Indium-Promoted ZnZrOx Solid Solution Catalyst for CO2 Hydrogenation to Methanol

Indium-Promoted ZnZrOx Solid Solution Catalyst for CO2 Hydrogenation to Methanol

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The lattice oxygen determines the methanol selectivity in CO₂ hydrogenation over ZnZrO_x catalysts

Indium-Promoted ZnZrO_x Solid Solution Catalyst for CO₂ Hydrogenation to Methanol

Indium-Promoted ZnZrO_x Solid Solution Catalyst for CO₂ Hydrogenation to Methanol