Mechanism of CO<sub>2</sub> hydrogenation over a Zr<sub>1</sub>–Cu single-atom catalyst

Liu, Lingna; Wang, Xu‐Jia; Lu, Shuwei; Li, Jiawei; Zhang, Hui; Su, Xuanyue; Xue, Fan; Cao, Baowei; Fang, Tao

doi:10.1039/d1nj05938f

Cited by 9 publications

(4 citation statements)

References 48 publications

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“…Moreover, some results of DFT calculations [71,83,84] and kinetic study [83] also confirm the mechanism via CO*. Thus, researchers also studied the co-existence of the two mechanisms.…”

Section: Reaction Mechanismmentioning

confidence: 75%

Perspective on CO2 Hydrogenation for Dimethyl Ether Economy

Liu

2022

Catalysts

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The CO2 hydrogenation to dimethyl ether (DME) is a potentially promising process for efficiently utilizing CO2 as a renewable and cheap carbon resource. Currently, the one-step heterogeneous catalytic conversion of CO2 to value-added chemicals exhibits higher efficiency than photocatalytic or electrocatalytic routes. However, typical catalysts for the one-step CO2 hydrogenation to DME still suffer from the deficient space–time yield and stability in industrial demonstrations/applications. In this perspective, the recent development of the one-step CO2 hydrogenation to DME is focused on different catalytic systems by examining the reported experimental results and the reaction mechanism including the catalytic nature of active sites, activation modes and of CO2 molecules under relevant conditions; surface intermediates are comparatively analyzed and discussed. In addition to the more traditional Cu-based, Pd-based, and oxide-derived bifunctional catalysts, a further emphasis is given to the characteristics of the recently emerged In2O3-based bifunctional catalysts for the one-step conversion of CO2 to DME. Moreover, GaN itself, as a bifunctional catalyst, shows over 90% DME selectivity and a reasonably high activity for one-step CO2 hydrogenation, and the direct hydrogenation of CO2 via the unique non-methanol intermediate mechanism is highlighted as an important illustration for exploring new catalytic systems. With these analyses and current understandings, the research directions in the aspects of catalysis and DME economy are suggested for the further development of one-step DME synthesis from CO2 hydrogenation.

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“…Moreover, some results of DFT calculations [71,83,84] and kinetic study [83] also confirm the mechanism via CO*. Thus, researchers also studied the co-existence of the two mechanisms.…”

Section: Reaction Mechanismmentioning

confidence: 75%

Perspective on CO2 Hydrogenation for Dimethyl Ether Economy

Liu

2022

Catalysts

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“…In addition, the H atoms spilled over to the support surface at the metal-support interface region, participated in the formation of the carbonaceous intermediate species, and were finally converted to HCOO*, CH 2 O*, CH 3 O*, and CH 3 OH. Liu et al [127] systematically explored three possible paths of CO 2 hydrogenation to methanol over a single-atom Zr-doped Cu-based catalyst from the kinetic and thermodynamic aspects of each elementary reaction by the DFT method (Figure 9). The results showed that methanol was produced by the HCOO pathway, which involved the intermediates of bi-HCOO*, HCOOH*, H 2 COO*, H 2 COOH*, H 2 CO*, and H 3 CO*.…”

Section: The Hcoo Mechanism and R-hcoo Mechanismmentioning

confidence: 99%

Hydrogenation of Carbon Dioxide to Methanol over Non-Noble Catalysts: A State-of-the-Art Review

Chen

Deng

et al. 2023

Atmosphere

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The malignant environmental changes caused by the ever-increasing amount of anthropogenic CO2 emissions have been particularly prominent in recent years. To achieve carbon mitigation and carbon neutrality, CO2 hydrogenation to methanol is regarded as a promising and sustainable route. However, the development of catalysts with exceptional performance and the establishment of a clear structure–activity relationship remain formidable challenges. Considering the lack of a state-of-the-art review on the catalytic progress of CO2 hydrogenation to methanol over non-noble catalysts, we conducted a detailed review in terms of the thermodynamic analysis, catalytic development, and reaction mechanism. In this work, we mainly reviewed the latest research progress of different catalysts including Cu-based, In2O3-based, bimetallic, solid solution, and other catalysts. Meanwhile, we summarized the effects of the support materials, promoters, and preparation methods on the catalytic performance. In addition, we also summarized the possible reaction mechanisms of direct hydrogenation of CO2 to methanol. Overall, this work would be of importance for the researchers to obtain a comprehensive understanding of the design and development of efficient catalysts for CO2 hydrogenation to methanol.

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“…Elementary reactions, activation energies, and reaction energy of CO 2 hydrogenation to methanol over the Zr/Cu (111) catalyst168 …”

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confidence: 99%