Dataset Information

Room-Temperature CO₂ Hydrogenation to Methanol over Air-Stable hcp-PdMo Intermetallic Catalyst.

ABSTRACT: CO₂ hydrogenation to methanol is one of the most promising routes to CO₂ utilization. However, difficulty in CO₂ activation at low temperature, catalyst stability, catalyst preparation, and product separation are obstacles to the realization of a practical hydrogenation process under mild conditions. Here, we report a PdMo intermetallic catalyst for low-temperature CO₂ hydrogenation. This catalyst can be synthesized by the facile ammonolysis of an oxide precursor and exhibits excellent stability in air and the reaction atmosphere and significantly enhances the catalytic activity for CO₂ hydrogenation to methanol and CO compared with a Pd catalyst. A turnover frequency of 0.15 h^-1 was achieved for methanol synthesis at 0.9 MPa and 25 °C, which is comparable to or higher than that of the state-of-the-art heterogeneous catalysts under higher-pressure conditions (4-5 MPa).

SUBMITTER: Sugiyama H

PROVIDER: S-EPMC10161205 | biostudies-literature | 2023 May

REPOSITORIES: biostudies-literature

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Room-Temperature CO2 Hydrogenation to Methanol over Air-Stable hcp-PdMo Intermetallic Catalyst.

Sugiyama Hironobu H Miyazaki Masayoshi M Sasase Masato M Kitano Masaaki M Hosono Hideo H

Journal of the American Chemical Society 20230330 17

CO2 hydrogenation to methanol is one of the most promising routes to CO2 utilization. However, difficulty in CO2 activation at low temperature, catalyst stability, catalyst preparation, and product separation are obstacles to the realization of a practical hydrogenation process under mild conditions. Here, we report a PdMo intermetallic catalyst for low-temperature CO2 hydrogenation. This catalyst can be synthesized by the facile ammonolysis of an oxid ...[more]

PMID: 36995761

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Project description:Methanol synthesized from carbonate hydrogenation is of great importance for CO2 utilization indirectly. Herein, a series of Cu/Zn/Al heterogeneous catalysts were prepared by co-precipitation with a synchronous aging step, and were applied for hydrogenation of diethyl carbonate (DEC) to produce methanol. Furthermore, the catalysts were characterized by physicochemical methods, such as N2 adsorption, ICP-OES, N2O titration, SEM, TEM, XRD, H2-TPR and XPS in detail. Higher copper concentration led to a higher ratio of bulk CuOx species in the calcined samples, which resulted in different copper species distribution after the reduction process. Structure activity relationship analysis indicated that the balance of surface Cu0 and Cu+ species influenced the formation rate of methanol. A higher proportion of Cu+ to (Cu+ + Cu0) was conductive to methanol formation, while excessive Cu0 site density played a negative influence on the methanol synthesized from DEC. Cu/Zn/Al with a 45.2% weight fraction of copper showed better performance with a total methanol formation rate of 131.0 mg gcat. -1 h-1. The reaction temperature and reaction time could obviously affect the reaction performance and the results suggested that 200 °C and 6 h were suitable. Furthermore, the long-term stability and activity of the catalyst was also studied on a fixed bed, and the yield of total methanol reached to 88.5% and the selectivity of total methanol gradually decreased to 74.0% within 200 h, which could be attributed to the detrimental influence derived from the increase of Cu0. The reaction pathways involved in the hydrogenation of DEC process were proposed. The substance scope was also extended to other carbonates and the catalyst exhibited superior catalytic performance toward linear carbonates. This work provided insights into carbonate hydrogenation over an effective Cu/Zn/Al catalyst, which could be utilized into upgrading CO2 indirectly to produce commodity methanol under relatively mild reaction conditions.

Dataset Information

Room-Temperature CO₂ Hydrogenation to Methanol over Air-Stable hcp-PdMo Intermetallic Catalyst.

Publications

Room-Temperature CO<sub>2</sub> Hydrogenation to Methanol over Air-Stable hcp-PdMo Intermetallic Catalyst.

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