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).
Methanol is a key chemical in C1 chemistry and energy carrier. The industrial synthesis of methanol uses a heterogeneous catalyst, Cu/ZnO/Al2O3, under harsh conditions of high temperature and high pressure. Here, we propose a design concept for a catalyst to achieve low-temperature synthesis of methanol and report that Cu-loaded rare-earth hydrides (Cu/REH2+x ) work as effective catalysts for methanol synthesis from CO and H2 at temperatures below 100 °C, where the conventional Cu/ZnO/Al2O3 industrial catalyst does not work well. This catalytic activity is due to negatively charged Cu sites that originate from the highly electron-donating support material and hydride ions directly reactive with CO. The activation energy and turn over frequency for the catalyst are less than half and ∼20 times higher than that for conventional Cu-based catalysts, respectively. The present work demonstrates that anionic electrons with a low work function, the metallic nature of the support material, and hydride ions in the support play key roles for low-temperature methanol synthesis.
Methanol, a raw material for C1 chemistry, is industrially produced under harsh conditions using Cu/ZnO-based catalysts. The synthesis of methanol under mild conditions is a challenging subject using an improved catalyst. Here, Zn1–x Si x O (ZSO) nanoparticles were synthesized by a thermal plasma method, and their work function and carrier concentration could be tuned by the Zn:Si ratio. The electrically conductive ZSO nanoparticles with a low work function enhanced the donation of electrons to loaded Cu and significantly promoted hydrogenation of CO to methanol, whereas insulating ZSO nanoparticles with a similar low work function did not. These results reveal that efficient electronic promotion by the transfer of electrons from a support to loaded Cu plays a key role in low-temperature methanol synthesis.
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