MDX Research Center for Element Strategy, International Research Frontiers Initiative, Tokyo Institute of Technology, Yokohama 226-8503, Japan.
Advanced Institute for Materials Research (WPI-AIMR), Tohoku University, Sendai 980-8577, Japan.
J Am Chem Soc. 2023 May 3;145(17):9410-9416. doi: 10.1021/jacs.2c13801. Epub 2023 Mar 30.
CO hydrogenation to methanol is one of the most promising routes to CO utilization. However, difficulty in CO 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 CO 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 CO hydrogenation to methanol and CO compared with a Pd catalyst. A turnover frequency of 0.15 h 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).
CO 加氢合成甲醇是 CO 利用最有前景的路线之一。然而，低温下 CO 活化、催化剂稳定性、催化剂制备和产物分离等问题，阻碍了在温和条件下实现该加氢过程的工业化。在此，我们报道了一种用于低温 CO 加氢的 PdMo 金属间化合物催化剂。该催化剂可通过氧化物前体的简单氨解合成，并在空气和反应气氛中表现出优异的稳定性，显著提高了 CO 加氢合成甲醇和 CO 的催化活性，优于 Pd 催化剂。在 0.9 MPa 和 25°C 下，甲醇的合成周转频率达到 0.15 h，与在更高压力条件（4-5 MPa）下的最先进的多相催化剂相当或更高。
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