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Room-Temperature CO2 Hydrogenation to Methanol over Air-Stable hcp-PdMo Intermetallic Catalyst
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-03-30 , DOI: 10.1021/jacs.2c13801 Hironobu Sugiyama 1 , Masayoshi Miyazaki 1 , Masato Sasase 1 , Masaaki Kitano 1, 2 , Hideo Hosono 1, 3
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-03-30 , DOI: 10.1021/jacs.2c13801 Hironobu Sugiyama 1 , Masayoshi Miyazaki 1 , Masato Sasase 1 , Masaaki Kitano 1, 2 , Hideo Hosono 1, 3
Affiliation
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).
中文翻译:
在空气稳定的 hcp-PdMo 金属间催化剂上室温 CO2 加氢制甲醇
CO 2加氢制甲醇是最有前途的CO 2利用途径之一。然而,CO 2的低温活化、催化剂稳定性、催化剂制备和产物分离等困难是实现温和条件下加氢工艺实用化的障碍。在这里,我们报告了一种用于低温 CO 2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,在空气和反应气氛中表现出优异的稳定性,与 Pd 催化剂相比,显着提高了 CO 2加氢生成甲醇和 CO 的催化活性。周转频率为 0.15 小时–1在 0.9 MPa 和 25 °C 下实现了甲醇合成,这与高压条件(4-5 MPa)下最先进的非均相催化剂相当或更高。
更新日期:2023-03-30
中文翻译:
在空气稳定的 hcp-PdMo 金属间催化剂上室温 CO2 加氢制甲醇
CO 2加氢制甲醇是最有前途的CO 2利用途径之一。然而,CO 2的低温活化、催化剂稳定性、催化剂制备和产物分离等困难是实现温和条件下加氢工艺实用化的障碍。在这里,我们报告了一种用于低温 CO 2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,在空气和反应气氛中表现出优异的稳定性,与 Pd 催化剂相比,显着提高了 CO 2加氢生成甲醇和 CO 的催化活性。周转频率为 0.15 小时–1在 0.9 MPa 和 25 °C 下实现了甲醇合成,这与高压条件(4-5 MPa)下最先进的非均相催化剂相当或更高。