Liu Hao-Xin, Wang Wei-Wei, Fu Xin-Pu, Liu Jin-Cheng, Jia Chun-Jiang
Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, P. R. China.
Center for Rare Earth and Inorganic Functional Materials, School of Materials Science and Engineering & National Institute for Advanced Materials, Nankai University, Tianjin, 300350, P. R. China.
Nat Commun. 2024 Oct 23;15(1):9126. doi: 10.1038/s41467-024-53484-y.
Compared to H-assisted activation mode, the direct dissociation of CO into carbonyl (*CO) with a simplified reaction route is advantageous for CO-related synthetic processes and catalyst upgrading, while the stable C = O double bond makes it very challenging. Herein, we construct a subnano MoO layer on the surface of MoN, which provides a dynamically changing surface of MoO↔MoO (x < 3) for catalyzing CO hydrogenation. Rich oxygen vacancies on the subnano MoO surface with a high electron donating capacity served as a scissor to directly shear the C = O double bond of CO to form CO at a high rate. The O atoms leached in CO dissociation are removed timely by H to regenerate active oxygen vacancies. Owing to the greatly enhanced dissociative activation of CO, this MoO/MoN catalyst without any supported active metals shows excellent performance for catalyzing CO hydrogenation to CO. The construction of highly disordered defective surface on heterostructures paves a new pathway for molecule activation.
与氢辅助活化模式相比，通过简化反应路线将一氧化碳直接解离为羰基（*CO），对与一氧化碳相关的合成过程和催化剂升级具有优势，而稳定的碳氧双键使其极具挑战性。在此，我们在氮化钼表面构建了一个亚纳米氧化钼层，该层为催化一氧化碳加氢提供了一个动态变化的MoO↔MoO（x < 3）表面。亚纳米氧化钼表面具有丰富的氧空位且供电子能力高，充当剪刀直接高速剪切一氧化碳的碳氧双键以形成一氧化碳。一氧化碳解离过程中浸出的氧原子被氢及时去除以再生活性氧空位。由于一氧化碳的解离活化大大增强，这种不含任何负载活性金属的氧化钼/氮化钼催化剂在催化一氧化碳加氢生成一氧化碳方面表现出优异性能。在异质结构上构建高度无序的缺陷表面为分子活化开辟了一条新途径。
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