Xu Dong, Li Qi-Yuan, Su Qing-Xu, Xia Si-Yuan, Xu Yu-Shuai, Leng Bing-Liang, Lin Xiu, Fan Liu-Yin, Chen Jie-Sheng, Li Xin-Hao
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
Student Innovation Center, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
Angew Chem Int Ed Engl. 2025 Feb 10;64(7):e202419816. doi: 10.1002/anie.202419816. Epub 2024 Nov 13.
Nonoxidative dehydrogenation of propane is useful for the high selectivity to propylene but is suffering from the heavy coke deposition on the catalyst surface. Herein, we present a proof-of-concept application of a hole-hydrogen (H) couple on a metallic cobalt surface to decrease the deactivation rate. The coupled H atoms on the Cobalt (Co) surface, partially resulting from propane dehydrogenation, enabled the desorption of propylene to avoid deep hydrogenolysis and coke deposition and realize selective and durable propylene production, while conventional Co metal-based catalysts do not generate propylene. The optimized hole-H coupled Co catalyst provided a low deactivation rate (0.0036 h) and a high turnover frequency (55.6 h) for propylene production with a high propane flux (48 vol.% CH in gas feeds) at 550 °C.
丙烷的非氧化脱氢反应对于高选择性制备丙烯很有用，但存在催化剂表面严重积碳的问题。在此，我们展示了在金属钴表面空穴 - 氢（H）偶联的概念验证应用，以降低失活速率。钴（Co）表面的偶联氢原子部分源自丙烷脱氢，这使得丙烯能够脱附，从而避免深度氢解和积碳，并实现选择性且持久的丙烯生产，而传统的钴基金属催化剂则无法生成丙烯。优化后的空穴 - H偶联钴催化剂在550℃下，对于高丙烷通量（气体进料中48体积%的CH）的丙烯生产提供了低失活速率（0.0036 h）和高周转频率（55.6 h）。
