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Carburization in the Crystalline Structure of the Metal Ag for Efficient Selective Hydrogenation of Acetylene
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2024-07-20 , DOI: 10.1021/acs.iecr.4c01880 Shihong Zhou 1 , Wenyu Zhou 1, 2 , Chenyang Lu 1 , Yuping Chen 1 , Cailong Zhou 1 , Aonan Zeng 3 , Anjie Wang 3 , Yong-Wei Zhang 2 , Luxi Tan 1 , Lichun Dong 1
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2024-07-20 , DOI: 10.1021/acs.iecr.4c01880 Shihong Zhou 1 , Wenyu Zhou 1, 2 , Chenyang Lu 1 , Yuping Chen 1 , Cailong Zhou 1 , Aonan Zeng 3 , Anjie Wang 3 , Yong-Wei Zhang 2 , Luxi Tan 1 , Lichun Dong 1
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The selective hydrogenation of acetylene to ethylene plays a pivotal role in the petrochemical industry. Metal Ag catalysts always show a high ethylene selectivity in acetylene hydrogenation, while the low hydrogen dissociation ability limits its application in hydrogenation reactions. Herein, a new silver carbide-like active phase (AgxC) was prepared through a crystalline phase transformation method, which is achieved by reducing silver acetylide to AgxC with H2. Surprisingly, the AgxC-containing catalyst exhibits an outstanding hydrogenation activity and selectivity simultaneously, achieving an acetylene conversion of 100% and an ethylene selectivity of 88.7% with exceptional long-term stability over at least 30 h. Density functional theory calculations reveal that the AgxC phase significantly lowers the activation barrier of H2 dissociation, leading to a substantially higher hydrogenation activity compared to the metal Ag catalyst. Furthermore, the excellent ethylene selectivity is attributed to the facile ethylene desorption rather than overhydrogenation. The results presented here encourage the pursuit of an Ag-based catalytic system for hydrogenation reactions.
中文翻译：
金属银晶体结构的渗碳用于乙炔的高效选择性加氢
乙炔选择性加氢制乙烯在石化工业中发挥着关键作用。金属银催化剂在乙炔加氢反应中始终表现出较高的乙烯选择性，但较低的氢解离能力限制了其在加氢反应中的应用。在此，通过结晶相变方法制备了新的碳化银类活性相(Ag x C)，该方法是通过用H 2将乙炔银还原为Ag x C来实现的。令人惊讶的是，含Ag x C的催化剂同时表现出出色的加氢活性和选择性，实现了100%的乙炔转化率和88.7%的乙烯选择性，并且在至少30小时内具有优异的长期稳定性。密度泛函理论计算表明，Ag x C相显着降低了H 2解离的活化势垒，从而导致与金属Ag催化剂相比显着更高的加氢活性。此外，优异的乙烯选择性归因于乙烯容易解吸而不是过度氢化。这里提出的结果鼓励人们追求基于银的氢化反应催化系统。
更新日期：2024-07-20
中文翻译：
金属银晶体结构的渗碳用于乙炔的高效选择性加氢
乙炔选择性加氢制乙烯在石化工业中发挥着关键作用。金属银催化剂在乙炔加氢反应中始终表现出较高的乙烯选择性，但较低的氢解离能力限制了其在加氢反应中的应用。在此，通过结晶相变方法制备了新的碳化银类活性相(Ag x C)，该方法是通过用H 2将乙炔银还原为Ag x C来实现的。令人惊讶的是，含Ag x C的催化剂同时表现出出色的加氢活性和选择性，实现了100%的乙炔转化率和88.7%的乙烯选择性，并且在至少30小时内具有优异的长期稳定性。密度泛函理论计算表明，Ag x C相显着降低了H 2解离的活化势垒，从而导致与金属Ag催化剂相比显着更高的加氢活性。此外，优异的乙烯选择性归因于乙烯容易解吸而不是过度氢化。这里提出的结果鼓励人们追求基于银的氢化反应催化系统。
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