Defect-Dependent Selective C–H/C–C Bond Cleavage of Propane in the Presence of CO2 over FeNi/Ceria Catalysts
Defect-Dependent Selective C–H/C–C Bond Cleavage of Propane in the Presence of CO2 over FeNi/Ceria Catalysts
复制标题
DOI：
10.1021/acssuschemeng.1c06095
复制
发表时间：
2021-12
影响因子：
8.4
通讯作者：
Yehong Wang;Zhixin Zhang;Lijun Lei;W. Liu;Shuyan Du;Xiangxue Zhu;Xiujie Li;Feng Wang
中科院分区：
文献类型：
--
作者：
Yehong Wang;Zhixin Zhang;Lijun Lei;W. Liu;Shuyan Du;Xiangxue Zhu;Xiujie Li;Feng Wang
二氧化碳辅助丙烷转化是最有趣的化学过程之一，通过C-H键裂解生成丙烯或通过丙烷的C-C键裂解生成合成气。然而，控制高选择性的转换仍然是一个重大的挑战。在这项工作中，我们开发了一种策略，以co2为氧化剂，通过控制氧化铈载体的缺陷浓度，在FeNi/ceria催化剂上实现丙烷C-H / C-C键的选择性裂解。成功制备了两种缺陷浓度不同的氧化铈。在550℃条件下，在富缺陷铈负载的FeNi催化剂上裂解C - h键，丙烷转化率达到25.2%，丙烯选择性为49%。相比之下，当使用缺陷铈作为载体时，CO通过C-C键裂解生成，选择性为95%。通过紫外拉曼光谱、x射线光电子能谱和h2 -程序升温还原等方法研究了缺陷在铈载体中的重要作用。这项工作为铈基催化剂的缺陷调整提供了一种方法，实现了二氧化碳和烷烃选择性转化为增值化学品。
CO2-assisted propane conversion is one of the most interesting chemical processes, generating either propylene via C–H bond cleavage or syngas via C–C bond cleavage of propane. However, controlling the conversion with high selectivity is still a significant challenge. In this work, we developed a strategy to realize selective C–H/C–C bond cleavage of propane with CO2as the oxidant by controlling the defect concentrations of ceria supports over FeNi/ceria catalysts. Two types of ceria with distinct defect concentrations were prepared successfully. The propane conversion achieved 25.2% with 49% propylene selectivity via C–H bond cleavage over the defect-rich ceria-supported FeNi catalyst at 550 °C. In contrast, CO is generated via C–C bond cleavage with 95% selectivity when defect-deficient ceria was used as the support. The essential role of defects in the ceria support was investigated carefully by UV–Raman, X-ray photoelectron spectroscopy, and H2-temperature-programmed reduction. This work provides a method for defect tuning of ceria-based catalysts and realizes the selective conversion of CO2and alkanes to value-added chemicals.