Bai Shuxing, Liu Fangfang, Huang Bolong, Li Fan, Lin Haiping, Wu Tong, Sun Mingzi, Wu Jianbo, Shao Qi, Xu Yong, Huang Xiaoqing
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Jiangsu, 215123, China.
Institute of Functional Nano&Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Jiangsu, 215123, China.
Nat Commun. 2020 Feb 19;11(1):954. doi: 10.1038/s41467-020-14742-x.
Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C-H activation of CH. The quest for high-efficiency catalysts for this process is limited by the current drawbacks including poor activity and low selectivity. Here we show a cerium dioxide (CeO) nanowires supported rhodium (Rh) single-atom (SAs Rh-CeO NWs) that can serve as a high-efficiency catalyst for DMC to oxygenates (i.e., CHOH and CHOOH) under mild conditions. Compared to Rh/CeO nanowires (Rh clusters) prepared by a conventional wet-impregnation method, CeO nanowires supported Rh single-atom exhibits 6.5 times higher of the oxygenates yield (1231.7 vs. 189.4 mmol g h), which largely outperforms that of the reported catalysts in the same class. This work demonstrates a highly efficient DMC process and promotes the research on Rh single-atom catalysts in heterogeneous catalysis.
将甲烷直接转化（DMC）为高附加值产品对于有效利用甲烷以应对能源危机具有重要意义。然而，DMC中与甲烷选择性C-H活化相关的挑战依然存在。目前该过程高效催化剂的研发受到包括活性差和选择性低等缺点的限制。在此，我们展示了一种二氧化铈（CeO₂）纳米线负载的铑（Rh）单原子（SAs Rh-CeO₂ NWs），其可作为一种高效催化剂，在温和条件下将DMC转化为含氧化合物（即CH₃OH和CH₃COOH）。与通过传统湿浸渍法制备的Rh/CeO₂纳米线（Rh团簇）相比，CeO₂纳米线负载的Rh单原子的含氧化合物产率高出6.5倍（1231.7对189.4 mmol g⁻¹ h⁻¹），这在很大程度上优于同类已报道的催化剂。这项工作展示了一种高效的DMC过程，并推动了非均相催化中Rh单原子催化剂的研究。
