TY - JOUR
T1 - High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst
AU - Bai, Shuxing
AU - Liu, Fangfang
AU - Huang, Bolong
AU - Li, Fan
AU - Lin, Haiping
AU - Wu, Tong
AU - Sun, Mingzi
AU - Wu, Jianbo
AU - Shao, Qi
AU - Xu, Yong
AU - Huang, Xiaoqing
PY - 2020
Y1 - 2020
N2 - Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH4 to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C−H activation of CH4. 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 (CeO2) nanowires supported rhodium (Rh) single-atom (SAs Rh-CeO2 NWs) that can serve as a high-efficiency catalyst for DMC to oxygenates (i.e., CH3OH and CH3OOH) under mild conditions. Compared to Rh/CeO2 nanowires (Rh clusters) prepared by a conventional wet-impregnation method, CeO2 nanowires supported Rh single-atom exhibits 6.5 times higher of the oxygenates yield (1231.7 vs. 189.4 mmol gRh −1 h−1), 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. © 2020, The Author(s).
AB - Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH4 to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C−H activation of CH4. 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 (CeO2) nanowires supported rhodium (Rh) single-atom (SAs Rh-CeO2 NWs) that can serve as a high-efficiency catalyst for DMC to oxygenates (i.e., CH3OH and CH3OOH) under mild conditions. Compared to Rh/CeO2 nanowires (Rh clusters) prepared by a conventional wet-impregnation method, CeO2 nanowires supported Rh single-atom exhibits 6.5 times higher of the oxygenates yield (1231.7 vs. 189.4 mmol gRh −1 h−1), 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. © 2020, The Author(s).
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U2 - 10.1038/s41467-020-14742-x
DO - 10.1038/s41467-020-14742-x
M3 - RGC 21 - Publication in refereed journal
C2 - 32075982
SN - 2041-1723
VL - 11
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 954
ER -