选择性
催化作用
产量(工程)
纳米线
吸附
甲烷
化学工程
化学
激进的
材料科学
光化学
纳米技术
物理化学
有机化学
冶金
工程类
作者
Yueshan Xu,Daoxiong Wu,Peilin Deng,Jing Li,Junming Luo,Qi Chen,Wei Huang,Chong Michael Shim,Chunman Jia,Zhongxin Liu,Yijun Shen,Xinlong Tian
标识
DOI:10.1016/j.apcatb.2022.121223
摘要
The direct methane (CH 4 ) oxidation to high value-added C1 chemicals is a great promising strategy to explore the CH 4 resource utilization. However, the low activity and selectivity of catalytic performance remains a great conundrum due to the difficulty to activate the C H bond and the unmanageable over oxidation. Herein, Pd x Au y nanowires (NWs) with various Pd/Au atomic ratios are presented as ideal models to explore the atomic-level effect of PdAu atoms for the direct CH 4 oxidation. The influence of reaction parameters are systematically investigated, and Pd 9 Au 1 NWs display a maximum yield of 2890.3 μmol g −1 h −1 with 99% selectivity for the liquid C1 oxygenated products. This enhanced performance is attributed to the combination of one-dimensional structure and the synergistic effect from the suitable portion of Au on Pd sites, which regulates bond strength between adsorbed radicals (•OH, •OOH, •CH 3 ) and PdAu atoms, confirmed by the density function theory calculations. Au decorated Pd NWs for methane direct oxidation to liquid C1 products with high activity and selectivity. • High quality Pd x Au y NWs with different Pd/Au atomic ratios are prepared by galvanic replacement reaction. • The Pd 9 Au 1 NWs show a maximum yield of 2890.3 μmol g -1 h -1 and a 99% selectivity for liquid C1 products. • The incorporation of Au moderates binding strength of intermediates, facilitating the C-H activation.
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