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Gold plasmon-induced photocatalytic dehydrogenative coupling of methane to ethane on polar oxide surfaces†
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2017-12-22 00:00:00 , DOI: 10.1039/c7ee02951a
Lingshu Meng 1, 2, 3, 4, 5 , Zhenye Chen 1, 2, 3, 4, 5 , Zhiyun Ma 1, 2, 3, 4, 5 , Sha He 1, 2, 3, 4, 5 , Yidong Hou 1, 2, 3, 4, 5 , Hao-Hong Li 1, 2, 3, 4, 5 , Rusheng Yuan 1, 2, 3, 4, 5 , Xi-He Huang 1, 2, 3, 4, 5 , Xuxu Wang 1, 2, 3, 4, 5 , Xinchen Wang 1, 2, 3, 4, 5 , Jinlin Long 1, 2, 3, 4, 5
Affiliation  

This work shows the solar-driven dehydrogenative coupling of methane to ethane at room temperature. A solar-to-C2H6 energy conversion efficiency of 0.08% was achieved on the polar surface of Au/ZnO porous nanosheets (NSs), where methane C–H bonds are polarized and dissociated by the local electric field normal to the polar {001} plane, and finally converted into ethane and hydrogen through a radical coupling pathway. Mechanistic studies suggest that the Au-plasmon-induced resonance energy transfer modulates charge carrier energetics to trigger the stoichiometric conversion. Hot electrons reduce protons to H2, which is the rate-determining step of methane coupling.

中文翻译:

金等离激元诱导的极性氧化物表面上甲烷与乙烷的光催化脱氢偶联

这项工作显示了室温下甲烷与乙烷在太阳能驱动下的脱氢偶联作用。在Au / ZnO多孔纳米片(NSs)的极性表面上实现了0.08%的太阳能到C 2 H 6的能量转换效率,其中甲烷C–H键被垂直于极性的局部电场极化并解离{001}面,最后通过自由基偶联途径转化为乙烷和氢。机理研究表明,Au-等离子体激元引起的共振能量转移调节电荷载流子的能量,从而触发化学计量转换。热电子将质子还原为H 2,这是甲烷偶联的决定速率的步骤。
更新日期:2017-12-22
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