Gold plasmon-induced photocatalytic dehydrogenative coupling of methane to ethane on polar oxide surfaces
Gold plasmon-induced photocatalytic dehydrogenative coupling of methane to ethane on polar oxide surfaces
复制标题
金等离子体诱导的极性氧化物表面上甲烷与乙烷的光催化脱氢偶联
DOI：
10.1039/c7ee02951a
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发表时间：
2018-02-01
影响因子：
32.5
通讯作者：
Long, Jinlin
中科院分区：
文献类型：
--
作者：
Meng, Lingshu;Chen, Zhenye;Long, Jinlin
这项工作显示了在室温下甲烷与乙烷的太阳能驱动的热偶联反应。在Au/ZnO多孔纳米片（NS）的极性表面上，甲烷C-H键被垂直于极性{001}面的局部电场极化解离，最终通过自由基耦合途径转化为乙烷和氢气，太阳能转化为C2 H6的能量转换效率为0.08%.机制研究表明，金等离子体激元诱导的共振能量转移调节电荷载流子能量来触发化学计量转换。热电子将质子还原为H-2，这是甲烷偶联的速率决定步骤。
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 H-2, which is the rate-determining step of methane coupling.