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Electrochemical Reduction of CO2 on Ni- and Pt-Epitaxially Grown Cu(111) Surfaces

机译:在Ni和Pt外延生长的Cu(111)表面上电化学还原CO2

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摘要

The electroreduction of CO2 on well-defined M/Cu(111) (M= Ni and Pt) bimetallic surface systems fabricated using molecular beam epitaxy was studied. The total faradic efficiency for CO2 reduction using one-monolayer (ML)-thick Pt epitaxially grown on a Cu(111) substrate (1-ML Pt/Cu(111)) was nearly the same as that for clean Pt(111). In contrast, the 1-ML-thick Ni/Cu(111) system exhibited increased selectivity for CH4 production compared with that of clean Ni(111), which may stem from the geometric tensile strain induced by the underlying Cu(111) substrate. Notably, bimetallic surfaces consisting of 0.1-ML-thick Ni or Pt grown on Cu(111) exhibited significantly different reduction behaviors compared with those of Cu because of the presence of the a small amount of epitaxially grown metal. For the 0.1-ML-thick Ni/Cu(111) system, the total faradaic efficiency for CO2 reduction and the production rate for CO were enhanced compared with those for clean Cu(111), whereas the production of CH4 decreased. In contrast, the total faradaic efficiency was significantly suppressed for the 0.1-ML-thick Pt/Cu(111) bimetallic substrate, with only a very small amount of CH4 production. The difference in the catalytic properties is attributed to the difference in the adsorption energies for CO, which is an intermediate in the electrochemical production of CH4 and C2H4.
机译:研究了使用分子束外延技术在定义明确的M / Cu(111)(M = Ni和Pt)双金属表面系统上对CO2的电还原。使用外延生长在Cu(111)基板上的单层(ML)厚的Pt(1-ML Pt / Cu(111))还原CO2的总法拉第效率几乎与纯净Pt(111)相同。相比之下,与干净的Ni(111)相比,1-ML厚的Ni / Cu(111)系统对CH4的生产表现出更高的选择性,这可能源于下面的Cu(111)基底引起的几何拉伸应变。值得注意的是,由Cu(111)上生长的0.1-ML厚的Ni或Pt构成的双金属表面与Cu相比具有明显不同的还原行为,因为存在少量的外延生长金属。对于厚度为0.1-ML的Ni / Cu(111)系统,与纯净的Cu(111)相比,用于还原CO2的总法拉第效率和CO的生产率均得到提高,而CH4的产生则下降。相比之下,厚度仅为0.1-ML的Pt / Cu(111)双金属基材的总法拉第效率得到了显着抑制,而CH4的生成量却很少。催化性能的差异归因于CO的吸附能的差异,CO是CH4和C2H4电化学生产的中间产物。

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