Hydrogenation of cyclohexene catalyzed by nanoporous SPE-PtNi/C membrane electrode
Hydrogenation of cyclohexene catalyzed by nanoporous SPE-PtNi/C membrane electrode
复制标题
纳米多孔SPE-PtNi/C膜电极催化环己烯加氢
DOI：
10.1016/j.ijhydene.2021.10.179
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发表时间：
2021-11
影响因子：
7.2
通讯作者：
Xudong Li
中科院分区：
文献类型：
--
作者：
Bin Yang;Liudang Fang;Linhan Zan;Jiaxian Cai;Yunhao Feng;Xudong Li
实施大规模合成纳米多孔PtNi/C催化剂用于在常压和低于100 ° C的温度下的不饱和有机化合物的氢化过程是一项紧迫的任务。本文采用离子束溅射、超声波辅助电化学脱合金、热压等方法制备了纳米多孔SPE-PtNi/C膜电极。特别注意的是支付的电化学性能，相结构，表面形貌，活性组分分布，并与商业Pt/C催化剂的环己烯加氢的催化效率进行比较，制备的电极的分析。结果表明，超声辅助电化学刻蚀温度对所研究催化剂的催化活性影响最为显着。在50 ° C下，用0.7mol/LHClO4处理PtNi/C 1.5h，催化活性提高了25.20%，Pt负载量降低了88.85%。此外，PtNi/C表面的纳米多孔结构使Pt 4f7/2的结合能降低了0.23 eV，这是由于Ni的损失和NiPt的晶面收缩，这增强了暴露的Pt的晶格结构的压缩应变，增加了活性位点的数量.最后，使用纳米多孔SPE-PtNi/C膜电极可以在加氢反应中将环己烯的产率提高179%，同时将电流效率提高69%。
Implementing large-scale synthesis of nanoporous PtNi/C catalysts for hydrogenation processes of unsaturated organic compounds under atmospheric pressure at temperatures below 100 °C is an urgent task. In this paper, a nanoporous SPE-PtNi/C membrane electrode is prepared by ion beam sputtering, ultrasonic-assisted electrochemical dealloying, and hotpressing. Special attention is paid to the analysis of the electrochemical properties, phase structure, surface morphology, active constituent distribution, and catalytic efficiency for cyclohexene hydrogenation of the produced electrode in comparison with those of commercial Pt/C catalysts. The results show that the ultrasonic-assisted electrochemical etching temperature exerts the most significant effect on the catalytic activity of the catalyst under consideration. In particular, the treatment of PtNi/C in 0.7 mol/L HClO4for 1.5 h at the optimized temperature of 50 °C enables one to increase the catalytic activity by 25.20% at decreasing the Pt-loading content by 88.85% compared with commercial Pt/C. Furthermore, the nanoporous structure of the PtNi/C surface allows the binding energy of Pt 4f7/2to be reduced by 0.23 eV due to the Ni loss and the crystal plane shrinkage from NiPt, which enhances the compressive strain of the lattice structure of exposed Pt and increases the number of active sites. Finally, the use of a nanoporous SPE-PtNi/C membrane electrode could increase the yield of cyclohexene during the hydrogenation reaction by 179% at simultaneously improving the current efficiency by 69%.
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