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Zhou Ling Zhu Xiaorong Su Hui Lin Hongzhen Lyu Yanhong Zhao Xu Chen Chen Zhang Nana Xie Chao Li Yingying Lu Yuxuan Zheng Jianyun Johannessen Benrt Jiang San Ping Liu Qinghua Li Yafei Zou Yuqin Wang Shuangyin 《中国科学:化学(英文版)》2021,64(9):1586-1595
Electrochemical hydrogenation(ECH) of biomass-derived platform molecules is a burgeoning route for the sustainable utilization of hydrogen. However, the noble-metal-catalyzed ECH of phenolic compounds suffers from intense competition with hydrogen evolution reaction. We prepared Pt Rh bimetallic nanoparticles dispersed on highly ordered mesoporous carbon nanospheres, which improves the utilization efficiency of adsorbed hydrogen(Had) to ECH in H–UPD region(0 V vs. RHE).Further analysis reveals(i) the strong overlapping between the d-orbitals of Pt and Rh enhances specific adsorption of phenol;(ii)incorporation of Rh devotes an electronic effect on weakening the alloy–Hadinteraction to increase the FE of ECH. DFT calculations confirm the selectivity difference and the ECH parallel pathways: cyclohexanol and cyclohexanone are formed via hydrogenation/dehydrogenation of the intermediate *C6 H10 OH. These findings deepen our fundamental understanding of the ECH process, and cast new light on exploration of highly efficient electrocatalysts for biomass upgrading. 相似文献
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