题目: | Phase-Dependent Electrocatalytic CO2 Reduction on Pd3Bi Nanocrystals |
作者: | Lin Jia,1,+ Mingzi Sun,2,+ Jie Xu,1,+ Xuan Zhao,1 Rui Zhou,1 Binbin Pan,1 Lu Wang,1 Na Han,1 Bolong Huang,2,* and Yanguang Li1,* |
单位: | 1Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, Suzhou 215123 (China) 2Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR (China) |
摘要: | Alloying is a general strategy for modulating the electronic structures of catalyst materials. Compared to more common solid–solution alloys, intermetallic alloys feature well-defined atomic arrangements and provide the unique platform for studying the structure-performance correlations. It is, unfortunately, synthetically challenging to prepare the nanostructures of intermetallic alloys for catalysis research. In this contribution, we prepare intermetallic Pd3Bi nanocrystals of a uniform size via a facile solvothermal method. These nanocrystals can phase-transform into solid solution alloy via thermal annealing while retaining a similar composition and size. In 0.1 M KHCO3 aqueous solution, the intermetallic Pd3Bi can selectively reduce CO2 to formate with high selectivity (≈100%) and stability even at <-0.35 V versus reversible hydrogen electrode, whereas the solid solution alloy has limited formate selectivity of < 60%. Such unique phase-dependence is understood via theoretical simulations showing that the crystallographic ordering of Pd and Bi atoms within intermetallic alloys can suppress CO poisoning and enhance the *OCHO adsorption during electrochemical CO2 reduction to formate. |
影响因子: | 12.959 |
分区情况: | 一区 |
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