李彦光教授课题组及其合作者在Angew. Chem. Int. Ed. 上发表论文

发布时间:2021-09-10访问量:809设置

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

链接:

https://doi.org/10.1002/anie.202109288


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