Unmasking the Critical Role of the Ordering Degree of Bimetallic Nanocatalysts on Oxygen Reduction Reaction by In Situ Raman Spectroscopy

被引：66

作者：

Chen, Heng-Quan ^{[1
]}

Ze, Huajie ^{[1
]}

Yue, Mu-Fei ^{[1
]}

Wei, Di-Ye ^{[1
]}

Yao-Lin, A. ^{[1
]}

Wu, Yuan-Fei ^{[1
]}

Dong, Jin-Chao ^{[1
]}

Zhang, Yue-Jiao ^{[1
]}

Zhang, Hua ^{[1
]}

Tian, Zhong-Qun ^{[1
,2
]}

Li, Jian-Feng ^{[1
,2
,3
,4
]}

机构：

[1] Xiamen Univ, Coll Chem & Chem Engn, Coll Mat,MOE Key Lab Spectrochem Anal & Instrumen, Coll Energy,State Key Lab Phys Chem Solid Surface, Xiamen 361005, Peoples R China

[2] Innovat Lab Sci & Technol Energy Mat Fujian Prov, Xiamen 361005, Peoples R China

[3] China Jiliang Univ, Coll Opt & Elect Technol, Hangzhou 310018, Zhejiang, Peoples R China

[4] Xiamen Univ, Shenzhen Res Inst, Shenzhen 518000, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2022年 / 61卷 / 16期

关键词：

Intermediates; ORR; Ordering Degree; Raman Spectroscopy; In Situ; INTERMETALLIC NANOPARTICLES; ELECTROCATALYTIC ACTIVITY; CATALYST; CONVERSION; PERFORMANCE; PLATINUM; ALLOY;

D O I：

10.1002/anie.202117834

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Precise control and accurate understanding of the ordering degree of bimetallic nanocatalysts (BNs) are challenging yet crucial to acquire advanced materials for the oxygen reduction reaction (ORR). AuCu BNs with various ordering degrees were synthesized to evaluate the influence of ordering degree on the ORR at a molecular level using in situ Raman spectroscopy. The activity of AuCu BNs was improved by over 2 times after a disorder-to-order transition, making the performance of highly ordered AuCu BNs exceed that of benchmark Pt/C. Direct Raman spectroscopic evidence of key intermediate (*OH) demonstrates that the active site is the combination site of Au and Cu. Moreover, two distinct *OH species are observed on the ordered and disordered structure, and the ordered site is more beneficial for ORR due to its lower affinity to *OH. This work deepens the understanding on the important role of ordering degree on BNs and enables the design of improved catalysts.

引用

页数：7

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