Breaking the Linear Scaling Relationship by Compositional and Structural Crafting of Ternary Cu-Au/Ag Nanoframes for Electrocatalytic Ethylene Production

被引：136

作者：

Xiong, Likun ^{[1
,2
]}

Zhang, Xiang ^{[1
,2
]}

Yuan, Hao ^{[3
]}

Wang, Juan ^{[4
]}

Yuan, Xuzhou ^{[1
,2
]}

Lian, Yuebin ^{[1
,2
]}

Jin, Huidong ^{[1
,2
]}

Sun, Hao ^{[1
,2
]}

Deng, Zhao ^{[1
,2
]}

Wang, Dan ^{[1
,2
]}

Hu, Jiapeng ^{[1
,2
]}

Hu, Huimin ^{[1
,2
]}

Choi, Jinho ^{[1
,2
]}

Li, Jiong ^{[4
]}

Chen, Yufeng ^{[3
]}

Zhong, Jun ^{[3
]}

Guo, Jun ^{[5
]}

Rummerli, Mark H. ^{[1
,2
]}

Xu, Lai ^{[3
]}

Peng, Yang ^{[1
,2
]}

机构：

[1] Soochow Univ, Coll Energy, Soochow Inst Energy & Mat Innovat SIEMIS, Suzhou, Jiangsu, Peoples R China

[2] Soochow Univ, Key Lab Adv Carbon Mat & Wearable Energy Technol, Suzhou, Jiangsu, Peoples R China

[3] Soochow Univ, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Inst Funct Nano & Soft Mat FUNSOM, Suzhou, Jiangsu, Peoples R China

[4] Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Beijing, Peoples R China

[5] Soochow Univ, Anal & Testing Ctr, Suzhou, Jiangsu, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2021年 / 60卷 / 05期

关键词：

carbon dioxide; metal nanoframes; electroreduction; heterogeneous catalysis; linear scaling relationships; CO2; ELECTROREDUCTION; CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; SPECTROSCOPIC OBSERVATION; GOLD NANOFRAMES; ACTIVE-SITES; AU; CATALYST; INTERMEDIATE; NANOCRYSTALS;

D O I：

10.1002/anie.202012631

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Electrocatalytic conversion of carbon dioxide into high-value multicarbon (C2+) chemical feedstocks offers a promising avenue to liberate the chemical industry from fossil-resource dependence and eventually close the anthropogenic carbon cycle but is severely impeded by the lack of high-performance catalysts. To break the linear scaling relationship of intermediate binding and minimize the kinetic barrier of CO2 reduction reactions, ternary Cu-Au/Ag nanoframes were fabricated to decouple the functions of CO generation and C-C coupling, whereby the former is promoted by the alloyed Ag/Au substrate and the latter is facilitated by the highly strained and positively charged Cu domains. Thus, C2H4 production in an H-cell and a flow cell occurred with high Faradic efficiencies of 69 +/- 5 and 77 +/- 2 %, respectively, as well as good electrocatalytic stability and material durability. In situ IR and DFT calculations unveiled two competing pathways for C2H4 generation, of which direct CO dimerization is energetically favored.

引用

页码：2508 / 2518

页数：11

共 68 条

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