Structurally ordered high-entropy intermetallic nanoparticles with enhanced C-C bond cleavage for ethanol oxidation

被引:47
作者
Wang, Dongdong [1 ]
Chen, Zhiwen [2 ]
Wu, Yujie [1 ]
Huang, Yu-Cheng [3 ]
Tao, Li [1 ,5 ]
Chen, Jun [4 ]
Dong, Chung-Li [3 ]
Singh, Chandra Veer [2 ,6 ]
Wang, Shuangyin [1 ,5 ]
机构
[1] Hunan Univ, Coll Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Adv Catalyt Engn Res Ctr Minist Educ, Changsha, Hunan, Peoples R China
[2] Univ Toronto, Dept Mat Sci & Engn, Toronto, ON, Canada
[3] Tamkang Univ, Res Ctr X Ray Sci, Dept Phys, New Taipei City, Taiwan
[4] Univ Wollongong, Intelligent Polymer Res Inst IPRI, Australian Inst Innovat Mat AIIM, ARC Ctr Excellence Electromat Sci, Wollongong, NSW, Australia
[5] Hunan Univ, Coll Chem & Chem Engn, Adv Catalyt Engn Res Ctr Minist Educ, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Hunan, Peoples R China
[6] Univ Toronto, Dept Mat Sci & Engn, Toronto, ON M5S 3E4, Canada
来源
SMARTMAT | 2023年 / 4卷 / 01期
基金
加拿大自然科学与工程研究理事会; 澳大利亚研究理事会; 中国国家自然科学基金;
关键词
C-C bond; electrocatalysis; ethanol oxidation; high-entropy alloys; high-entropy intermetallic; ELECTROCATALYSTS; CATALYSTS; FRAMEWORK; GRAPHENE; ALLOYS; CARBON;
D O I
10.1002/smm2.1117
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Efficient ethanol oxidation reaction (EOR) is challenging due to the multiple reaction steps required to accomplish full oxidation to CO2 in fuel cells. High-entropy materials with the adjustable composition and unique chemical structure provide a large configurational space for designing high-performance electrocatalysts. Herein, a new class of structurally ordered PtRhFeNiCu high-entropy intermetallics (HEIs) is developed as electrocatalyst, which exhibits excellent electrocatalytic activity and CO tolerance for EOR compared to high-entropy alloys (HEAs) comprising of same elements. When the HEIs are used as anode catalysts to be assembled into a high-temperature polybenzimidazole-based direct ethanol fuel cell, the HEIs achieve a high power density of 47.50 mW/cm(2), which is 2.97 times of Pt/C (16.0 mW/cm(2)). Online gas chromatography measurements show that the developed HEIs have a stronger C-C bond-breaking ability than corresponding HEAs and Pt/C catalysts, which is further verified by density functional theory (DFT) calculations. Moreover, DFT results indicate that HEIs possess higher stability and electrochemical activity for EOR than HEAs. These results demonstrate that the HEIs could provide a new platform to develop high-performance electrocatalysts for broader applications.
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页数:10
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共 43 条
[1]   Recent progress of high-entropy materials for energy storage and conversion [J].
Amiri, Azadeh ;
Shahbazian-Yassar, Reza .
JOURNAL OF MATERIALS CHEMISTRY A, 2021, 9 (02) :782-823
[2]   Catalysts for direct ethanol fuel cells [J].
Antolini, Ermete .
JOURNAL OF POWER SOURCES, 2007, 170 (01) :1-12
[3]   Bimetallic Platinum-Rhodium Alloy Nanodendrites as Highly Active Electrocatalyst for the Ethanol Oxidation Reaction [J].
Bai, Juan ;
Xiao, Xue ;
Xue, Yuan-Yuan ;
Jiang, Jia-Xing ;
Zeng, Jing-Hui ;
Li, Xi-Fei ;
Chen, Yu .
ACS APPLIED MATERIALS & INTERFACES, 2018, 10 (23) :19755-19763
[4]   Selective Ethanol Oxidation Reaction at the Rh-SnO2 Interface [J].
Bai, Shuxing ;
Xu, Yong ;
Cao, Kailei ;
Huang, Xiaoqing .
ADVANCED MATERIALS, 2021, 33 (05)
[5]   Enhancing C-C Bond Scission for Efficient Ethanol Oxidation using PtIr Nanocube Electrocatalysts [J].
Chang, Qiaowan ;
Kattel, Shyam ;
Li, Xing ;
Liang, Zhixiu ;
Tackett, Brian M. ;
Denny, Steven R. ;
Zhang, Pu ;
Su, Dong ;
Chen, Jingguang G. ;
Chen, Zheng .
ACS CATALYSIS, 2019, 9 (09) :7618-7625
[6]   Lattice-strained metal-organic-framework arrays for bifunctional oxygen electrocatalysis [J].
Cheng, Weiren ;
Zhao, Xu ;
Su, Hui ;
Tang, Fumin ;
Che, Wei ;
Zhang, Hui ;
Liu, Qinghua .
NATURE ENERGY, 2019, 4 (02) :115-122
[7]   Unusually High Activity of Pt Islands on Rh(111) Electrodes for Ethanol Oxidation [J].
Del Colle, Vinicius ;
Grozovski, Vitali ;
Herrero, Enrique ;
Feliu, Juan M. .
CHEMCATCHEM, 2013, 5 (06) :1350-1353
[8]   Porous Trimetallic PtRhCu Cubic Nanoboxes for Ethanol Electrooxidation [J].
Han, Shu-He ;
Liu, Hui-Min ;
Chen, Pei ;
Jiang, Jia-Xing ;
Chen, Yu .
ADVANCED ENERGY MATERIALS, 2018, 8 (24)
[9]   Newly-Designed Complex Ternary Pt/PdCu Nanoboxes Anchored on Three-Dimensional Graphene Framework for Highly Efficient Ethanol Oxidation [J].
Hu, Chuangang ;
Cheng, Huhu ;
Zhao, Yang ;
Hu, Yue ;
Liu, Yong ;
Dai, Liming ;
Qu, Liangti .
ADVANCED MATERIALS, 2012, 24 (40) :5493-5498
[10]   Roles of Mo Surface Dopants in Enhancing the ORR Performance of Octahedral PtNi Nanoparticles [J].
Jia, Qingying ;
Zhao, Zipeng ;
Cao, Liang ;
Li, Jingkun ;
Ghoshal, Shraboni ;
Davies, Veronica ;
Stavitski, Eli ;
Attenkofer, Klaus ;
Liu, Zeyan ;
Li, Mufan ;
Duan, Xiangfeng ;
Mukerjee, Sanjeev ;
Mueller, Tim ;
Huang, Yu .
NANO LETTERS, 2018, 18 (02) :798-804