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

Abstract 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 h...

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Main Authors: Dongdong Wang, Zhiwen Chen, Yujie Wu, Yu‐Cheng Huang, Li Tao, Jun Chen, Chung‐Li Dong, Chandra Veer Singh, Shuangyin Wang
Format: Article
Language:English
Published: Wiley 2023-02-01
Series:SmartMat
Subjects:
Online Access:https://doi.org/10.1002/smm2.1117
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author Dongdong Wang
Zhiwen Chen
Yujie Wu
Yu‐Cheng Huang
Li Tao
Jun Chen
Chung‐Li Dong
Chandra Veer Singh
Shuangyin Wang
author_facet Dongdong Wang
Zhiwen Chen
Yujie Wu
Yu‐Cheng Huang
Li Tao
Jun Chen
Chung‐Li Dong
Chandra Veer Singh
Shuangyin Wang
author_sort Dongdong Wang
collection DOAJ
description Abstract 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/cm2, which is 2.97 times of Pt/C (16.0 mW/cm2). 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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spelling doaj.art-3a7d6978f90f438a9932f7dac17cc6802022-12-26T11:27:48ZengWileySmartMat2688-819X2023-02-0141n/an/a10.1002/smm2.1117Structurally ordered high‐entropy intermetallic nanoparticles with enhanced C–C bond cleavage for ethanol oxidationDongdong Wang0Zhiwen Chen1Yujie Wu2Yu‐Cheng Huang3Li Tao4Jun Chen5Chung‐Li Dong6Chandra Veer Singh7Shuangyin Wang8State Key Laboratory of Chemo/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha Hunan ChinaDepartment of Materials Science and Engineering University of Toronto Toronto Ontario CanadaState Key Laboratory of Chemo/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha Hunan ChinaDepartment of Physics, Research Center for X‐Ray Science Tamkang University New Taipei City ChinaState Key Laboratory of Chemo/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha Hunan ChinaARC Centre of Excellence for Electromaterials Science, Intelligent Polymer Research Institute (IPRI), Australian Institute of Innovative Mate‐rials (AIIM) University of Wollongong Wollongong New South Wales AustraliaDepartment of Physics, Research Center for X‐Ray Science Tamkang University New Taipei City ChinaDepartment of Materials Science and Engineering University of Toronto Toronto Ontario CanadaState Key Laboratory of Chemo/Bio‐Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering Hunan University Changsha Hunan ChinaAbstract 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/cm2, which is 2.97 times of Pt/C (16.0 mW/cm2). 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.https://doi.org/10.1002/smm2.1117C–C bondelectrocatalysisethanol oxidationhigh‐entropy alloyshigh‐entropy intermetallic
spellingShingle Dongdong Wang
Zhiwen Chen
Yujie Wu
Yu‐Cheng Huang
Li Tao
Jun Chen
Chung‐Li Dong
Chandra Veer Singh
Shuangyin Wang
Structurally ordered high‐entropy intermetallic nanoparticles with enhanced C–C bond cleavage for ethanol oxidation
SmartMat
C–C bond
electrocatalysis
ethanol oxidation
high‐entropy alloys
high‐entropy intermetallic
title Structurally ordered high‐entropy intermetallic nanoparticles with enhanced C–C bond cleavage for ethanol oxidation
title_full Structurally ordered high‐entropy intermetallic nanoparticles with enhanced C–C bond cleavage for ethanol oxidation
title_fullStr Structurally ordered high‐entropy intermetallic nanoparticles with enhanced C–C bond cleavage for ethanol oxidation
title_full_unstemmed Structurally ordered high‐entropy intermetallic nanoparticles with enhanced C–C bond cleavage for ethanol oxidation
title_short Structurally ordered high‐entropy intermetallic nanoparticles with enhanced C–C bond cleavage for ethanol oxidation
title_sort structurally ordered high entropy intermetallic nanoparticles with enhanced c c bond cleavage for ethanol oxidation
topic C–C bond
electrocatalysis
ethanol oxidation
high‐entropy alloys
high‐entropy intermetallic
url https://doi.org/10.1002/smm2.1117
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