Antisite defect unleashes catalytic potential in high-entropy intermetallics for oxygen reduction reaction

Abstract Developing highly active, low-cost, and durable catalysts for efficient oxygen reduction reactions remain a challenge, hindering the commercial viability of proton exchange membrane fuel cells (PEMFCs). In this study, an ordered PtZnFeCoNiCr high-entropy intermetallic electrocatalyst with P...

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Main Authors: Tao Chen, Xinkai Zhang, Hangchao Wang, Chonglin Yuan, Yuxuan Zuo, Chuan Gao, Wukun Xiao, Yue Yu, Junfei Cai, Tie Luo, Yan Xiang, Dingguo Xia
Format: Article
Language:English
Published: Nature Portfolio 2025-04-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-58679-5
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author Tao Chen
Xinkai Zhang
Hangchao Wang
Chonglin Yuan
Yuxuan Zuo
Chuan Gao
Wukun Xiao
Yue Yu
Junfei Cai
Tie Luo
Yan Xiang
Dingguo Xia
author_facet Tao Chen
Xinkai Zhang
Hangchao Wang
Chonglin Yuan
Yuxuan Zuo
Chuan Gao
Wukun Xiao
Yue Yu
Junfei Cai
Tie Luo
Yan Xiang
Dingguo Xia
author_sort Tao Chen
collection DOAJ
description Abstract Developing highly active, low-cost, and durable catalysts for efficient oxygen reduction reactions remain a challenge, hindering the commercial viability of proton exchange membrane fuel cells (PEMFCs). In this study, an ordered PtZnFeCoNiCr high-entropy intermetallic electrocatalyst with Pt antisite point defects (PD-PZFCNC-HEI) is synthesized. The electrocatalyst shows high mass activity of 4.12 A mgPt -1 toward the oxygen reduction reaction (ORR), which is 33 times that of the commercial Pt/C. PEMFC, assembled with PD-PZFCNC-HEI as the cathode (0.05 mgPt cm-2), exhibits a peak power density of 1.9 W cm-2 and a high mass activity of 3.0 A mgPt -1 at 0.9 V. Theoretical calculations combined with in situ X-ray absorption fine structure results reveal that defect engineering optimizes Pt’s electronic structure and activates non-noble metal site active centers, achieving exceptionally high ORR catalytic activity. This study provides guidance for the development of nanostructured ordered high-entropy intermetallic catalysts.
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spelling doaj-art-e9e926c7c14d43cb8799cd961b83bce12025-08-20T02:12:02ZengNature PortfolioNature Communications2041-17232025-04-0116111110.1038/s41467-025-58679-5Antisite defect unleashes catalytic potential in high-entropy intermetallics for oxygen reduction reactionTao Chen0Xinkai Zhang1Hangchao Wang2Chonglin Yuan3Yuxuan Zuo4Chuan Gao5Wukun Xiao6Yue Yu7Junfei Cai8Tie Luo9Yan Xiang10Dingguo Xia11Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityBeijing Key Laboratory of Bio-inspired Energy Materials and Devices, School of Space and Environment, Beihang UniversityBeijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityBeijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityBeijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityBeijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityBeijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityBeijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityBeijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityBeijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityBeijing Key Laboratory of Bio-inspired Energy Materials and Devices, School of Space and Environment, Beihang UniversityBeijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking UniversityAbstract Developing highly active, low-cost, and durable catalysts for efficient oxygen reduction reactions remain a challenge, hindering the commercial viability of proton exchange membrane fuel cells (PEMFCs). In this study, an ordered PtZnFeCoNiCr high-entropy intermetallic electrocatalyst with Pt antisite point defects (PD-PZFCNC-HEI) is synthesized. The electrocatalyst shows high mass activity of 4.12 A mgPt -1 toward the oxygen reduction reaction (ORR), which is 33 times that of the commercial Pt/C. PEMFC, assembled with PD-PZFCNC-HEI as the cathode (0.05 mgPt cm-2), exhibits a peak power density of 1.9 W cm-2 and a high mass activity of 3.0 A mgPt -1 at 0.9 V. Theoretical calculations combined with in situ X-ray absorption fine structure results reveal that defect engineering optimizes Pt’s electronic structure and activates non-noble metal site active centers, achieving exceptionally high ORR catalytic activity. This study provides guidance for the development of nanostructured ordered high-entropy intermetallic catalysts.https://doi.org/10.1038/s41467-025-58679-5
spellingShingle Tao Chen
Xinkai Zhang
Hangchao Wang
Chonglin Yuan
Yuxuan Zuo
Chuan Gao
Wukun Xiao
Yue Yu
Junfei Cai
Tie Luo
Yan Xiang
Dingguo Xia
Antisite defect unleashes catalytic potential in high-entropy intermetallics for oxygen reduction reaction
Nature Communications
title Antisite defect unleashes catalytic potential in high-entropy intermetallics for oxygen reduction reaction
title_full Antisite defect unleashes catalytic potential in high-entropy intermetallics for oxygen reduction reaction
title_fullStr Antisite defect unleashes catalytic potential in high-entropy intermetallics for oxygen reduction reaction
title_full_unstemmed Antisite defect unleashes catalytic potential in high-entropy intermetallics for oxygen reduction reaction
title_short Antisite defect unleashes catalytic potential in high-entropy intermetallics for oxygen reduction reaction
title_sort antisite defect unleashes catalytic potential in high entropy intermetallics for oxygen reduction reaction
url https://doi.org/10.1038/s41467-025-58679-5
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