Theory-guided design of atomically dispersed dual-metal catalysts for superior oxygen reduction reaction activity
The widespread application of electrochemical energy conversion devices, such as proton exchange membrane fuel cells, is hindered by the kinetically sluggish oxygen reduction reaction (ORR) at the cathode. Transition-metal and nitrogen codoped carbon materials (TM−N−C) are among the most promising c...
| Main Authors: | , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
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2023
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| Online Access: | https://hdl.handle.net/10356/171457 |
| _version_ | 1826110189977206784 |
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| author | Yang, Yuqi Wang, Qing Mei, Bingbao Han, Zengyu Sun, Fanfei Shang, Lu Yang, Shuai Wei, Yao Wu, Dongshuang Jiang, Zheng |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Yang, Yuqi Wang, Qing Mei, Bingbao Han, Zengyu Sun, Fanfei Shang, Lu Yang, Shuai Wei, Yao Wu, Dongshuang Jiang, Zheng |
| author_sort | Yang, Yuqi |
| collection | NTU |
| description | The widespread application of electrochemical energy conversion devices, such as proton exchange membrane fuel cells, is hindered by the kinetically sluggish oxygen reduction reaction (ORR) at the cathode. Transition-metal and nitrogen codoped carbon materials (TM−N−C) are among the most promising catalysts to solve this problem. Particularly, dual-metal TM−N−C have already displayed excellent performance. However, further knowledge on the reaction mechanism and the structure−activity relationship is still required. In this study, we established three dual-metal TM−N−C models (FeMn−N−C, FeCo−N−C, and FeNi−N−C) to investigate the electronic interaction between the metallic sites and their corresponding adsorption strength for oxygenated intermediates in ORR electrocatalysis. Then, using density functional theory calculations, we determined that the ORR activity of the dual-metal TM−N−C models followed the order of FeCo−N−C > FeNi−N−C > FeMn−N−C. We confirmed the theoretically predicted activity by synthesizing atomically dispersed FeMn−N−C, FeCo−N−C, and FeNi−N−C catalysts using metal-organic framework precursors, among which FeCo−N−C showed the best results in terms of ORR onset potential and half-wave potential (0.92 and 0.81 V vs. the reference hydrogen electrode in 0.1 M HClO4, respectively.). The results demonstrate the feasibility of the theory-guided rational design of efficient dual-metal catalysts for ORR electrocatalysis. |
| first_indexed | 2024-10-01T02:30:21Z |
| format | Journal Article |
| id | ntu-10356/171457 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T02:30:21Z |
| publishDate | 2023 |
| record_format | dspace |
| spelling | ntu-10356/1714572023-10-26T08:19:25Z Theory-guided design of atomically dispersed dual-metal catalysts for superior oxygen reduction reaction activity Yang, Yuqi Wang, Qing Mei, Bingbao Han, Zengyu Sun, Fanfei Shang, Lu Yang, Shuai Wei, Yao Wu, Dongshuang Jiang, Zheng School of Materials Science and Engineering Engineering::Materials Density Functional Theory Dual-Metal Catalysts The widespread application of electrochemical energy conversion devices, such as proton exchange membrane fuel cells, is hindered by the kinetically sluggish oxygen reduction reaction (ORR) at the cathode. Transition-metal and nitrogen codoped carbon materials (TM−N−C) are among the most promising catalysts to solve this problem. Particularly, dual-metal TM−N−C have already displayed excellent performance. However, further knowledge on the reaction mechanism and the structure−activity relationship is still required. In this study, we established three dual-metal TM−N−C models (FeMn−N−C, FeCo−N−C, and FeNi−N−C) to investigate the electronic interaction between the metallic sites and their corresponding adsorption strength for oxygenated intermediates in ORR electrocatalysis. Then, using density functional theory calculations, we determined that the ORR activity of the dual-metal TM−N−C models followed the order of FeCo−N−C > FeNi−N−C > FeMn−N−C. We confirmed the theoretically predicted activity by synthesizing atomically dispersed FeMn−N−C, FeCo−N−C, and FeNi−N−C catalysts using metal-organic framework precursors, among which FeCo−N−C showed the best results in terms of ORR onset potential and half-wave potential (0.92 and 0.81 V vs. the reference hydrogen electrode in 0.1 M HClO4, respectively.). The results demonstrate the feasibility of the theory-guided rational design of efficient dual-metal catalysts for ORR electrocatalysis. This work has been financially supported by the National Key Research and Development Program of China (2022YFA1503801), the National Natural Science Foundation of China (12205359) and Natural Science Foundation of Shanghai (23ZR1471400). 2023-10-26T08:19:24Z 2023-10-26T08:19:24Z 2023 Journal Article Yang, Y., Wang, Q., Mei, B., Han, Z., Sun, F., Shang, L., Yang, S., Wei, Y., Wu, D. & Jiang, Z. (2023). Theory-guided design of atomically dispersed dual-metal catalysts for superior oxygen reduction reaction activity. ChemCatChem, 15(15), e202300534-. https://dx.doi.org/10.1002/cctc.202300534 1867-3880 https://hdl.handle.net/10356/171457 10.1002/cctc.202300534 2-s2.0-85163810598 15 15 e202300534 en ChemCatChem © 2023 Wiley-VCH GmbH. All rights reserved. |
| spellingShingle | Engineering::Materials Density Functional Theory Dual-Metal Catalysts Yang, Yuqi Wang, Qing Mei, Bingbao Han, Zengyu Sun, Fanfei Shang, Lu Yang, Shuai Wei, Yao Wu, Dongshuang Jiang, Zheng Theory-guided design of atomically dispersed dual-metal catalysts for superior oxygen reduction reaction activity |
| title | Theory-guided design of atomically dispersed dual-metal catalysts for superior oxygen reduction reaction activity |
| title_full | Theory-guided design of atomically dispersed dual-metal catalysts for superior oxygen reduction reaction activity |
| title_fullStr | Theory-guided design of atomically dispersed dual-metal catalysts for superior oxygen reduction reaction activity |
| title_full_unstemmed | Theory-guided design of atomically dispersed dual-metal catalysts for superior oxygen reduction reaction activity |
| title_short | Theory-guided design of atomically dispersed dual-metal catalysts for superior oxygen reduction reaction activity |
| title_sort | theory guided design of atomically dispersed dual metal catalysts for superior oxygen reduction reaction activity |
| topic | Engineering::Materials Density Functional Theory Dual-Metal Catalysts |
| url | https://hdl.handle.net/10356/171457 |
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