Size-dependent activity of Fe-N-doped mesoporous carbon nanoparticles towards oxygen reduction reaction

The rational design of Fe–N–C catalysts that possess easily accessible active sites and favorable mass transfer, which are usually determined by the structure of catalyst supports, is crucial for the oxygen reduction reaction (ORR). In this study, an oleic acid-assisted soft-templating approach is d...

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Main Authors: Yilun Zhao, Zhengbin Tian, Wenquan Wang, Xiaohui Deng, Jo-Chi Tseng, Guanghui Wang
Format: Article
Language:English
Published: KeAi Communications Co., Ltd. 2024-06-01
Series:Green Carbon
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Online Access:http://www.sciencedirect.com/science/article/pii/S2950155524000260
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author Yilun Zhao
Zhengbin Tian
Wenquan Wang
Xiaohui Deng
Jo-Chi Tseng
Guanghui Wang
author_facet Yilun Zhao
Zhengbin Tian
Wenquan Wang
Xiaohui Deng
Jo-Chi Tseng
Guanghui Wang
author_sort Yilun Zhao
collection DOAJ
description The rational design of Fe–N–C catalysts that possess easily accessible active sites and favorable mass transfer, which are usually determined by the structure of catalyst supports, is crucial for the oxygen reduction reaction (ORR). In this study, an oleic acid-assisted soft-templating approach is developed to synthesize size-controlled nitrogen-doped carbon nanoparticles (ranging from 130 nm to 60 nm and 35 nm, respectively) that feature spiral mesopores on their surface (SMCs). Next, atomically dispersed Fe–Nx sites are fabricated on the size-tunable SMCs (Fe1/SMC-x, where x represents the SMC size) and the size-dependent activity toward ORR is investigated. It is found that the catalytic performance of Fe1/SMCs is significantly influenced by the size of SMCs, where the Fe1/SMC-60 catalyst shows the highest ORR activity with a half-wave potential of 0.90 V vs. RHE in KOH electrolyte, indicating that the gas-liquid-solid three-phase interface on the Fe1/SMC-60 enhances the accessibility of Fe–Nx sites. In addition, when using Fe1/SMC-60 as the cathode catalyst in aqueous zinc-air batteries (ZABs), it delivers a higher open-circuit voltage (1.514 V), a greater power density (223 mW cm−2), and a larger specific capacity/energy than Pt/C-based counterparts. These results further highlight the potential of Fe1/SMC-60 for practical energy devices associated with ORR and the importance of size-controlled synthesis of SMCs.
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publisher KeAi Communications Co., Ltd.
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spelling doaj-art-50e2ceda8f2349c29a910c8d91e7e67c2025-08-20T03:42:45ZengKeAi Communications Co., Ltd.Green Carbon2950-15552024-06-012222123010.1016/j.greenca.2024.03.002Size-dependent activity of Fe-N-doped mesoporous carbon nanoparticles towards oxygen reduction reactionYilun Zhao0Zhengbin Tian1Wenquan Wang2Xiaohui Deng3Jo-Chi Tseng4Guanghui Wang5Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China; Shandong Energy Institute, Qingdao 266101, China; Qingdao New Energy Shandong Laboratory, Qingdao 266101, China; University of Chinese Academy of Sciences, Beijing 100049, ChinaQingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China; Shandong Energy Institute, Qingdao 266101, China; Qingdao New Energy Shandong Laboratory, Qingdao 266101, China; Corresponding authors.Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China; Shandong Energy Institute, Qingdao 266101, China; Qingdao New Energy Shandong Laboratory, Qingdao 266101, China; University of Chinese Academy of Sciences, Beijing 100049, ChinaQingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China; Shandong Energy Institute, Qingdao 266101, China; Qingdao New Energy Shandong Laboratory, Qingdao 266101, ChinaJapan Synchrotron Radiation Research Institute, Hyogo 679-5198, JapanQingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China; Shandong Energy Institute, Qingdao 266101, China; Qingdao New Energy Shandong Laboratory, Qingdao 266101, China; University of Chinese Academy of Sciences, Beijing 100049, China; Corresponding authors.The rational design of Fe–N–C catalysts that possess easily accessible active sites and favorable mass transfer, which are usually determined by the structure of catalyst supports, is crucial for the oxygen reduction reaction (ORR). In this study, an oleic acid-assisted soft-templating approach is developed to synthesize size-controlled nitrogen-doped carbon nanoparticles (ranging from 130 nm to 60 nm and 35 nm, respectively) that feature spiral mesopores on their surface (SMCs). Next, atomically dispersed Fe–Nx sites are fabricated on the size-tunable SMCs (Fe1/SMC-x, where x represents the SMC size) and the size-dependent activity toward ORR is investigated. It is found that the catalytic performance of Fe1/SMCs is significantly influenced by the size of SMCs, where the Fe1/SMC-60 catalyst shows the highest ORR activity with a half-wave potential of 0.90 V vs. RHE in KOH electrolyte, indicating that the gas-liquid-solid three-phase interface on the Fe1/SMC-60 enhances the accessibility of Fe–Nx sites. In addition, when using Fe1/SMC-60 as the cathode catalyst in aqueous zinc-air batteries (ZABs), it delivers a higher open-circuit voltage (1.514 V), a greater power density (223 mW cm−2), and a larger specific capacity/energy than Pt/C-based counterparts. These results further highlight the potential of Fe1/SMC-60 for practical energy devices associated with ORR and the importance of size-controlled synthesis of SMCs.http://www.sciencedirect.com/science/article/pii/S2950155524000260Soft-templating approachSize-dependent activityFe–N–C catalystOxygen reduction reactionZinc-air battery
spellingShingle Yilun Zhao
Zhengbin Tian
Wenquan Wang
Xiaohui Deng
Jo-Chi Tseng
Guanghui Wang
Size-dependent activity of Fe-N-doped mesoporous carbon nanoparticles towards oxygen reduction reaction
Green Carbon
Soft-templating approach
Size-dependent activity
Fe–N–C catalyst
Oxygen reduction reaction
Zinc-air battery
title Size-dependent activity of Fe-N-doped mesoporous carbon nanoparticles towards oxygen reduction reaction
title_full Size-dependent activity of Fe-N-doped mesoporous carbon nanoparticles towards oxygen reduction reaction
title_fullStr Size-dependent activity of Fe-N-doped mesoporous carbon nanoparticles towards oxygen reduction reaction
title_full_unstemmed Size-dependent activity of Fe-N-doped mesoporous carbon nanoparticles towards oxygen reduction reaction
title_short Size-dependent activity of Fe-N-doped mesoporous carbon nanoparticles towards oxygen reduction reaction
title_sort size dependent activity of fe n doped mesoporous carbon nanoparticles towards oxygen reduction reaction
topic Soft-templating approach
Size-dependent activity
Fe–N–C catalyst
Oxygen reduction reaction
Zinc-air battery
url http://www.sciencedirect.com/science/article/pii/S2950155524000260
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AT zhengbintian sizedependentactivityoffendopedmesoporouscarbonnanoparticlestowardsoxygenreductionreaction
AT wenquanwang sizedependentactivityoffendopedmesoporouscarbonnanoparticlestowardsoxygenreductionreaction
AT xiaohuideng sizedependentactivityoffendopedmesoporouscarbonnanoparticlestowardsoxygenreductionreaction
AT jochitseng sizedependentactivityoffendopedmesoporouscarbonnanoparticlestowardsoxygenreductionreaction
AT guanghuiwang sizedependentactivityoffendopedmesoporouscarbonnanoparticlestowardsoxygenreductionreaction