Chunqiang Zhuang, Huanqiao Li, Xiaoming Zhang, Hong Zhang, Suli Wang and Gongquan Sun
{"title":"直接co进料高温质子交换膜燃料电池的优化负载铑单原子催化剂","authors":"Chunqiang Zhuang, Huanqiao Li, Xiaoming Zhang, Hong Zhang, Suli Wang and Gongquan Sun","doi":"10.1039/D5TA00897B","DOIUrl":null,"url":null,"abstract":"<p >The presence of carbon monoxide (CO) in crude hydrogen is a significant factor hindering the commercialization of hydrogen fuel cells. Introducing a direct CO fuel cell upstream can selectively oxidize and remove CO from crude hydrogen, thereby releasing electrical energy. The purified crude hydrogen is then fed into the downstream hydrogen fuel cell, which helps mitigate the poisoning effect on platinum (Pt) catalysts. Rhodium (Rh) and iridium (Ir) based single-atom catalysts (SACs) have demonstrated potential in the electrochemical CO oxidation reaction (COOR). However, the low density of SAC active sites (Rh metal loading <1 wt%) hinders their further development for use in direct CO fueled PEMFCs. To address this challenge, a two-step pyrolysis method was developed, yielding a series of atomically dispersed Rh on N-doped carbon with several different Rh metal loadings from 0.25 wt% to 7.43 wt%. Half-cell test results demonstrated that with the increment of Rh loading, the overpotential for the COOR at 1 mA cm<small><sup>−2</sup></small> of CO oxidation gradually decreased, while the limiting current density gradually increased, indicating the high COOR activity on the SAC with a higher metal loading. The optimum Rh metal loading was determined to be 2.88 wt% and the limiting current density was found to be 2.4 mA cm<small><sup>−2</sup></small> with a mass activity of up to 4.18 A mg<small><sub>Rh</sub></small><small><sup>−1</sup></small>. Furthermore, a peak power density of 208.4 mW cm<small><sup>−2</sup></small> was achieved in a high-temperature single cell utilizing direct CO feed, thereby demonstrating a stable performance over a 22-hours period. This finding indicates a potential robust CO removal capability.</p>","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":" 20","pages":" 14672-14680"},"PeriodicalIF":9.5000,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Rh single-atom catalysts with optimized metal loading for direct CO-feed high-temperature proton exchange membrane fuel cells†\",\"authors\":\"Chunqiang Zhuang, Huanqiao Li, Xiaoming Zhang, Hong Zhang, Suli Wang and Gongquan Sun\",\"doi\":\"10.1039/D5TA00897B\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The presence of carbon monoxide (CO) in crude hydrogen is a significant factor hindering the commercialization of hydrogen fuel cells. Introducing a direct CO fuel cell upstream can selectively oxidize and remove CO from crude hydrogen, thereby releasing electrical energy. The purified crude hydrogen is then fed into the downstream hydrogen fuel cell, which helps mitigate the poisoning effect on platinum (Pt) catalysts. Rhodium (Rh) and iridium (Ir) based single-atom catalysts (SACs) have demonstrated potential in the electrochemical CO oxidation reaction (COOR). However, the low density of SAC active sites (Rh metal loading <1 wt%) hinders their further development for use in direct CO fueled PEMFCs. To address this challenge, a two-step pyrolysis method was developed, yielding a series of atomically dispersed Rh on N-doped carbon with several different Rh metal loadings from 0.25 wt% to 7.43 wt%. Half-cell test results demonstrated that with the increment of Rh loading, the overpotential for the COOR at 1 mA cm<small><sup>−2</sup></small> of CO oxidation gradually decreased, while the limiting current density gradually increased, indicating the high COOR activity on the SAC with a higher metal loading. The optimum Rh metal loading was determined to be 2.88 wt% and the limiting current density was found to be 2.4 mA cm<small><sup>−2</sup></small> with a mass activity of up to 4.18 A mg<small><sub>Rh</sub></small><small><sup>−1</sup></small>. Furthermore, a peak power density of 208.4 mW cm<small><sup>−2</sup></small> was achieved in a high-temperature single cell utilizing direct CO feed, thereby demonstrating a stable performance over a 22-hours period. This finding indicates a potential robust CO removal capability.</p>\",\"PeriodicalId\":82,\"journal\":{\"name\":\"Journal of Materials Chemistry A\",\"volume\":\" 20\",\"pages\":\" 14672-14680\"},\"PeriodicalIF\":9.5000,\"publicationDate\":\"2025-04-07\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Materials Chemistry A\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2025/ta/d5ta00897b\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/ta/d5ta00897b","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Rh single-atom catalysts with optimized metal loading for direct CO-feed high-temperature proton exchange membrane fuel cells†
The presence of carbon monoxide (CO) in crude hydrogen is a significant factor hindering the commercialization of hydrogen fuel cells. Introducing a direct CO fuel cell upstream can selectively oxidize and remove CO from crude hydrogen, thereby releasing electrical energy. The purified crude hydrogen is then fed into the downstream hydrogen fuel cell, which helps mitigate the poisoning effect on platinum (Pt) catalysts. Rhodium (Rh) and iridium (Ir) based single-atom catalysts (SACs) have demonstrated potential in the electrochemical CO oxidation reaction (COOR). However, the low density of SAC active sites (Rh metal loading <1 wt%) hinders their further development for use in direct CO fueled PEMFCs. To address this challenge, a two-step pyrolysis method was developed, yielding a series of atomically dispersed Rh on N-doped carbon with several different Rh metal loadings from 0.25 wt% to 7.43 wt%. Half-cell test results demonstrated that with the increment of Rh loading, the overpotential for the COOR at 1 mA cm−2 of CO oxidation gradually decreased, while the limiting current density gradually increased, indicating the high COOR activity on the SAC with a higher metal loading. The optimum Rh metal loading was determined to be 2.88 wt% and the limiting current density was found to be 2.4 mA cm−2 with a mass activity of up to 4.18 A mgRh−1. Furthermore, a peak power density of 208.4 mW cm−2 was achieved in a high-temperature single cell utilizing direct CO feed, thereby demonstrating a stable performance over a 22-hours period. This finding indicates a potential robust CO removal capability.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.