{"title":"带有 KOH 蚀刻产生的缺陷的多孔和高掺杂 N,O 无定形碳材料对 ORR 催化剂稳定性的影响","authors":"Zhaonan Sun, Chen Guo, Fanghui Wang","doi":"10.1021/acs.energyfuels.4c02482","DOIUrl":null,"url":null,"abstract":"A porous N-doped carbon (PNC) carrier with high N content, a rich pore structure, and a high specific surface area was prepared by high-temperature carbonization of polyaniline (CPANI) and KOH activation. The influence of KOH activation on the structure of the carriers was discussed through structural and morphological characterization. The PNC-2 (the mass ratio of CPANI/KOH was 1:2) carrier had more pyridine N- and O-containing functional groups that were conducive to the oxygen reduction reaction (ORR) activity and stability of catalysts. Then, PtCo alloy was loaded into carriers by the immersion method, obtaining a series of catalysts for the ORR. In acidic media, PtCo/PNC-2 has the best performance (Tafel slope = 65.7 mV dec<sup>–1</sup>, electron-rich active surface area (ECSA) = 129.2 m<sup>2</sup>g<sub>Pt</sub><sup>–1</sup>, half-wave potential = 0.913 V), whose initial current density was 97 mA cm<sup>–2</sup> and maximum power density was 676 mW cm<sup>–2</sup> in a single-cell test. After 10,000 potential cycles, the mass activity of the PtCo/PNC-2 catalyst retained at 85%. Finally, it was confirmed that high pyridine N- and O-containing functional group contents could effectively inhibit the agglomeration and shedding of PtCo nanoparticles in the durability test. It can be seen that PNC carriers are beneficial for improving the performance of ORR catalysts.","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":null,"pages":null},"PeriodicalIF":5.2000,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effect of Porous and Highly N,O-Doped Amorphous Carbon Materials with Defects Generated by KOH Etching on the Stability of ORR Catalysts\",\"authors\":\"Zhaonan Sun, Chen Guo, Fanghui Wang\",\"doi\":\"10.1021/acs.energyfuels.4c02482\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"A porous N-doped carbon (PNC) carrier with high N content, a rich pore structure, and a high specific surface area was prepared by high-temperature carbonization of polyaniline (CPANI) and KOH activation. The influence of KOH activation on the structure of the carriers was discussed through structural and morphological characterization. The PNC-2 (the mass ratio of CPANI/KOH was 1:2) carrier had more pyridine N- and O-containing functional groups that were conducive to the oxygen reduction reaction (ORR) activity and stability of catalysts. Then, PtCo alloy was loaded into carriers by the immersion method, obtaining a series of catalysts for the ORR. In acidic media, PtCo/PNC-2 has the best performance (Tafel slope = 65.7 mV dec<sup>–1</sup>, electron-rich active surface area (ECSA) = 129.2 m<sup>2</sup>g<sub>Pt</sub><sup>–1</sup>, half-wave potential = 0.913 V), whose initial current density was 97 mA cm<sup>–2</sup> and maximum power density was 676 mW cm<sup>–2</sup> in a single-cell test. After 10,000 potential cycles, the mass activity of the PtCo/PNC-2 catalyst retained at 85%. Finally, it was confirmed that high pyridine N- and O-containing functional group contents could effectively inhibit the agglomeration and shedding of PtCo nanoparticles in the durability test. It can be seen that PNC carriers are beneficial for improving the performance of ORR catalysts.\",\"PeriodicalId\":35,\"journal\":{\"name\":\"Energy & Fuels\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2024-09-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Energy & Fuels\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.energyfuels.4c02482\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Fuels","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1021/acs.energyfuels.4c02482","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
引用次数: 0
摘要
通过对聚苯胺(CPANI)进行高温碳化和 KOH 活化,制备了一种具有高 N 含量、丰富孔隙结构和高比表面积的多孔 N 掺杂碳(PNC)载体。通过结构和形态表征讨论了 KOH 活化对载体结构的影响。PNC-2(CPANI/KOH 的质量比为 1:2)载体具有更多的含吡啶 N 和 O 的官能团,有利于提高氧还原反应(ORR)活性和催化剂的稳定性。然后,通过浸泡法将铂钴合金负载到载体中,得到了一系列用于 ORR 的催化剂。在酸性介质中,PtCo/PNC-2 的性能最佳(Tafel 斜率 = 65.7 mV dec-1,富电子活性表面积 (ECSA) = 129.2 m2gPt-1,半波电位 = 0.913 V),其初始电流密度为 97 mA cm-2,单电池测试的最大功率密度为 676 mW cm-2。经过 10,000 次电位循环后,PtCo/PNC-2 催化剂的质量活性保持在 85%。最后证实,在耐久性测试中,高含量的含吡啶 N 和 O 官能团可有效抑制铂钴纳米颗粒的团聚和脱落。由此可见,PNC 载体有利于提高 ORR 催化剂的性能。
Effect of Porous and Highly N,O-Doped Amorphous Carbon Materials with Defects Generated by KOH Etching on the Stability of ORR Catalysts
A porous N-doped carbon (PNC) carrier with high N content, a rich pore structure, and a high specific surface area was prepared by high-temperature carbonization of polyaniline (CPANI) and KOH activation. The influence of KOH activation on the structure of the carriers was discussed through structural and morphological characterization. The PNC-2 (the mass ratio of CPANI/KOH was 1:2) carrier had more pyridine N- and O-containing functional groups that were conducive to the oxygen reduction reaction (ORR) activity and stability of catalysts. Then, PtCo alloy was loaded into carriers by the immersion method, obtaining a series of catalysts for the ORR. In acidic media, PtCo/PNC-2 has the best performance (Tafel slope = 65.7 mV dec–1, electron-rich active surface area (ECSA) = 129.2 m2gPt–1, half-wave potential = 0.913 V), whose initial current density was 97 mA cm–2 and maximum power density was 676 mW cm–2 in a single-cell test. After 10,000 potential cycles, the mass activity of the PtCo/PNC-2 catalyst retained at 85%. Finally, it was confirmed that high pyridine N- and O-containing functional group contents could effectively inhibit the agglomeration and shedding of PtCo nanoparticles in the durability test. It can be seen that PNC carriers are beneficial for improving the performance of ORR catalysts.
期刊介绍:
Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.