{"title":"富吡啶氮介孔碳包覆碳布的高效析氧反应","authors":"Yingying Li , Chi Li , Qin Zhou , Yongfu Lian","doi":"10.1016/j.apsusc.2025.162444","DOIUrl":null,"url":null,"abstract":"<div><div>Electrochemical oxygen evolution reaction (OER) plays an important role in the field of energy conversion/storage, but highly efficient electrocatalysts are required to overcome the barrier out of slow four-electron transfer oxygen kinetics. Herein, pyridinic-N doped activated carbon cloth (NACC) is prepared by successive KOH activation and urea pyrolysis and applied as an efficient OER electrocatalyst. Experimental results reveal that NACC shows a lower overpotential of 239 mV at the current density of 10 mA cm<sup>−2</sup>, a small Tafel slope of 58 mV dec<sup>-1</sup> and excellent durability, which are significantly prior to those of pristine CC. The improved electrochemical behaviors of NACC could be ascribed to the pyridinic-N doping leaded large increase in active sites, efficient charge/mass transfer and easy adsorption of hydroxide anions as well as intermediate products on active sites. Moreover, the density functional theoretical (DFT) calculations conclude that pyridinic-N-doping occurs at the zigzag edges of structural defects in carbon sheets, and the <em>meta</em>- or <em>ortho</em>-carbon atoms of pyridinic-N atoms are the main active sites, which are responsible for the outstanding OER performance of NACC.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"689 ","pages":"Article 162444"},"PeriodicalIF":6.9000,"publicationDate":"2025-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Pyridinic-N-enriched mesoporous carbon coated carbon cloth for efficient oxygen evolution reactions\",\"authors\":\"Yingying Li , Chi Li , Qin Zhou , Yongfu Lian\",\"doi\":\"10.1016/j.apsusc.2025.162444\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Electrochemical oxygen evolution reaction (OER) plays an important role in the field of energy conversion/storage, but highly efficient electrocatalysts are required to overcome the barrier out of slow four-electron transfer oxygen kinetics. Herein, pyridinic-N doped activated carbon cloth (NACC) is prepared by successive KOH activation and urea pyrolysis and applied as an efficient OER electrocatalyst. Experimental results reveal that NACC shows a lower overpotential of 239 mV at the current density of 10 mA cm<sup>−2</sup>, a small Tafel slope of 58 mV dec<sup>-1</sup> and excellent durability, which are significantly prior to those of pristine CC. The improved electrochemical behaviors of NACC could be ascribed to the pyridinic-N doping leaded large increase in active sites, efficient charge/mass transfer and easy adsorption of hydroxide anions as well as intermediate products on active sites. Moreover, the density functional theoretical (DFT) calculations conclude that pyridinic-N-doping occurs at the zigzag edges of structural defects in carbon sheets, and the <em>meta</em>- or <em>ortho</em>-carbon atoms of pyridinic-N atoms are the main active sites, which are responsible for the outstanding OER performance of NACC.</div></div>\",\"PeriodicalId\":247,\"journal\":{\"name\":\"Applied Surface Science\",\"volume\":\"689 \",\"pages\":\"Article 162444\"},\"PeriodicalIF\":6.9000,\"publicationDate\":\"2025-01-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Surface Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0169433225001576\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0169433225001576","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
电化学析氧反应(OER)在能量转换/存储领域发挥着重要作用,但要克服缓慢的四电子转移氧动力学障碍,需要高效的电催化剂。本文通过KOH活化和尿素热解制备了吡啶- n掺杂活性炭布(NACC),并将其作为高效的OER电催化剂。实验结果表明,在电流密度为10 mA cm−2时,NACC的过电位为239 mV, Tafel斜率为58 mV·dec1,耐久性明显优于原始CC。NACC电化学性能的改善可归因于吡啶- n掺杂导致活性位点的大量增加,有效的电荷/质量传递以及羟基阴离子和中间产物在活性位点上的易于吸附。此外,密度泛函理论(DFT)计算表明,吡啶- n掺杂发生在碳片结构缺陷的锯齿状边缘,并且吡啶- n原子的间位或邻位碳原子是主要的活性位点,这是NACC具有优异OER性能的原因。
Electrochemical oxygen evolution reaction (OER) plays an important role in the field of energy conversion/storage, but highly efficient electrocatalysts are required to overcome the barrier out of slow four-electron transfer oxygen kinetics. Herein, pyridinic-N doped activated carbon cloth (NACC) is prepared by successive KOH activation and urea pyrolysis and applied as an efficient OER electrocatalyst. Experimental results reveal that NACC shows a lower overpotential of 239 mV at the current density of 10 mA cm−2, a small Tafel slope of 58 mV dec-1 and excellent durability, which are significantly prior to those of pristine CC. The improved electrochemical behaviors of NACC could be ascribed to the pyridinic-N doping leaded large increase in active sites, efficient charge/mass transfer and easy adsorption of hydroxide anions as well as intermediate products on active sites. Moreover, the density functional theoretical (DFT) calculations conclude that pyridinic-N-doping occurs at the zigzag edges of structural defects in carbon sheets, and the meta- or ortho-carbon atoms of pyridinic-N atoms are the main active sites, which are responsible for the outstanding OER performance of NACC.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.