文献类型：期刊文献

英文题名：Ultrastable Fe-N-C Fuel Cell Electrocatalysts by Eliminating Non-Coordinating Nitrogen and Regulating Coordination Structures at High Temperatures

作者：Xia, Dongsheng[1];Tang, Xuan[2,3];Dai, Sheng[2,3];Ge, Rile[4];Rykov, Alexander[4];Wang, Junhu[4];Huang, Tzu-Hsi[5];Wang, Kuan-Wen[5];Wei, Yinping[1];Zhang, Kai[1];Li, Jia[1];Gan, Lin[1];Kang, Feiyu[1]

机构：[1]Tsinghua Univ, Inst Mat Res, Tsinghua Shenzhen Int Grad Sch, Shenzhen Geim Graphene Res Ctr, Shenzhen 518055, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Inst Fine Chem, Frontiers Sci Ctr Materiobiol & Dynam Chem,Feringa, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Inst Fine Chem, Frontiers Sci Ctr Materiobiol & Dynam Chem,Feringa, Shanghai 200237, Peoples R China;[4]Chinese Acad Sci, Dalian Inst Chem Phys, Ctr Adv Mossbauer Spect, Mossbauer Effect Data Ctr, Dalian 116023, Peoples R China;[5]Natl Cent Univ, Inst Mat Sci & Engn, Taoyuan 320, Taiwan

年份：2023

卷号：35

期号：5

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20225113278580);WOS:【SCI-EXPANDED(收录号:WOS:000899653800001)】；

基金：This work was supported by the National Natural Science Foundation of China (grant nos. 52173222, 22109088, and 11874036), the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (grant no. 2017BT01N111), Basic Research Project of Shenzhen, China (WDZ20200819115243002, JCYJ20200109142816479 and JCYJ20170817161445322), China Postdoctoral Science Foundation (grant no. 2020M680545), Fundamental Research Funds for the Central Universities, Shanghai Rising-star Program (20QA1402400), and the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning. The authors also appreciate the help from the Materials and Devices Testing Center at Tsinghua Shenzhen International Graduate School (SIGS).

语种：英文

外文关键词：coordination structures; Fe-N-C single atom catalysts; operation; storage stability; oxygen reduction reaction; proton exchange membrane fuel cells

摘要：Pyrolyzed Fe-N-C materials have attracted considerable interest as one of the most active noble-metal-free electrocatalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). Despite significant progress is made in improving their catalytic activity during past decades, the Fe-N-C catalysts still suffer from fairly poor electrochemical and storage stability, which greatly hurdles their practical application. Here, an effective strategy is developed to greatly improve their catalytic stability in PEMFCs and storage stability by virtue of previously unexplored high-temperature synthetic chemistry between 1100 and 1200 degrees C. Pyrolysis at this rarely adopted temperature range not only enables the elimination of less active nitrogen-doped carbon sites that generate detrimental peroxide byproduct but also regulates the coordination structure of Fe-N-C from less stable D1 (O-FeN4C12) to a more stable D2 structure (FeN4C10). The optimized Fe-N-C catalyst exhibits excellent stability in PEMFCs (>80% performance retention after 30 h under H-2/O-2 condition) and no activity loss after 35 day storage while maintaining a competitive ORR activity and PEMFC performance.