Dual Metal Site Fe Single Atom Catalyst with Improved Stability in Acidic Conditions
Yuehua Wang,
Shuang Li,
Rui Xu,
Junpeng Chen,
Yifan Hao,
Ke Li,
Yan Li,
Yingmei Li,
Jing Wang
Affiliations
Yuehua Wang
State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, China
Shuang Li
Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemistry Engineering, Yanshan University, Qinhuangdao 066004, China
Rui Xu
Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemistry Engineering, Yanshan University, Qinhuangdao 066004, China
Junpeng Chen
Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemistry Engineering, Yanshan University, Qinhuangdao 066004, China
Yifan Hao
Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemistry Engineering, Yanshan University, Qinhuangdao 066004, China
Ke Li
Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemistry Engineering, Yanshan University, Qinhuangdao 066004, China
Yan Li
Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemistry Engineering, Yanshan University, Qinhuangdao 066004, China
Yingmei Li
State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, China
Jing Wang
State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, China
Dual atom catalysts (DACs) not only retain uniform active sites and high atomic utilization efficiency as the single atom catalysts, but the two adjacent metal sites also cooperate and play a synergistic role to achieve additional benefits. However, the relationships connecting their dual-site synergistic effects on catalytic performance are not well rationalized due to limited pairs available from experiments. Herein, Fe/M dual sites supported by nitrogen doped carbon (Fe/M-N-C whereby M from 3 d–5 d electron containing transition metals) have been screened as an oxygen reduction reaction (ORR) catalyst. The results show that the absorption strength of ORR intermediates on four nitrogen coordinated metals is weaker than the three coordinated metals, which promotes favourable ORR activities. As a result, we recommended FeIr, FeRh, FeRu and FeOs as promising ORR catalysts. Ab initio molecular dynamic (AIMD) simulations suggest Fe/M-N-C (M = Ir, Rh, Ru and Os) catalysts with encouraging structural stability at room temperature. Furthermore, it is found that the nitrogen atoms in-between metals are vulnerable sites for proton attacking, yet the protonation process demands high energy, even under O2 atmosphere, which underlines good tolerance under acidic conditions. This work provides a broad understanding of Fe based catalyst and a new direction for catalytic design.
