青岛科技大学化学与分子工程学院王磊研究组取得一项新突破。他们的研究显示,微孔硬碳载体激发了先进空气阴极单原子电催化剂的卓越性能。相关论文于2025年4月1日发表于国际顶尖学术期刊《德国应用化学》杂志上。
包含金属-氮(MNx)基团的单原子催化剂在氧还原反应(ORR)中表现出良好的性能。在空间受限的微环境上的修饰,在获得高效催化剂方面赢得了共同的关注,但对于MNx部分从调节ORR的能量学和动力学方面还有待检验。将Fe单原子(SAs)固定在微孔硬碳(Fe-SAs/MPC)中,其微孔结构具有皱褶的石墨烯片,为催化提供了受限的微环境。Fe-SAs/MPC具有0.927 V的半波电位和良好的ORR稳定性。理论研究揭示了O*中间体与微孔内表面之间的氢键能显著促进其质子化,加速整体ORR动力学。Fe-SAs/MPC空气阴极驱动的水电池和准固态锌空气电池均表现出良好的稳定性和较小的充放电电压间隙。重要的是,当作为工业氯碱工艺的空气阴极时,基于Fe-SAs/ MPC的液流电池的施加电压达到300 mA cm2为1.57 V,比Pt/ c基电压小210 mV。这些发现为提高MNx基团的电化学性能提供了深入的微环境见解,并为未来满足工业应用要求的催化剂开发铺平了道路。
附:英文原文
Title: Microporous Hard Carbon Support Provokes Exceptional Performance of Single Atom Electrocatalysts for Advanced Air Cathodes
Author: Haijing Liu, Ping Li, Kaicai Fan, Fenghong Lu, Qi Sun, Qi Zhang, Bin Li, Yajie Shu, Lingbo Zong, Lei Wang
Issue&Volume: 2025-04-01
Abstract: Single atom catalysts embracing metal-nitrogen (MNx) moieties show promising performance for oxygen reduction reaction (ORR). The modification on spatially confined microenvironments, which won copious attention with respect to achieving efficient catalysts, are auspicious but yet to be inspected for MNx moieties from modulating the energetics and kinetics of ORR. Here, Fe single atoms (SAs) are immobilized in microporous hard carbon (Fe-SAs/MPC), in which the microporous structure with crumpled graphene sheets serves confined microenvironment for catalysis. Fe-SAs/MPC holds a remarkable half-wave potential of 0.927 V and excellent stability for ORR. Theoretical studies unveil that hydrogen bonding between the intermediate of O* and micropore interior surfaces substantially promotes its protonation and accelerates overall ORR kinetics. Both the aqueous and quasi-solid-state zinc-air batteries driven by Fe-SAs/MPC air cathode show excellent stability with small charging/discharging voltage gaps. Importantly, when used as the air cathode for industrial chlor-alkali process, the applied voltage of Fe-SAs/MPC-based flow cell to reach 300 mA cm2 is 1.57 V, which is 210 mV smaller than Pt/C-based one. These findings provide in-depth insights into the confined microenvironment of MNx moieties for boosted electrochemical performance, and pave the pathways for future catalyst development satisfying the requirement of industrial applications.
DOI: 10.1002/anie.202501307
Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202501307
Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx