A robust asymmetric diatomic electrocatalyst for oxygen reduction reaction in both acidic and alkaline media

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-12-20 DOI:10.1016/j.apcatb.2023.123645

Pianpian Zhang , Tingting Sun , Rong Jiang , Tianyu Zheng , Qingmei Xu , Ruanbo Hu , Xinxin Wang , Kang Wang , Lianbin Xu , Dingsheng Wang , Jianzhuang Jiang

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Abstract

Herein, an asymmetric diatomic site oxygen reduction reaction (ORR) electrocatalyst with atomically dispersed Fe and Cu species co-anchored on porous nitrogen-doped polyhedra carbon was successfully prepared through a facile cooperation of post-adsorption and two-step pyrolysis method. Density functional theory (DFT) calculations reveal that the asymmetric FeCu dual atomic site experiences a symmetry destruction of electron transfer due to the existing Cu-N₄ sites and thus results in the electron redistribution in Fe_SACu_SA/NC, contributing significantly to the optimization of intermediates adsorption and acceleration of kinetics during ORR process. Attributed to the structural advantages of Fe_SA-N₄&Cu_SA-N₄ sites and highly porous carbon matrix, the Fe_SACu_SA/NC catalyst exhibits excellent electrocatalytic ORR performance with half-wave potentials (E_1/2) of 0.86 and 0.88 V versus reversible hydrogen electrode in 0.1 M HClO₄ and 0.1 M KOH solutions as well as high durability. Moreover, Fe_SACu_SA/NC-based H₂/O₂ fuel cell and zinc-air battery present superior performance with high peak power density.

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用于酸性和碱性介质中氧还原反应的强效不对称二原子电催化剂

本文通过后吸附法和两步热解法的简便合作，成功制备了一种非对称双原子位点氧还原反应（ORR）电催化剂，其原子分散的铁和铜物种共锚在多孔掺氮多面体碳上。密度泛函理论（DFT）计算表明，由于存在 Cu-N4 位点，不对称的 FeCu 双原子位点在电子传递过程中发生了对称性破坏，从而导致了 FeSACuSA/NC 中电子的重新分布，这极大地促进了 ORR 过程中中间产物吸附的优化和动力学的加速。得益于 FeSA-N4&CuSA-N4 位点和高多孔碳基质的结构优势，FeSACuSA/NC 催化剂表现出优异的电催化 ORR 性能，在 0.1 M HClO4 和 0.1 M KOH 溶液中与可逆氢电极相比，半波电位（E1/2）分别为 0.86 V 和 0.88 V，并且具有很高的耐久性。此外，基于 FeSACuSA/NC 的 H2/O2 燃料电池和锌-空气电池性能优越，峰值功率密度高。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.