磷介导的硒双原子双功能氧反应和长寿命低温能量转换

IF 19.9 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Advanced Functional Materials Pub Date : 2025-01-17 DOI:10.1002/adfm.202423476
Lingzhi Xia, Jianhua Zhang, Pengfei Yan, Kai-Ling Zhou, Yuhong Jin, Xiaoxing Ke, Jingbin Liu, Hao Wang
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摘要

对于双功能氧反应和能量转换装置来说,快速的动力学和稳定的原子构型是必不可少的,但目前还不尽如人意。本文采用P定向介导的单原子沉积策略,构建了由周期性排列的Se-P-Se组态组成的石墨氮碳骨架Se双原子结构(P-Se双原子- nc)。原位/非原位实验结合理论计算表明,NC中相邻Se原子的位间距离效应和Se-P结合效应使P-Se双原子-NC具有稳定的原子构型和超持久的寿命,而P 2p-Se 3d-C 2p轨道杂化和电子转移所建立的局部极化电子微环境显著促进了H2O-O2耦合。促进o -中间体的吸附/解吸,加速电子传递动力学。此外,相邻的Se原子具有周期性排列的结构,可以为反应物的吸收和转化提供更多的位点。因此,所制备的催化剂表现出顶级的双功能活性,超低电位差(ΔE)为0.58 V,并提供了出色的低温比容量796.41 mAh gZn - 1,以及在- 40°C下组装锌-空气电池的超耐用寿命超过1000 h。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Phosphorus-Mediated Selenium Dual Atoms for Bifunctional Oxygen Reactions and Long-Life Low-Temperature Energy Conversion

Rapid kinetics and stable atom configuration of the catalysts are essential and greatly sought after for bifunctional oxygen reactions and energy conversion devices, but remain unsatisfactory. Herein, the Se dual atoms structure consisting of the periodically arranged Se-P-Se configurations within graphitic nitrogen carbon framework (P-Se dual atoms-NC) is constructed by P directionally mediated single atoms deposition strategy. The in situ/ex situ experiments combining the theoretical calculations reveal that both the inter-site distance effect of the adjacent Se atoms in the NC and the Se-P binding effect endow P-Se dual atoms-NC with a stable atom configuration and ultra-durable lifespan, and the locally polarized electronic micro-environment built by P 2p-Se 3d-C 2p orbital hybridization and the electrons transfer significantly promotes H2O-O2 coupling, boosts the adsorption/desorption of O-intermediates and accelerates the electron transport kinetics. Moreover, the adjacent Se atoms with a periodically arranged structure could provide more sites for the absorption and conversion of reactants. Thus, the as-prepared catalyst exhibits the top-level bifunctional activity with an ultra-low potential difference (ΔE) of 0.58 V and delivers the outstandingly low-temperature specific capacity of 796.41 mAh gZn−1 and the ultra-durable lifespan over 1000 h for assembled zinc-air batteries at −40 °C.

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来源期刊
Advanced Functional Materials
Advanced Functional Materials 工程技术-材料科学:综合
CiteScore
29.50
自引率
4.20%
发文量
2086
审稿时长
2.1 months
期刊介绍: Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week. Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.
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