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非对称的Mn/Fe双单原子催化剂用于pH-通用氧电还原和可持续的金属空气电池

Qichen Wang^1,2, Bingxian Chu^1,2, Chunyan Shang^1,2

¹Department of Chemistry, Southern University of Science and Technology, Shenzhen, 518055, China.

Advanced materials (Deerfield Beach, Fla.)

|July 22, 2025

概括

一种新型的催化剂具有不对称的N,P-协调的Mn和Fe双单个原子 (MnFe-PNC) 显著提高了可持续的金属空气电池的氧降解反应 (ORR) 动力学,证明了卓越的pH-通用性能和稳定性.

科学领域:

电化学电化学电化学
材料科学材料科学材料科学
储能储能储能储能储能储能

背景情况:

氧降解反应 (ORR) 动力学对于可持续的金属空气电池至关重要,但在开发高效,无Pt电催化剂方面面临的挑战阻碍了它们.
目前的无PtORR催化剂在内在活性,活性站点可访问性和结构完整性方面面临限制.

研究的目的:

合成和描述一种新型不对称的N,P-协调的Mn和Fe双单原子催化剂 (MnFe-PNC),以提高ORR性能.
通过理论计算来研究MnFe-PNC增强的ORR活动的潜在机制.
在各种条件下评估MnFe-PNC在水性Zn/Al-空气电池和准固态Zn-空气电池中的性能.

主要方法:

金属有机框架 (MOF) 是合成MnFe-PNC的热解策略.
在广泛的pH范围内进行电化学表征 (0.1M KOH,0.1M HClO4,1M酸盐缓冲区).
密度函数理论 (DFT) 计算以阐明反应机制.
装配和测试含有有机液电解质的水性Zn/Al-空气电池和准固态Zn-空气电池.

主要成果:

MnFe-PNC表现出卓越的pH-通用ORR性能,具有高的半波潜力 (KOH中的0.923V,HClO4中的0.803V,PBS中的0.774V).
理论计算表明,Mn-N3P和Fe-N3P位点之间的电子相互作用是优化*OH中间吸附的关键.
水性Zn/Al-空气电池显示出超长的放电稳定性和广泛的温度适应性.
准固态Zn-空气电池表现出强大的循环稳定性 (130小时在50 mA cm-2,70小时在100 mA cm-2) 和显著的低温性能 (-40 °C).

结论:

非对称的N,P协调双单原子策略有效地提高了ORR动力学和稳定性.
MnFe-PNC是一种有前途的无Pt电催化剂,用于高性能,pH-通用和广泛温度适应性金属空气电池.
开发的准固态Zn-空气电池提供了卓越的循环稳定性和特殊的低温放电能力.

关键词:

不对称的协调协调.双双的单原子催化剂.氧减少反应反应的氧减少反应.超低温Zn空气电池超低温Zn空气电池

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