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双原子Fe催化剂的升华转化合成,以实现高效的氧降解反应

Li Yan¹, Yu Mao², Yingxin Li²

¹State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, 100029, Beijing, China.

Angewandte Chemie (International ed. in English)

|September 3, 2024

概括

一个新的合成策略可以精确制造双原子铁催化剂 (Fe2/NC) 以最佳的Fe-Fe距离. 这一突破提高了氧气减少性能,超越了基催化剂,并提供了对双位点催化物的见解.

科学领域:

材料科学材料科学材料科学
催化剂是一种催化剂.
电化学电化学电化学

背景情况:

双原子催化剂 (DAC) 对催化应用具有很大的前景.
对DAC制造的精确控制是一个重大挑战.
了解DAC中的结构-活动关系对于性能优化至关重要.

研究的目的:

开发一个简单的合成原子精确的双原子铁催化剂 (Fe2/NC).
研究合成Fe2/NC的结构特征和催化性能.
阐明Fe-Fe原子间距离对催化活性的影响.

主要方法:

使用现场生成的Fe2Cl6 (g) 模聚物进行升华转化合成.
偏差校正传输电子显微镜 (TEM) 用于结构分析.
用X射线吸收细结构 (XAFS) 光谱进行详细的结构特征.
氧降解反应 (ORR) 的电化学测试性能评估.
密度函数理论 (DFT) 计算和微动力学分析.

主要成果:

成功合成了一种具有0.3nm延长Fe-Fe距离的新型Fe2/NC催化剂.
铁2/NC催化剂表现出优越的ORR性能 (0.90V与RHE),表现优于Pt/C和Fe单原子催化剂.
DFT的计算证实,延长的Fe-Fe距离增强了O2吸附和质子化动力学.
较短的Fe-Fe距离 (~0.25nm) 导致催化活性较低.

结论:

为原子精确的DAC建立了一个简单的合成路线.
铁-铁原子间距离显著影响DAC中的催化活性.
优化的Fe-Fe距离对于提高氧降解反应效率至关重要.

关键词:

远距离效应的影响.双原子Fe催化剂是双原子的微动力学分析微动力学分析氧降解反应是氧降解反应.升华转化合成合成的合成

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