轴性酸盐协调驱动的旋转状态变化FeN4 站点稳定氧气减少
Pengxiang Zhang1, Shuling Liu1, Lebin Cai2
1College of Chemistry, Zhengzhou University, 100 Science Road, Zhengzhou, 450001, P.R. China.
Angewandte Chemie (International ed. in English)
|December 13, 2025
概括
将酸盐组引入铁单原子催化剂 (SAC) 增强了氧降解反应. 这种修改改善了催化剂活性,选择性和稳定性,用于空气电池等应用.
科学领域:
- 电触媒溶解是一种电触媒.
- 材料科学 材料科学 材料科学
- 纳米技术纳米技术
背景情况:
- 在工作条件下了解单原子催化剂 (SAC) 的结构性能关系至关重要,但具有挑战性.
- 纤维素衍生的碳上的Fe单原子位是有希望的电催化剂.
研究的目的:
- 调查轴性酸盐组对基于Fe的SAC电子结构和催化性能的影响.
- 增强氧降解反应 (ORR) 的SACs的活性,选择性和稳定性.
主要方法:
- 在Fe-SAC微环境中引入轴性酸盐组 (PO4) (P-FeN4/CC).
- 调制Fe中心的晶场 (D4h到C4v) 和旋转状态.
- 对ORR进行电催化测试,包括半波电位和电流密度测量.
- 长期稳定性测试和空气电池 (ZAB) 的应用.
- 理论计算和现场光谱学用于机械洞察力.
主要成果:
- P-FeN4/CC催化剂的半波潜力为0.97V,在0.85V时的极高动力电流密度为179.2mA cm-2.
- 催化剂在136小时后保持了超过90.5%的电流,超过了商业Pt/C-20%.
- 液体ZAB的峰值功率密度为280.1 mW cm-2和11,130个周期,而柔性ZAB的峰值功率密度为81 mW cm-2和160多小时的稳定运行.
结论:
- 轴性酸盐组动态调节Fe中心的电子结构和旋转状态,显著提高ORR性能.
- 联体诱导的自旋可调性和磁场控制为设计高性能SAC提供了新的策略.
- 这种P-FeN4/CC催化剂在ZAB等储能装置中的实际应用具有很大的潜力.
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