A plasma bombing strategy to synthesize high-loading single-atom catalysts for oxygen reduction reaction
A plasma bombing strategy to synthesize high-loading single-atom catalysts for oxygen reduction reaction
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DOI：
10.1016/j.xcrp.2022.100880
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发表时间：
2022-05-18
影响因子：
8.9
通讯作者：
Tian, Xinlong
中科院分区：
文献类型：
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作者：
Rao, Peng;Wu, Daoxiong;Tian, Xinlong
单原子催化剂（SACs）因其独特的内在性质而引起了人们的极大关注，但其简单的合成方法，特别是将金属盐直接转化为单金属原子的方法仍然是一个巨大的挑战。在这里，我们报告了一个实用的方法来访问大规模合成的SAC，其中的金属盐被激发和剥离作为移动的单金属原子流动下的“等离子体轰炸“处理。同时，它们被载体的缺陷和含氮位点捕获和锚定。更重要的是，该合成方法具有很强的通用性，可以推广到各种SAC的制备。作为示例，所制备的SAC-Fe/NC提供了显著的氧还原反应（ORR）性能。结合理论分析，提出了吸附诱导自旋交叉ORR机理，证明了Fe物种与四个吡啶型N原子的配位是SAC-Fe/NC高性能的主要贡献者。
Single-atom catalysts (SACs) have attracted tremendous attention owing to their unique intrinsic properties, while the facile synthesis, especially the direct transformation of metal salts into single-metal atoms, is still a huge challenge. Here we report a practical approach to access the large-scale synthesis of SACs, in which the metal salts are excited and stripped as mobile single-metal atoms flow under the "plasma bombing"treatment. Simultaneously, they are trapped and anchored by the defective and nitrogenous sites of the supports. More importantly, the synthesis approach is quite general, and it can be extended to the fabrication of various SACs. As an illustration, the prepared SAC-Fe/NC delivers a remarkable oxygen reduction reaction (ORR) performance. In combination with the theoretical analysis, an adsorbent-induced spin-crossover ORR mechanism is proposed, and the Fe species coordination with four pyridinic-type N atoms is demonstrated as the main contributor to the high performance of the prepared SAC-Fe/NC.