Single Cobalt Atoms with Precise N‐Coordination as Superior Oxygen Reduction Reaction Catalysts,Angewandte Chemie International Edition

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Single Cobalt Atoms with Precise N‐Coordination as Superior Oxygen Reduction Reaction Catalysts
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2016-08-04 , DOI: 10.1002/anie.201604802
Peiqun Yin _{1,

2} , Tao Yao ₃ , Yuen Wu _{1,

2} , Lirong Zheng ₄ , Yue Lin ₃ , Wei Liu ₃ , Huanxin Ju ₃ , Junfa Zhu ₃ , Xun Hong _{1,

2} , Zhaoxiang Deng , Gang Zhou ₅ , Shiqiang Wei ₃ , Yadong Li _{1,

2}

Affiliation

A new strategy for achieving stable Co single atoms (SAs) on nitrogen‐doped porous carbon with high metal loading over 4 wt % is reported. The strategy is based on a pyrolysis process of predesigned bimetallic Zn/Co metal–organic frameworks, during which Co can be reduced by carbonization of the organic linker and Zn is selectively evaporated away at high temperatures above 800 °C. The spherical aberration correction electron microscopy and extended X‐ray absorption fine structure measurements both confirm the atomic dispersion of Co atoms stabilized by as‐generated N‐doped porous carbon. Surprisingly, the obtained Co‐N_x single sites exhibit superior ORR performance with a half‐wave potential (0.881 V) that is more positive than commercial Pt/C (0.811 V) and most reported non‐precious metal catalysts. Durability tests revealed that the Co single atoms exhibit outstanding chemical stability during electrocatalysis and thermal stability that resists sintering at 900 °C. Our findings open up a new routine for general and practical synthesis of a variety of materials bearing single atoms, which could facilitate new discoveries at the atomic scale in condensed materials.

中文翻译：

具有精确N配位的单钴原子可作为优异的氧还原反应催化剂

据报道，一种新的策略可在氮掺杂的多孔碳上实现稳定的Co单原子（SA），且金属负载量超过4 wt％。该策略基于预先设计的双金属Zn / Co金属-有机骨架的热解过程，在此过程中，有机连接剂的碳化可还原Co，而Zn在高于800°C的高温下会选择性蒸发掉。球面像差校正电子显微镜和扩展的X射线吸收精细结构测量均证实了生成的N掺杂多孔碳稳定了Co原子的原子色散。令人惊讶的是，获得的Co‐N _x单个位点具有优异的ORR性能，半波电势（0.881 V）比市售Pt / C（0.811 V）和大多数报道的非贵金属催化剂更具有正电性。耐久性测试表明，Co单原子在电催化过程中表现出出色的化学稳定性，并且在900°C的温度下仍能抵抗烧结。我们的发现开辟了一个新的程序，可以对各种带有单个原子的材料进行常规和实际合成，这可能有助于在凝聚态材料中原子级的新发现。

更新日期：2016-08-04

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