催化作用
电催化剂
钴
纳米技术
电化学
材料科学
贵金属
过渡金属
Atom(片上系统)
电化学能量转换
化学
物理化学
电极
计算机科学
有机化学
嵌入式系统
冶金
作者
Gang Wan,Pengfei Yu,Hangrong Chen,Jianguo Wen,Chengjun Sun,Hua Zhou,Nian Zhang,Qianru Li,Weixia Zhao,Bing Xie,Tao Li,Jianlin Shi
出处
期刊:Small
[Wiley]
日期:2018-03-05
卷期号:14 (15)
被引量:96
标识
DOI:10.1002/smll.201704319
摘要
The development of cost-effective catalysts to replace noble metal is attracting increasing interests in many fields of catalysis and energy, and intensive efforts are focused on the integration of transition-metal sites in carbon as noble-metal-free candidates. Recently, the discovery of single-atom dispersed catalyst (SAC) provides a new frontier in heterogeneous catalysis. However, the electrocatalytic application of SAC is still subject to several theoretical and experimental limitations. Further advances depend on a better design of SAC through optimizing its interaction with adsorbates during catalysis. Here, distinctive from previous studies, favorable 3d electronic occupation and enhanced metal-adsorbates interactions in single-atom centers via the construction of nonplanar coordination is achieved, which is confirmed by advanced X-ray spectroscopic and electrochemical studies. The as-designed atomically dispersed cobalt sites within nonplanar coordination show significantly improved catalytic activity and selectivity toward the oxygen reduction reaction, approaching the benchmark Pt-based catalysts. More importantly, the illustration of the active sites in SAC indicates metal-natured catalytic sites and a media-dependent catalytic pathway. Achieving structural and electronic engineering on SAC that promotes its catalytic performances provides a paradigm to bridge the gap between single-atom catalysts design and electrocatalytic applications.
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