Journal
ACS ENERGY LETTERS
Volume 4, Issue 8, Pages 1793-1802Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.9b00893
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Funding
- U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0019019]
- Camille Dreyfus Teacher Scholar Award
- National Natural Science Foundation of China [21777108]
- China Scholarship Council [201706240160]
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Great efforts have been devoted to unveiling structural contributions of transition heterometallic materials to enhanced catalysis, while effective in situ approaches are still urgently demanded to probe the intrinsic activity on individual electrolyte-accessible sites. Here, we report cobalt-iron subnanoclusters (CoFe-PPy) incorporated on nitrogen-rich nanotubular carbon from dual cross-linked polypyrrole hydrogels. The bimetallic catalyst exhibits obviously improved oxygen electrocatalysis largely attributed to the electronic interaction between cobalt and iron at the atomic scale. Furthermore, the site information and catalytic kinetics of CoFe-PPy were in situ quantified by a surface-interrogation scanning electro-chemical microscopy (SI-SECM) technique. Consequently, CoFe-PPy not only provides higher active site density but also achieves rapid kinetics to activate O-2, greatly promoting the oxygen electroreduction turnover frequency compared with monometallic catalysts. Our work offers an opportunity to investigate important catalytic parameters of bimetallic electrocatalysis and highlights the heterometallic interaction at the subnanometer scale to promote enhanced electrocatalytic reactivity.
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