Journal
ACS CATALYSIS
Volume 10, Issue 10, Pages 5862-5870Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c00936
Keywords
single-atom catalysis; electrocatalysis; atomic structure engineering; accelerated kinetics; oxygen reduction reaction
Categories
Funding
- MOE [A75-114, R-144000-410-114]
- NUS green energy program [R-143-000-A63-114, R-143-000-A55-733]
- National Natural Science Foundation of China [21601193]
- Fundamental Research Funds for the Central Universities [31020190QD013]
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The ability to tune both local and global environments of a single metal active center on a support is crucial for the development of highly robust and efficient single-atom electrocatalysts (SAECs) that can surmount both thermodynamic and kinetic constraints in electrocatalysis. Here, we designed a core-shell-structured SAEC (Co-1-SAC) with superior oxygen reduction reaction (ORR) performance. Co-1-SAC consists of a locally engineered single Co-N3C1 site on a N-doped microporous amorphous carbon support enveloped by a globally engineered highly conductive mesoporous graphitic carbon shell. Theoretical calculations reveal that Co-N3C1 exhibits near-Fermi electronic states distinct from those of Co-N2C2 and Co-N-4, which facilitate both the electronic hybridization with O-2 and the subsequent protonation of adsorbed O-2* toward the formation of OOH*. Engineering Co-N3C1-SAC into a micro/mesoporous structure dramatically enhances the mass transport and electron transfer, which further boosts the ORR and Zn-air battery performance (slightly outperforming Pt/C). Our findings open an avenue toward engineering of the local and global environment of SACs for a wide range of efficient electrochemical conversions.
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