Details

Autor(en) / Beteiligte

• Hai, Xiao
• Zhao, Xiaoxu
• Guo, Na
• Yao, Chuanhao
• Chen, Cheng
• Liu, Wei
• Du, Yonghua
• Yan, Huan
• Li, Jing
• Chen, Zhongxin
• Li, Xing
• Li, Zejun
• Xu, Haomin
• Lyu, Pin
• Zhang, Jia
• Lin, Ming
• Su, Chenliang
• Pennycook, Stephen J
• Zhang, Chun
• Xi, Shibo
• Lu, Jiong

Titel

Engineering Local and Global Structures of Single Co Atoms for a Superior Oxygen Reduction Reaction

Ist Teil von

• ACS catalysis, 2020-05, Vol.10 (10), p.5862-5870

Ort / Verlag

American Chemical Society

Erscheinungsjahr

2020

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• 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 (Co1-SAC) with superior oxygen reduction reaction (ORR) performance. Co1-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-N4, which facilitate both the electronic hybridization with O2 and the subsequent protonation of adsorbed O2* toward the formation of OOH*. Engineering Co-N3C1-SAC into a micro/mesoporous core–shell 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.