Abstract
Atomic interface regulation is thought to be an efficient method to adjust the performance of single atom catalysts. Herein, a practical strategy was reported to rationally design single copper atoms coordinated with both sulfur and nitrogen atoms in metal-organic framework derived hierarchically porous carbon (S-Cu-ISA/SNC). The atomic interface configuration of the copper site in S-Cu-ISA/SNC is detected to be an unsymmetrically arranged Cu-S1N3 moiety. The catalyst exhibits excellent oxygen reduction reaction activity with a half-wave potential of 0.918 V vs. RHE. Additionally, through in situ X-ray absorption fine structure tests, we discover that the low-valent Cuprous-S1N3 moiety acts as an active center during the oxygen reduction process. Our discovery provides a universal scheme for the controllable synthesis and performance regulation of single metal atom catalysts toward energy applications.
Highlights
Atomic interface regulation is thought to be an efficient method to adjust the performance of single atom catalysts
X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) revealed that the outstanding oxygen reduction reaction (ORR) activity originated from the formation of the unsymmetrical Cu-S1N3 atomic interface in the carbon matrix, and we discovered that low-valent Cu (+1) species worked as active sites for ORR
Cu-ZIF-8 and sulfur powder were jointly dispersed in carbon tetrachloride (CCl4) and dried by stirring, ensuring the sulfur was absorbed on the surface of Cu-ZIF-8 powder
Summary
Atomic interface regulation is thought to be an efficient method to adjust the performance of single atom catalysts. Due to the high atomic utilization, single atom catalysts have gained great attention in heterogeneous catalysis, and significantly, they provide new horizons for the discovery of innovative materials to energy applications[11,12,13,14,15,16,17,18,19,20] Both theoretical and experimental explorations have suggested that isolated single metal-Nx (M-Nx) modified carbon-based materials can serve as desirable oxygen electrocatalysts with promising performance[21,22,23,24,25,26,27,28,29]. We developed a hierarchically porous carbon based single copper atom catalyst toward ORR, by rationally controlling the unsymmetrical interface structure of central metal atoms, in which Cu was directly bonded with both sulfur and nitrogen atoms (denoted as S-Cu-ISA/SNC). This strategy of atomic interface engineering could be used to other metals (Mn, Fe, Co, Ni, etc.)
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