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Efficient ambient ammonia synthesis by Lewis acid pair over cobalt single atom catalyst with suppressed proton reduction

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Title
Efficient ambient ammonia synthesis by Lewis acid pair over cobalt single atom catalyst with suppressed proton reduction
Author(s)
Ngoc Quang Tran; Xinghui Liu; Yunhee Cho; Duy, Le Thai; Zheng, Lirong; Jianmin Yu; Sara Ajmal; Xiaodong Shao; Jinsun Lee; Hyoyoung Lee
Publication Date
2022-04
Journal
JOURNAL OF MATERIALS CHEMISTRY A, v.10, no.15, pp.8432 - 8439
Publisher
ROYAL SOC CHEMISTRY
Abstract
© Royal Society of Chemistry 2022. Improving the ammonia yield and Faraday efficiency of ambient electrochemical nitrogen fixation is a priority for altering the energy-intensive Haber-Bosch process. In this work, positively charged single cobalt atoms anchored on sponge-like nitrogen-doped mesoporous interconnected hollow carbon nanofibers (serving as a Lewis acid pair) were intentionally designed as catalytic centers that can suppress the side effect of the competing hydrogen evolution reaction and simultaneously boost the electrochemical conversion of nitrogen (N-2) to ammonia (NH3). The Lewis acid pair catalyst exhibits an NH3 production rate of 67.6 mu g h(-1) mg(-1) and a maximum Faraday efficiency of 56.9% at a peak potential of -0.1 V vs. RHE, which outperforms previously reported nitrogen reduction reaction (NRR) catalysts. First-principles DFT calculations suggest the regulation of the local electronic structure that induces Lewis acid pair formation upon charge transfer between the single Co atom and substrate, confirming a high intrinsic NRR by both experiments and theoretical calculations.
URI
https://pr.ibs.re.kr/handle/8788114/11578
DOI
10.1039/d2ta00308b
ISSN
2050-7488
Appears in Collections:
Center for Integrated Nanostructure Physics(나노구조물리 연구단) > 1. Journal Papers (저널논문)
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