In-situ spectroscopic insights into the dual-site synergistic electrocatalytic mechanism of propylene epoxidation over single-Ag-atom catalyst

Dengwen Pi; Xiaobo Yang; Meixin Chen; Jian Zhao; Jiuyi Wang; Shifu Wang; Wen-Cheng Shih; Wei Xu; Yanqiang Huang; Bin Liu; Xuning Li

doi:10.1038/s41467-025-67338-8

In-situ spectroscopic insights into the dual-site synergistic electrocatalytic mechanism of propylene epoxidation over single-Ag-atom catalyst

Dengwen Pi (Co-first Author), Xiaobo Yang (Co-first Author), Meixin Chen (Co-first Author), Jian Zhao, Jiuyi Wang, Shifu Wang, Wen-Cheng Shih, Wei Xu, Yanqiang Huang, Bin Liu^*, Xuning Li^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

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Abstract

The electrochemical oxidation of propylene presents a promising strategy for propylene oxide (PO) synthesis, but is severely hindered by the complex reaction pathways and the low PO selectivity. In this work, a series of Ag-decorated FeOOH catalysts is designed to elucidate the reaction mechanism of the electrochemical propylene oxidation reaction for PO electrosynthesis. An optimal Faradaic efficiency of PO of 32.0% is achieved over the single-Ag-atom decorated FeOOH catalyst (Ag₁-FeOOH) at 2.4 V versus reversible hydrogen electrode. The in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy and in-situ ⁵⁷Fe Mössbauer spectroscopy measurements combined with density functional theory calculations reveal the dual-site synergistic catalytic mechanism for electrochemical propylene epoxidation over Ag₁-FeOOH, where single-Ag-atom sites catalyze water oxidation to generate reactive oxygen species, while the adjacent Fe sites serve as adsorption sites for propylene activation. This study provides clear insights into the dual-site synergistic electrocatalytic mechanism of propylene epoxidation and sheds light on the rational design of single-atom catalysts for electrochemical organic synthesis. © The Author(s) 2025.

Original language	English
Article number	691
Number of pages	12
Journal	Nature Communications
Volume	17
Online published	12 Dec 2025
DOIs	https://doi.org/10.1038/s41467-025-67338-8
Publication status	Published - 2026

Funding

This work was financially supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB0600200 (X.L.)), the National Natural Science Foundation of China (22522815 (X.L.), 22478377 (X.L.)), the NSFC Center for Single-Atom Catalysis (grant No. 22388102 (X.L.)), CAS Project for Young Scientists in Basic Research (YSBR-051 (X.L.)), and the DICP. CAS-Cardiff Joint Research Units (121421ZYLH20230008 (X.L.)), the Liaoning Foundation for Excellent Young Scholars (2025JH6/101000018 (X.L.)), and DICP Founding (DICP I202331 (X.L.)). The authors gratefully acknowledge the support of Photon Science Center for Carbon Neutrality.

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title = "In-situ spectroscopic insights into the dual-site synergistic electrocatalytic mechanism of propylene epoxidation over single-Ag-atom catalyst",

abstract = "The electrochemical oxidation of propylene presents a promising strategy for propylene oxide (PO) synthesis, but is severely hindered by the complex reaction pathways and the low PO selectivity. In this work, a series of Ag-decorated FeOOH catalysts is designed to elucidate the reaction mechanism of the electrochemical propylene oxidation reaction for PO electrosynthesis. An optimal Faradaic efficiency of PO of 32.0% is achieved over the single-Ag-atom decorated FeOOH catalyst (Ag1-FeOOH) at 2.4 V versus reversible hydrogen electrode. The in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy and in-situ 57Fe M{\"o}ssbauer spectroscopy measurements combined with density functional theory calculations reveal the dual-site synergistic catalytic mechanism for electrochemical propylene epoxidation over Ag1-FeOOH, where single-Ag-atom sites catalyze water oxidation to generate reactive oxygen species, while the adjacent Fe sites serve as adsorption sites for propylene activation. This study provides clear insights into the dual-site synergistic electrocatalytic mechanism of propylene epoxidation and sheds light on the rational design of single-atom catalysts for electrochemical organic synthesis. {\textcopyright} The Author(s) 2025.",

author = "Dengwen Pi and Xiaobo Yang and Meixin Chen and Jian Zhao and Jiuyi Wang and Shifu Wang and Wen-Cheng Shih and Wei Xu and Yanqiang Huang and Bin Liu and Xuning Li",

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In-situ spectroscopic insights into the dual-site synergistic electrocatalytic mechanism of propylene epoxidation over single-Ag-atom catalyst. / Pi, Dengwen (Co-first Author); Yang, Xiaobo (Co-first Author); Chen, Meixin (Co-first Author) et al.
In: Nature Communications, Vol. 17, 691, 2026.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

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AU - Yang, Xiaobo

AU - Chen, Meixin

AU - Zhao, Jian

AU - Wang, Jiuyi

AU - Wang, Shifu

AU - Shih, Wen-Cheng

AU - Xu, Wei

AU - Huang, Yanqiang

AU - Liu, Bin

AU - Li, Xuning

PY - 2026

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N2 - The electrochemical oxidation of propylene presents a promising strategy for propylene oxide (PO) synthesis, but is severely hindered by the complex reaction pathways and the low PO selectivity. In this work, a series of Ag-decorated FeOOH catalysts is designed to elucidate the reaction mechanism of the electrochemical propylene oxidation reaction for PO electrosynthesis. An optimal Faradaic efficiency of PO of 32.0% is achieved over the single-Ag-atom decorated FeOOH catalyst (Ag1-FeOOH) at 2.4 V versus reversible hydrogen electrode. The in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy and in-situ 57Fe Mössbauer spectroscopy measurements combined with density functional theory calculations reveal the dual-site synergistic catalytic mechanism for electrochemical propylene epoxidation over Ag1-FeOOH, where single-Ag-atom sites catalyze water oxidation to generate reactive oxygen species, while the adjacent Fe sites serve as adsorption sites for propylene activation. This study provides clear insights into the dual-site synergistic electrocatalytic mechanism of propylene epoxidation and sheds light on the rational design of single-atom catalysts for electrochemical organic synthesis. © The Author(s) 2025.

AB - The electrochemical oxidation of propylene presents a promising strategy for propylene oxide (PO) synthesis, but is severely hindered by the complex reaction pathways and the low PO selectivity. In this work, a series of Ag-decorated FeOOH catalysts is designed to elucidate the reaction mechanism of the electrochemical propylene oxidation reaction for PO electrosynthesis. An optimal Faradaic efficiency of PO of 32.0% is achieved over the single-Ag-atom decorated FeOOH catalyst (Ag1-FeOOH) at 2.4 V versus reversible hydrogen electrode. The in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy and in-situ 57Fe Mössbauer spectroscopy measurements combined with density functional theory calculations reveal the dual-site synergistic catalytic mechanism for electrochemical propylene epoxidation over Ag1-FeOOH, where single-Ag-atom sites catalyze water oxidation to generate reactive oxygen species, while the adjacent Fe sites serve as adsorption sites for propylene activation. This study provides clear insights into the dual-site synergistic electrocatalytic mechanism of propylene epoxidation and sheds light on the rational design of single-atom catalysts for electrochemical organic synthesis. © The Author(s) 2025.

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In-situ spectroscopic insights into the dual-site synergistic electrocatalytic mechanism of propylene epoxidation over single-Ag-atom catalyst

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