CO2-Induced Reverse Lattice Oxygen Spillover on Pt/CeO2 Enables Sulfur-Resistant Dry Reforming of Methane

Jun Liu; Jiang Deng; Jiajia Zheng; Mohsen Beladi Mousavi; Chunning Sun; Jin Li; Xin Chen; Yongjie Shen; Haotian Huang; Ming Xie; Emiliano Cortés; Dengsong Zhang

doi:10.1002/anie.1664469

CO₂-Induced Reverse Lattice Oxygen Spillover on Pt/CeO₂ Enables Sulfur-Resistant Dry Reforming of Methane

Jun Liu
, Jiang Deng^*
, Jiajia Zheng
, Mohsen Beladi Mousavi
, Chunning Sun
, Jin Li
, Xin Chen
, Yongjie Shen
, Haotian Huang
, Ming Xie
, Emiliano Cortés^*
, Dengsong Zhang^*

^*Corresponding author for this work

Shanghai University
Ludwig Maximilian University of Munich
University of Bath, Department of Chemical Engineering

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

Overcoming sulfur poisoning in dry reforming of methane (DRM), which is a critical process for biogas upgrading, is particularly challenging. In this study, we illustrate that a reverse lattice oxygen spillover (RLOS) from CeO₂ to Pt on the Pt-O-Ce interface, induced by CO₂, can oxidize S into SO₂, aiding in the removal of S deposits. A low oxygen migration barrier at the Pt–O–Ce interface and Pt's high activity for oxidizing sulfur to SO₂ make Pt/CeO₂ uniquely effective at self-recovering after H₂S poisoning. Furthermore, the atomically dispersed Pt/CeO₂ catalyst undergoes reaction driven adaptive restructuring, which amplifies the RLOS effect and enables dynamic S deposition and removal. As a result, the catalysts maintain constant DRM activity for 100 h, even in the presence of H₂S. This discovery paves the way for designing catalysts that resist sulfur poisoning in H₂S-containing streams.

Original language	English
Article number	e1664469
Journal	Angewandte Chemie - International Edition
Volume	65
Issue number	31
Early online date	31 May 2026
DOIs	https://doi.org/10.1002/anie.1664469
Publication status	Published - 26 Jul 2026

Bibliographical note

Publisher Copyright:
© 2026 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH.

Funding

This work was financially supported by the National Natural Science Foundation of China (22125604 and 22476121) and the Science & Technology Commission of Shanghai Municipality (23230713700, 24230711600) and the Shanghai Pujiang Programme (24PJD033). Jiang Deng acknowledges support from the China Scholarship Council (CSC). We acknowledge funding and support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy—EXC 2089/2–390776260, the Bavarian program Solar Technologies Go Hybrid (SolTech), and the Center for NanoScience (CeNS). The Shanghai Technical Service Center of Science and Engineering Computing, Shanghai University, supported this work. ESRF is kindly acknowledged for providing XAS beamtime at the BM23 beamline. Prof. Bert M. Weckhuysen is acknowledged for providing the beamline time. thanks Dr. Zhiqiang Wang from ECUST for the fruitful discussion. Dr. Davide Salusso, Dr. Jiaorong Yan, and Joëlle Siewe are kindly acknowledged for their help with XAS characterization. Jiang Deng

Funders	Funder number
Centre for Nano and Soft Matter Sciences
China Scholarship Council
Shanghai Pujiang Programme	24PJD033
Deutsche Forschungsgemeinschaft	EXC 2089/2–390776260
Science and Technology Commission of Shanghai Municipality	24230711600, 23230713700
National Natural Science Foundation of China	22476121, 22125604

Keywords

biogas upgrading
dry reforming of methane
HS poisoning-resistance
platinum

Access to Document

10.1002/anie.1664469Licence: CC BY

Angew Chem Int Ed - 2026 - Liu - CO2‐Induced Reverse Lattice Oxygen Spillover on Pt CeO2 Enables Sulfur‐Resistant DryFinal published version, 2.7 MBLicence: CC BY

Cite this

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title = "CO2-Induced Reverse Lattice Oxygen Spillover on Pt/CeO2 Enables Sulfur-Resistant Dry Reforming of Methane",

abstract = "Overcoming sulfur poisoning in dry reforming of methane (DRM), which is a critical process for biogas upgrading, is particularly challenging. In this study, we illustrate that a reverse lattice oxygen spillover (RLOS) from CeO2 to Pt on the Pt-O-Ce interface, induced by CO2, can oxidize S into SO2, aiding in the removal of S deposits. A low oxygen migration barrier at the Pt{\textendash}O{\textendash}Ce interface and Pt's high activity for oxidizing sulfur to SO2 make Pt/CeO2 uniquely effective at self-recovering after H2S poisoning. Furthermore, the atomically dispersed Pt/CeO2 catalyst undergoes reaction driven adaptive restructuring, which amplifies the RLOS effect and enables dynamic S deposition and removal. As a result, the catalysts maintain constant DRM activity for 100 h, even in the presence of H2S. This discovery paves the way for designing catalysts that resist sulfur poisoning in H2S-containing streams.",

keywords = "biogas upgrading, dry reforming of methane, HS poisoning-resistance, platinum",

author = "Jun Liu and Jiang Deng and Jiajia Zheng and Mousavi, \{Mohsen Beladi\} and Chunning Sun and Jin Li and Xin Chen and Yongjie Shen and Haotian Huang and Ming Xie and Emiliano Cort{\'e}s and Dengsong Zhang",

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T1 - CO2-Induced Reverse Lattice Oxygen Spillover on Pt/CeO2 Enables Sulfur-Resistant Dry Reforming of Methane

AU - Liu, Jun

AU - Deng, Jiang

AU - Zheng, Jiajia

AU - Mousavi, Mohsen Beladi

AU - Sun, Chunning

AU - Li, Jin

AU - Chen, Xin

AU - Shen, Yongjie

AU - Huang, Haotian

AU - Xie, Ming

AU - Cortés, Emiliano

AU - Zhang, Dengsong

PY - 2026/7/26

Y1 - 2026/7/26

N2 - Overcoming sulfur poisoning in dry reforming of methane (DRM), which is a critical process for biogas upgrading, is particularly challenging. In this study, we illustrate that a reverse lattice oxygen spillover (RLOS) from CeO2 to Pt on the Pt-O-Ce interface, induced by CO2, can oxidize S into SO2, aiding in the removal of S deposits. A low oxygen migration barrier at the Pt–O–Ce interface and Pt's high activity for oxidizing sulfur to SO2 make Pt/CeO2 uniquely effective at self-recovering after H2S poisoning. Furthermore, the atomically dispersed Pt/CeO2 catalyst undergoes reaction driven adaptive restructuring, which amplifies the RLOS effect and enables dynamic S deposition and removal. As a result, the catalysts maintain constant DRM activity for 100 h, even in the presence of H2S. This discovery paves the way for designing catalysts that resist sulfur poisoning in H2S-containing streams.

AB - Overcoming sulfur poisoning in dry reforming of methane (DRM), which is a critical process for biogas upgrading, is particularly challenging. In this study, we illustrate that a reverse lattice oxygen spillover (RLOS) from CeO2 to Pt on the Pt-O-Ce interface, induced by CO2, can oxidize S into SO2, aiding in the removal of S deposits. A low oxygen migration barrier at the Pt–O–Ce interface and Pt's high activity for oxidizing sulfur to SO2 make Pt/CeO2 uniquely effective at self-recovering after H2S poisoning. Furthermore, the atomically dispersed Pt/CeO2 catalyst undergoes reaction driven adaptive restructuring, which amplifies the RLOS effect and enables dynamic S deposition and removal. As a result, the catalysts maintain constant DRM activity for 100 h, even in the presence of H2S. This discovery paves the way for designing catalysts that resist sulfur poisoning in H2S-containing streams.

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KW - dry reforming of methane

KW - HS poisoning-resistance

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