Accelerated Zeolite Defect Healing Suppresses Oxygen-Containing Species Trapping for Tandem Propene Epoxidation.
5 affiliations
- 1State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Qingdao266580, China.
- 2Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University, CardiffCF24 4HQ, U.K.
- 3College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao266100, China.
- 4National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan430071, China.
- 5Department of Chemical Engineering, Norwegian University of Science and Technology, Trondheim7491, Norway.
Abstract
Selective oxidation of chemical feedstocks with in situ-generated H2O2 offers a sustainable route to high-value oxygenates, yet such tandem catalysis is often fundamentally limited by the trapping of oxygen-containing species, including H2O2-derived intermediates and oxygenated products in zeolite microenvironments, where they undergo nonproductive decomposition and side reactions. Herein, we overcome this limitation by accelerating titanosilicalite hydroxyl defect healing through intensified nucleation and subsequent accelerated crystal growth. The resulting defect-healed microenvironment facilitates the transport of in situ-generated H2O2 between bifunctional active sites while suppressing its nonproductive decomposition to H2O. Moreover, it accelerates product propylene oxide (PO) desorption by weakening hydrogen bond interactions between PO and hydroxyl defects, thereby suppressing ring-opening and overoxidation side reactions. Consequently, the defect-healed Au/TS-1 catalyst exhibits a 1.8-fold enhancement in the PO formation rate and a 2.1-fold increase in Au-based productivity. This defect-healing strategy is broadly applicable to titanosilicates, aluminosilicates, and pure-silica zeolites and can be readily extended to a 10 L scale process, delivering reductions of 21% in production cost and 54% in carbon emissions compared with conventional TS-1 synthesis. Overall, this work establishes a sustainable, scalable, and cost-effective route for zeolite defect healing and provides a general strategy to overcome the long-standing transport-decomposition trade-off in tandem catalysis with in situ-generated H2O2.
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BibTeX
@article{lin2026accelerated,
title = {{Accelerated Zeolite Defect Healing Suppresses Oxygen-Containing Species Trapping for Tandem Propene Epoxidation.}},
author = {Dong Lin and Xin Zhou and Yang Xu and Richard J Lewis and Zongzhuang Sun and Defu Yin and Yongxiang Wang and Zhenyi Liu and Jingyuan Shang and Zhe Ma and Qiang Wang and Feng Deng and Chaohe Yang and De Chen and Graham J Hutchings and Xiang Feng},
journal = {Journal of the American Chemical Society},
year = {2026},
month = oct,
doi = {10.1021/jacs.6c17355},
url = {https://europepmc.org/article/MED/42954582},
note = {CC BY},
}
RIS
TY - JOUR
TI - Accelerated Zeolite Defect Healing Suppresses Oxygen-Containing Species Trapping for Tandem Propene Epoxidation.
AU - Dong Lin
AU - Xin Zhou
AU - Yang Xu
AU - Richard J Lewis
AU - Zongzhuang Sun
AU - Defu Yin
AU - Yongxiang Wang
AU - Zhenyi Liu
AU - Jingyuan Shang
AU - Zhe Ma
AU - Qiang Wang
AU - Feng Deng
AU - Chaohe Yang
AU - De Chen
AU - Graham J Hutchings
AU - Xiang Feng
PY - 2026
DA - 2026/10/01
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c17355
UR - https://europepmc.org/article/MED/42954582
AB - Selective oxidation of chemical feedstocks with in situ-generated H2O2 offers a sustainable route to high-value oxygenates, yet such tandem catalysis is often fundamentally limited by the trapping of oxygen-containing species, including H2O2-derived intermediates and oxygenated products in zeolite microenvironments, where they undergo nonproductive decomposition and side reactions. Herein, we overcome this limitation by accelerating titanosilicalite hydroxyl defect healing through intensified nucleation and subsequent accelerated crystal growth. The resulting defect-healed microenvironment facilitates the transport of in situ-generated H2O2 between bifunctional active sites while suppressing its nonproductive decomposition to H2O. Moreover, it accelerates product propylene oxide (PO) desorption by weakening hydrogen bond interactions between PO and hydroxyl defects, thereby suppressing ring-opening and overoxidation side reactions. Consequently, the defect-healed Au/TS-1 catalyst exhibits a 1.8-fold enhancement in the PO formation rate and a 2.1-fold increase in Au-based productivity. This defect-healing strategy is broadly applicable to titanosilicates, aluminosilicates, and pure-silica zeolites and can be readily extended to a 10 L scale process, delivering reductions of 21% in production cost and 54% in carbon emissions compared with conventional TS-1 synthesis. Overall, this work establishes a sustainable, scalable, and cost-effective route for zeolite defect healing and provides a general strategy to overcome the long-standing transport-decomposition trade-off in tandem catalysis with in situ-generated H2O2.
SN - 0002-7863
SN - 1520-5126
ER -