A Titanium Silicalite‐1 (TS‐1) Catalyst with Abundant Active Ti‐VI Species for Efficient Conversion of Ethylene to Glycol
One-pot synthesis of glycol from ethylene and H<sub>2</sub>O<sub>2</sub> is simple and environmentally friendly, making it a potential alternative for glycol production. The key to the success of this is to have a bifunctional catalyst with both oxidative activity for ethylene epoxidation and acidic centers for the hydration of ethylene oxide. Typically, the incorporation of trivalent metal ions into titanium silicalite-1 (TS-1) framework can provide the two types of active centers, but this often results in decreased oxidative activity. Here, we propose a dual-chemical post-treatment regime to introduce acid centers in TS-1 while simultaneously improving oxidative activity. The combined tetrapropylammonium hydroxide (TPAOH) + (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub> post-treatment not only produces abundant Ti(OSi)<sub>2</sub>(OH)<sub>4</sub> (Ti-VI) species from Ti(OSi)<sub>4</sub>, but also creates internal cavities within TS-1. Ti-VI possesses both high oxidative activity and acidic sites. The presence of internal cavities enhances the diffusion on the catalyst as well as increases the accessibility of Ti-VI species. Consequently, when applied as a catalyst, the combined-treated TS-1 demonstrates an outstanding catalytic performance, achieving 98.6 % conversion of H<sub>2</sub>O<sub>2</sub> and 99.8 % selectivity of EG, which is ≈2 times of the conventional TS-1. This study also unveils the formation mechanism of Ti-VI during the post-treatment.
Authors
- Fei Song (ORCID: https://orcid.org/0000-0002-6408-7796)
- Hong Sun Yang (ORCID: https://orcid.org/0000-0003-0169-6479)
- Lingling Guo (ORCID: https://orcid.org/0000-0002-3444-9733)
- Bosong Zhang (ORCID: https://orcid.org/0000-0002-0334-7128)
- Yi Zuo (ORCID: https://orcid.org/0000-0002-3368-132X)
- Hongyi Tan (ORCID: https://orcid.org/0000-0002-6318-3161)
- Jianrong Zeng (ORCID: https://orcid.org/0000-0003-4867-1893)
- Gudan Li
- Lina Li (ORCID: https://orcid.org/0000-0002-4962-2906)
- Xinwen Guo (ORCID: https://orcid.org/0000-0002-6597-4979)
Institutions
- The University of Western Australia (AU)
- Dalian University of Technology (CN)
- Dalian University (CN)
- Shanghai Advanced Research Institute (CN)
- Shanghai Synchrotron Radiation Facility
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-03-16
- DOI
- https://doi.org/10.1002/anie.202502003
- Citations
- 8
- Primary Topic
- Mesoporous Materials and Catalysis
- Type
- article
- Field-Weighted Citation Impact
- 4.14