Academic Journal
Metal‐Oxo Electronic Tuning via In Situ CO Decoration for Promoting Methane Conversion to Oxygenates over Single‐Atom Catalysts
| العنوان: | Metal‐Oxo Electronic Tuning via In Situ CO Decoration for Promoting Methane Conversion to Oxygenates over Single‐Atom Catalysts |
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| المؤلفون: | Xu, Weibin, Liu, Han‐Xuan, Hu, Yue, Wang, Zhen, Huang, Zheng‐Qing, Huang, Chuande, Lin, Jian, Chang, Chun‐Ran, Wang, Aiqin, Wang, Xiaodong, Zhang, Tao |
| المساهمون: | National Natural Science Foundation of China, Youth Innovation Promotion Association of the Chinese Academy of Sciences |
| المصدر: | Angewandte Chemie International Edition ; volume 63, issue 16 ; ISSN 1433-7851 1521-3773 |
| بيانات النشر: | Wiley |
| سنة النشر: | 2024 |
| المجموعة: | Wiley Online Library (Open Access Articles via Crossref) |
| الوصف: | Direct methane conversion (DMC) to oxygenates at low temperature is of great value but remains challenging due to the high energy barrier for C−H bond activation. Here, we report that in situ decoration of Pd 1 ‐ZSM‐5 single atom catalyst (SAC) by CO molecules significantly promoted the DMC reaction, giving the highest turnover frequency of 207 h −1 ever reported at room temperature and ~100 % oxygenates selectivity with H 2 O 2 as oxidant. Combined characterizations and DFT calculations illustrate that the C‐atom of CO prefers to coordinate with Pd 1 , which donates electrons to the Pd 1 −O active center (L−Pd 1 −O, L=CO) generated by H 2 O 2 oxidation. The correspondingly improved electron density over Pd−O pair renders a favorable heterolytic dissociation of C−H bond with low energy barrier of 0.48 eV. Applying CO decoration strategy to M 1 ‐ZSM‐5 (M=Pd, Rh, Ru, Fe) enables improvement of oxygenates productivity by 3.2–11.3 times, highlighting the generalizability of this method in tuning metal‐oxo electronic structure of SACs for efficient DMC process. |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | English |
| DOI: | 10.1002/anie.202315343 |
| الاتاحة: | http://dx.doi.org/10.1002/anie.202315343 https://onlinelibrary.wiley.com/doi/pdf/10.1002/anie.202315343 |
| Rights: | http://onlinelibrary.wiley.com/termsAndConditions#vor |
| رقم الانضمام: | edsbas.5A7067EB |
| قاعدة البيانات: | BASE |
| DOI: | 10.1002/anie.202315343 |
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