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Published on: June 12, 2019
Ti3+-O Acid-Base Pairs for Efficient Solar-Driven Photothermal Nonoxidative Ethane Dehydrogenation
Yuwen Sun1,2, Kun Gong1, Tianyu Li3
1Center of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai201210, China.
Noble metal-free catalysts with Ti3+-O acid-base pairs on reduced rutile TiO2 enable efficient solar-driven nonoxidative ethane dehydrogenation (NOEDH) for ethene production without external heating.
Area of Science:
- Catalysis
- Materials Science
- Photochemistry
Background:
- Nonoxidative ethane dehydrogenation (NOEDH) is a carbon-efficient route to ethene but requires severe thermodynamic conditions.
- Solar-driven NOEDH is a promising alternative, but achieving high activity and selectivity with noble metal-free catalysts without external heating is challenging.
Purpose of the Study:
- To develop a noble metal-free catalyst for efficient solar-driven nonoxidative ethane dehydrogenation (NOEDH) without external heating.
- To investigate the mechanism of enhanced catalytic activity and selectivity.
Main Methods:
- Synthesis of reduced rutile TiO2 with Ti3+-O acid-base pairs.
- Full-spectrum solar irradiation for photothermal NOEDH.
- Comprehensive characterizations including spectroscopy and kinetics analysis.
Main Results:
- Optimally reduced TiO2 exhibited an ethene production rate of 392.0 mmol g-1 h-1 with 94.9% selectivity, significantly outperforming pristine TiO2.
- Ti3+-O acid-base pairs enhanced light absorption, charge carrier separation, and C-H bond activation.
- Surface acid-base pairs facilitated product desorption and suppressed deep dehydrogenation and coke formation.
- Apparent activation energy was reduced from 157.6 kJ mol-1 in the dark to 75.0 kJ mol-1 under illumination.
Conclusions:
- Surface Ti3+-O acid-base pairs on reduced rutile TiO2 are effective for highly efficient solar-driven NOEDH without external heating.
- This approach offers a sustainable platform for light-driven alkane upgrading using noble metal-free catalysts.
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