期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 8, 期 26, 页码 13292-13298出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ta03914d
关键词
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资金
- Fundamental Research Funds for the Central Universities [2652017331]
- Photoexcitonix Project in Hokkaido University
The bottleneck of photocatalytic nitrogen fixation lies in the rate-limiting reductive activation of robust N equivalent to N triple bonds with high bond energy. Herein, polymeric carbon nitride with frustrated-Lewis-pairs was constructed by intercalation of electron-deficient boron (B) into metal-free carbon nitride. NH3-temperature programmed desorption (TPD) and pyridine-adsorption diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results demonstrated that B heteroatoms (Lewis acid) and proximal amino groups (Lewis base) were more likely to form frustrated Lewis pairs, which would capture, activate and reduce N(2)to NH(3)through a pull-push effect. Molybdenum-based oxide was further employed as a co-catalyst to improve the charge separation efficiency of site-engineered photocatalysts. The synergistic effect between intercalated B and defective MoO(2)resulted in an 8-fold increased photoactivity of carbon nitride for N(2)fixation. This work provides a new avenue for the rational design and engineering of frustrated Lewis pair sites on polymeric photocatalysts toward efficient N(2)fixation.
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