Binghua Ye, Cheng Liu, Yueling Chen, Qi Chen, Kaiqiang Jing, Jimmy C. Yu, Jionghua Wu* and Ling Wu*,
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引用次数: 0
Abstract
Photocatalytic N2 fixation is a green and sustainable pathway for the synthesis of ammonia. However, its efficiency is considerably restricted by the energy-intensive activation of N2 molecules. Herein, a series of MOF-74(Co) with varying contents of coordinatively unsaturated Co sites were synthesized through the thermal treatment at different temperatures (T = 100, 150, 200, 250 °C). These photocatalysts were used for the photocatalytic fixation of N2 in the absence of a sacrificial agent. The experimental results and theoretical computations indicate that the amount of coordinatively unsaturated Co sites increases as the temperature elevates by the removal of coordinated H2O from MOF-74(Co). These Co sites can function as active sites to promote chemisorption and activation of N2 molecules. The sample MOF-74(Co)-200 exhibits the highest NH4+ production rate of 84 μmol·g–1·h–1, which is six times higher than that of the pristine MOF-74(Co) (13.9 μmol·g–1·h–1). The enhanced performance can be ascribed to the abundance of active sites and the optimal mobility of the photogenerated charges. Finally, a mechanism is proposed for the photocatalytic N2 activation at the molecular level.
期刊介绍:
ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment.
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