Han Yi, Li Wen, Bi Chuanzhou, Liu Jinyuan, Xu Hangmin, Song Hao, Zhong Kang, Yang Jinman, Jiang Weiyi, Yi Jianjian, Wang Bin, Chu Paul K, Ding Penghui, Xu Hui, Zhu Xingwang
College of Environmental Science and Engineering, Institute of Technology for Carbon Neutralization, Yangzhou University, Yangzhou 225009, PR China.
Department of Physics, Department of Materials Science and Engineering, and Department of Biomedical Engineering, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong, PR China.
J Colloid Interface Sci. 2024 Sep 15;670:348-356. doi: 10.1016/j.jcis.2024.05.003. Epub 2024 May 8.
The depressed directional separation of photogenerated carriers and weak CO adsorption/activation activity are the main factors hampering the development of artificial photosynthesis. Herein, Na ions are embedded in graphitic carbon nitride (g-CN) to achieve directional migration of the photogenerated electrons to Na sites, while the electron-rich Na sites enhance CO adsorption and activation. Na/g-CN (NaCN) shows improved photocatalytic reduction activity of CO to CO and CH, and under simulated sunlight irradiation, the CO yield of NaCN synthesized by embedding Na at 550°C (NaCN-550) is 371.2 μmol g h, which is 58.9 times more than that of the monomer g-CN. By means of theoretical calculations and experiments including in situ fourier transform infrared spectroscopy, the mechanism is investigated. This strategy which improves carrier separation and reduces the energy barrier at the same time is important to the development of artificial photosynthesis.
光生载流子的定向分离受阻以及一氧化碳吸附/活化活性较弱是阻碍人工光合作用发展的主要因素。在此，将钠离子嵌入石墨相氮化碳（g-CN）中，以实现光生电子向钠位点的定向迁移，而富电子的钠位点增强了一氧化碳的吸附和活化。钠/石墨相氮化碳（NaCN）对一氧化碳还原为一氧化碳和甲烷的光催化活性有所提高，在模拟太阳光照射下，550℃嵌入钠合成的NaCN（NaCN-550）的一氧化碳产率为371.2 μmol g⁻¹ h⁻¹，是单体g-CN的58.9倍。通过理论计算以及包括原位傅里叶变换红外光谱在内的实验对其机理进行了研究。这种同时改善载流子分离并降低能垒的策略对人工光合作用的发展具有重要意义。
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