Wan Shipeng, Ou Man, Wang Xinming, Wang Yanan, Zeng Yiqing, Ding Jie, Zhang Shule, Zhong Qin
School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing, Jiangsu 210094, PR China.
School of Energy Science and Engineering, Nanjing Tech University, Nanjing, Jiangsu 211816, PR China.
Dalton Trans. 2019 Aug 28;48(32):12070-12079. doi: 10.1039/c9dt02507c. Epub 2019 Jul 19.
In this study, to overcome the low charge transportation efficiency and poor visible light absorption ability, and achieve highly efficient photocatalytic applications, carbon nitride nanosheets with oxygen and carbon co-doping were successfully designed and fabricated. The resultant carbon nitride nanosheets exhibited efficient photocatalytic H evolution and CO reduction performance, highlighting the efficacy of such a strategy. The highest H evolution rate could reach 698.43 μmol g h, higher than that for graphitic carbon nitride (GCN). For CO reduction, the photocatalytic system shows a high CO selectivity, and MG achieves the largest CO generation amount of 55.2 μmol g. This enhanced photocatalytic reduction performance could be attributed to oxygen and carbon co-doping, which achieves fast electron extraction and transfer, and improved visible light absorption ability. It should be noted that the excessive addition of glucose in the synthesis process could enhance conductivity and promote visible light absorption of carbon nitride, but suppress the H evolution and CO reduction ability. Simultaneously, the photocatalytic reduction mechanism is discussed. This work confirms that a carbon nitride semiconductor with oxygen and carbon co-doping could be easily prepared by this strategy, achieving efficient photocatalytic applications.
在本研究中，为了克服电荷传输效率低和可见光吸收能力差的问题，并实现高效的光催化应用，成功设计并制备了氧碳共掺杂的氮化碳纳米片。所得的氮化碳纳米片表现出高效的光催化析氢和一氧化碳还原性能，突出了该策略的有效性。最高析氢速率可达698.43 μmol g⁻¹ h⁻¹，高于石墨相氮化碳（GCN）。对于一氧化碳还原，光催化体系表现出高的一氧化碳选择性，且三聚氰胺氰尿酸盐实现了最大一氧化碳生成量55.2 μmol g⁻¹。这种增强的光催化还原性能可归因于氧碳共掺杂，其实现了快速的电子提取和转移，并提高了可见光吸收能力。需要注意的是，合成过程中葡萄糖的过量添加可提高导电性并促进氮化碳对可见光的吸收，但会抑制析氢和一氧化碳还原能力。同时，对光催化还原机理进行了探讨。这项工作证实，通过该策略可以轻松制备氧碳共掺杂的氮化碳半导体，实现高效的光催化应用。
