Li Jinhe, Lu Zhongxi, Jin Cheng, Shen Jun, Jiang Haopeng, Yu Xiaohui, Sun Lijuan, Wang Weikang, Wang Lele, Liu Qinqin
School of Materials Science & Engineering, Jiangsu University, Zhenjiang212013, China.
School of Pharmacy, Suzhou Vocational Health College, Suzhou215009, P. R. China.
Inorg Chem. 2022 Nov 28;61(47):18979-18989. doi: 10.1021/acs.inorgchem.2c03268. Epub 2022 Nov 14.
Charge separation and transfer are the dominating factors in achieving high activity of solar energy-based photocatalysis. Here, a plasmonic transition metal nitride, NiN, nanosheet was fabricated and employed as an efficient cocatalyst to couple with CdZnS (CZS) solid solution via a self-assembly method to form a novel NiN/CZS heterojunction with an intimate interface. On one hand, localized surface plasmon resonance of the NiN nanosheets endowed the fabricated NiN/CZS composite with a wide-spectrum light absorption capacity, even to the near-infrared range. On the other hand, NiN as a cocatalyst can not only effectively induce the directional electron transfer from CZS to NiN active sites but also enhance the surface charge separation efficiency of the NiN/CZS heterojunction by 4.1 times compared to that of pure CZS. Plasmonic NiN also provided a photothermal effect to enhance the surface temperature of the composite for boosting the catalytic reaction kinetics. As a result, under visible light irradiation, the optimal NiN/CZS composite exhibited simultaneous H generation and benzaldehyde formation rates of 35.08 and 16.44 mmol g h, which were 9.4 and 5.9 times those of CZS, respectively; and the composite also demonstrated a strong antibacterial ability with a sterilization rate of 99.7% toward . Besides that, under NIR light, plasmonic NiN offered extra hot electrons that can transfer back to CZS to take part in the photocatalytic reaction, leading to the NiN/CZS composite still having a high H production of 179.6 μmol g h. This work focuses on developing and applying novel plasmonic cocatalysts in photocatalysis for achieving adjustable electron transfer and fast charge separation for extensive practical application.
电荷分离和转移是实现基于太阳能的光催化高活性的主导因素。在此,制备了一种等离子体过渡金属氮化物NiN纳米片,并通过自组装方法将其用作高效助催化剂与CdZnS(CZS)固溶体耦合,形成具有紧密界面的新型NiN/CZS异质结。一方面,NiN纳米片的局域表面等离子体共振赋予制备的NiN/CZS复合材料宽光谱光吸收能力,甚至延伸至近红外范围。另一方面,NiN作为助催化剂不仅能有效诱导电子从CZS定向转移至NiN活性位点,还能使NiN/CZS异质结的表面电荷分离效率相比纯CZS提高4.1倍。等离子体NiN还提供光热效应以提高复合材料的表面温度,从而加快催化反应动力学。结果,在可见光照射下,最佳的NiN/CZS复合材料同时产生H2和苯甲醛的速率分别为35.08和16.44 mmol g-1 h-1,分别是CZS的9.4倍和5.9倍;该复合材料还表现出强大的抗菌能力,对……的杀菌率为99.7%。此外,在近红外光下,等离子体NiN提供额外的热电子,这些热电子可转移回CZS参与光催化反应,使得NiN/CZS复合材料仍具有179.6 μmol g-1 h-1的高H2产率。这项工作致力于在光催化中开发和应用新型等离子体助催化剂,以实现可调节的电子转移和快速的电荷分离,从而实现广泛的实际应用。