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等离子体氮化镍助催化剂促进定向电荷转移与分离,实现协同光催化-光热产氢、产苯甲醛及细菌灭活性能

Plasmonic NiN Cocatalyst Boosting Directional Charge Transfer and Separation toward Synergistic Photocatalytic-Photothermal Performance of Hydrogen and Benzaldehyde Production as Well as Bacterial Inactivation.

作者信息

Li Jinhe, Lu Zhongxi, Jin Cheng, Shen Jun, Jiang Haopeng, Yu Xiaohui, Sun Lijuan, Wang Weikang, Wang Lele, Liu Qinqin

机构信息

School of Materials Science & Engineering, Jiangsu University, Zhenjiang212013, China.

School of Pharmacy, Suzhou Vocational Health College, Suzhou215009, P. R. China.

出版信息

Inorg Chem. 2022 Nov 28;61(47):18979-18989. doi: 10.1021/acs.inorgchem.2c03268. Epub 2022 Nov 14.

DOI:10.1021/acs.inorgchem.2c03268
PMID:36375108
Abstract

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.

摘要

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。

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