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一锅原位水热合成三元InS/NbO/NbC肖特基/S型复合异质结用于高效光催化产氢

One-pot in-situ hydrothermal synthesis of ternary InS/NbO/NbC Schottky/S-scheme integrated heterojunction for efficient photocatalytic hydrogen production.

作者信息

Tayyab Muhammad, Liu Yujie, Liu Zhiguo, Pan Lihan, Xu Zehong, Yue Wenhui, Zhou Liang, Lei Juying, Zhang Jinlong

机构信息

Key Laboratory for Advanced Materials, Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization, Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science & Technology, Shanghai 200237, PR China.

National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery, School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai 200237, PR China; State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, PR China.

出版信息

J Colloid Interface Sci. 2022 Dec 15;628(Pt B):500-512. doi: 10.1016/j.jcis.2022.08.071. Epub 2022 Aug 17.

Abstract

MXene-derived photocatalysts continue to fascinate the research community in developing photo-driven green and sustainable fuel production. However, the efficiency of MXene-derived photocatalyst is still low due to the wide bandgap and high recombination rate of photo-excited charge carriers. Here, we have synthesized the NbC MXene-derived ternary photocatalyst via one-pot in-situ hydrothermal method for photocatalytic hydrogen (H) evolution. The partial oxidation of NbC MXene into NbO nanorods and coupling with InS nanoparticles via in-situ chemical anchoring were the key factors toward high efficiency and long-term stability during photocatalytic H evolution. The optimized ternary photocatalyst composite manifested the highest H evolution efficiency at 68.8 µmol g h, which was 11 and 7.5 times higher than the NbO/NbC (NNC) and pure InS photocatalyst, respectively. Moreover, the photocatalytic stability of the optimized ternary photocatalyst composite was analyzed for five consecutive cycles, and above 87% activity retention was observed even after the fifth cycle without any obvious decline. The separation efficiency of photoexcited charge carriers could be attributed to the synergic effect of the InS/NbO heterojunction and the redox reactions at different sites of the composite. More importantly, the participation of Schottky junction and S-scheme heterojunction charge transfer for the obtained novel ternary photocatalyst was evaluated via ultraviolet photoelectron spectroscopy (UPS) and electron paramagnetic resonance (EPR). This research will provide additional insight into the extended potential of MXene-derived ternary photocatalysts towards efficient H production to meet future global energy demands.

摘要

源自MXene的光催化剂在开发光驱动绿色可持续燃料生产方面持续吸引着研究界。然而,由于光激发电荷载流子的宽带隙和高复合率,源自MXene的光催化剂效率仍然较低。在此,我们通过一锅原位水热法合成了用于光催化析氢的源自NbC MXene的三元光催化剂。NbC MXene部分氧化成NbO纳米棒并通过原位化学锚定与InS纳米颗粒耦合是光催化析氢过程中实现高效率和长期稳定性的关键因素。优化后的三元光催化剂复合材料表现出最高的析氢效率,为68.8 μmol g⁻¹ h⁻¹,分别是NbO/NbC(NNC)和纯InS光催化剂的11倍和7.5倍。此外,对优化后的三元光催化剂复合材料的光催化稳定性进行了连续五个循环的分析,即使在第五个循环后仍观察到87%以上的活性保留,且无明显下降。光激发电荷载流子的分离效率可归因于InS/NbO异质结的协同效应以及复合材料不同位点的氧化还原反应。更重要的是,通过紫外光电子能谱(UPS)和电子顺磁共振(EPR)评估了所制备的新型三元光催化剂中肖特基结和S型异质结电荷转移的参与情况。这项研究将为源自MXene的三元光催化剂在高效制氢方面的扩展潜力提供更多见解,以满足未来全球能源需求。

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