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具有CdMoSe量子点的结构调制NiV-LDH:在S型异质结处解锁活性中心以刺激光催化产生HO和H演化

Structurally Modulated NiV-LDH with CdMoSe-Quantum Dots: Unlocking the Active Centers at S-Scheme Heterojunctions for Stimulating Photocatalytic HO Production and H Evolution.

作者信息

Sarangi Preeti Prabha, Das Kundan Kumar, Sahu Jyotirmayee, Mohanty Upali Aparajita, Sahoo Dipti Prava, Parida Kulamani

机构信息

Centre for Nano Science and Nano Technology, ITER, Siksha 'O' Anusandhan Deemed to be University, Bhubaneswar, Odisha 751030, India.

出版信息

Inorg Chem. 2025 Feb 17;64(6):2723-2736. doi: 10.1021/acs.inorgchem.4c04513. Epub 2025 Feb 3.

Abstract

Designing and accumulating quantum dots (QD) onto layered double hydroxide (LDH) for the photocatalytic production of H and HO is a formidable task. Here, we intended the synthesis procedure of CdMoSe-QD (CMS)-incorporated NiV-LDH (NV) through a facile in situ reflux method and explored the photocatalytic activities of the CMS/NV (CNV) heterostructure. CNV-1 exhibits a large interface contact area and assures excellent interfacial charge transfer ability. Moreover, CNV-1 exhibits outstanding H and HO production rates, i.e., 6.4 and 2.5 times higher than that of pristine NV, respectively, due to formation of an S-scheme heterojunction between NV and CMS. Both NV and CMS function as n-type semiconductors and extend photoresponse to visible regions. The CNV-1 composite achieves 1.67% SCC for photocatalytic HO generation and 7.36% ACE for photocatalytic H evolution. The excellent activity is ascribed to higher anodic photocurrent, the quantum confinement effect of CMS, large surface-active sites, and delayed recombination of excitons as supported by PL and EIS measurements. Further, the S-scheme mechanism was authenticated through a radical scavenging test and work function, evaluated by UPS measurement. Altogether, this study exemplifies the concepts of designing a CNV heterostructure, which operates via an n-n-based S-scheme mechanism and aims to enhance photocatalytic H and HO production.

摘要

将量子点(QD)设计并累积到层状双氢氧化物(LDH)上以光催化产生H₂和H₂O₂是一项艰巨的任务。在此,我们旨在通过简便的原位回流法合成掺入CdMoSe-QD(CMS)的NiV-LDH(NV),并探索CMS/NV(CNV)异质结构的光催化活性。CNV-1具有较大的界面接触面积,并确保了优异的界面电荷转移能力。此外,由于NV和CMS之间形成了S型异质结,CNV-1表现出出色的H₂和H₂O₂产率,分别比原始NV高6.4倍和2.5倍。NV和CMS均作为n型半导体,并将光响应扩展到可见光区域。CNV-1复合材料在光催化产生H₂O₂方面实现了1.67%的SCC,在光催化H₂析出方面实现了7.36%的ACE。优异的活性归因于更高的阳极光电流、CMS的量子限制效应、大的表面活性位点以及PL和EIS测量所支持的激子延迟复合。此外,通过自由基清除试验和UPS测量评估的功函数验证了S型机制。总之,本研究例证了设计CNV异质结构的概念,该结构通过基于n-n的S型机制运行,旨在提高光催化H₂和H₂O₂的产生。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f4cf/11836927/de06430b5a99/ic4c04513_0007.jpg

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