A Visible Light-Responsive Mixed-Valence Bimetallic Eu–Zr MOF-Based Nanoarchitecture toward Efficacious H2O2 and H2 Production

IF 3.9 3区 工程技术 Q2 ENGINEERING, CHEMICAL Industrial & Engineering Chemistry Research Pub Date : 2025-03-06 DOI:10.1021/acs.iecr.4c04234
Srabani Dash, Suraj Prakash Tripathy, Satyabrata Subudhi, Kulamani Parida
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Abstract

A mixed-valence bimetallic Eu/Zr MOF has been fabricated via a one-step solvothermal method by incorporating Eu3+ ions into the Zr-MOF, thereby making a single-component photocatalyst that can be utilized toward robust photon utilization from the visible light spectrum for the photocatalytic production of green energy like H2 and H2O2. The one-step synthesized bimetallic Eu/Zr-MOF exhibits more visible light captivation properties along with improved charge carrier separation, confined band gap, and excellent ligand-to-metal charge transfer (LMCT) because of the existence of an interconvertible Eu3+/Eu2+ ion pair compared with the pristine MOF counterparts. The addition of Eu ions directed to an upsurge in the electron density around Zr4+ ion, as seen from XPS analysis. Moreover, the introduction of Eu3+ enhanced the exciton segregation, as seen from PL and EIS analyses, thereby leading to superior catalytic performances. An increased photocatalytic H2 generation efficacy of 331.26 μmol h–1 (ACE = 2.42%) was demonstrated by the synthesized EZUNH-2 MOF, which is approximately three times greater than pristine MOFs. As a result, the bimetallic EZUNH-2 MOF can be easily utilized as a robust photocatalyst that has increased inclinations to produce H2O2 at 35.2 μmol h–1, around 4 times more than that of the parent material. Consequently, the one-pot synthesized bimetallic MOF paves a suitable mechanistic pathway for paramount performance toward photocatalytic H2O2 and H2 production.

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一种可见光响应的混合价双金属铕-锆mof纳米结构高效产氢
通过一步溶剂热法,将Eu3+离子掺入Zr-MOF中,制备了一种混合价双金属Eu/Zr MOF,从而制备了一种单组分光催化剂,该光催化剂可以利用可见光光谱中的强大光子,用于光催化生产H2和H2O2等绿色能源。一步合成的双金属Eu/Zr-MOF与原始MOF相比,由于存在可互转换的Eu3+/Eu2+离子对,具有更好的可见光俘获性能,改善了载流子分离,限制了带隙,并具有良好的配体-金属电荷转移(LMCT)。从XPS分析可以看出,Eu离子的加入导致Zr4+离子周围的电子密度激增。此外,从PL和EIS分析可以看出,Eu3+的引入增强了激子的偏析,从而导致了优异的催化性能。合成的EZUNH-2 MOF光催化H2生成效率为331.26 μmol h-1 (ACE = 2.42%),约为原始MOF的3倍。结果表明,双金属EZUNH-2 MOF可以很容易地用作光催化剂,其产生H2O2的倾向为35.2 μmol h-1,约为母体材料的4倍。因此,一锅合成的双金属MOF为光催化生产H2O2和H2的最佳性能铺平了合适的机制途径。
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来源期刊
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
期刊介绍: ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.
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