A Novel Ti12-Based Metal-Organic Framework for Photocatalytic Hydrogen Evolution

IF 24.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Advanced Energy Materials Pub Date : 2025-04-01 DOI:10.1002/aenm.202500211

Bingbing Chen, Asma Mansouri, Celia M. Rueda-Navarro, Iurii Dovgaliuk, Philippe Boullay, Arianna Melillo, Juan José Ramírez-Hernández, Beibei Xiao, Dong Fan, Lokuge Aravindani Fernando, Gilles Patriarche, Ieuan Cornu, Pierre Florian, Guillaume Maurin, Sergio Navalón, Hermenegildo Garcia, Georges Mouchaham, Christian Serre

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引用次数: 0

Abstract

A new microporous titanium-based metal-organic framework (Ti-MOF), labeled as MIP-209(Ti) (MIP: Materials from Institute of Porous Materials of Paris), features nitro terephthalate ligands and Ti₁₂O₁₅ oxo-clusters, as revealed by continuous rotation electron diffraction (cRED). MIP-209(Ti) can be obtained using two different terephthalate (1, 4-BDC²⁻) derivatives such as NO₂-BDC and 2Cl-BDC in an eco-friendly solvent, suggesting the isostructural versatility of Ti₁₂-MOFs. Alternatively, its Ti-oxo-cluster can be tuned, similarly to MIP-177(Ti)-LT bearing the same Ti₁₂O₁₅ sub-unit. Typically, low percentage Cr³⁺ doping (≤5 at%) in MIP-209(Ti) favorably enhances the water stability. MIP-209(Ti-Cr)-NO₂ shows a significant hydrogen production rate, with good reusability and stability under simulated solar light irradiation. Compared to the benchmark Ti-MOF IEF-11, the hydrogen production of MIP-209(Ti-Cr)-NO₂ with 5 at% Cr doping has a fourfold enhancement in photocatalytic hydrogen evolution from water splitting reaction (HER) during 5 h in presence of methanol (5 812 µmol/g_cat against 1 391 µmol/g_cat), as well as, without any noble metal co-catalyst, a sixfold enhancement in overall water splitting reaction (OWS) (681 and 325 µmol/g_cat of H₂ and O₂, respectively, against 94 and 53 µmol/g_cat of H₂ and O₂, respectively). This work represents a leap forward in the synthesis of Ti-MOFs and their practical photocatalytic applications.

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来源期刊

Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS

CiteScore

41.90

自引率

4.00%

发文量

889

审稿时长

1.4 months

期刊介绍： Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.