Nitro functionalized chromium terephthalate metal-organic framework as multifunctional solid acid for the synthesis of benzimidazoles

Autor: Sergio Navalón, Hermenegildo García, Mercedes Alvaro, María Cabrero-Antonino, Amarajothi Dhakshinamoorthy, Cristina Vallés-García
Přispěvatelé: Ministerio de Economía y Competitividad (España), Generalitat Valenciana, Ministerio de Ciencia, Innovación y Universidades (España)
Jazyk: angličtina
Rok vydání: 2020
Předmět:
Zdroj: RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
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Digital.CSIC. Repositorio Institucional del CSIC
Popis: [EN] In the present work, nitro functionalized chromium terephthalate [MIL-101(Cr)-NO2] metal-organic framework is prepared and characterized by powder X-ray diffraction (XRD), elemental analysis, infrared spectroscopy (IR), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and Brun auer-Emmett-Teller (BET) surface area. The inherent Lewis acidity of MIL-101(Cr)-NO2 is confirmed by FT-IR spectroscopy using CD3CN as a probe molecule. The performance of MIL-101(Cr)-NO2 as bifunctional catalyst (acid and redox) promoting the synthesis of wide range of benzimidazoles has been examined by catalyzed condensation on acid sites and subsequent oxidative dehydrogenation. The catalytic activity of MIL-101(Cr)-NO2 is found to be superior than analogues catalysts like MIL-101(Cr)-S0(3)H, MIL-101(Cr)-NH2, U10-66(Zr), Ui0-66(Zr)-NO2, MIL-100(Fe) and Cu-3(BTC)(2) (BTC: 1,35-benzenetricarboxylate) under identical reaction conditions, The structural stability of MIL-101(Cr)-NO2 is supported by leaching analysis and reusability tests. MIL-101(Cr)-NO2 solid is used five times without decay in its activity. Comparison of the fresh and five times used MIL-101(Cr)-NO2 solids by powder XRD, SEM and elemental analysis indicate identical crystallinity, morphology and the absence of chromium leaching, respectively. (C) 2019 Elsevier Inc. All rights reserved.
AD thanks the University Grants Commission, New Delhi, for the award of an Assistant Professorship under its Faculty Recharge Programme. AD also thanks the Department of Science and Technology, India, for the financial support through Extra Mural Research Funding (EMR/2016/006500). Financial support by the Spanish Ministry of Science and Innovation (Severo Ochoa and RTI2018-098237-CO21) and Generalitat Valenciana (Prometeo 2017/083) is gratefully acknowledged. S.N. thanks financial support by the Fundacion Ramon Areces (XVIII Concurso Nacional para la Adjudication de Ayudas a la Investigacion en Ciencias de la Vida y de la Materia, 2016), Ministerio de Ciencia, Innovation y Universidades RTI2018-099482-A-I00 project and Generalitat Valenciana grupos de investigacion consolidables 2019 (AICO/2019/214) project.
Databáze: OpenAIRE