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一种与多层石墨烯共价键合的钌配合物的制备及其作为光催化剂的评估。

Preparation of a ruthenium complex covalently bonded to multilayer graphene and its evaluation as a photocatalyst.

作者信息

Rodríguez-Flórez Lesly V, de Gracia Retamosa María, Navlani-García Miriam, Cazorla-Amorós Diego, Nájera Carmen, Yus Miguel, Sansano José M

机构信息

Departamento de Química Orgánica e Instituto de Síntesis Orgánica (ISO), University of Alicante E-03080 Alicante Spain

Centro de Innovación en Química Avanzada (ORFEO-CINQA), University of Alicante E-03080 Alicante Spain.

出版信息

Nanoscale Adv. 2024 Feb 9;6(6):1648-1652. doi: 10.1039/d4na00075g. eCollection 2024 Mar 12.

DOI:10.1039/d4na00075g
PMID:38482040
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10929589/
Abstract

Multilayer graphene (MLG), obtained by mild sonication of graphite in NMP, was functionalised 1,3-dipolar cycloaddition with azomethine ylides generated by thermal 1,2-prototropy from various imino esters. The microwave-assisted functionalisation took place in five hours at 100 °C. The resulting MLG, containing substituted proline-based amine functional groups, was characterized using XPS and showed a nitrogen loading three times that obtained for the same transformation performed for five days using convection-assisted heating. The preparation of the imino ester containing a bipyridine unit at the arylidene position allowed for the preparation of the corresponding functionalised MLG, which incorporated the ruthenium atom to achieve a heterogeneous MLG-Ru complex. This supported complex was tested, as a proof of concept, as a photocatalyst of the aerobic oxidative hydroxylation of 4-methoxyphenylboronic acid.

摘要

通过在NMP中对石墨进行温和超声处理获得的多层石墨烯(MLG),通过与各种亚氨基酯经热1,2-质子转移生成的甲亚胺叶立德进行1,3-偶极环加成反应进行功能化。微波辅助功能化在100°C下进行了5小时。所得含有取代脯氨酸基胺官能团的MLG使用XPS进行了表征,结果表明,与使用对流辅助加热进行5天的相同转化相比,氮负载量提高了三倍。在亚芳基位置含有联吡啶单元的亚氨基酯的制备使得能够制备相应的功能化MLG,其并入钌原子以形成多相MLG-Ru络合物。作为概念验证,对这种负载型络合物作为4-甲氧基苯硼酸需氧氧化羟基化的光催化剂进行了测试。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66f4/10929589/f60c7f4d5191/d4na00075g-s3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66f4/10929589/eb7bb30408d1/d4na00075g-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66f4/10929589/dfbf656ef51d/d4na00075g-s2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66f4/10929589/f60c7f4d5191/d4na00075g-s3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66f4/10929589/eb7bb30408d1/d4na00075g-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66f4/10929589/dfbf656ef51d/d4na00075g-s2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/66f4/10929589/f60c7f4d5191/d4na00075g-s3.jpg

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