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氧化石墨烯负载钼簇:用于由二氧化碳和甲醇合成碳酸二甲酯的首个均相催化剂多相化实例

Graphene oxide supported molybdenum cluster: first heterogenized homogeneous catalyst for the synthesis of dimethylcarbonate from CO2 and methanol.

作者信息

Kumar Subodh, Khatri Om P, Cordier Stéphane, Boukherroub Rabah, Jain Suman L

机构信息

Chemical Sciences Division, CSIR-Indian Institute of Petroleum, Mohkampur, Dehradun-248005 (India).

出版信息

Chemistry. 2015 Feb 16;21(8):3488-94. doi: 10.1002/chem.201404949. Epub 2014 Dec 23.

DOI:10.1002/chem.201404949
PMID:25537229
Abstract

The octahedral molybdenum cluster-based compound, Cs2 Mo6 Br(i) 8 Br(a) 6 was immobilized on graphene oxide (GO) by using a facile approach. High resolution transmission electron microscopy results revealed that molybdenum clusters were uniformly distributed on the GO nanosheets. Cs2 Mo6 Br(i) 8 Br(a) 6 was attached to the GO support via chemical interaction between apical ligands of Mo6 Br(i) 8 Br(a) 6 cluster units and oxygen functionalities of GO, as revealed by XPS studies. The developed material was used for the synthesis of dimethyl carbonate by reduction of carbon dioxide. The synthesized catalyst, that is, GO-Cs2 Mo6 Br(i) 8 Br(a) x , exhibited higher catalytic efficiency than its homogeneous analogue without using dehydrating agent. The catalyst was found to be efficiently recyclable without significant loss of catalytic activity.

摘要

通过一种简便的方法将基于八面体钼簇的化合物Cs2Mo6Br(i)8Br(a)6固定在氧化石墨烯(GO)上。高分辨率透射电子显微镜结果表明,钼簇均匀分布在GO纳米片上。XPS研究表明,Cs2Mo6Br(i)8Br(a)6通过Mo6Br(i)8Br(a)6簇单元的顶端配体与GO的氧官能团之间的化学相互作用附着在GO载体上。所制备的材料用于通过二氧化碳还原合成碳酸二甲酯。合成的催化剂,即GO-Cs2Mo6Br(i)8Br(a)x,在不使用脱水剂的情况下表现出比其均相类似物更高的催化效率。发现该催化剂可有效循环使用,且催化活性无明显损失。

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