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Structural and mechanistic understanding of an active and durable graphene carbocatalyst for reduction of 4-nitrophenol at room temperature

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Nano Research 2015年第12期8卷 3992-4006页

作者： Huawen Hu John H. Xin Hong Hu Xiaowen Wang Nanotechnology Centre Institute of Textiles and Clothing The Hong Kong Polytechnic University Hong Kong SAR 999077 China

The development of an active, durable, and metal-free carbocatalyst that is able to replace metal-based catalysts is of increasing scientific and technological importance. The use of such a catalyst would avoid problems caused by metal- containing catalysts, for example, environmental pollution by heavy metals and depletion of rare metal resources. Herein, an active and durable graphene carbocatalyst is presented for the carbocatalytic conversion of 4-nitrophenol to 4-aminophenol at ambient temperature. The carbocatalyst was prepared via a mild, water-based reaction between L-ascorbic acid （AA） and graphene oxide （GO） and did not involve any other reactants. During the structure and catalytic property optimization, a series of carbocatalysts were fabricated at various reaction temperatures and AA/GO ratios. Using several characterization techniques, detailed structural features of these carbocatalysts were identified. Possible active species and sites on the carbocatalysts were also identified such as certain oxygen-containing groups, the ~x-conjugated system, and graphene sheet edges. In addition, the synergistic effect between these active species and sites on the resulting catalytic activity is highlighted. Furthermore, we clarified the origin of the high stability and durability of the optimized carbocatalyst. The work presented here aids the design of high-performance carbocatalysts for hydrogenation reactions, and increases understanding of the structural and mechanistic aspects at the molecular level that lead to high catalyst activity and durability.

关键词： metal-free graphene carbocatalyst activity and durability L-ascorbic acid active sites and domains synergistic effect carbocatalytic conversion of 4-nitrophenol (4NP) to 4-aminophenol (4AP)

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