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

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• 作者：Huawen Hu ; John H. Xin ; Hong Hu ; Xiaowen Wang
• 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)
• 刊名：Nano Research
• 出版年：2015
• 出版时间：December 2015
• 年：2015
• 卷：8
• 期：12
• 页码：3992-4006
• 全文大小：3,262 KB
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• 作者单位：Huawen Hu (1)
  John H. Xin (1)
  Hong Hu (1)
  Xiaowen Wang (1)
  
  1. Nanotechnology Centre, Institute of Textiles and Clothing, The Hong Kong Polytechnic University, Hong Kong SAR, 999077, China
  
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Chinese Library of Science
  Chemistry
  Nanotechnology
  
• 出版者：Tsinghua University Press, co-published with Springer-Verlag GmbH
• ISSN：1998-0000

文摘

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 π-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.