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用于催化应用的氮功能化石墨烯纳米片的连续生产。

Continuous production of nitrogen-functionalized graphene nanosheets for catalysis applications.

作者信息

Sanjeeva Rao Kodepelly, Senthilnathan Jaganathan, Ting Jyh-Ming, Yoshimura Masahiro

机构信息

Promotion Center for Global Materials Research (PCGMR), Department of Material Science and Engineering, National Cheng Kung University, Tainan, Taiwan.

出版信息

Nanoscale. 2014 Nov 7;6(21):12758-68. doi: 10.1039/c4nr02824d.

Abstract

This study reports the "continuous production" of high-quality, few-layer nitrogen-functionalized graphene nanosheets in aqueous solutions directly from graphite via a two-step method. The initial step utilizes our recently developed peroxide-mediated soft and green electrochemical exfoliation approach for the production of few-layer graphene nanosheets. The subsequent step, developed here, produces nitrogen-functionalized graphene nanosheets via selective alkylation/basic hydrolysis reactions using rather a simple nitrogen precursor bromoacetonitrile, which was never reported in the literature. A possible reaction mechanism of the nitrogen-functionalized graphene formation is proposed. The proposed method allows the quantification of the phenolic and hydroxyl functional groups of anodic few-layer graphene via the derivatization chemistry approach. Additionally, a nitrogen-functionalized graphene-gold nanocrystal hybrid is prepared using gold nanocrystals obtained via the microwave irradiation of H[AuCl4] and trisodium citrate solution. A systematic investigation demonstrates that the nitrogen-functionalized graphene-gold nanocrystal hybrid shows enhanced catalytic reduction of carbonyl compounds such as benzaldehyde.

摘要

本研究报告了通过两步法直接从石墨在水溶液中“连续生产”高质量、少层氮功能化石墨烯纳米片。第一步利用我们最近开发的过氧化物介导的温和绿色电化学剥离方法来制备少层石墨烯纳米片。在此开发的后续步骤通过使用相当简单的氮前驱体溴乙腈进行选择性烷基化/碱性水解反应来生产氮功能化石墨烯纳米片,这在文献中从未有过报道。提出了氮功能化石墨烯形成的可能反应机理。所提出的方法允许通过衍生化化学方法对阳极少层石墨烯的酚羟基和羟基官能团进行定量。此外,使用通过微波辐照氯金酸和柠檬酸钠溶液获得的金纳米晶体制备了氮功能化石墨烯-金纳米晶体杂化物。系统研究表明,氮功能化石墨烯-金纳米晶体杂化物对苯甲醛等羰基化合物的催化还原性能增强。

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