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Nucleobase derived boron and nitrogen co-doped carbon nanosheets as efficient catalysts for selective oxidation and reduction reactions
Nanoscale ( IF 6.7 ) Pub Date : 2020/03/04 , DOI: 10.1039/d0nr00516a
Guangming Wang 1, 2, 3, 4 , Peng Wang 1, 2, 3, 4 , Xuefei Zhang 1, 2, 3, 4 , Qiao-Hua Wei 1, 2, 3, 4 , Shuchang Wu 4, 5, 6, 7 , Zailai Xie 1, 2, 3, 4
Affiliation  

The search for active, stable and cost-efficient carbocatalysts for selective oxidation and reduction reactions could make a substantial impact on the catalytic technologies that do not rely on conventional metal based catalysts. Here we report a facile strategy for the synthesis of boron (B) and nitrogen (N) co-doped carbon nanosheets (BNC) by using biomolecule guanine as a carbon (C) and N source and boric acid as the B precursor. The whole synthesis process which leads to the formation of a two dimensional (2D) structure and mesoporosity with high surface areas is simple, metal-free and template-free. The as-synthesized carbon nanosheets possess a series of merits, such as relatively high specific surface area, satisfactory pore structure, enough structural defects, abundant B and N dopants as well as oxygen functional groups. The catalytic assessments demonstrate that the presented carbon catalyst is highly active and selective for the liquid phase oxidation of ethyl lactate to ethyl pyruvate and the reduction of nitrobenzene to aniline and outperforms other equivalent benchmarks. Control experiments confirm the importance of the B and N co-doping as well as the carbon matrix which benefit the electron transfer. The carbonyl group masking test indicates that carbonyl groups play an important role in both the selective oxidation and reductions. Given the diversity in the structure of the nucleobase moiety, they represent ideal building blocks for the catalyst-free and metal-free formation of 2D carbon architectures, only induced by hydrogen bonds. This B and N co-doped synthesis strategy provides guidance for the design of carbon-based catalysts for selective oxidation and reductions.

中文翻译:

核碱衍生的硼和氮共掺杂碳纳米片,作为选择性氧化和还原反应的有效催化剂

寻找用于选择性氧化和还原反应的活性,稳定和成本有效的碳催化剂可能会对不依赖常规金属基催化剂的催化技术产生重大影响。在这里,我们报告了一种利用生物分子鸟嘌呤作为碳(C)和N源以及硼酸作为B前体来合成硼(B)和氮(N)共掺杂碳纳米片(BNC)的简便策略。导致形成二维(2D)结构和具有高表面积的介孔的整个合成过程简单,无金属且无模板。所合成的碳纳米片具有一系列优点,例如相对较高的比表面积,令人满意的孔结构,足够的结构缺陷,丰富的B和N掺杂剂以及氧官能团。催化评估表明,所提出的碳催化剂对于乳酸乙酯液相氧化成丙酮酸乙酯和硝基苯还原成苯胺具有很高的活性和选择性,并且优于其他等效基准。对照实验证实了B和N共掺杂以及碳基体对电子转移有利的重要性。羰基掩蔽试验表明,羰基在选择性氧化和还原中均起着重要作用。考虑到核碱基部分结构的多样性,它们代表了仅由氢键诱导的无催化剂和无金属的2D碳结构形成的理想构件。
更新日期:2020-04-09
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