Wang Guangming, Wang Peng, Zhang Xuefei, Wei Qiao-Hua, Wu Shuchang, Xie Zailai
Fujian Provincial Key Laboratory of Electrochemical Energy Storage Materials, College of Chemistry, Fuzhou University, 2 Xueyuan Road, Fuzhou 350116, China.
Nanoscale. 2020 Apr 14;12(14):7797-7803. doi: 10.1039/d0nr00516a. Epub 2020 Mar 27.
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.
寻找用于选择性氧化和还原反应的活性高、稳定性好且成本效益高的碳催化剂,可能会对不依赖传统金属基催化剂的催化技术产生重大影响。在此,我们报告了一种简便的策略,通过使用生物分子鸟嘌呤作为碳(C)和氮源,硼酸作为硼前驱体,合成硼(B)和氮(N)共掺杂的碳纳米片(BNC)。整个合成过程简单、无金属且无模板,能够形成二维(2D)结构和具有高比表面积的介孔。所合成的碳纳米片具有一系列优点,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,所展示的碳催化剂对乳酸乙酯液相氧化为丙酮酸乙酯以及硝基苯还原为苯胺具有高活性和选择性,并且优于其他等效基准。对照实验证实了B和N共掺杂以及有利于电子转移的碳基质的重要性。羰基掩蔽试验表明羰基在选择性氧化和还原中都起着重要作用。鉴于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形成二维碳结构的理想构建块。这种B和N共掺杂的合成策略为设计用于选择性氧化和还原的碳基催化剂提供了指导。