Boron- and Fluorine-Containing Mesoporous Carbon Nitride Polymers: Metal-Free Catalysts for Cyclohexane Oxidation

Boron- and Fluorine-Containing Mesoporous Carbon Nitride Polymers: Metal-Free Catalysts for Cyclohexane Oxidation
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含硼和氟介孔氮化碳聚合物:用于环己烷氧化的无金属催化剂

DOI:
10.1002/anie.201000120
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发表时间:
2010-01-01
影响因子:
16.6
通讯作者:
Li, Haoran
Li, Haoran
中科院分区:
化学1区
文献类型:
--
作者:
Wang, Yong;Zhang, Jinshui;Li, Haoran

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最近,具有不同纳米形态的各种轻质材料,其含有诸如氮、硼或氟的杂原子,由于其不寻常的性质,诸如在催化应用中或作为半导体,已经被积极地追求。[1]例如,氮化碳(C3 N4)的有序和无序改性扩展了碳纳米结构的性质,并具有从半导体到燃料电池的许多潜在应用领域。[1a]A大量报道涉及本体CxNy材料的不同改性的合成。[2]这些富氮物质的合成通常包括富氮前体的热缩合,通常来自含有或产生三嗪环的分子。例如,通过2,4,6-三氨基-1,3,5-三嗪与2,4,6-三氯-1,3,5-三嗪在高压和高温下的固态反应,Wolf和同事获得了良好表征和高度结晶的石墨碳氮化物衍生物。[3]然而,研究表明,更理想的块状氮化碳固体在某些催化过程中表现得相当弱,而更无序的聚合物形式显示出良好的活性,因为结构缺陷或表面终止似乎对催化活化起着关键作用。[4]为了提高氮化碳作为载体和催化剂的性能,必须提高比表面积,最近已经探索了使用多孔二氧化硅的硬模板纳米铸造用于复制具有受控介孔结构的多孔氮化碳材料。[五]《中国日报》
Recently, various lightweight materials with diverse nanomorphologies that contain heteroatoms such as nitrogen, boron, or fluorine have been actively pursued because of their unusual properties, such as in catalytic applications or as semiconductors.[1] For example, ordered and disordered modifications of carbon nitride (C3N4) extend the property profile of carbon nanostructures and have numerous potential areas of applications ranging from semiconductors to fuel cells.[1a]A large number of reports deals with the synthesis of different modifications of bulk CxNy materials.[2] The synthesis of these nitrogen-rich species generally includes thermal condensation of nitrogen-rich precursors, often from molecules containing or generating triazine rings. For example, through a solid-state reaction of 2, 4, 6-triamino-1, 3, 5-triazine with 2, 4, 6-trichloro-1, 3, 5-triazine at high pressure and high temperature, Wolf and co-workers obtained a well-characterized and highly crystalline graphitic carbon nitride derivative.[3] However, it was shown that the more ideal bulk carbon nitride solids perform rather weakly in some catalytic processes, while more disordered, polymeric versions showed nice activity, as structural defects or surface terminations seemed to play a key role for the catalytic activation.[4] To enhance the performance of carbon nitride both as a support and as a catalyst, the specific surface had to be enhanced, and nanocasting with hard templates using porous silicas has been explored recently for the replication of porous carbon nitride materials with controlled mesopore structures.[5]