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Facile Synthesis of Self-Assembled g-C3N4 with Abundant Nitrogen Defects for Photocatalytic Hydrogen Evolution
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2018-06-21 00:00:00 , DOI: 10.1021/acssuschemeng.8b01499 Yanyun Wang 1 , Shuo Zhao 1 , Yiwei Zhang 1 , Jiasheng Fang 1 , Wenxia Chen 1 , Shenhao Yuan 1 , Yuming Zhou 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2018-06-21 00:00:00 , DOI: 10.1021/acssuschemeng.8b01499 Yanyun Wang 1 , Shuo Zhao 1 , Yiwei Zhang 1 , Jiasheng Fang 1 , Wenxia Chen 1 , Shenhao Yuan 1 , Yuming Zhou 1
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In this work, g-C3N4 with different morphologies is prepared using melamine as precursor via self-assembly and calcination. Compared with pristine g-C3N4, the resultant materials possess thinner lamellar structure and abundant nitrogen defects. Hydrolysis of partial melamine occurs in a hydrothermal process, and a consequent supramolecular intermediate is formed between melamine and its hydrolysates via hydrogen bonding. In addition to enlarging the π–π conjugated systems of the polymer, the formation of intermolecular hydrogen bonds is also interesting for increasing the lifetime of fluorescence as well as for decreasing the recombination rate of electron–hole pairs. Optical absorption characterization indicates that the samples formed by surface self-assembly show remarkably extended light absorption in the visible-light region in comparison with the original g-C3N4. Under visible-light irradiation, all modified materials have outstanding photocatalytic activity, especially the optimally modified catalyst; the hydrogen evolution activity is as high as 8910.7 μmol g–1, which is 9.9 times higher than that of g-C3N4. The improved photocatalytic performance benefits from the nitrogen defects and the structural advantages, more exposed active edges and higher surface area. This method opens a window for facile preparation of metal-free catalysts and inspires similar attempts for the modification of nanomaterials.
中文翻译：
自组装的具有大量氮缺陷的g -C 3 N 4的简便合成，可用于光催化制氢
在这项工作中，以三聚氰胺为前体通过自组装和煅烧制备了不同形态的g -C 3 N 4。与原始g -C 3 N 4相比，所得材料具有较薄的层状结构和丰富的氮缺陷。部分三聚氰胺的水解在水热过程中发生，结果三聚氰胺及其水解产物之间通过氢键形成超分子中间体。除了扩大聚合物的π-π共轭体系外，分子间氢键的形成对于延长荧光寿命以及降低电子-空穴对的复合速率也很有趣。光吸收特性表明，与原始g -C 3 N 4相比，通过表面自组装形成的样品在可见光区域显示出明显延长的光吸收。。在可见光照射下，所有改性材料都具有出色的光催化活性，尤其是最佳改性的催化剂。析氢活性高达8910.7μmolg –1，是g -C 3 N 4的9.9倍。改进的光催化性能得益于氮缺陷和结构优势，更多暴露的活性边缘和更大的表面积。该方法为方便地制备无金属催化剂打开了一个窗口，并激发了类似的尝试来修饰纳米材料。
更新日期：2018-06-21
中文翻译：
自组装的具有大量氮缺陷的g -C 3 N 4的简便合成，可用于光催化制氢
在这项工作中，以三聚氰胺为前体通过自组装和煅烧制备了不同形态的g -C 3 N 4。与原始g -C 3 N 4相比，所得材料具有较薄的层状结构和丰富的氮缺陷。部分三聚氰胺的水解在水热过程中发生，结果三聚氰胺及其水解产物之间通过氢键形成超分子中间体。除了扩大聚合物的π-π共轭体系外，分子间氢键的形成对于延长荧光寿命以及降低电子-空穴对的复合速率也很有趣。光吸收特性表明，与原始g -C 3 N 4相比，通过表面自组装形成的样品在可见光区域显示出明显延长的光吸收。。在可见光照射下，所有改性材料都具有出色的光催化活性，尤其是最佳改性的催化剂。析氢活性高达8910.7μmolg –1，是g -C 3 N 4的9.9倍。改进的光催化性能得益于氮缺陷和结构优势，更多暴露的活性边缘和更大的表面积。该方法为方便地制备无金属催化剂打开了一个窗口，并激发了类似的尝试来修饰纳米材料。
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