Facile one-step synthesis of porous graphene-like g-C3N4 rich in nitrogen vacancies for enhanced H2 production from photocatalytic aqueous-phase reforming of methanol
Facile one-step synthesis of porous graphene-like g-C3N4 rich in nitrogen vacancies for enhanced H2 production from photocatalytic aqueous-phase reforming of methanol
复制标题
轻松一步合成富含氮空位的多孔石墨烯类g-C3N4，以提高甲醇光催化水相重整中的氢气产量
DOI：
10.1016/j.ijhydene.2020.09.156
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发表时间：
2020-10
影响因子：
7.2
通讯作者：
Zheng Zhanfeng
中科院分区：
文献类型：
--
作者：
Wang Ruiyi;Wang Xiaoyu;Li Xincheng;Pei Linjuan;Gu Xianmo;Zheng Zhanfeng
将块状石墨氮化碳（g-C3N4）剥离成单层或多层结构是提高其光催化性能的有效途径。然而，少层g- c3n4的合成方法相对复杂且耗时，并且由于量子尺寸效应导致g- c3n4的带隙增大，阻碍了可见光的有效利用。在不失去其可见光吸收能力的情况下，有效地将g- c3n4体剥离成单层或多层结构仍然是一个挑战。本文以氧化石墨烯（GO）为牺牲模板，通过三聚氰胺的易热聚合制备了具有丰富氮空位的多孔类石墨烯g- c3n4纳米片。利用原子力显微镜（AFM）、扫描电镜（SEM）、透射电镜（TEM）、电子能谱（EA）、XPS和电子能谱（EPR）等技术对其二维层形貌和氮缺陷结构进行了表征。与块体g-C3N4相比，由于其独特的结构特征，制备的g-C3N4纳米片具有较高的比表面积，增强了对可见光的吸收能力，提高了载流子的产生和分离效率。它们的situDRIFT光谱表明，表面氮空位也是甲醇吸附和活化的绝佳位置。结果表明，甲醇水相重整制氢具有优异的光催化活性，其产氢率约为本体g-C3N4的14倍。
Exfoliation of bulk graphitic carbon nitride (g-C3N4) to single- or few-layered structures is an effective way to improve the photocatalytic performance. However, the synthesis methods for few-layer g-C3N4are relatively complicated and time-consuming, with the bandgap of g-C3N4increasing through quantum size effects, thus hampering effective utilization of visible light. To effectively exfoliate the bulk g-C3N4to single or few-layered structures in a facile way without losing its visible light absorption ability is still a challenge. Herein, porous graphene-like g-C3N4nanosheets with abundant nitrogen vacancies were prepared by facile thermal polymerization of melamine using graphene oxide (GO) as a sacrificial template. The two-dimensional (2D) layer morphology and nitrogen defect structure were proved using AFM, SEM, TEM, EA, XPS and EPR techniques. Compared with the bulk g-C3N4, the as-prepared g-C3N4nanosheet possesses a high specific surface area, enhanced absorption ability of visible light, and elevated charge carrier generation and separation efficiency because of the unique structural features. Thein situDRIFT spectrum indicates that the surface nitrogen vacancies also serve as excellent locations for methanol adsorption and activation. Consequently, an excellent photocatalytic activity of hydrogen production from methanol aqueous-phase reforming is obtained, which is about 14 times more productive than the bulk g-C3N4.
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