Department of Chemistry, University College London, London, UK.
London Centre for Nanotechnology and the Department of Electronic and Electrical Engineering, University College London, London, UK.
Nanoscale. 2017 Nov 9;9(43):16586-16590. doi: 10.1039/c7nr06489f.
Graphitic carbon nitrides (GCNs) represent a family of 2D materials composed of carbon and nitrogen with variable amounts of hydrogen, used in a wide variety of applications. We report a method of room temperature thin film deposition which allows ordered GCN layers to be deposited on a very wide variety of substrates, including conductive glass, flexible plastics, nanoparticles and nano-structured surfaces, where they form a highly conformal coating on the nanoscale. Film thicknesses of below 20 nm are achievable. In this way we construct functional nanoscale heterojunctions between TiO nanoparticles and GCN, capable of producing H photocatalytically under visible light irradiation. The films are hydrogen rich, have a band gap around 1.7 eV, display transmission electron microscopy lattice fringes as well as X-ray diffraction peaks despite being deposited at room temperature, and show characteristic Raman and IR bands. We use cluster etching to reveal the chemical environments of C and N in GCN using X-ray photoelectron spectroscopy. We elucidate the mechanism of this deposition, which operates via sequential surface adsorption and reaction analogous to atomic layer deposition. The mechanism may have implications for current models of carbon nitride formation.
石墨相氮化碳(GCNs)是一种由碳和氮组成的二维材料家族,其组成中含有不同数量的氢,可应用于各种不同的领域。我们报告了一种室温薄膜沉积方法,该方法可在非常广泛的基底上沉积有序的 GCN 层,包括导电玻璃、柔性塑料、纳米颗粒和纳米结构表面,在这些基底上 GCN 会在纳米尺度上形成高度适配的涂层。薄膜厚度可低于 20nm。通过这种方式,我们在 TiO2 纳米颗粒和 GCN 之间构建了功能型纳米级异质结,在可见光照射下可进行 H2 的光催化生产。薄膜富含氢,带隙约为 1.7eV,尽管是在室温下沉积的,但仍显示出透射电子显微镜晶格条纹和 X 射线衍射峰,并显示出特征拉曼和红外带。我们使用团簇刻蚀技术,通过 X 射线光电子能谱揭示了 GCN 中 C 和 N 的化学环境。我们阐明了这种沉积的机制,该机制通过类似于原子层沉积的顺序表面吸附和反应来进行。该机制可能对当前的氮化碳形成模型产生影响。