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Effect of morphology and non-metal doping (P and S) on the activity of graphitic carbon nitride toward photoelectrochemical water oxidation
Solar Energy Materials and Solar Cells ( IF 6.9 ) Pub Date : 2021-08-19 , DOI: 10.1016/j.solmat.2021.111326
Ahmed Esmail A. Aboubakr , Waleed M.A. El Rouby , Malik Dilshad Khan , Neerish Revaprasadu , Pierre Millet

The production of molecular hydrogen by photoelectrochemical dissociation (PEC) of water is a promising technique, which allows the direct transformation of solar energy into hydrogen, an energy vector acclaimed by the scientific community and policymakers. Hydrogen stores solar energy and will help overcome the energy crisis and associated environmental problems. Currently, the design and development of innovative photocatalysts with strong photoelectrochemical activity remain a major challenge, and the subject of intense research activity within the international scientific community. Here we describe the synthesis and photoelectrochemical properties of one-dimensional nanostructures of graphitic carbon nitride (1D-gC3N4) doped with phosphorus or sulfur (1D-P-gC3N4 &1D-S-gC3N4, respectively). A new synthesis method using supramolecular melamine, ammonium dihydrogen phosphate, and tri-thiocyanuric acid as precursors has been developed. The samples were characterized by powder-X Ray diffraction (p-XRD), X-Ray spectroscopy (EDS), transmission electron microscopy (TEM), Ultraviolet–visible (UV–Vis) spectroscopy, Fourier transform infrared spectra (FT-IR) and photoluminescence (PL) analysis. The activity towards the photo-oxidation of water was studied by linear scanning voltammetry (LSV). Compared to 3D material, the activity was found to be significantly improved, thanks in particular to the 1D morphology of gC3N4. It was further strengthened by doping with phosphorus and sulfur. The photo-oxidation mechanism of water was analyzed by photoelectrochemical impedance spectroscopy (PEIS). The measurements show that the resistance to charge transfer at the electrode/electrolyte interface can be greatly reduced by controlling the morphology of gC3N4, and that doping with phosphorus and sulfur also plays a positive role. The PEIS analysis makes it possible to demonstrate that the lifetime of the photo-generated electrons in 1D-gC3N4 is increased compared to 3D-gC3N4, and that doping with phosphorus or sulfur further improves it. The width of the forbidden bands and the position of the valence and conduction bands of the different materials were determined by Mott - Schottky type measurements.



中文翻译:

形貌和非金属掺杂(P和S)对石墨氮化碳光电化学水氧化活性的影响

通过水的光电化学解离 (PEC) 生产分子氢是一种很有前途的技术,它可以将太阳能直接转化为氢,这是一种受到科学界和政策制定者赞誉的能量载体。氢能储存太阳能,有助于克服能源危机和相关的环境问题。目前,具有强光电化学活性的创新光催化剂的设计和开发仍然是一项重大挑战,也是国际科学界研究活动的热点。在这里,我们描述了掺杂磷或硫的石墨氮化碳 (1D-gC 3 N 4 )一维纳米结构(1D-P-gC 3N 4 &1D-S-gC 3 N 4 )。开发了一种以超分子三聚氰胺、磷酸二氢铵和三硫氰尿酸为前驱体的合成新方法。通过粉末 X 射线衍射 (p-XRD)、X 射线光谱 (EDS)、透射电子显微镜 (TEM)、紫外-可见 (UV-Vis) 光谱、傅里叶变换红外光谱 (FT-IR) 对样品进行表征和光致发光 (PL) 分析。通过线性扫描伏安法(LSV)研究对水的光氧化的活性。与 3D 材料相比,发现活性显着提高,特别是由于 gC 3 N 4的 1D 形态. 通过掺杂磷和硫进一步强化。通过光电化学阻抗谱(PEIS)分析了水的光氧化机理。测量表明,通过控制gC 3 N 4的形貌可以大大降低电极/电解质界面处的电荷转移阻力,并且磷和硫的掺杂也起到了积极的作用。PEIS 分析可以证明与 3D-gC 3 N 4相比,1D-gC 3 N 4 中光生电子的寿命有所增加,并且掺杂磷或硫进一步改善了它。不同材料的禁带宽度和价带和导带的位置由莫特-肖特基型测量确定。

更新日期:2021-08-19
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