Sundararaj Sathiya Bama, Amir Humayun, Viswanathan Chinnuswamy, Thangavelu Selvaraju
Department of Chemistry, Bharathiar University, Coimbatore 641 046, India.
Department of Nanoscience and Technology, Bharathiar University, Coimbatore 641 046, India.
Langmuir. 2024 Aug 6;40(31):16582-16594. doi: 10.1021/acs.langmuir.4c02148. Epub 2024 Jul 24.
Harnessing solar energy can be efficiently used to generate hydrogen by photochemical water splitting, which is a sustainable and environmentally benign energy source. Here, a unique visible-light-driven CoTiO@g-CN (CTOCN)-based photoanode interface has been optimized and developed with modification to follow the type II heterojunction for the enhancement of photoelectrochemical water splitting. Initially, a graphitic carbon nitride-loaded CoTiO (with 10 wt % g-CN) composite was obtained using a one-pot solvothermal method. Accordingly, the type II heterojunction interface between g-CN and CoTiO has been successfully created and confirmed by the acquired phase, morphological, and optical examinations. Thereby, heterostructure generations with interfacial interaction were enabled to decrease photogenerated electron-hole pair recombination, leading to enhanced charge transfer for water oxidation kinetics. The minimal charge transfer resistance and hole relaxation lifetime () shown in Nyquist and Bode plots have further confirmed the rapid electron transport across the electrode/electrolyte interfaces, which is attributed to an enhanced absorption of holes for the water splitting process. Additionally, UV-vis spectroscopy, Mott-Schottky analysis, and UPS studies were used to determine the band edge locations of g-CN and CoTiO. In comparison to previously developed nanohybrids and their equivalents, the CTOCN-d photoanode follows the type II charge transfer mechanism, resulting in a higher photocurrent density of 55.51 mA cm.
利用太阳能通过光化学水分解高效地制氢,这是一种可持续且环境友好的能源。在此,一种独特的基于可见光驱动的CoTiO@g-CN(CTOCN)的光阳极界面已通过改性进行了优化和开发,以遵循II型异质结来增强光电化学水分解。最初,使用一锅溶剂热法获得了负载石墨相氮化碳的CoTiO(含10 wt% g-CN)复合材料。相应地,通过所获得的相、形态和光学检查成功创建并确认了g-CN和CoTiO之间的II型异质结界面。由此,具有界面相互作用的异质结构的生成能够减少光生电子-空穴对的复合,从而增强水氧化动力学的电荷转移。奈奎斯特图和博德图中显示的最小电荷转移电阻和空穴弛豫寿命进一步证实了电极/电解质界面间快速的电子传输,这归因于水分解过程中空穴吸收的增强。此外,利用紫外-可见光谱、莫特-肖特基分析和紫外光电子能谱研究来确定g-CN和CoTiO的能带边缘位置。与先前开发的纳米杂化物及其等效物相比,CTOCN-d光阳极遵循II型电荷转移机制,产生了更高的光电流密度55.51 mA cm。