N–TiO2 crystal seeds incorporated in amorphous matrix for enhanced solar hydrogen generation: Experimental & first-principles analysis. (26th June 2022)

• Record Type: Journal Article
• Authors: Biswas, Neeraj Kumar; Srivastav, Anupam; Saxena, Sakshi; Verma, Anuradha; Dutta, Runjhun; Srivastava, Manju; Upadhyay, Sumant; Satsangi, Vibha Rani; Shrivastav, Rohit; Dass, Sahab
• Is Part Of: International journal of hydrogen energy. Volume 47:Number 53(2022)
• Page Start: 22415
• Page End: 22429
• Publication Date: 2022-06-26
• Subjects: Partially crystalline -- TiO2 -- Highly crystalline -- Hydrogen -- Photoelectrochemical; Hydrogen as fuel -- Periodicals; Hydrogène (Combustible) -- Périodiques; Hydrogen as fuel; Periodicals; 665.81
• DOI: 10.1016/j.ijhydene.2022.05.064
• Languages: English
• ISSNs: 0360-3199

Abstract

Abstract: We present here a combined study on the photoelectrochemical activity of highly active Nitrogen doped titanium dioxide thin-film using experiments and First principle density (DFT) based calculation. Hybridization of N 2p with O 2p and localized valence band upshifting leads to the reduction in band-gap of N–TiO2 . To validate theoretical findings, the role of nitrogen in TiO2 is revisited with a focus on partial crystallinity. The best-case photoelectrode, nanostructured partially crystalline nitrogen-doped titanium dioxide (PCNDTO) offered photocurrent density of 24.3 mA/cm 2 at 1 V versus saturated calomel electrode (SCE). The absence of well-defined peaks and long-range order in XRD pattern and Raman spectrum respectively suggests partially crystallinity. High-resolution transmission electron microscopy (HR-TEM) images confirm the presence of TiO2 crystals in the amorphous matrix. High photoelectrochemical response can be attributed to the abundance of hydroxyl groups, high electrochemical active surface area, reduced charge transfer resistance, and reduced charge carrier recombination rate. Graphical abstract: Image 1 Highlights: Incorporation of N in TiO2 using DEA as a binder. Investigation of the effect of annealing atmosphere on the crystallinity of TiO2 . IPCE of 80.58% achieved in partially crystalline N–TiO2 . Presence of –OH groups in PCNDTO reduces charge carrier recombination. Oxygen vacancy in partially crystalline N–TiO2 enhances PEC activity.