Investigation of the Kinetic Properties and Photoelectrochemical Water Splitting of Cu3V2O8/ZnO Photoanode Modified by Cobalt Phosphate

doi:10.6023/A23090403

Abstract

Copper vanadate (Cu₃V₂O₈) has emerged as a promising material for photoelectrochemical applications due to its unique electronic and optical properties. In this study, the preparation of Cu₃V₂O₈ photoelectrodes with different thicknesses was reported and the factors that affect their photoelectrochemical performance were investigated. It is found that the primary limitation of Cu₃V₂O₈ as a photoanode material is the short diffusion distance of the photo-generated charge carriers, which leads to severe bulk recombination and limits the photocurrent density and efficiency. To overcome this limitation, a novel strategy of using one-dimensional ZnO nanorod arrays as a support framework and loading CoPi cocatalyst to enhance the photoelectrochemical performance of Cu₃V₂O₈ was proposed. The ZnO nanorod arrays serve as a rapid electron transfer channel to promote the bulk separation of photo-generated charge carriers, while the CoPi cocatalyst improves the surface separation efficiency of photo-generated charge carriers and enhances the oxidation kinetics. The incorporation of ZnO nanorod arrays and CoPi cocatalyst significantly enhances the photocurrent density and efficiency of Cu₃V₂O₈ photoelectrodes, resulting in a more than 2-fold increase in the photocurrent density and a 50% increase in the photoconversion efficiency. To further understand the underlying mechanisms behind the improved photoelectrochemical performance, a comprehensive analysis of the intensity-modulated photocurrent spectroscopy and electrochemical impedance spectroscopy data was performed. The results show that the incorporation of ZnO nanorod arrays and CoPi cocatalyst leads to a significant reduction in the charge transfer resistance and a decrease in the recombination rate of photo-generated charge carriers, which are responsible for the improved photocurrent density and efficiency. Overall, the study demonstrates the potential of using ZnO nanorod arrays and CoPi cocatalyst as a novel strategy to enhance the photoelectrochemical performance of Cu₃V₂O₈ photoelectrodes. The proposed approach provides a new direction for the development of high-performance photoanode materials for solar energy conversion and other photoelectrochemical applications.

Key words: Cu₃V₂O₈, ZnO, photoelectrochemical, kinetics, intensity modulated photocurrent spectroscopy

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Zhiqiang Wang, Jinzhan Su. Investigation of the Kinetic Properties and Photoelectrochemical Water Splitting of Cu₃V₂O₈/ZnO Photoanode Modified by Cobalt Phosphate[J]. Acta Chimica Sinica, 2024, 82(1): 26-35.

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Fig. & Tab. 8

Figure 1. (a) SEM image of CVO-3. SEM images of film cross section of (b) CVO-1, (c) CVO-2, (d) CVO-3, (e) CVO-4 and (f) CVO-5

Figure 2. (a) UV-Vis absorption spectra (The illustration shows the optical image of the CVO photoelectrode with different coating layers), (b) tauc-plot, (c) Raman spectrum, (d) X-ray photoelectron spectrum of Cu 2p, (e) X-ray photoelectron spectrum of V 2p and (f) X-ray diffraction patterns of CVO photoelectrode

Figure 3. (a) Photocurrent density spectrum, (b) applied bias photon-to-current efficiency spectrum, (c) Mott-Schottky plots, (d) transient photocurrent density curves, (e) electrochemical impedance spectra-Nyquist plot, (f) electrochemical impedance spectra-Bode-phase plot, (h) surface injection efficiency curves, (i) bulk phase separation efficiency curves and (j) intensity modulated photocurrent spectroscopy of CVO photoanode

样品	D_n/(cm²•s^-1)	τ_d/ms	k_tr	k_rec	η_tr/%	L_D/nm
CVO-1	1.20×10^-4	0.40	3.65	1.36	72.86	141.36
CVO-2	7.60×10^-5	0.63	3.73	2.58	59.05	112.28
CVO-3	7.60×10^-5	0.63	4.06	2.53	61.59	112.28
CVO-4	6.04×10^-5	0.80	2.96	3.35	46.85	100.08
CVO-5	6.04×10^-5	0.80	2.24	2.78	44.62	100.08

Table 1. Charge transfer and recombination kinetic parameters of photoelectrode

Figure 4. SEM images of (a) ZnO, (b) CVO/ZnO and (c) CoPi/CVO/ZnO. SEM images of film cross section of (d) ZnO, (e) CVO/ZnO and (f) CoPi/ CVO/ZnO

Figure 5. (a) X-ray diffraction patterns, (b) Raman spectra, (c) XPS wide survey spectra, (d) X-ray photoelectron spectrum of Zn element, (e) X-ray photoelectron spectrum of O element and (f) UV-Vis absorption spectra (the illustration shows the optical image of the CoPi/CVO/ZnO composite photoelectrodes)

Figure 6. (a) Photocurrent density spectrum, (b) applied bias photon-to-current efficiency spectrum, (c) Mott-Schottky plots, (d) electrochemical impedance spectra-Nyquist plot, (e) transient photocurrent density curves, (f) surface injection efficiency curves, (h) bulk phase separation efficiency curves, (i) intensity modulated photocurrent spectra, and (j) the VB and CB energy levels and the mechanism of charge transfer in CoPi/CVO/ZnO composite photoelectrode

样品	D_n/(cm²•s^-1)	τ_d/ms	k_tr	k_rec	η_tr/%
CVO-3	7.60×10^-5	0.63	4.06	2.53	61.59
ZnO	1.67×10^-4	0.29	3.61	1.40	72.23
CVO/ZnO	9.06×10^-5	0.53	3.73	2.15	63.41
CoPi/CVO/ZnO	1.14×10^-4	0.42	5.72	0.84	87.22

Table 2. Charge transfer and recombination kinetic parameters of photoelectrode

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磷酸钴修饰Cu₃V₂O₈/ZnO光阳极的动力学特性及光电化学水分解研究

Investigation of the Kinetic Properties and Photoelectrochemical Water Splitting of Cu₃V₂O₈/ZnO Photoanode Modified by Cobalt Phosphate

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磷酸钴修饰Cu3V2O8/ZnO光阳极的动力学特性及光电化学水分解研究