Ni(OH)2 quantum dots as a stable cocatalyst modified α-Fe2O3 for enhanced photoelectrochemical water-splitting

doi:10.1016/S1872-2067(21)63829-9

Abstract

Abstract:

Depositing a cocatalyst has proven to be an important strategy for improving the photoelectrochemical (PEC) water-splitting efficiency of photoanodes. In this study, Ni(OH)₂ quantum dots (Ni(OH)₂ QDs) were deposited in situ onto an α-Fe₂O₃ photoanode via a chelation-mediated hydrolysis method. The photocurrent density of the Ni(OH)₂ QDs/α-Fe₂O₃ photoanode reached 1.93 mA·cm^-2 at 1.23 V vs. RHE, which is 3.5 times that of α-Fe₂O₃, and an onset potential with a negative shift of ca. 100 mV was achieved. More importantly, the Ni(OH)₂ QDs exhibited excellent stability in maintaining PEC water oxidation at a high current density, which is attributed to the ultra-small crystalline size, allowing for the rapid acceptance of holes from α-Fe₂O₃ to Ni(OH)₂ QDs, formation of active sites for water oxidation, and hole transfer from the active sites to water molecules. Further (photo)electrochemical analysis suggests that Ni(OH)₂ QDs not only provide maximal active sites for water oxidation but also suppress charge recombination by passivating the surface states of α-Fe₂O₃, thereby significantly enhancing the water oxidation kinetics over the α-Fe₂O₃ surface.

Key words: Photoelectrochemical water splitting, α-Fe₂O₃, Cocatalyst, Ni(OH)₂, Quantum dots

Jiayue Rong, Zhenzhen Wang, Jiaqi Lv, Ming Fan, Ruifeng Chong, Zhixian Chang. Ni(OH)₂ quantum dots as a stable cocatalyst modified α-Fe₂O₃ for enhanced photoelectrochemical water-splitting[J]. Chinese Journal of Catalysis, 2021, 42(11): 1999-2009.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63829-9

https://www.cjcatal.com/EN/Y2021/V42/I11/1999

Figures/Tables 9

Fig. 1. (a) Illustration of fabrication of Ni(OH)2 QDs/α-Fe2O3; TEM images of Ni(OH)2 QDs/α-Fe2O3 under different successive dipping frequencies: (b) 1, (c) 3, and (d) 5 times; (e) HRTEM image of Ni(OH)2 QDs/α-Fe2O3; photographs of Ni(OH)2 QDs with a Tyndall effect (f) and fresh NO3--Ni(OH)2 precipitate (g).

Fig. 2. XRD patterns of different samples. (a) α-Fe2O3, NO3--Ni(OH)2/α-Fe2O3, and Ni(OH)2 QDs/α-Fe2O3; (b) EDTA-Ni(OH)2 and NO3--Ni(OH)2.

Fig. 3. High-resolution XPS spectra of (a) Ni 2p in EDTA-Ni(OH)2 and NO3--Ni(OH)2 (a), Fe 2p (b) and O 1s (c) in α-Fe2O3 and Ni(OH)2 QDs/α-Fe2O3; (d) UV-vis absorption of α-Fe2O3, NO3--Ni(OH)2/α-Fe2O3 and Ni(OH)2 QDs/α-Fe2O3.

Fig. 4. (a) LSV curves for α-Fe2O3 and Ni(OH)2 QDs/α-Fe2O3 with 1, 3, and 5 dipping times; (b) amperometric I-t curves for α-Fe2O3 and Ni(OH)2 QDs/α-Fe2O3; (c) LSV curves and (d) I-t curves under chopped light illumination for α-Fe2O3, Ni(OH)2 QDs/α-Fe2O3, and NO3--Ni(OH)2/α-Fe2O3.

Fig. 5. CVs ofα-Fe2O3 (a) and Ni(OH)2 QDs/α-Fe2O3 (b) in the non-Faradaic potential range from 0.85 to 1.05 V vs. RHE at scan rates of 20, 40, 60, 80, and 100 mV·s-1; (c) half capacitive current differences (Δj/2) vs. scan rates; (d) OCP profiles of α-Fe2O3 and Ni(OH)2 QDs/α-Fe2O3.

Fig. 6. Nyquist plots (a) and Bode plots (b) for α-Fe2O3 and Ni(OH)2 QDs/α-Fe2O3 at 0.85 V vs. RHE under illumination.

Fig. 7. ηbulk (a) and ηsurface (b) for α-Fe2O3 and Ni(OH)2 QDs/α-Fe2O3.

Fig. 8. (a) IMPS curves for α-Fe2O3 and Ni(OH)2 QDs/α-Fe2O3 photoanodes under the applied potential of 1.2 V vs. RHE; (b) Charge transfer rate constant (ktr) and recombination rate constant (krec) for α-Fe2O3 and Ni(OH)2 QDs/α-Fe2O3.

Fig. 9. The possible water oxidation mechanism over Ni(OH)2 QDs/α-Fe2O3.

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Ni(OH)₂ quantum dots as a stable cocatalyst modified α-Fe₂O₃ for enhanced photoelectrochemical water-splitting

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