Unveiling the multiple effects of MOF-derived TiO2 on Ti-Fe2O3 photoanodes for efficient and stable photoelectrochemical water oxidation

doi:10.1016/S1872-2067(24)60005-7

Abstract

Abstract:

α-Fe₂O₃ is a promising photoanode that is limited by its high surface charge recombination and slow water oxidation kinetics. In this study, we synthesized a TiO₂ layer on Ti-Fe₂O₃ by annealing Ti-MOFs, followed by ZIF-67 as a co-catalyst, to fabricate a ZIF-67/TiO₂/Ti-Fe₂O₃ photoanode for photoelectrochemical (PEC) water splitting. The systematic experimental and theoretical results revealed that the improvement in performance was due to multiple effects of the MOF-derived TiO₂. This molecule not only passivates the acceptor surface states of Ti-Fe₂O₃, thereby reducing the number of surface recombination centers, but also acts as an electron barrier to promote charge separation in the Ti-Fe₂O₃ bulk. Moreover, MOF-derived TiO₂ can dramatically reduce the energy barrier for the OER of Ti-Fe₂O₃, thus promoting the conversion of the intermediate *OH into *O. The synergistic improvement in the bulk and surface properties effectively enhanced the water oxidation performance of Ti-Fe₂O₃. The ZIF-67/TiO₂/Ti-Fe₂O₃ photoanode exhibits a photocurrent density of up to 4.04 mA cm^‒2 at 1.23 V vs. RHE, which is 9.4 times as that of pure Ti-Fe₂O₃, and has long-term stability. Our work provides a feasible strategy for constructing efficient organic-inorganic hybrid photoelectrodes.

Key words: Ti-Fe₂O₃ photoanode, Charge separation, Porous TiO₂, Multiple effects, Water oxidation

Kaikai Ba, Yuʼnan Liu, Kai Zhang, Ping Wang, Yanhong Lin, Dejun Wang, Ziheng Li, Tengfeng Xie. Unveiling the multiple effects of MOF-derived TiO₂ on Ti-Fe₂O₃photoanodes for efficient and stable photoelectrochemical water oxidation[J]. Chinese Journal of Catalysis, 2024, 61: 179-191.

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Figures/Tables 12

Scheme 1. The preparation of the ZIF-67/TiO2/Ti-Fe2O3 photoanode.

Fig. 1. SEM images of Ti-Fe2O3 (a), Ti-MOF/Ti-Fe2O3 (b), TiO2/Ti-Fe2O3 (c), and ZIF-67/TiO2/Ti-Fe2O3 (d). TEM image (e), HRTEM image (f), and elemental mapping (g) of ZIF-67/TiO2/Ti-Fe2O3.

Fig. 2. XRD patterns (a), Raman spectra (b), and FTIR spectra (c) of ZIF-67/TiO2/Ti-Fe2O3, TiO2/Ti-Fe2O3, and Ti-Fe2O3. (d) N2 adsorption-desorption isotherms of MOF-derived TiO2. (e) Comparison of contact angles of TiO2/Ti-Fe2O3 and Ti-Fe2O3. (f) UV-vis absorption spectra.

Fig. 3. XPS spectra of ZIF-67/TiO2/Ti-Fe2O3: (a) survey; (b) Fe 2p; (c) Ti 2p; (d) O 1s; (e) Co 2p; (f) N 1s.

Fig. 4. LSV curves (the solid lines represent testing under illumination, while the dashed lines were run in the dark) (a), IPCE values (b), ABPE values (c) of Ti-Fe2O3, TiO2/Ti-Fe2O3, and ZIF-67/TiO2/Ti-Fe2O3, and stability test (d) of ZIF-67/TiO2/Ti-Fe2O3.

Table 1 Comparison of the photocurrent densities of Fe2O3-based photoanodes in the literature with our results at 1.23 V vs. RHE.

Photoanode	Photocurrent density (mA cm^-2)	Stability	Ref.
Ti:Fe₂O₃@CoFe-cMOFs	3.32	10 h stability ca. 95% of the original	[35]
CoPi/H₂TCPP/Ti-Fe₂O₃	1.84	2 h stability ca. 84% of the original	[36]
Fe_xNi_1‒_xOOH/B/Ti-Fe₂O₃	3.39	2 h stability ca. 93% of the original	[37]
Co-Sil/CTF/Gd-Fe₂O₃	2.74	5 h stability ca. 99% of the original	[38]
CoAl-LDH/F-Fe₂O₃	2.46	6 h stability ca. 90% of the original the original	[39]
Ti: Fe₂O₃@g-C₃N₄	3.38	5 h stability ca. 85% of the original	[40]
Ti-Fe₂O₃/CoFePi	2.15	3 h stability ca. 95% of the original	[41]
Co-Pi/CQDs/Fe₂O₃/TiO₂	3.00	3 h stability ca. 100% of the original	[42]
F:FeOOH/Zr:Fe₂O₃	2.11	2 h stability ca. 100% of the original	[43]
Fe₂O₃/FePO₄/FeOOH	2.00	1.3 h stability ca. 99% of the original	[44]
Fe₂O₃/Fe₂TiO₅/CoFe	1.25	24 h stability ca. 80% of the original	[45]
ZnFe₂O₄/Fe₂O₃	3.17	3 h stability ca. 86% of the original	[46]
NiFe(OH)_x/PSi/Ge-Fe₂O₃	4.57	65 h stability ca. 97% of the original	[47]
Ta:Fe₂O₃@CaFe₂O₄/FeNiO_x	2.70	50 h stability ca. 88% of the original	[48]
NiCoP/Fe₂O₃	3.80	4 h stability ca. 99% of the original	[49]
ZIF-67/TiO₂/Ti-Fe₂O₃	4.04	40 h stability ca. 90% of the original	this work

Fig. 5. TPV spectra (a) and the enlarged part (b) of peak 1 in the TPV spectra of Ti-Fe2O3, TiO2/Ti-Fe2O3, and ZIF-67/TiO2/Ti-Fe2O3. (c) Work function measurements of pure Ti-Fe2O3 and MOF-derived TiO2. (d) Open-circuit photovoltage (Voc) of Ti-Fe2O3, TiO2/Ti-Fe2O3, and ZIF-67/TiO2/Ti-Fe2O3. PL spectra (e) and PA spectra (f) of Ti-Fe2O3 and TiO2/Ti-Fe2O3.

Fig. 6. fs-TA spectra of Ti-Fe2O3 (a) and TiO2/Ti-Fe2O3 (b) excited at 400 nm. Transient absorption decays observed at 625 nm for Ti-Fe2O3 (c) and TiO2/Ti-Fe2O3 (d).

Fig. 7. Bode phase plots (a), bulk resistance of the photoanode (R1) (b), charge transfer resistance (c) at the solid-liquid interface (R2), charge transfer efficiency (ηCT) (d) of Ti-Fe2O3, TiO2/Ti-Fe2O3, and ZIF-67/TiO2/Ti-Fe2O3. CV curves (e) of ZIF-67/TiO2/Ti-Fe2O3, and measured capacitive currents plotted as a function of scan rates (f) for Ti-Fe2O3, TiO2/Ti-Fe2O3, and ZIF-67/TiO2/Ti-Fe2O3.

Fig. 8. J-t curves at 1.23 V vs. RHE under chopping light (a), accumulated charge density (b), ηinj (c), Nyquist plots (d) at 1.0 V vs. RHE, and enlarged Nyquist plots (e) of Ti-Fe2O3, TiO2/Ti-Fe2O3, and ZIF-67/TiO2/Ti-Fe2O3.

Fig. 9. Gibbs free energy changes during the OER for Ti-Fe2O3 and TiO2/Ti-Fe2O3.

Scheme 2. The charge transfer schematic mechanism diagram of Ti-Fe2O3 (a), TiO2/Ti-Fe2O3 (b), and ZIF-67/TiO2/Ti-Fe2O3 (c).

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Unveiling the multiple effects of MOF-derived TiO₂ on Ti-Fe₂O₃photoanodes for efficient and stable photoelectrochemical water oxidation

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