Intrinsic photocatalytic water oxidation activity of Mn-doped ferroelectric BiFeO3

doi:10.1016/S1872-2067(20)63713-5

Abstract

Abstract:

The development of stable and efficient visible light-absorbing oxide-based semiconductor photocatalysts is a desirable task for solar water splitting applications. Recently, we proposed that the low photocurrent density in film-based BiFeO₃ (BFO) is due to charge recombination at the interface of the domain walls, which could be largely reduced in particulate photocatalyst systems. To demonstrate this hypothesis, in this work we synthesized particulate BFO and Mn-doped BiFeO₃ (Mn-BFO) by the sol-gel method. Photocatalytic water oxidation tests showed that pure BFO had an intrinsic photocatalytic oxygen evolution reaction (OER) activity of 70 μmol h^-1g^-1, while BFO-2, with an optimum amount of Mn doping (0.05%), showed an OER activity of 255 μmol h ^-1g^-1under visible light (λ ≥ 420 nm) irradiation. The bandgap of Mn-doped BFO could be reduced from 2.1 to 1.36 eV by varying the amount of Mn doping. Density functional theory (DFT) calculations suggested that surface Fe (rather than Mn) species serve as the active sites for water oxidation, because the overpotential for water oxidation on Fe species after Mn doping is 0.51 V, which is the lowest value measured for the different Fe and Mn species examined in this study. The improved photocatalytic water oxidation activity of Mn-BFO is ascribed to the synergistic effect of the bandgap narrowing, which increases the absorption of visible light, reduces the activation energy of water oxidation, and inhibits the recombination of photogenerated charges. This work demonstrates that Mn doping is an effective strategy to enhance the intrinsic photocatalytic water oxidation activity of particulate ferroelectric BFO photocatalysts.

Key words: Photocatalytic water oxidation, Bandgap engineering, Bismuth ferrite, Ferroelectric materials, Cation doping

Jafar Hussain Shah, Anum Shahid Malik, Ahmed Mahmoud Idris, Saadia Rasheed, Hongxian Han, Can Li. Intrinsic photocatalytic water oxidation activity of Mn-doped ferroelectric BiFeO₃[J]. Chinese Journal of Catalysis, 2021, 42(6): 945-952.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63713-5

https://www.cjcatal.com/EN/Y2021/V42/I6/945

Figures/Tables 8

Fig. 1. (a) XRD patterns of the BFO, BFO-1, BFO-2, BFO-3 and BFO-4; (b) Enlarged patterns of (104) and (110) peaks for BFO, BFO-1, BFO-2, BFO-3 and BFO-4.

Fig. 2. (a) DRS of the BFO, BFO-1, BFO-2, BFO-3 and BFO-4; (b) Tauc’s plot for bandgap calculations of the BFO, BFO-1, BFO-2, BFO-3 and BFO-4. Partial and total DOS calculations using DFT for BFO (c) and BFO-2 (d); (e) Mott-Schottky plots of BFO and BFO-2; (f) Energy band diagram showing the band edges of BFO and BFO-2.

Table 1 Particle sizes and bandgap energies of all samples.

Sample	Particle Size (nm)	Bandgap (eV)
BFO	130	2.1
BFO-1	50	1.52
BFO-2	40	1.46
BFO-3	38	1.4
BFO-4	34	1.36

Fig. 3. HR-SEM images of BFO (a,b), BFO-1 (c), BFO-2 (d), BFO-3 (e), and BFO-3 (f). (Scale bar 1 μm). Insets in (a-f) show the distribution of particle size of all the samples, respectively.

Fig. 4. EDS elemental mapping for BFO-2. (a) Bi; (b) Fe; (c) Mn; (d) O. (scale bar 3 μm). (e) EDS analysis graph indicating the presence of Bi, Fe, O and Mn.

Fig. 5. XPS analysis of BFO-2. (a) Bi 4f; (b) Fe 2p3/2 and 2p1/2; (c) O 1s; (f) Mn 2p.

Fig. 6. (a) Photocatalytic water oxidation activity results of BFO, BFO-1, BFO-2, BFO-3 and BFO-4; (b) Time course of water oxidation activity test for BFO and BFO-2. (Reaction conditions: 0.1 g photocatalyst + 0.04 M Na2S2O8 + 150 mL H2O under visible light irradiation ≥ 420 nm at pH~13.5). PL studies of BFO and BFO-2: (c) PLE spectra for BFO using 290 nm excitation wavelength; (d) PL spectrum for BFO and BFO-2.

Fig. 7. (a) Free energy diagram for BFO; (b) BFO-2 with Mn as the metal active site; (c) BFO-2 with Fe as metal active site.

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Intrinsic photocatalytic water oxidation activity of Mn-doped ferroelectric BiFeO₃

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