Built in electric field boosted photocatalytic performance in a ferroelectric layered material SrBi2Ta2O9 with oriented facets: Charge separation and mechanism insights

doi:10.1016/j.jmst.2022.01.023

Abstract

Abstract:

Antibiotics have received increasing attention due to their potential adverse effects on aquatic life and human health. How to efficiently degrade them into harmless substances is a challenging subject. Ferroelectric materials with a built-in electric field can offer a strong separation ability for the photoinduced-charge pairs and are now found to be used as photocatalysts. Herein, a series of different morphologies of SrBi₂Ta₂O₉ ferroelectric photocatalysts with high antibiotic degradation efficiency have been successfully synthesized through a molten salt method. With the addition of KCl, SrBi₂Ta₂O₉ (SBTO 3) with exposed (001) facets shows the most excellent photocatalytic activity for decomposing tetracycline (TC) and ciprofloxacin (CIP) under visible light illumination (λ > 420 nm). The rate constants of SBTO 3 for TC and CIP degradation are 1.38 × 10^-1 and 4.54 × 10^-2 min^-1, which are 18 and 138 times that of the unmodified sample, respectively. The enhancement of photocatalytic performance is mainly attributed to the spontaneous polarization electric field along the [001] direction which provides a strong driven force for the separation of photoinduced charges. The KPFM results also confirm that the superior photocatalytic activity is consistent with the big large surface potential changes before and after light irradiation. The possible degradation pathways and intermediates of TC and CIP were well analyzed by DFT calculation and LC-MS. The results highlight that morphology control of the ferroelectric materials exhibits enhanced photocatalytic performance for the degradation of the antibiotic.

Key words: SrBi₂Ta₂O₉, Morphology, Ferroelectric, Photocatalysis, Antibiotics, Built-in electric field

Biru Liao, Xiaomin Liao, Huiyuan Xie, Yuanchu Qin, Yi Zhu, Yang Yu, Sen Hou, Yuanming Zhang, Xiaoyun Fan. Built in electric field boosted photocatalytic performance in a ferroelectric layered material SrBi₂Ta₂O₉ with oriented facets: Charge separation and mechanism insights[J]. J. Mater. Sci. Technol., 2022, 123: 222-233.

Figures/Tables 13

Fig. 1. Synthesis process of SBTO synthesized by the molten salt method.

Fig. 2. Structural analysis of series of SBTO samples. (a) XRD patterns; (b) Raman spectra; (c) FTIR spectra; (d) crystal structure; (e) UV-vis DRS patterns with the enlarged view of SBTO 2-SBTO 7 in the inset figure; (f) band structures.

Fig. 3. SEM images of (a) SBTO 3 and (e) SBTO 4; (b) TEM image, (c) HRTEM image, and (d) SAED pattern of SBTO 3; (f) TEM image and (g) HRTEM image of SBTO 4; (h) schematic illustration of the crystal orientation of the SBTO nanocube.

Fig. 4. Photocatalytic degradation efficiency of (a) TC and (c) CIP; rate constants of (b) TC and (d) CIP on series of SBTO samples under visible light irradiation.

Fig. 5. (a) Transient photocurrent responses; (b) EIS Nyquist plots; (c) PL spectra; and (d) TRPL decay spectra of SBTO 1, SBTO 3, and SBTO 4.

Table 1. Photocatalytic performance in TC and CIP compared in different reported Aurivillius-type layered photocatalysts.

Photocatalysts	Antibiotics and concentration	Dosage(g/L)	Reaction conditions	Degradation rate (%)	Rate constants	Refs.
SBTO 3	TC, 10 ppm	0.1	λ > 420 nm	99, 20 min	0.138 min^-1	This work
BFTO/2% Ag/10% UCN	TC, 20 ppm	0.1	λ > 420 nm	86, 20 min	0.0465 min^-1	[44]
BON-S	TC, 10 ppm	0.1	UV- vis	97.75, 25 min	/	[18]
0.4C-BMO	TC, 10 ppm	0.04	Visible light	99.8, 120 min	2.16032 h^-1	[45]
SBNCN-3	TC, 10 ppm	0.1	λ > 420 nm	76, 240 min	0.0095 min^-1	[46]
Bi₂NbO₅F	TC, 30 ppm	0.05	UV-vis	80.73, 120 min	0.0227 min^-1	[14]
Na-Bi₂MoO₆	TC, 10 ppm	0.1	Visible light	98, 300 min	0.42302 h^-1	[47]
SBTO 3	CIP, 10 ppm	0.1	λ > 420 nm	95, 60 min	0.0454 min^-1	This work
NCQDs/BOC	CIP, 10 ppm	0.05	Visible light	91.9, 120 min	-	[48]
1.0Bi-Ta	CIP, 20 ppm	0.04	λ > 400 nm	81.1, 150 min	0.0105 min^-1	[49]
BCN-200/rGO	CIP, 10 ppm	0.06	UV-vis	90, 110 min	0.014 min^-1	[50]
PbBiO₂Br-0.10	CIP, 10 ppm	0.03	λ > 400 nm	86.7, 150 min	0.01381 min^-1	[51]
5wt% CNT/PbBiO₂Br	CIP, 10 ppm	0.03	λ > 400 nm	88, 150 min	0.01652 min^-1	[52]
10%Bi₂MoO₆/CuBi₂O₄	CIP, 10 ppm	0.1	Visible light	90.2, 180 min	0.01263 min^-1	[53]

Fig. 6. AFM, KPFM, and surface potential change for SBTO. (a1) Topographic image, surface potential (a2) in dark and (a3) under irradiation of SBTO 1; (a4) differential image obtained by subtracting panel from panel (a3); (a5) the surface potential distribution on the selected line for the sample; Corresponding SBTO 3 (b1-b5); SBTO 4 (c1-c5).

Table 2. Summary of ΔCPD, degradation efficiency, and degradation rate constant in SrBi2Ta2O9 series samples.

Material		ΔCPD (mV)	Degradation efficiency		Degradation rate constant (min^-1)
Material		ΔCPD (mV)	TC(20 min)	CIP(60 min)	TC	CIP
Amorphous	SBTO 1	0.6	21%	2%	7.64 × 10^-3	3.29 × 10^-4
Nanocube	SBTO 2	-	93%	71%	8.58 × 10^-2	1.76 × 10^-2
Nanocube	SBTO 3	146.1	99%	96%	1.38 × 10^-1	4.54 × 10^-2
Nanoplate	SBTO 4	38.4	75%	37%	5.15 × 10^-2	6.23 × 10^-3
	SBTO 5	-	86%	51%	6.55 × 10^-2	9.28 × 10^-3
	SBTO 6	-	57%	55%	3.03 × 10^-2	1.22 × 10^-2
	SBTO 7	-	57%	49%	2.57 × 10^-2	9.53 × 10^-3

Fig. 7. ESR spin-trapping signals of DMPO-·OH and DMPO-·O2- for (a), (b) SBTO 3 and (c), (d) SBTO 4; photodegradation efficiency and rate constants of (e) and (f) TC, (g) and (h) CIP with different scavengers ((NH4)2C2O4→h+, TBA→·OH, p-BQ→·O2-) under visible light irradiation for SBTO 3.

Fig. 8. (a) and (b) Schematic diagrams for the possible photocatalytic mechanism over SrBi2Ta2O9 with ferroelectric polarization field under visible light irradiation; (c) top views of (001) and (115) surface terminations of SBTO.

Fig. 9. Proposed photocatalytic degradation pathways of TC in SBTO 3, the red circles represent the main attacked sites.

Fig. 10. Proposed photocatalytic degradation pathways of CIP in SBTO 3, the red circles represent the main attacked sites.

Fig. 11. Fathead minnow LC50 of (a) TC and (c) CIP degradation intermediates and bioconcentration factor of (b) TC degradation intermediates and (d) CIP degradation intermediates.

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Built in electric field boosted photocatalytic performance in a ferroelectric layered material SrBi₂Ta₂O₉ with oriented facets: Charge separation and mechanism insights

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