High visible light photocatalytic activities obtained by integrating g-C3N4 with ferroelectric PbTiO3

doi:10.1016/j.jmst.2020.10.036

Abstract

Abstract:

Graphitic carbon nitride (g-C₃N₄) with the merits of high visible light absorption, proper electronic band structure with high conduction band edge and variable modulation, is viewed as a promising photocatalyst for practical use. To alleviate its high recombination rate of photo-excited charge carriers and maximize the photocatalytic performances, it is paramount to design highly effective transfer channels for photo-excited charge carriers. Ferroelectric materials can have the charge carriers transport in opposite directions owing to the internal spontaneous polarization, which may be suitable for constructing the heterostructure with g-C₃N₄ for efficient charge separation. Inspired by this concept, herein ferroelectric PbTiO₃, which can be the visible-light absorber, is coupled with g-C₃N₄ to construct PbTiO₃/g-C₃N₄ heterostructure with close contact via Pb-N bond by the facile post thermal treatment. The optimized PbTiO₃/g-C₃N₄ heterostructure exhibited excellent photocatalytic and photoelectrochemical activities under visible light irradiation. Moreover, the simultaneous application of ultrasound-induced mechanical waves can further improve its photocatalytic activities through reinforcing the built-in piezoelectric field. This work proposes a widely applicable strategy for the fabrication of high-performance ferroelectric based photocatalysts and also provides some new ideas for developing the understanding of ferroelectric photocatalysis.

Key words: Photocatalysis, Ferroelectric, Piezoelectric, Carbon nitride, Lead titanate

Tingting Xu, Ping Niu, Shulan Wang, Li Li. High visible light photocatalytic activities obtained by integrating g-C₃N₄ with ferroelectric PbTiO₃[J]. J. Mater. Sci. Technol., 2021, 74: 128-135.

Figures/Tables 6

Fig. 1. (a) The Scheme of the synthesis process and photochemical characterization of the composite; (b) XRD patterns of PTO, CN and PTO/CN; SEM images of (c) PTO and (d) CN; (e) SEM image and EDX elemental mapping of PTO/CN; (f) Bright field TEM image of PTO/CN with selected area electron diffraction (SAED) pattern shown in the inset; (g) TEM image of PTO/CN; (h) High resolution TEM image with the lattice fringes of PTO/CN.

Fig. 2. (a) UV-vis absorption spectra and (b) valence band spectra of PTO, CN and PTO/CN; (c) Schematic of the band structure and possible charge carrier transfer within PTO/CN composite; (d) PL spectra of CN and PTO/CN; (e) Electrochemical impedance spectroscopic spectra and (f) nitrogen adsorption-desorption isotherms of CN, PTO and PTO/CN.

Table 1 The surface area and pore structure of PTO, CN, PTO/CN.

Samples	S_BET (m² g^-1)	S_micro^a) (m² g^-1)	S_meso ^b) (m² g^-1)	V_pore ^c) (cm³ g^-1)	V_micro ^d) (cm³ g^-1)	V_meso ^e) (cm³ g^-1)
PTO	2.8148	0.6268	2.1880	0.0239	0.0011	0.0232
CN	17.7531	2.0565	15.6966	0.1273	0.0010	0.1259
PTO/CN	26.2042	6.1020	20.1023	0.2357	0.0031	0.2324

Fig. 3. High-resolution XPS spectra of (a) Pb 4f (PTO); (b) Ti 2p (PTO); (c) N 1s (CN); (d) Pb 4f (PTO/CN); (e) Ti 2p (PTO/CN); and (f) N 1s (PTO/CN).

Fig. 4. Evaluation of visible light activities of the samples. (a) Photocatalytic RhB degradation activities of CN, PTO and PTO/CN; (b) Photocatalytic hydrogen production of CN, PTO and PTO/CN loaded with 2% Pt as co-catalyst; (c) Photocurrent response of CN, PTO and PTO/CN during repeated measurements; (d) Photocatalytic RhB degradation comparison of PTO/CN under ultrasonic and stir condition; Schematic band structure alignment of PTO/CN (e) without and (f) with ultrasonic treatment.

Table 2 The photocatalytic activity of PTO/CN with different molar ratios of PbTiO3 to g-C3N4 for RhB degradation under visible light irradiation.

Photocatalyst	Vis (Stir) Slope (min^-1)	Vis (Ultrasonic) Slope (min^-1)	Ultrasonic/Stir
g-C₃N₄ ^a	0.0493	0.0552	112 %
PbTiO₃ ^b	0.0027	0.0038	141 %
PbTiO₃ 520-2 h	0.0035	0.0068	194 %
PbTiO₃/(g-C₃N₄+PbTiO₃) = 2 % 520-2 h	0.0722	0.0794	110 %
PbTiO₃/(g-C₃N₄+PbTiO₃) = 4 % 520-2 h	0.0863	0.1036	120 %
PbTiO₃/(g-C₃N₄+PbTiO₃) = 6 % 520-2 h	0.0981	0.1177	120 %
PbTiO₃/(g-C₃N₄+PbTiO₃) = 8 % 520-2 h	0.1044	0.1357	130 %
PbTiO3/(g-C3N4+PbTiO3) = 10 % 520-2 h	0.0672	0.0874	130 %
PbTiO3/(g-C3N4+PbTiO3) = 50 % 520-2 h	0.0362	0.0402	111 %
g-C₃N₄ 520-2 h	0.0669	0.0704	105 %
PbTiO₃/(g-C₃N₄+PbTiO₃) = 8 % 400-2 h	0.0463	0.0556	120 %
PbTiO₃/(g-C₃N₄+PbTiO₃) = 8 % 450-2 h	0.0484	0.0629	130 %
PbTiO₃/(g-C₃N₄+PbTiO₃) = 8 % 550-2 h	0.0669	0.0837	125 %

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High visible light photocatalytic activities obtained by integrating g-C₃N₄ with ferroelectric PbTiO₃

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