Two-dimensional g-C3N4 Compositing with Ag-TiO2 as Deactivation Resistant Photocatalyst for Degradation of Gaseous Acetaldehyde

doi:10.15541/jim20220123

Abstract

Abstract:

The photocatalysts deactivation is one of the major issues, which lowers the usefulness of photocatalytic oxidation technology for the removal of low content volatile organic compounds (VOCs). Here, we carried out a series of experiments to demonstrate that the photocatalysts stability could be significantly improved via coupling the oxide base semiconductors, i.e., TiO₂ with 2D materials such as graphitic carbon nitride (g-C₃N₄). Initially, when Ag modified TiO₂ (AT) was used for the gaseous acetaldehyde degradation, a robust deactivation was observed within 60 min. The AT catalyst completely lost its activity when the reaction time was extended to 400 min. On the contrary, the g-C₃N₄ modified AT (CAT) showed superior photocatalytic performance and improved stability (600 min). The in-situ FT-IR, PL, and photocurrent studies suggested that the accumulation of reaction intermediates in the case of AT fundamentally caused the deactivation. However, the g-C₃N₄ provided excessive adsorption sites for the reaction by-products which improved the stability. Additionally, the PL and ESR studies suggested that the existence of g-C₃N₄ improved the charge separation and production of reactive oxygen species, which facilitated the photodegradation of acetaldehyde and ultimate reaction products. This study realizes the usefulness of 2D materials for developing stable and visible light active photocatalysts for applications in sustainable VOC abatement technology.

Key words: photocatalysis, titanium dioxide, g-C₃N₄, deactivation-resistant, in-situ diffuse reflectance infrared Fourier transform spectroscopy

CLC Number:

TQ174

XUE Hongyun, WANG Congyu, MAHMOOD Asad, YU Jiajun, WANG Yan, XIE Xiaofeng, SUN Jing. Two-dimensional g-C₃N₄ Compositing with Ag-TiO₂ as Deactivation Resistant Photocatalyst for Degradation of Gaseous Acetaldehyde[J]. Journal of Inorganic Materials, 2022, 37(8): 865-872.

Figures/Tables 7

Fig. 1 Activation maintained by CAT for gaseous acetaldehyde (a) Adsorption, photodegradation and CO2 generation curves of acetaldehyde gas by AT and CAT samples; (b) Photocatalytic degradation of acetaldehyde by AT sample under visible light irradiation for 400 min and CAT sample under visible light irradiation for 600 min; (c) XRD patterns of AT and CAT samples before and after degradation of acetaldehyde gas (160 min) under visible light irradiation; (d) Photocatalytic degradation of acetaldehyde by AT sample under visible light irradiation for 360 min, and cutting off acetaldehyde inlet at 180 min

Fig. 2 In-situ DRIFTS spectra of (a) AT and (b) CAT photocatalysts degrading acetaldehyde gas under visible light irradiation, and (c) photocatalytic reaction routes of acetaldehyde

Fig. 3 Photocurrent and PL plots of the photocatalytic degradation of acetaldehyde (a) Photocurrent and (c) PL plots of AT sample for the photocatalytic degradation of acetaldehyde under visible light irradiation; (b) Photocurrent and (d) PL plots of the photocatalytic degradation of acetaldehyde by CAT sample under visible light irradiation for 300 min 0, 60, 120, 180 min represent the photocatalytic reaction time of which the dotted lines of 240 and 300 min represent 1 and 2 h, respectively, when acetaldehyde was stopped but the light was kept on

Fig. 4 ESR profiles of (a, c) DMPO-•O2- and (b, d) DMPO-•OH for the photocatalytic degradation of acetaldehyde by AT(a, b) and CAT (c, d) sample Under visible light irradiation for 300 min 0, 60, 120, 180 min represent the photocatalytic reaction time, of which the dotted lines of 240 and 300 min represent 1 and 2 h, respectively, when acetaldehyde was stopped but the light was kept on

Fig. 5 Schematic of photocatalytic reaction mechanism

Table S1 Assignment of FT-IR bands observed for AT sample in the process of dark adsorption and photocatalytic degradation for acetaldehyde

Product	Wavenumber/cm^-1	Mode of vibration
1	1072	β(CH₃)
2	1128, 1166	v(C-C)
3	1315	δ(CH₃)
4	1339	δ_as(CH₃)
5	1377	v_s(COO)
6	1419	δ_s(CH₃)
7	1458, 1473	δ(CH₂)
8	1541, 1558	v_as(COO)
9	1603	v(C=C)
10	1732, 1716, 1699, 1650	v(C=O)

Table S2 Assignment of FT-IR bands observed for CAT sample in the process of dark adsorption and photocatalytic degradation for acetaldehyde

Product	Wavenumber/cm^-1	Mode of vibration
1	1050, 1100	β(CH₃)
2	1200	r(CH₂)
3	1221, 1294	v(C-O)
4	1316	δ(CH₃)
5	1339, 1371	v_s(COO)
6	1361	δ(CH)
7	1419	δ_s(CH₃)
8	1458	δ(CH₂)
9	1522, 1558,1573	v_as(COO)
10	1620	v(C=C)
11	1771, 1732, 1716, 1699, 1650	v(C=O)

References 31

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Two-dimensional g-C₃N₄ Compositing with Ag-TiO₂ as Deactivation Resistant Photocatalyst for Degradation of Gaseous Acetaldehyde

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