Insight into the Photodegradation Mechanism of Bisphenol-A by Oxygen Doped Mesoporous Carbon Nitride Under Visible Light Irradiation and DFT Calculations

Overview

Journal RSC Adv

Publisher Royal Society of Chemistry

Specialty Chemistry

Date 2022 Apr 15

PMID 35424996

Authors

Fatimah Bukola Shittu

Anwar Iqbal

Mohammad Norazmi Ahmad

Muhammad Rahimi Yusop

Mohamad Nasir Mohamad Ibrahim

Sumiyyah Sabar

Lee D Wilson

Dede Heri Yuli Yanto

Affiliations

Soon will be listed here.

Abstract

Oxygen doped mesoporous carbon nitride (O-MCN) was successfully synthesized through one-step thermal polymerization of urea and glucose utilizing nanodisc silica (NDS) from rice husk ash as a hard template. The CO gas, NH and water vapor produced during the thermal process reshaped the morphology and textural properties of the of O-MCN compared to pristine mesoporous carbon nitride (MCN). Highest bisphenol A (BPA) removal achieved under visible light irradiation was 97%, with 60% mineralization ([BPA] = 10 mg L: catalyst dosage = 40 mg L; pH = 10; 180 min). In addition to mesoporosity, the sub-gap impurity states created from the oxygen doping reduced recombination rate of photogenerated carriers. Holes (h) and superoxide (O˙) were identified as the predominant active species responsible for the photodegradation process. The photodegradation route was proposed based on the intermediates detected by LC-time-of-flight/mass spectrometry (LC/TOF-MS). The Density of States (DOS) showed that oxygen doping resulted in a higher photoactivity due to the stronger localization and delocalization of the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO). The adsorption pathway of the BPA on the O-MCN and MCN was successfully predicted using the DFT calculations, namely molecular electrostatic potential (MEP), global and local descriptors.

References

He F, Chen G, Yu Y, Zhou Y, Zheng Y, Hao S . The sulfur-bubble template-mediated synthesis of uniform porous g-C3N4 with superior photocatalytic performance. Chem Commun (Camb). 2014; 51(2):425-7. DOI: 10.1039/c4cc07106a. View

Mohammad Alwi M, Normaya E, Ismail H, Iqbal A, Mat Piah B, Samah M . Two-Dimensional Infrared Correlation Spectroscopy, Conductor-like Screening Model for Real Solvents, and Density Functional Theory Study on the Adsorption Mechanism of Polyvinylpolypyrrolidone for Effective Phenol Removal in an Aqueous Medium. ACS Omega. 2021; 6(39):25179-25192. PMC: 8495713. DOI: 10.1021/acsomega.1c02699. View

Sahu R, Shih Y, Chen W . New insights of metal free 2D graphitic carbon nitride for photocatalytic degradation of bisphenol A. J Hazard Mater. 2020; 402:123509. DOI: 10.1016/j.jhazmat.2020.123509. View

Wang X, Sun M, Guo Y, Hu J, Zhu M . Three dimensional Pt island-on-Au architectures coupled with graphite carbon nitride nanosheets for effective photo-accelerated methanol electro-oxidation. J Colloid Interface Sci. 2019; 558:38-46. DOI: 10.1016/j.jcis.2019.09.085. View

Li Y, Wang S, Wu J, Wang Q, Ma C, Jiang D . Metal-free porous phosphorus-doped g-CN photocatalyst achieving efficient synthesis of benzoin. RSC Adv. 2022; 11(21):12682-12686. PMC: 8696882. DOI: 10.1039/d1ra00701g. View

Poerschmann J, Trommler U, Gorecki T . Aromatic intermediate formation during oxidative degradation of Bisphenol A by homogeneous sub-stoichiometric Fenton reaction. Chemosphere. 2010; 79(10):975-86. DOI: 10.1016/j.chemosphere.2010.03.030. View

Li S, Hu C, Peng Y, Chen Z . One-step scalable synthesis of honeycomb-like g-CN with broad sub-bandgap absorption for superior visible-light-driven photocatalytic hydrogen evolution. RSC Adv. 2022; 9(56):32674-32682. PMC: 9073371. DOI: 10.1039/c9ra07068k. View

Tan K, Iqbal A, Adam F, Abu Bakar N, Ahmad M, Yusop R . Influence of Mg/CTAB ratio on the structural, physicochemical properties and catalytic activity of amorphous mesoporous magnesium silicate catalysts. RSC Adv. 2022; 9(66):38760-38771. PMC: 9075996. DOI: 10.1039/c9ra08024d. View

Zhu Y, Yue M, Natarajan V, Kong L, Ma L, Zhang Y . Efficient activation of persulfate by FeO@β-cyclodextrin nanocomposite for removal of bisphenol A. RSC Adv. 2022; 8(27):14879-14887. PMC: 9079925. DOI: 10.1039/c8ra01696h. View

10.

Fu J, Zhu B, Jiang C, Cheng B, You W, Yu J . Hierarchical Porous O-Doped g-C N with Enhanced Photocatalytic CO Reduction Activity. Small. 2017; 13(15). DOI: 10.1002/smll.201603938. View

11.

Zheng X, Zhang Q, Chen T, Wu Y, Hao J, Tan C . A novel synthetic carbon and oxygen doped stalactite-like g-CN for broad-spectrum-driven indometacin degradation. J Hazard Mater. 2020; 386:121961. DOI: 10.1016/j.jhazmat.2019.121961. View

12.

Zhang L, Jin Z, Lu H, Lin T, Ruan S, Zhao X . Improving the Visible-Light Photocatalytic Activity of Graphitic Carbon Nitride by Carbon Black Doping. ACS Omega. 2019; 3(11):15009-15017. PMC: 6643869. DOI: 10.1021/acsomega.8b01933. View

13.

Ismail H, Ahmad M, Normaya E . A highly sensitive and selective thiosemicarbazone chemosensor for detection of Co in aqueous environments using RSM and TD/DFT approaches. Sci Rep. 2021; 11(1):20963. PMC: 8545950. DOI: 10.1038/s41598-021-00264-z. View

14.

Sharma J, Mishra I, Kumar V . Mechanistic study of photo-oxidation of Bisphenol-A (BPA) with hydrogen peroxide (H2O2) and sodium persulfate (SPS). J Environ Manage. 2015; 166:12-22. DOI: 10.1016/j.jenvman.2015.09.043. View

15.

Ahmad M, Karim N, Normaya E, Mat Piah B, Iqbal A, Bulat K . Artocarpus altilis extracts as a food-borne pathogen and oxidation inhibitors: RSM, COSMO RS, and molecular docking approaches. Sci Rep. 2020; 10(1):9566. PMC: 7293230. DOI: 10.1038/s41598-020-66488-7. View

16.

Jourshabani M, Shariatinia Z, Badiei A . Controllable Synthesis of Mesoporous Sulfur-Doped Carbon Nitride Materials for Enhanced Visible Light Photocatalytic Degradation. Langmuir. 2017; 33(28):7062-7078. DOI: 10.1021/acs.langmuir.7b01767. View

17.

Lauretta R, Sansone A, Sansone M, Romanelli F, Appetecchia M . Endocrine Disrupting Chemicals: Effects on Endocrine Glands. Front Endocrinol (Lausanne). 2019; 10:178. PMC: 6448049. DOI: 10.3389/fendo.2019.00178. View

18.

Li J, Shen B, Hong Z, Lin B, Gao B, Chen Y . A facile approach to synthesize novel oxygen-doped g-C3N4 with superior visible-light photoreactivity. Chem Commun (Camb). 2012; 48(98):12017-9. DOI: 10.1039/c2cc35862j. View

19.

Sunasee S, Wong K, Lee G, Pichiah S, Ibrahim S, Park C . Titanium dioxide-based sonophotocatalytic mineralization of bisphenol A and its intermediates. Environ Sci Pollut Res Int. 2017; 24(18):15488-15499. DOI: 10.1007/s11356-017-9124-0. View

20.

He J, Yang J, Jiang F, Liu P, Zhu M . Photo-assisted peroxymonosulfate activation via 2D/2D heterostructure of TiC/g-CN for degradation of diclofenac. Chemosphere. 2020; 258:127339. DOI: 10.1016/j.chemosphere.2020.127339. View