Visible Light-Induced Photocatalysis: Self-Fenton Degradation of p-ClPhOH Over Graphitic Carbon Nitride by a Polyethylenimine Bifunctional Catalyst

Yuan Bai, Shuangjun Li, Bolin Yin, Jinpeng Zhao, Hexing Li

Transactions of Tianjin University ›› 2024, Vol. 30 ›› Issue (2) : 130-139.

Transactions of Tianjin University ›› 2024, Vol. 30 ›› Issue (2) : 130-139. DOI: 10.1007/s12209-024-00386-1
Research Article

Visible Light-Induced Photocatalysis: Self-Fenton Degradation of p-ClPhOH Over Graphitic Carbon Nitride by a Polyethylenimine Bifunctional Catalyst

Author information +
History +

Abstract

Deep degradation of organic pollutants by sunlight-induced coupled photocatalytic and Fenton (photo-Fenton) reactions is of immense importance for water purification. In this work, we report a novel bifunctional catalyst (Fe-PEI-CN) by codoping graphitic carbon nitride (CN) with polyethyleneimine ethoxylated (PEI) and Fe species, which demonstrated high activity during p-chlorophenol (p-ClPhOH) degradation via H2O2 from the photocatalytic process. The relationship between the catalytic efficiency and the structure was explored using different characterization methods. The Fe modification of CN was achieved through Fe–N coordination, which ensured high dispersion of Fe species and strong stability against leaching during liquid-phase reactions. The Fe modification initiated the Fenton reaction by activating H2O2 into ·OH radicals for deep degradation of p-ClPhOH. In addition, it effectively promoted light absorption and photoelectron–hole (e–h+) separation, corresponding to improved photocatalytic activity. On the other hand, PEI could significantly improve the ability of CN to generate H2O2 through visible light photocatalysis. The maximum H2O2 yield reached up to 102.6 μmol/L, which was 22 times higher than that of primitive CN. The cooperation of photocatalysis and the self-Fenton reaction has led to high-activity mineralizing organic pollutants with strong durability, indicating good potential for practical application in wastewater treatment.

Keywords

Fe-PEI-CN bifunctional catalyst / Photo-Fenton / p-chlorophenol (p-ClPhOH) degradation / Synergetic effect

Cite this article

Download citation ▾
Yuan Bai, Shuangjun Li, Bolin Yin, Jinpeng Zhao, Hexing Li. Visible Light-Induced Photocatalysis: Self-Fenton Degradation of p-ClPhOH Over Graphitic Carbon Nitride by a Polyethylenimine Bifunctional Catalyst. Transactions of Tianjin University, 2024, 30(2): 130‒139 https://doi.org/10.1007/s12209-024-00386-1

References

[1.]
Saravanakumar K, Yun K, Maheskumar V, et al.. Construction of novel In2S3/Ti3C2 MXene quantum dots/SmFeO3 Z-scheme heterojunctions for efficient photocatalytic removal of sulfamethoxazole and 4-chlorophenol: degradation pathways and mechanism insights. Chem Eng J, 2023, 451: 138933,
CrossRef Google scholar
[2.]
Liu X, Mo J, Wu W, et al.. Triboelectric pulsed direct-current enhanced radical generation for efficient degradation of organic pollutants in wastewater. Appl Catal B Environ, 2022, 312: 121422,
CrossRef Google scholar
[3.]
Liu JJ, Sun SN, Liu J, et al.. Achieving high-efficient photoelectrocatalytic degradation of 4-chlorophenol via functional reformation of titanium-oxo clusters. J Am Chem Soc, 2023, 145(11): 6112-6122,
CrossRef Google scholar
[4.]
Abazari R, Esrafili L, Morsali A, et al.. PMo12@UiO-67 nanocomposite as a novel non-leaching catalyst with enhanced performance durability for sulfur removal from liquid fuels with exceptionally diluted oxidant. Appl Catal B Environ, 2021, 283: 119582,
CrossRef Google scholar
[5.]
Eryılmaz C, Genç A. Review of treatment technologies for the removal of phenol from wastewaters. J Water Chem Technol, 2021, 43(2): 145-154,
CrossRef Google scholar
[6.]
Matos J, Garcia A, Cordero T, et al.. Eco-friendly TiO2–AC photocatalyst for the selective photooxidation of 4-chlorophenol. Catal Lett, 2009, 130(3): 568-574,
CrossRef Google scholar
[7.]
Ling C, Liu X, Li H, et al.. Atomic-layered Cu5 nanoclusters on FeS2 with dual catalytic sites for efficient and selective H2O2 activation. Angew Chem Int Ed Engl, 2022, 61(21): e202200670,
CrossRef Google scholar
[8.]
Aioub M, Panikkanvalappil SR, El-Sayed MA. Platinum-coated gold nanorods: efficient reactive oxygen scavengers that prevent oxidative damage toward healthy, untreated cells during plasmonic photothermal therapy. ACS Nano, 2017, 11(1): 579-586,
CrossRef Google scholar
[9.]
Charkoudian LK, Pham DM, Franz KJ. A pro-chelator triggered by hydrogen peroxide inhibits iron-promoted hydroxyl radical formation. J Am Chem Soc, 2006, 128(38): 12424-12425,
CrossRef Google scholar
[10.]
Xie Y, Chen L, Zhang X, et al.. Photosynergetic bimetallic Fe-Cu codoped melem polymer for boosting Fenton-like catalytic performance: insights into the enhancement mechanism. Appl Surf Sci, 2023, 612: 155899,
CrossRef Google scholar
[11.]
Du C, Zhang Y, Zhang Z, et al.. Fe-based metal organic frameworks (Fe-MOFs) for organic pollutants removal via photo-Fenton: a review. Chem Eng J, 2022, 431: 133932,
CrossRef Google scholar
[12.]
Wang F, Xu J, Wang Z, et al.. Unprecedentedly efficient mineralization performance of photocatalysis-self-Fenton system towards organic pollutants over oxygen-doped porous g-C3N4 nanosheets. Appl Catal B Environ, 2022, 312: 121438,
CrossRef Google scholar
[13.]
Zhu L, Ji J, Liu J, et al.. Designing 3D-MoS2 sponge as excellent cocatalysts in advanced oxidation processes for pollutant control. Angew Chem Int Ed Engl, 2020, 59(33): 13968-13976,
CrossRef Google scholar
[14.]
Yang XJ, Xu XM, Xu J, et al.. Iron oxychloride (FeOCl):an efficient Fenton-like catalyst for producing hydroxyl radicals in degradation of organic contaminants. J Am Chem Soc, 2013, 135(43): 16058-16061,
CrossRef Google scholar
[15.]
Xie Y, Li Y, Huang Z, et al.. Two types of cooperative nitrogen vacancies in polymeric carbon nitride for efficient solar-driven H2O2 evolution. Appl Catal B Environ, 2020, 265: 118581,
CrossRef Google scholar
[16.]
Rizi NS, Shahzeydi A, Ghiaci M, et al.. Photocatalytic degradation of cationic and anionic organic pollutants in water via Fe-g-C3N4/CF as a macroscopic photo-Fenton catalyst under visible light irradiation. J Environ Chem Eng, 2020, 8: 104219,
CrossRef Google scholar
[17.]
Sun S, Hu Y, Xu M, et al.. Photo-Fenton degradation of carbamazepine and ibuprofen by iron-based metal-organic framework under alkaline condition. J Hazard Mater, 2022, 424: 127698,
CrossRef Google scholar
[18.]
Wang J, Wang J, Zuo S, et al.. Cooperative coupling of photocatalytic production of H2O2 and oxidation of organic pollutants over gadolinium ion doped WO3 nanocomposite. Chinese Chem Lett, 2023, 34(9): 108157,
CrossRef Google scholar
[19.]
Li L, Sun Z, Cai C, et al.. 3D rectangular WO3 hybridized by PrFeO3 nanoparticles with efficient dual charge transfer for enhanced photo-Fenton-like activity. Ceram Int, 2023, 49(16): 26683-26693,
CrossRef Google scholar
[20.]
Li Y, Ouyang S, Xu H, et al.. Constructing solid-gas-interfacial Fenton reaction over alkalinized-C3N4 photocatalyst to achieve apparent quantum yield of 49% at 420 nm. J Am Chem Soc, 2016, 138(40): 13289-13297,
CrossRef Google scholar
[21.]
Chu Y, Zheng X, Fan J. Preparation of sodium and boron Co-doped graphitic carbon nitride for the enhanced production of H2O2 via two-electron oxygen reduction and the degradation of 2, 4-DCP via photocatalytic oxidation coupled with Fenton oxidation. Chem Eng J, 2022, 431: 134020,
CrossRef Google scholar
[22.]
Zeng X, Liu Y, Xia Y, et al.. Cooperatively modulating reactive oxygen species generation and bacteria-photocatalyst contact over graphitic carbon nitride by polyethylenimine for rapid water disinfection. Appl Catal B Environ, 2020, 274: 119095,
CrossRef Google scholar
[23.]
Chen F, Liu LL, Wu JH, et al.. Single-atom iron anchored tubular g-C3N4 catalysts for ultrafast fenton-like reaction: roles of high-valency iron-oxo species and organic radicals. Adv Mater, 2022, 34(31): 2202891,
CrossRef Google scholar
[24.]
Zeng X, Liu Y, Kang Y, et al.. Simultaneously tuning charge separation and oxygen reduction pathway on graphitic carbon nitride by polyethylenimine for boosted photocatalytic hydrogen peroxide production. ACS Catal, 2020, 10(6): 3697-3706,
CrossRef Google scholar
[25.]
Sanati S, Rezvani Z. G-C3N4 nanosheet@CoAl-layered double hydroxide composites for electrochemical energy storage in supercapacitors. Chem Eng J, 2019, 362(15): 743-757,
CrossRef Google scholar
[26.]
Li Y, Zhang M, Chen B, et al.. An ultrafast carrier dynamics system from oxygen vacancies modified SnO2 QDs and Zn2SnO4 heterojunction for deeply photocatalytic oxidation of NO. J Mater Sci Technol, 2023, 165(1): 85-93,
CrossRef Google scholar
[27.]
Li Y, Chen B, Ouyang P, et al.. Engineering ZnSn(OH)6 with ternary active sites-directed hydroxyl vacancies for robust deep C6H6 photo-oxidation: experiment and DFT calculations. Chem Eng J, 2023, 451: 138695,
CrossRef Google scholar
[28.]
Zhao X, Fan Y, Zhang W, et al.. Nanoengineering construction of Cu2O nanowire arrays encapsulated with g-C3N4 as 3D spatial reticulation all-solid-state direct Z-scheme photocatalysts for photocatalytic reduction of carbon dioxide. ACS Catal, 2020, 10(11): 6367-6376,
CrossRef Google scholar
[29.]
Wang Q, Ma J, Li G, et al.. Unsaturated iron ion-based coordination polymer for highly efficient photocatalytic hydrogen evolution with simultaneous real wastewater degradation: mechanistic insight into multifunctional Fe–N sites. J Mater Chem A, 2021, 9(47): 27041-27048,
CrossRef Google scholar
[30.]
Wan X, Liu Q, Liu J, et al.. Iron atom-cluster interactions increase activity and improve durability in Fe-N-C fuel cells. Nat Commun, 2022, 13(1): 2963,
CrossRef Google scholar
[31.]
He T, Chen Y, Liu Q, et al.. Theory-guided regulation of FeN4 spin state by neighboring Cu atoms for enhanced oxygen reduction electrocatalysis in flexible metal-air batteries. Angew Chem Int Ed Engl, 2022, 61(27): e202201007,
CrossRef Google scholar
[32.]
Su H, Chen L, Chen Y, et al.. Single atoms of iron on MoS2 nanosheets for N2 electroreduction into ammonia. Angew Chem Int Ed Engl, 2020, 59(46): 20411-20416,
CrossRef Google scholar
[33.]
Ji S, Chen Y, Fu Q, et al.. Confined pyrolysis within metal-organic frameworks to form uniform Ru3 clusters for efficient oxidation of alcohols. J Am Chem Soc, 2017, 139(29): 9795-9798,
CrossRef Google scholar
[34.]
Gu J, Jian M, Huang L, et al.. Synergizing metal-support interactions and spatial confinement boosts dynamics of atomic nickel for hydrogenations. Nat Nanotechnol, 2021, 16(10): 1141-1149,
CrossRef Google scholar
[35.]
Chen X, Kondo Y, Li S, et al.. Visible-light-driven hydrogen peroxide production from water and dioxygen by perylenetetracarboxylic diimide modified titanium-based metal–organic frameworks. J Mater Chem A, 2021, 9(46): 26371-26380,
CrossRef Google scholar
[36.]
Yang Q, Li S, Liang R, et al.. Microwave assisted synthesis of PQ-GDY@NH2-UIO-66(Zr) for improved photocatalytic removal of NO x under visible light. J Environ Sci (China), 2023, 134: 126-137,
CrossRef Google scholar
[37.]
Li S, Shang H, Tao Y, et al.. Hydroxyl radical-mediated efficient photoelectrocatalytic NO oxidation with simultaneous nitrate storage using A flow photoanode reactor. Angew Chem Int Ed Engl, 2023, 62(28): e202305538,
CrossRef Google scholar
[38.]
Li X, Shi H, Yan X, et al.. Rational construction of direct Z-scheme doped perovskite/palygorskite nanocatalyst for photo-SCR removal of NO: insight into the effect of Ce incorporation. J Catal, 2019, 369: 190-200,
CrossRef Google scholar
[39.]
Li X, Shi H, Yan X, et al.. Palygorskite immobilized direct Z-scheme nitrogen-doped carbon quantum dots/PrFeO3 for photo-SCR removal of NO x. ACS Sustainable Chem Eng, 2018, 6(8): 10616-10627,
CrossRef Google scholar
[40.]
Giannakopoulou T, Papailias I, Todorova N, et al.. Tailoring the energy band gap and edges’ potentials of g-C3N4/TiO2 composite photocatalysts for NO x removal. Chem Eng J, 2017, 310: 571-580,
CrossRef Google scholar
[41.]
Xie P, Ding J, Yao Z, et al.. Oxo dicopper anchored on carbon nitride for selective oxidation of methane. Nat Commun, 2022, 13(1): 1375,
CrossRef Google scholar
[42.]
Dai W, Zhang S, Shang H, et al.. Breaking the selectivity barrier: reactive oxygen species control in photocatalytic nitric oxide conversion. Adv Funct Mater, 2024, 34(4): 2309426,
CrossRef Google scholar
[43.]
Chen Y, Li Y, Luo N, et al.. Kinetic comparison of photocatalysis with H2O2-free photo-Fenton process on BiVO4 and the effective antibiotic degradation. Chem Eng J, 2022, 429(1): 132577,
CrossRef Google scholar
[44.]
Chen F, Wu XL, Shi C, et al.. Molecular engineering toward pyrrolic N-rich M-N4 (M = Cr, Mn, Fe Co, Cu) single-atom sites for enhanced heterogeneous Fenton-like reaction. Adv Funct Mater, 2021, 31(13): 2007877,
CrossRef Google scholar

Accesses

Citations

Detail

Sections
Recommended

/