Persulfate-Based Advanced Oxidation Reforming of Polyethylene Terephthalate Fiber into Formate via Singlet Oxygen Activation

Luyao Zhang , Li Wang , Junliang Chen , Jinzhou Li , Peng Huang , Xinming Nie , Jianping Yang

Advanced Fiber Materials ›› 2025, Vol. 7 ›› Issue (2) : 664 -677.

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Advanced Fiber Materials ›› 2025, Vol. 7 ›› Issue (2) : 664 -677. DOI: 10.1007/s42765-025-00525-w
Research Article

Persulfate-Based Advanced Oxidation Reforming of Polyethylene Terephthalate Fiber into Formate via Singlet Oxygen Activation

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Abstract

Due to the shortage of rational waste management, plastic waste has become increasingly serious, posing a serious threat to the environment and humans. The catalytic oxidation of polyethylene terephthalate (PET) waste has been reported to reduce environmental stress and produce valuable products. However, obtaining valuable chemicals from waste plastics under mild conditions driven by specific reactive oxygen species is a great challenge. Herein, N, P-doped Mo2C@porous carbon was designed and employed in the peroxymonosulfate-based advanced oxidation reforming of PET hydrolysate. The ethylene glycol (EG) derived from PET fiber was catalytically oxidized to formate via singlet oxygen activation during the peroxymonosulfate-based advanced oxidation process. Compared with Mo2C, the N, P-doped Mo2C@porous carbon catalyst with a large specific surface area provides more active sites, which has the characteristic of high catalytic activity. It presents the tetracycline degradation efficiency of ~ 80% under a wide pH range (6.8–10.6) and, further, the formate generation rate of ~ 56.5 mmol gcat−1 in the advanced oxidation reforming process of EG in 8 h. The detection and quenching experiments on the oxygen active species comprehensively confirmed that singlet oxygen is the key reactive oxygen species during the advanced catalytic oxidation reactions. This work provided a constructive demonstration for designing advanced oxidation catalysts to catalyze the reforming of waste PET fiber plastics into valuable chemicals.

Graphical Abstract

The catalytic reforming of polyethylene terephthalate (PET) waste and proper treatment of fiber-based microplastics have emerged as critical areas of research and innovation to alleviate environmental stress and generate valuable products. This work sheds light on the efficient Mo2C@porous C catalyst design via singlet oxygen activation for persulfate-based advanced oxidation reforming of EG from PET fiber waste, providing a potential countermeasure to address plastic waste pollution and achieve carbon neutrality

Keywords

Plastic waste / PET fiber reforming / PMS activation / Singlet oxygen species / Formate / Engineering / Environmental Engineering / Chemical Sciences / Other Chemical Sciences

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Luyao Zhang, Li Wang, Junliang Chen, Jinzhou Li, Peng Huang, Xinming Nie, Jianping Yang. Persulfate-Based Advanced Oxidation Reforming of Polyethylene Terephthalate Fiber into Formate via Singlet Oxygen Activation. Advanced Fiber Materials, 2025, 7(2): 664-677 DOI:10.1007/s42765-025-00525-w

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References

[1]

ZhaoX, BoruahB, ChinKF, ĐokićM, ModakJM, SooHS. Upcycling to sustainably reuse plastics. Adv Mater, 2021, 34: 2100843.

[2]

GeyerR, JambeckJR, LawKL. Production, use, and fate of all plastics ever made. Sci Adv, 2017, 3. e1700782

[3]

QiuZT, LinSY, ChenZ, ChenAQ, ZhouYT, CaoXD, WangY, LinBL. A reusable, impurity-tolerant and noble metal-free catalyst for hydrocracking of waste polyolefins. Sci Adv, 2023, 9: eadg5332.

[4]

ChenJL, WuJ, SherrellPC, ChenJ, WangHP, ZhangWX, YangJP. How to build a microplastic-free environment: strategies for microplastics degradation and plastics recycling. Adv Sci, 2022, 9: 2103764.

[5]

ChenJL, ZhangLY, WangL, KuangM, WangSB, YangJP. Toward carbon neutrality: selective conversion of waste plastics into value-added chemicals. Matter, 2023, 6: 3322.

[6]

ZhouDW, LuoHX, ZhangFZ, WuJ, YangJP, WangHP. Efficient photocatalytic degradation of the persistent PET fiber-based microplastics over Pt nanoparticles decorated N-doped TiO2 nanoflowers. Adv Fiber Mater, 2022, 4: 1094.

[7]

WenJ, SunH, YangBW, SongE, SongY, JiangGB. Environmentally relevant concentrations of microplastic exposure cause cholestasis and bile acid metabolism dysregulation through a gut-liver loop in mice. Environ Sci Technol, 1832, 2024: 58

[8]

DuMM, XueR, YuanWF, ChengY, CuiZ, DongWL, QiuBC. Tandem integration of biological and electrochemical catalysis for efficient polyester upcycling under ambient conditions. Nano Lett, 2024, 24319768-9775.

[9]

DuMM, ZhangY, KangSL, GuoXY, MaYX, XingMY, ZhuY, ChaiY, QiuBC. Trash to treasure: photoreforming of plastic waste into commodity chemicals and hydrogen over MoS2-tipped CdS nanorods. ACS Catal, 2022, 122012823-12832.

[10]

UekertT, KasapH, ReisnerE. Photoreforming of nonrecyclable plastic waste over a carbon nitride/nickel phosphide catalyst. J Am Chem Soc, 2019, 141: 15201.

[11]

WangGH, ChenZJ, WeiW, NiBJ. Electrocatalysis-driven sustainable plastic waste upcycling. Electron, 2024, 22. e34

[12]

FanZF, HePP, BaiHY, LiuJ, LiuHJ, LiuLJ, NiuR, GongJ. Green recycling of waste poly(ethylene terephthalate) into Ni-MOF nanorod for simultaneous interfacial solar evaporation and photocatalytic degradation of organic pollutants. EcoMat, 2024, 6. e12422

[13]

XiongLQ, QiHF, ZhangSX, ZhangLL, LiuXY, WangAQ, TangJW. Highly selective transformation of biomass derivatives to valuable chemicals by single-atom photocatalyst Ni/TiO2. Adv Mater, 2023, 35: 2209646.

[14]

LiuFL, GaoXT, ShiR, GuoZX, EdmundCMT, ChenY. Concerted and selective electrooxidation of polyethylene-terephthalate-derived alcohol to glycolic acid at an industry-level current density over a Pd-Ni(OH)2 catalyst. Angew Chem Int Ed, 2023, 62. e202300094

[15]

LiuKS, GaoXT, LiuCX, ShiR, EdmundCMT, LiuFL, ChenY. Energy-saving hydrogen production by seawater splitting coupled with PET plastic upcycling. Adv Energy Mater, 2024, 2024: 2304065.

[16]

ChenJL, ZhangFZ, KuangM, WangL, WangHP, LiW, YangJP. Unveiling synergy of strain and ligand effects in metallic aerogel for electrocatalytic polyethylene terephthalate upcycling. Proc Natl Acad Sci USA, 2024, 121. e2318853121

[17]

PuC, LuG, QiH, IsaevAB, ZhuMS. Enhanced persulfate activation process by magnetically separable catalysts for water purification: a review. Chinese J Struc Chem, 2023, 42100093

[18]

FangQZ, YangHL, YeSJ, ZhangP, DaiMY, HuXJ, GuYL, TanXF. Generation and identification of 1O2 in catalysts/peroxymonosulfate systems for water purification. Water Res, 2023, 245. 120614

[19]

LuoHX, ChenJ, YangJP. Recent advances in transition metal-based catalysts for electrocatalytic nitrate reduction reaction. J Donghua Univ (Eng Ed), 2024, 41: 333

[20]

WangLX, RaoLJ, RanMX, ShentuQK, WuZL, SongWK, ZhangZW, LiH, YaoYY, LvWY, XingMY. A polymer tethering strategy to achieve high metal loading on catalysts for Fenton reactions. Nat Commun, 2023, 14: 7841.

[21]

DongCC, BaoY, ShengT, YiQY, ZhuQH, ShenB, XingMY, LoIMC, ZhangJL. Singlet oxygen triggered by robust bimetallic MoFe/TiO2 nanoparticles of highly efficacy in solar-light-driven peroxymonosulfate activation for organic pollutants removal. Appl Catal B Environ, 2021, 286. 119930

[22]

WengZL, LinYF, GuoSY, ZhangXF, GuoQ, LuoY, OuXW, MaJX, ZhouY, JiangJ, HanB. Site engineering of covalent organic frameworks for regulating peroxymonosulfate activation to generate singlet oxygen with 100% selectivity. Angew Chem Int Ed, 2023, 62. e202310934

[23]

MiXY, WangPF, XuSZ, SuLN, ZhongH, WangHT, LiY, ZhanSH. Almost 100% peroxymonosulfate conversion to singlet oxygen on single-atom CoN2+2 sites. Angew Chem Int Ed, 2021, 60: 4588-4593.

[24]

ZhangLS, JiangXH, ZhongZA, TianL, SunQ, CuiYT, LuX, ZouJP, LuoSL. Carbon nitride supported high-loading Fe single-atom catalyst for activation of peroxymonosulfate to generate 1O2 with 100% selectivity. Angew Chem Int Ed, 2021, 60: 21751-21755.

[25]

HeYZ, QinH, WangZW, WangH, ZhuY, ZhouCY, ZengY, LiYC, XuP, ZengGM. Fe-Mn oxycarbide anchored on N-doped carbon for enhanced Fenton-like catalysis: Importance of high-valent metal-oxo species and singlet oxygen. Appl Catal B Environ, 2024, 340. 123204

[26]

ZhengNC, TangXH, LianYK, OuZS, ZhouQ, WangRL, HuZF. Low-valent copper on molybdenum triggers molecular oxygen activation to selectively generate singlet oxygen for advanced oxidation processes. J Hazard Mater, 2023, 452. 131210

[27]

LiHL, ZhangSH, LiuBH, LiXH, ShangNZ, ZhaoXX, EguchiM, YamauchiY, XuXT. Nanoarchitectonics of ultrafine molybdenum carbide nanocrystals into three-dimensional nitrogen-doped carbon framework for capacitive deionization. Chem Sci, 2024, 15: 11540-11549.

[28]

KallitsakisMG, GioftsidouDK, TzaniMA, AngaridisPA, TerzidisMA, LykakisIN. Mo2C as pre-catalyst for the C–H allylic oxygenation of alkenes and terpenoids in the presence of H2O2. Organics, 2022, 3: 173.

[29]

MengJY, ChengCQ, WangYT, YuYF, ZhangB. Carbon support enhanced mass transfer and metal-support interaction promoted activation for low-concentrated nitric oxide electroreduction to ammonia. J Am Chem Soc, 2024, 146: 10044.

[30]

YangWL, GuoBR, GuoZY, WangX, ZengYL, GuoJN, WuMX. Hollow porous carbon nanofibers with Fe–N–C modified by Fe3O4 nanoparticles for enhancing mass transfer for boosting the oxygen reduction reaction. ACS Sustain Chem Eng, 2023, 11: 8884.

[31]

ZhouH, RenY, LiZH, XuM, WangY, GeRX, KongXG, ZhengLR, DuanHH. Electrocatalytic upcycling of polyethylene terephthalate to commodity chemicals and H2 fuel. Nat Commun, 2021, 12: 4679.

[32]

ChenYY, ZhangY, JiangWJ, ZhangX, DaiZH, WanLJ, HuJS. Pomegranate-like N, P-doped Mo2C@C nanoparticles as highly active electrocatalysts for alkaline hydrogen evolution. ACS Nano, 2016, 10: 8851.

[33]

CongW, DongW, YanY, CaoX, XuY, LiuZ, LiuJ, YangJ, LiuX, YangY, FuL, WangM, ZhangT, ZhouJ. Adjacent-confined pyrolysis for high-density phase boundaries in Mo2C nanosheets to boost oxygen evolution. Adv Func Mater, 2024, 34362401990.

[34]

HuangY, SongX, DengJ, ZhaC, HuangW, WuY, LiY. Ultra-dispersed molybdenum phosphide and phosphosulfide nanoparticles on hierarchical carbonaceous scaffolds for hydrogen evolution electrocatalysis. Appl Catal B Environ, 2019, 245: 656-661.

[35]

QuGJ, JiaP, TangS, PervezMN, PangYX, LiB, CaoCJ, ZhaoYP. Enhanced peroxymonosulfate activation via heteroatomic doping defects of pyridinic and pyrrolic N in 2D N-doped carbon nanosheets for BPA degradation. J Hazard Mater, 2024, 461. 132626

[36]

FuC, SunGW, YinGF, WangC, RanGX, SongQJ. P/N co-doped carbon sheet for peroxymonosulfate activation: Edge sites enhanced adsorption and subsequent electron transfer. Sep Purif Technol, 2022, 292. 120922

[37]

YeGY, LiuSQ, HuangK, WangSY, ZhaoKM, ZhuWW, SuYK, WangJ, HeZ. Domain-confined etching strategy to regulate defective sites in carbon for high-efficiency electrocatalytic oxygen reduction. Adv Funct Mater, 2022, 32: 2111396.

[38]

WangCY, ChenWX, XiaKL, XieNH, WangHM, ZhangYY. Silk-derived 2D porous carbon nanosheets with atomically-dispersed Fe–Nx–C sites for highly efficient oxygen reaction catalysts. Small, 2019, 15: 1804966.

[39]

YangX, WangF, JingZ, ChenM, WangB, WangL, QuG, KongY, XuL. A general “In situ etch-adsorption-phosphatization” strategy for the fabrication of metal phosphides/hollow carbon composite for high performance liquid/flexible Zn–Air batteries. Small, 2023, 19: 2301985.

[40]

SunXT, YuJF, CaoS, ZiminaA, SarmaBB, GrunwaldtJD, XuHY, LiSY, LiuYF, SunJ. In situ investigations on structural evolutions during the facile synthesis of cubic α-MoC1x catalysts. J Am Chem Soc, 2022, 144: 22589.

[41]

ChangJL, WangLL, WuDP, XuF, JiangK, GuoYM, GaoZY. Concurrent electrocatalytic hydrogen evolution and polyethylene terephthalate plastics reforming by self-supported amorphous cobalt iron phosphide electrode. J Colloid Interface Sci, 2024, 655: 555.

[42]

LiJZ, DuLG, GuoST, ChangJL, WuDP, JiangK, GaoZY. Molybdenum iron carbide-copper hybrid as efficient electrooxidation catalyst for oxygen evolution reaction and synthesis of cinnamaldehyde/benzalacetone. J Colloid Interface Sci, 2024, 673: 616.

[43]

FangJJ, WangHY, DangQ, WangH, WangXD, PeiJJ, XuZY, ChenCJ, ZhuW, LiH, YanYS, ZhuangZB. Atomically dispersed Iridium on Mo2C as an efficient and stable alkaline hydrogen oxidation reaction catalyst. Nat Commun, 2024, 15: 4236.

[44]

HuangYF, WuP, TangJP, YangJ, LiJ, ChenS, ZhaoXL, ChenC, ZhangBW, MaYY, ShiWH, LinDH, SunSG. MOF-derived Cu embedded into N-doped mesoporous carbon as a robust support of PdAu nanocatalysts for ethanol electrooxidation. Rare Met, 2023, 43: 1083.

[45]

ChenLL, HuangYC, DingYP, YuP, HuangF, ZhouWB, WangLM, JiangYY, LiHT, CaiHQ, WangL, WangH, LiaoMH, ZhaoLM, FanZJ. Interfacial engineering of atomic platinum-doped molybdenum carbide quantum dots for high-rate and stable hydrogen evolution reaction in proton exchange membrane water electrolysis. Nano Res, 2023, 16: 12186.

[46]

YangCF, ZhaoR, XiangH, WuJ, ZhongWD, LiXK, ZhangQ. Structural transformation of molybdenum carbide with extensive active centers for superior hydrogen evolution. Nano Energy, 2022, 98. 107232

[47]

HaoHC, WangYX, KatyalN, YangG, DongH, LiuPC, HwangS, ManthaJ, HenkelmanG, XuYX, BoscoboinikJA, NandaJ, MitlinD. Molybdenum carbide electrocatalyst in situ embedded in Pnitrogen-rich carbon nanotubes promotes rapid kinetics in sodium-metal-sulfur batteries. Adv Mater, 2022, 34: 2106572.

[48]

WuHB, XiaBY, YuL, YuXY, LouXW. Porous molybdenum carbide nano-octahedrons synthesized via confined carburization in metal-organic frameworks for efficient hydrogen production. Nat Commun, 2015, 6: 6512.

[49]

BellarditaM, García-LópezEI, MarcìG, KrivtsovI, GarcíaJR, PalmisanoL. Selective photocatalytic oxidation of aromatic alcohols in water by using P-doped g-C3N4. Appl Catal B Environ, 2018, 220: 222.

[50]

ZhaoXR, CaoYQ, DuanLL, YangRO, JiangZ, TianC, ChenSJ, DuanXZ, ChenD, WanY. Unleash electron transfer in C–H functionalization by mesoporous carbon-supported palladium interstitial catalysts. Natl Sci Rev, 2021, 8: nwaa126.

[51]

YanQY, LianC, HuangK, LiangLH, YuHR, YinPC, ZhangJL, XingMY. Constructing an acidic microenvironment by MoS2 in heterogeneous Fenton reaction for pollutant control. Angew Chem Int Ed, 2021, 60: 17155.

[52]

BuYG, LiHC, YuWJ, PanYF, LiLJ, WangYF, PuLT, DingJ, GaoGD, PanBC. Peroxydisulfate activation and singlet oxygen generation by oxygen vacancy for degradation of contaminants. Environ Sci Technol, 2021, 5532110.

[53]

YiQY, JiJH, ShenB, DongCC, LiuJ, ZhangJL, XingMY. Singlet oxygen triggered by superoxide radicals in a molybdenum cocatalytic Fenton reaction with enhanced redox activity in the environment. Environ Sci Technol, 2019, 53: 9725.

[54]

XieLB, WangPF, LiY, ZhangDP, ShangDH, ZhengWW, XiaYG, ZhanSH, HuWP. Pauling-type adsorption of O2 induced electrocatalytic singlet oxygen production on N-CuO for organic pollutants degradation. Nat Commun, 2022, 13: 5560.

[55]

HuangYX, ChenKY, WangSX, ZhaoSY, YuLQ, HuangBC, JinRC. Synergizing electron transfer with singlet oxygen to expedite refractory contaminant mineralization in peroxymonosulfate based heterogeneous oxidation system. Appl Catal B Environ, 2024, 341. 123324

[56]

LiuTC, XiaoSZ, LiN, ChenJB, ZhouXF, QianYJ, HuangCH, ZhangYL. Water decontamination via nonradical process by nanoconfined Fenton-like catalysts. Nat Commun, 2023, 14: 2881.

[57]

YueS, ZhaoZY, ZhangT, LiF, LiuKW, ZhanSH. Selective photoreforming of waste plastics into diesel olefins via single reactive oxygen species. Angew Chem Int Ed, 2024, 2024: e202406795

[58]

XuH, ZhangSB, ZhangXY, XuM, HanMM, ZhengLR, ZhangYX, WangGZ, ZhangHM, ZhaoHJ. Atomically dispersed iron regulating electronic structure of iron atom clusters for electrocatalytic H2O2 production and biomass upgrading. Angew Chem Int Ed, 2023, 2023: e202314414

[59]

LiJZ, ChenJL, ZhangLY, MatosJ, WangL, YangJP. Electrocatalytic upcycling of plastic waste: progress, challenges, and future. Electron, 2024, 23. e63

[60]

MaFH, LiZQ, HuRM, WangZQ, WangJP, LiJK, NieY, ZhengZK, JiangXC. Electrocatalytic waste-treating-waste strategy for concurrently upgrading of polyethylene terephthalate plastic and CO2 into value-added formic acid. ACS Catal, 2023, 13: 14163.

[61]

WangJY, LiX, WangML, ZhangT, ChaiXY, LuJL, WangTF, ZhaoYX, MaD. Electrocatalytic valorization of poly(ethylene terephthalate) plastic and CO2 for simultaneous production of formic acid. ACS Catal, 2022, 12: 6722.

[62]

SiD, XiongBY, ChenLS, ShiJL. Highly selective and efficient electrocatalytic synthesis of glycolic acid in coupling with hydrogen evolution. Chem Catal, 2021, 1: 941.

[63]

ZhuJX, XiaLX, YuRH, LuRH, LiJT, HeRH, WuYC, ZhangW, HongXF, ChenW, ZhaoY, ZhouL, MaiLQ, WangZY. Ultrahigh stable methanol oxidation enabled by a high hydroxyl concentration on Pt clusters/MXene interfaces. J Am Chem Soc, 2022, 144: 15529.

[64]

LiangX, WangM, MaD. One-pot conversion of polyester and carbonate into formate without external H2. J Am Chem Soc, 2024, 146: 2711.

[65]

LiuFL, GaoXT, ShiR, TseECM, ChenY. A general electrochemical strategy for upcycling polyester plastics into added-value chemicals by a CuCo2O4 catalyst. Green Chem, 2022, 24: 6571.

[66]

DuMM, XingMY, YuanWF, ZhangL, SunT, ShengT, ZhouCY, QiuBC. Upgrading polyethylene terephthalate plastic into commodity chemicals paired with hydrogen evolution over a partially oxidized CuIn5S8 nanosheet photocatalyst. Green Chem, 2023, 25: 9818.

[67]

BeheraS, DindaS, SahaR, MondalB. Quantitative electrocatalytic upcycling of polyethylene terephthalate plastic and its oligomer with a cobalt-based one-dimensional coordination polymer having open metal sites along with coproduction of hydrogen. ACS Catal, 2022, 13: 469.

[68]

YanYF, ZhouH, XuSM, YangJR, HaoPJ, CaiX, RenY, XuM, KongXG, ShaoMF, LiZH, DuanHH. Electrocatalytic upcycling of biomass and plastic wastes to biodegradable polymer monomers and hydrogen fuel at high current densities. J Am Chem Soc, 2023, 145: 6144.

[69]

KangHX, HeD, YanXX, DaoB, WilliamsNB, ElliottGI, StreaterD, NyakuchenaJ, HuangJ, PanXQ, XiaoXH, GuJ. Cu promoted the dynamic evolution of Ni-based catalysts for polyethylene terephthalate plastic upcycling. ACS Catal, 2024, 14: 5314.

[70]

ChenZJ, WeiW, ShenYS, NiBJ. Defective nickel sulfide hierarchical structures for efficient electrochemical conversion of plastic waste to value-added chemicals and hydrogen fuel. Green Chem, 2023, 25: 5979.

[71]

ChaukeNM, RaphuluM. A review: simultaneous “one-pot” pollution mitigation and hydrogen production from industrial wastewater using photoelectrocatalysis process. Mater Today Catal, 2024, 5. 100052

[72]

ChenJL, JiangMM, ZhangFZ, WangL, YangJP. Interstitial boron atoms in Pd aerogel selectively switch the pathway for glycolic acid synthesis from waste plastics. Adv Mater, 2024, 36: 2401867.

[73]

LiHZ, JiangS, HeS, ZhangYB, ChenY, WangL, YangJP. Accelerated solar-driven polyolefin degradation via self-activated hydroxy-rich ZnIn2S4. Nano Lett, 2024, 24: 11624.

Funding

Shanghai Committee of Science and Technology, China(21ZR1480000)

National Natural Science Foundation of China(52122312)

State Key Laboratory of Advanced Fiber Materials, Donghua University (KF2508)

RIGHTS & PERMISSIONS

Donghua University, Shanghai, China

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