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Yong GUO


Ying GUO


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Journal of Zhejiang University SCIENCE A 2024 Vol.25 No.4 P.340-356


N-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies

Author(s):  Yong GUO, Mengxia CHEN, Ting CHEN, Ying GUO, Zixuan XU, Guowei XU, Soukthakhane SINSONESACK, Keophoungeun KANMANY

Affiliation(s):  Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Ministry of Education, College of Environment, Hohai University, Nanjing 210093, China; more

Corresponding email(s):   guoyong@hhu.edu.cn, guoyinghhu@163.com

Key Words:  Dissolved black carbon (DBC), N-doping, Organic pollutants, Band gap, Photodegradation

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Yong GUO, Mengxia CHEN, Ting CHEN, Ying GUO, Zixuan XU, Guowei XU, Soukthakhane SINSONESACK, Keophoungeun KANMANY. N-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies[J]. Journal of Zhejiang University Science A, 2024, 25(4): 340-356.

@article{title="N-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies",
author="Yong GUO, Mengxia CHEN, Ting CHEN, Ying GUO, Zixuan XU, Guowei XU, Soukthakhane SINSONESACK, Keophoungeun KANMANY",
journal="Journal of Zhejiang University Science A",
publisher="Zhejiang University Press & Springer",

%0 Journal Article
%T N-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies
%A Yong GUO
%A Mengxia CHEN
%A Ting CHEN
%A Ying GUO
%A Zixuan XU
%A Guowei XU
%A Soukthakhane SINSONESACK
%A Keophoungeun KANMANY
%J Journal of Zhejiang University SCIENCE A
%V 25
%N 4
%P 340-356
%@ 1673-565X
%D 2024
%I Zhejiang University Press & Springer
%DOI 10.1631/jzus.A2300081

T1 - N-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies
A1 - Yong GUO
A1 - Mengxia CHEN
A1 - Ting CHEN
A1 - Ying GUO
A1 - Zixuan XU
A1 - Guowei XU
A1 - Soukthakhane SINSONESACK
A1 - Keophoungeun KANMANY
J0 - Journal of Zhejiang University Science A
VL - 25
IS - 4
SP - 340
EP - 356
%@ 1673-565X
Y1 - 2024
PB - Zhejiang University Press & Springer
ER -
DOI - 10.1631/jzus.A2300081

We investigated the influence mechanism of n-doping for dissolved black carbon (DBC) photodegradation of organic pollutants. The degradation performance of N-doped dissolved black carbon (NDBC) for tetracycline (TC) (71%) is better than that for methylene blue (MB) (28%) under irradiation. These levels are both better than DBC degradation performances for TC (68%) and MB (18%) under irradiation. Reactive species quenching experiments suggest that h+ and O2- are the main reactive species for NDBC photodegraded TC, while ·OH and h+ are the main reactive species for NDBC photodegraded MB. ·OH is not observed during DBC photodegradation of MB. This is likely because n-doping increases valence-band (VB) energy from 1.55 eV in DBC to 2.04 eV in NDBC; the latter is strong enough to oxidize water to form ·OH. Additionally, n-doping increases the DBC band gap of 2.29 to 2.62 eV in NDBC, resulting in a higher separation efficiency of photo-generated electrons-holes in NDBC than in DBC. All these factors give NDBC stronger photodegradation performance for TC and MB than DBC. High-performance liquid chromatography-mass spectrometry (HPLC-MS) characterization and toxicity evaluation with the quantitative structure-activity relationship (QSAR) method suggest that TC photodegradation intermediates produced by NDBC have less aromatic structure and are less toxic than those produced by DBC. We adopted a theoretical approach to clarify the relationship between the surface groups of NDBC and the photoactive species produced. Our results add to the understanding of the photochemical behavior of NDBC.


作者:郭勇1,3,陈孟霞1,陈婷2,郭颖2,徐子璇1,徐国威1,Soukthakhane SINSONESACK4, Keophoungeun KANMANY4
结论:氮掺杂促进了生物炭衍生的DBC对四环素(TC)和亚甲基蓝(MB)的光降解性能。这可能是由于以下原因:(1)氮掺杂使DBC的价带能量从1.55 eV增加到氮掺杂的可溶性黑炭(NDBC)的2.04 eV,这足以使NDBC的水氧化形成·OH。换句话说,NDBC可以产生-OH和,而DBC只能产生。(2)氮掺杂使DBC的带隙从2.29 eV增加到2.62 eV,从而导致光生电子孔的分离效率提高,最终促进光降解效率。(3)氮掺杂降低DBC在光照下的稳定性,使DBC对可见光的反应更加灵敏。


Darkslateblue:Affiliate; Royal Blue:Author; Turquoise:Article


[1]AraiW, KameyaH, HashimR, et al., 2022. Reactive oxygen species scavenging capacities of oil palm trunk sap evaluated using the electron spin resonance spin trapping method. Industrial Crops and Products, 182:114887.

[2]Barroso-MartínezJS, RomoAIB, PudarS, et al., 2022. Real-time detection of hydroxyl radical generated at operating electrodes via redox-active adduct formation using scanning electrochemical microscopy. Journal of the American Chemical Society, 144(41):18896-18907.

[3]Ben OuaghremM, de VaugeladeS, BourcierS, et al., 2022. Characterization of photoproducts and global ecotoxicity of chlorphenesin: a preservative used in skin care products. International Journal of Cosmetic Science, 44(1):10-19.

[4]ChenW, YangHP, ChenYQ, et al., 2016. Biomass pyrolysis for nitrogen-containing liquid chemicals and nitrogen-doped carbon materials. Journal of Analytical and Applied Pyrolysis, 120:186-193.

[5]de OliveiraJA, da CruzJC, NascimentoOR, et al., 2022. Selective CH4 reform to methanol through partial oxidation over Bi2O3 at room temperature and pressure. Applied Catalysis B: Environmental, 318:121827.

[6]DengSY, LiZZ, ZhaoTS, et al., 2022. Direct Z-scheme covalent triazine-based framework/Bi2WO6 heterostructure for efficient photocatalytic degradation of tetracycline: kinetics, mechanism and toxicity. Journal of Water Process Engineering, 49:103021.

[7]FangGD, GaoJ, LiuC, et al., 2014. Key role of persistent free radicals in hydrogen peroxide activation by biochar: implications to organic contaminant degradation. Environmental Science & Technology, 48(3):1902-1910.

[8]FangGD, LiuC, GaoJ, et al., 2015. Manipulation of persistent free radicals in biochar to activate persulfate for contaminant degradation. Environmental Science & Technology, 49(9):5645-5653.

[9]FangGD, LiuC, WangYJ, et al., 2017. Photogeneration of reactive oxygen species from biochar suspension for diethyl phthalate degradation. Applied Catalysis B: Environmental, 214:34-45.

[10]FatimahS, BilqisSM, Isnaeni, et al., 2019. Luminescence properties of carbon dots synthesis from sugar for enhancing glows in paints. Materials Research Express, 6(9):095006.

[11]FowlesM, 2007. Black carbon sequestration as an alternative to bioenergy. Biomass and Bioenergy, 31(6):426-432.

[12]FrischMJ, TrucksG, SchlegelHS, et al., 2009. Gaussian 09, Revision A.02. Gaussian Inc., Wallingford, USA.

[13]FuHY, LiuHT, MaoJD, et al., 2016. Photochemistry of dissolved black carbon released from biochar: reactive oxygen species generation and phototransformation. Environmental Science & Technology, 50(3):1218-1226.

[14]GeedSR, SamalK, TagadeA, 2019. Development of adsorption-biodegradation hybrid process for removal of methylene blue from wastewater. Journal of Environmental Chemical Engineering, 7(6):103439.

[15]GolshanM, KakavandiB, AhmadiM, et al., 2018. Photocatalytic activation of peroxymonosulfate by TiO2 anchored on cupper ferrite (TiO2@CuFe2O4) into 2,4-D degradation: process feasibility, mechanism and pathway. Journal of Hazardous Materials, 359:325-337.

[16]GuJM, YanJ, ChenZG, et al., 2017. Construction and preparation of novel 2D metal-free few-layer BN modified graphene-like g-C3N4 with enhanced photocatalytic performance. Dalton Transactions, 46(34):11250-11258.

[17]GuoHH, CuiJ, ChaiX, et al., 2023. Preparation of multilayer strontium-doped TiO2/CDs with enhanced photocatalytic efficiency for enrofloxacin removal. Environmental Science and Pollution Research, 30(26):68403-68416.

[18]GuoMY, YuanBH, SuiY, et al., 2023. Rational design of molybdenum sulfide/tungsten oxide solar absorber with enhanced photocatalytic degradation toward dye wastewater purification. Journal of Colloid and Interface Science, 631:33-43.

[19]GuoY, GuoY, HuaSG, et al., 2022. Coupling band structure and oxidation-reduction potential to expound photodegradation performance difference of biochar-derived dissolved black carbon for organic pollutants under light irradiation. Science of the Total Environment, 820:153300.

[20]GuoYX, WenH, ZhongT, et al., 2022. Edge-rich atomic-layered biobr quantum dots for photocatalytic molecular oxygen activation. Chemical Engineering Journal, 445:136776.

[21]HuSL, TianRX, WuLL, et al., 2013. Chemical regulation of carbon quantum dots from synthesis to photocatalytic activity. Chemistry-An Asian Journal, 8(5):1035-1041.

[22]HuSL, ZhangWY, ChangQ, et al., 2016. A chemical method for identifying the photocatalytic active sites on carbon dots. Carbon, 103:391-393.

[23]ImrichT, KrysovaH, Neumann-SpallartM, et al., 2023. Pseudobrookite (Fe2TiO5) films: synthesis, properties and photoelectrochemical characterization. Catalysis Today, 413-415:113982.

[24]KasinathanM, ThiripuranthaganS, SivakumarA, 2020. Fabrication of sphere-like Bi2MoO6/ZnO composite catalyst with strong photocatalytic behavior for the detoxification of harmful organic dyes. Optical Materials, 109:110218.

[25]KhanMA, AlqadamiAA, WabaidurSM, et al., 2020. Oil industry waste based non-magnetic and magnetic hydrochar to sequester potentially toxic post-transition metal ions from water. Journal of Hazardous Materials, 400:123247.

[26]KöhlerT, ZschornakM, RöderC, et al., 2023. Chemical environment and occupation sites of hydrogen in LiMO3. Journal of Materials Chemistry C, 11(2):520-538.

[27]KumarG, DuttaRK, 2022. Sunlight mediated photo-Fenton degradation of tetracycline antibiotic and methylene blue dye in aqueous medium using FeWO4/Bi2MoO6 nanocomposite. Process Safety and Environmental Protection, 159:862-873.

[28]LarssonDGJ, FlachCF, 2022. Antibiotic resistance in the environment. Nature Reviews Microbiology, 20(5):257-269.

[29]LiHT, LiuRH, LianSY, et al., 2013. Near-infrared light controlled photocatalytic activity of carbon quantum dots for highly selective oxidation reaction. Nanoscale, 5(8):3289-3297.

[30]LiL, ChengM, QinL, et al., 2022. Enhancing hydrogen peroxide activation of Cu‍–‍Co layered double hydroxide by compositing with biochar: performance and mechanism. Science of the Total Environment, 828:154188.

[31]LiRH, WangJJ, ZhouBY, et al., 2017. Simultaneous capture removal of phosphate, ammonium and organic substances by MgO impregnated biochar and its potential use in swine wastewater treatment. Journal of Cleaner Production, 147:96-107.

[32]LinZL, WuYL, JinXY, et al., 2023. Facile synthesis of direct Z-scheme UiO-66-NH2/PhC2Cu heterojunction with ultrahigh redox potential for enhanced photocatalytic Cr(VI) reduction and NOR degradation. Journal of Hazardous Materials, 443:130195.

[33]LiuSH, HuangYY, 2018. Valorization of coffee grounds to biochar-derived adsorbents for Co2 adsorption. Journal of Cleaner Production, 175:354-360.

[34]LiuXJ, LiuJY, ChuHP, et al., 2015. Enhanced photocatalytic activity of Bi2O3-Ag2O hybrid photocatalysts. Applied Surface Science, 347:269-274.

[35]LiuY, GuoHG, ZhangYL, et al., 2019. Fe@C carbonized resin for peroxymonosulfate activation and bisphenol S degradation. Environmental Pollution, 252:1042-1050.

[36]LiuY, LiuXH, LuSY, et al., 2020. Adsorption and biodegradation of sulfamethoxazole and ofloxacin on zeolite: influence of particle diameter and redox potential. Chemical Engineering Journal, 384:123346.

[37]MaWJ, XuXY, AnBY, et al., 2021. Single and ternary competitive adsorption-desorption and degradation of amphenicol antibiotics in three agricultural soils. Journal of Environmental Management, 297:113366.

[38]MeyerS, BrightRM, FischerD, et al., 2012. Albedo impact on the suitability of biochar systems to mitigate global warming. Environmental Science & Technology, 46(22):12726-12734.

[39]OrtizGR, Lartundo-RojasL, Samaniego-BenítezJE, et al., 2021. Photocatalytic behavior for the phenol degradation of ZnAl layered double hydroxide functionalized with SDS. Journal of Environmental Management, 277:111399.

[40]QambraniNA, RahmanMM, WonS, et al., 2017. Biochar properties and eco-friendly applications for climate change mitigation, waste management, and wastewater treatment: a review. Renewable and Sustainable Energy Reviews, 79:255-273.

[41]QinL, ZhouZP, DaiJD, et al., 2016. Novel N-doped hierarchically porous carbons derived from sustainable shrimp shell for high-performance removal of sulfamethazine and chloramphenicol. Journal of the Taiwan Institute of Chemical Engineers, 62:228-238.

[42]QinL, HuangCH, LiuCQ, et al., 2023. Molecular mechanism for the activation of the potent hepatotoxin acetylhydrazine: identification of the initial N-centered radical and the secondary C-centered radical intermediates. Free Radical Biology and Medicine, 204:20-27.

[43]QuXL, FuHY, MaoJD, et al., 2016. Chemical and structural properties of dissolved black carbon released from biochars. Carbon, 96:759-767.

[44]RafiqA, IkramM, AliS, et al., 2021. Photocatalytic degradation of dyes using semiconductor photocatalysts to clean industrial water pollution. Journal of Industrial and Engineering Chemistry, 97:111-128.

[45]ShahidMK, KashifA, FuwadA, et al., 2021. Current advances in treatment technologies for removal of emerging contaminants from water–a critical review. Coordination Chemistry Reviews, 442:213993.

[46]ShaoJG, ZhangJJ, ZhangX, et al., 2018. Enhance SO2 adsorption performance of biochar modified by CO2 activation and amine impregnation. Fuel, 224:138-146.

[47]ShiHH, WangMJ, WangBB, et al., 2020. Insights on photochemical activities of organic components and minerals in dissolved state biochar in the degradation of atorvastatin in aqueous solution. Journal of Hazardous Materials, 392:122277.

[48]SuHS, YiH, GuWY, et al., 2022. Cost of raising discharge standards: a plant-by-plant assessment from wastewater sector in China. Journal of Environmental Management, 308:114642.

[49]SunSM, WangWZ, LiDZ, et al., 2014. Solar light driven pure water splitting on quantum sized BiVO4 without any cocatalyst. ACS Catalysis, 4(10):3498-3503.

[50]TanXF, LiuSB, LiuYG, et al., 2017. Biochar as potential sustainable precursors for activated carbon production: multiple applications in environmental protection and energy storage. Bioresource Technology, 227:359-372.

[51]TangCQ, ZhangYM, HanJG, et al., 2020. Monitoring graphene oxide’s efficiency for removing Re(VII) and Cr(VI) with fluorescent silica hydrogels. Environmental Pollution, 262:114246.

[52]TangSF, WangZT, YuanDL, et al., 2020. Ferrous ion-tartaric acid chelation promoted calcium peroxide fenton-like reactions for simulated organic wastewater treatment. Journal of Cleaner Production, 268:122253.

[53]TianYJ, FengL, WangC, et al., 2019. Dissolved black carbon enhanced the aquatic photo-transformation of chlortetracycline via triplet excited-state species: the role of chemical composition. Environmental Research, 179:108855.

[54]TuYN, LiuHY, LiYJ, et al., 2022. Radical chemistry of dissolved black carbon under sunlight irradiation: quantum yield prediction and effects on sulfadiazine photodegradation. Environmental Science and Pollution Research, 29(15):21517-21527.

[55]WanD, WangJ, ChenT, et al., 2022. Effect of disinfection on the photoreactivity of effluent organic matter and photodegradation of organic contaminants. Water Research, 219:118552.

[56]WanZH, SunYQ, TsangDCW, et al., 2020. Customised fabrication of nitrogen-doped biochar for environmental and energy applications. Chemical Engineering Journal, 401:126136.

[57]WangH, ZhouHX, MaJZ, et al., 2020. Triplet photochemistry of dissolved black carbon and its effects on the photochemical formation of reactive oxygen species. Environmental Science & Technology, 54(8):4903-4911.

[58]WangJT, CaiYL, LiuXJ, et al., 2022. Unveiling the visible-light-driven photodegradation pathway and products toxicity of tetracycline in the system of Pt/BiVO4 nanosheets. Journal of Hazardous Materials, 424:127596.

[59]WangLL, WangL, ShiYW, et al., 2022. Blue TiO2 nanotube electrocatalytic membrane electrode for efficient electrochemical degradation of organic pollutants. Chemosphere, 306:135628.

[60]WengXL, CaiWL, LanRF, et al., 2018. Simultaneous removal of amoxicillin, ampicillin and penicillin by clay supported Fe/Ni bimetallic nanoparticles. Environmental Pollution, 236:562-569.

[61]WoolfD, AmonetteJE, Street-PerrottFA, et al., 2010. Sustainable biochar to mitigate global climate change. Nature Communications, 1:56.

[62]WuZZ, FeiH, WangDZ, 2019. MoS2/Cu2O nanohybrid as a highly efficient catalyst for the photoelectrocatalytic hydrogen generation. Materials Letters, 256:126622.

[63]XiaoCF, ChenXQ, TaoXM, et al., 2023. In situ generation of hydroxyl radicals by B-doped TiO2 for efficient photocatalytic degradation of acetaminophen in wastewater. Environmental Science and Pollution Research, 30(16):46997-47011.

[64]XuXY, CaoXD, ZhaoL, et al., 2014. Interaction of organic and inorganic fractions of biochar with Pb(II) ion: further elucidation of mechanisms for Pb(II) removal by biochar. RSC Advances, 4(85):44930-44937.

[65]YanM, HuaYQ, ZhuFF, et al., 2017. Fabrication of nitrogen doped graphene quantum dots-BiOI/MnNb2O6 p-n junction photocatalysts with enhanced visible light efficiency in photocatalytic degradation of antibiotics. Applied Catalysis B: Environmental, 202:518-527.

[66]YanYB, ChenJ, LiN, et al., 2018. Systematic bandgap engineering of graphene quantum dots and applications for photocatalytic water splitting and CO2 reduction. ACS Nano, 12(4):3523-3532.

[67]YangF, SunLL, XieWL, et al., 2017. Nitrogen-functionalization biochars derived from wheat straws via molten salt synthesis: an efficient adsorbent for atrazine removal. Science of the Total Environment, 607-608:1391-1399.

[68]YaoB, LuoZR, DuSZ, et al., 2022. Magnetic MgFe2O4/biochar derived from pomelo peel as a persulfate activator for levofloxacin degradation: effects and mechanistic consideration. Bioresource Technology, 346:126547.

[69]YaoYJ, ChenH, LianC, et al., 2016. Fe, Co, Ni nanocrystals encapsulated in nitrogen-doped carbon nanotubes as Fenton-like catalysts for organic pollutant removal. Journal of Hazardous Materials, 314:129-139.

[70]YeRQ, PengZW, MetzgerA, et al., 2015. Bandgap engineering of coal-derived graphene quantum dots. ACS Applied Materials & Interfaces, 7(12):7041-7048.

[71]YeWJ, ZhangWW, HuXX, et al., 2020. Efficient electrochemical-catalytic reduction of nitrate using Co/AC0.9-AB0.1 particle electrode. Science of the Total Environment, 732:139245.

[72]YuanH, ShiWL, LuJL, et al., 2023. Dual-channels separated mechanism of photo-generated charges over semiconductor photocatalyst for hydrogen evolution: interfacial charge transfer and transport dynamics insight. Chemical Engineering Journal, 454:140442.

[73]ZhangJ, WangC, HuangNN, et al., 2022. Humic acid promoted activation of peroxymonosulfate by Fe3S4 for degradation of 2,4,6-trichlorophenol: an experimental and theoretical study. Journal of Hazardous Materials, 434:128913.

[74]ZhangJJ, GaoYF, JiaXR, et al., 2018. Oxygen vacancy-rich mesoporous ZrO2 with remarkably enhanced visible-light photocatalytic performance. Solar Energy Materials and Solar Cells, 182:113-120.

[75]ZhangKK, KhanA, SunP, et al., 2020. Simultaneous reduction of Cr(VI) and oxidization of organic pollutants by rice husk derived biochar and the interactive influences of coexisting Cr(VI). Science of the Total Environment, 706:135763.

[76]ZhangZC, WangFX, WangF, et al., 2023. Efficient atrazine degradation via photoactivated SR-AOP over S-BUC-21(Fe): the formation and contribution of different reactive oxygen species. Separation and Purification Technology, 307:122864.

[77]ZhangZF, ZhaoW, ZhaoWW, 2014. Commercialization development of crop straw gasification technologies in China. Sustainability, 6(12):9159-9178.

[78]ZhaoPJ, YangY, PeiY, et al., 2023. TEMPO-oxidized cellulose beads embedded with Au-doped TiO2 nanoparticles for photocatalytic degradation of Tylosin. Cellulose, 30(2):1133-1147.

[79]ZhaoY, TruhlarDG, 2008. The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals. Theoretical Chemistry Accounts, 120(1-3):215-241.

[80]ZhengY, ZhangZS, LiCH, 2017. A comparison of graphitic carbon nitrides synthesized from different precursors through pyrolysis. Journal of Photochemistry and Photobiology A: Chemistry, 332:32-44.

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