Abstract
This study developed nitrogen-doped graphene/Pt/TiO2 (N-GN/Pt/TiO2) as anode to effectively degrade aminophenol (APAP) in electrocatalytic process. Due to the different physicochemical properties of graphene with various N species loading, the efficiency of catalysts was novelty discussed. The morphology, N-doped content/species, and the graphene defects of the catalyst were analyzed by TEM, FTIR, XPS, EA, and Raman spectroscopy. The results show that the doping morphology of the N atoms gradually shifted from pyridinic N and pyrrolic N to graphitic N with increased hydrothermal time, in order to decrease the defect degrees and redox activity. However, the conductivity of material increased with the graphitic N generation. The best APAP degradation efficiency (100% with 20 mA, 1 g/L NaCl, and initial pH 3.0) can be achieved with 1.5-N-GN/Pt/TiO2 (mainly pyridinic N and pyrrolic N doping). A detailed investigation was conducted to determine the oxidation intermediates of APAP using GC-MS analysis. Finally, a possible degradation pathway was proposed.
Graphical Abstract
Similar content being viewed by others
References
Rajkumar D, Palanivelu K (2004) Electrochemical treatment of industrial wastewater. J Hazard Mater 113:123–129
Feng YJ, Li XY (2003) Electro-catalytic oxidation of phenol on several metal-oxide electrodes in aqueous solution. Water Res 37:2399–2407
Huang C, Li C, Shi G (2012) Graphene based catalysts. Energ Environ Sci 5:8848–8868
Yan Y, Yin Y, Xin S, Guo Y, Wan L (2012) Ionothermal synthesis of sulfur-doped porous carbons hybridized with graphene as superior anode materials for lithium-ion batteries. Chem Commun 48:10663
Liu Q, Lin Y, Fan J, Lv D, Min Y, Wu T, Xu Q (2016) Well-dispersed palladium nanoparticles on three-dimensional hollow N-doped graphene frameworks for enhancement of methanol electro-oxidation. Electrochem Commun 73:75–79
Liu D, Li L, You T (2017) Superior catalytic performances of platinum nanoparticles loaded nitrogen-doped graphene toward methanol oxidation and hydrogen evolution reaction. J Colloid Interface Sci 487:330–335
Sheng Z, Shao L, Chen J, Bao W, Wang F, Xia X (2011) Catalyst-free synthesis of nitrogen-doped graphene via thermal annealing graphite oxide with melamine and its excellent electrocatalysis. ACS Nano 5:4350–4358
Lin Z, Waller G, Liu Y, Liu M, Wong C (2012) Facile synthesis of nitrogen-doped graphene via pyrolysis of graphene oxide and urea, and its electrocatalytic activity toward the oxygen-reduction reaction. Adv Energy Mater 2:884–888
Zheng Y, Jiao Y, Ge L, Jaroniec M, Qiao SZ (2013) Two-step boron and nitrogen doping in graphene for enhanced synergistic catalysis. Angew Chem Int Ed Engl 52:3110–3116
Chen D, Feng H, Li J (2012) Graphene oxide: preparation, functionalization, and electrochemical applications. Chem Rev 112:6027–6053
Li J, Li Y, Tang L (2009) Preparation and electrochemical performance for methanol oxidation of pt/graphene nanocomposites. Electrochem Commun 11:846–849
Sun L, Wang L, Tian C, Tan T, Xie Y, Shi K, Li M, Fu H (2012) Nitrogen-doped graphene with high nitrogen level via a one-step hydrothermal reaction of graphene oxide with urea for superior capacitive energy storage. RSC Adv 2:4498
Zhang L, Xia Z (2011) Mechanisms of oxygen reduction reaction on nitrogen-doped graphene for fuel cells. J Phys Chem C 115:11170–11176
Li TS, Loh KS, Mohamad AB, Wan RWD (2016) The effect of varying N/C ratios of nitrogen precursors during non-metal graphene catalyst synthesis. Int J Hydrog Energy 42:9069–9076
Kim H, Lee K, Woo SI, Jung Y (2011) On the mechanism of enhanced oxygen reduction reaction in nitrogen-doped graphene nanoribbons. Phys Chem Chem Phys 13:17505
Tao H, Liang X, Zhang Q, Chang CT (2015) Enhanced photoactivity of graphene/titanium dioxide nanotubes for removal of acetaminophen. Appl Surf Sci 324:258–264
Zhang Q, Huang W, Chen BY, Hong JM (2018) Deciphering acetaminophen electrical catalytic degradation using single-form S doped graphene/Pt/TiO2. Chem Eng J 343:662–675
Joshi AA, Locke BR, Arce P, Finney WC (1995) Formation of hydroxyl radicals, hydrogen peroxide and aqueous electrons by pulsed streamer corona discharge in aqueous solution. J Hazard Mater 41:3–30
Zhao L, Wang Z, Liu J, Zhang J, Sui X, Zhang L, Gu D (2015) Facile one-pot synthesis of Pt/graphene-TiO2 hybrid catalyst with enhanced methanol electrooxidation performance. J Power Sources 279:210–217
Wang P, Zhan S, Xia Y, Ma S, Zhou Q, Li Y (2017) The fundamental role and mechanism of reduced graphene oxide in rGO/Pt-TiO2 nanocomposite for high-performance photocatalytic water splitting. Appl Catal B 207:335–346
Maldonado S, Stevenson KJ (2005) Influence of nitrogen doping on oxygen reduction electrocatalysis at carbon nanofiber electrodes. J Phys Chem B 109:4707–4716
Shao Y, Sui J, Yin G, Gao (2008) Nitrogen-doped carbon nanostructures and their composites as catalytic materials for proton exchange membrane fuel cell. Appl Catal B 79:89–99
Brindha A, Sivakumar T (2017) Visible active N, S co-doped TiO2/graphene photocatalysts for the degradation of hazardous dyes. J Photochem Photobiol A 340:146–156
Zhang T, Li C, Gu Y, Yan X, Zheng B, Li Y, Liu H, Lu N, Zhang Z, Feng G (2017) Fabrication of novel metal-free “graphene alloy” for the highly efficient electrocatalytic reduction of H2O2. Talanta 165:143–151
Nguyen-Phan TD, Pham VH, Shin EW, Pham HD, Kim S (2011) The role of graphene oxide content on the adsorption-enhanced photocatalysis of titanium dioxide/graphene oxide composites. Chem Eng J 170:226–232
Min S, Lu G (2012) Dye-cosensitized graphene/Pt photocatalyst for high efficient visible light hydrogen evolution. Int J Hydrog Energy 37:10564–10574
Vinodgopal K, Neppolian B, Salleh N, Lightcap IV, Grieser F, Ashokkumar M, Ding TT, Kamat PV (2012) Dual-frequency ultrasound for designing two dimensional catalyst surface: Reduced graphene oxide–Pt composite. Colloids Surf A 409:81–87
Chekin F, Bagheri S, Abd Hamid SB (2013) Synthesis of Pt doped TiO2 nanoparticles: characterization and application for electrocatalytic oxidation of l-methionine. Sens Actuators B 177:898–903
Wohlgemuth S, White RJ, Willinger M, Titirici M, Antonietti M (2012) A one-pot hydrothermal synthesis of sulfur and nitrogen doped carbon aerogels with enhanced electrocatalytic activity in the oxygen reduction reaction. Green Chem 14:1515
Xiong B, Zhou Y, O’ Hayre R, Shao Z (2013) Facile single-step ammonia heat-treatment and quenching process for the synthesis of improved Pt/N-graphene catalysts. Appl Surf Sci 266:433–439
Kudin KN, Ozbas B, Schniepp HC, Prud’Homme RK, Aksay IA, Car R (2008) Raman spectra of graphite oxide and functionalized graphene sheets. Nano Lett 8:36–41
Kang Y, Wang W, Pu Y, Li J, Chai D, Lei Z (2017) An effective Pd-NiOx-P composite catalyst for glycerol electrooxidation: co-existed phosphorus and nickel oxide to enhance performance of Pd. Chem Eng J 308:419–427
Liu Y, Zhu Y, Fan X, Wang S, Li Y, Zhang F, Peng W (2017) (0D/3D) MoS2 on porous graphene as catalysts for enhanced electrochemical hydrogen evolution. Carbon 121:163–169
Wei Y, Li X, Sun X, Ma H, Zhang Y, Wei Q (2017) Dual-responsive electrochemical immunosensor for prostate specific antigen detection based on Au-CoS/graphene and CeO2/ionic liquids doped with carboxymethyl chitosan complex. Biosens Bioelectron 94:141–147
Chen Z, Zhang Y, Zhou L, Zhu H, Wan F, Wang Y, Zhang D (2017) Performance of nitrogen-doped graphene aerogel particle electrodes for electro-catalytic oxidation of simulated Bisphenol A wastewaters. J Hazard Mater 332:70–78
Wu W, Huang Z, Lim T (2016) A comparative study on electrochemical oxidation of bisphenol A by boron-doped diamond anode and modified SnO2-Sb anodes: Influencing parameters and reaction pathways. J Environ Chem Eng 4:2807–2815
Khongthon W, Jovanovic G, Yokochi A, Sangvanich P, Pavarajarn V (2016) Degradation of diuron via an electrochemical advanced oxidation process in a microscale-based reactor. Chem Eng J 292:298–307
Martínez-Huitle CA, Rodrigo MA, Sirés I, Scialdone O (2015) Single and coupled electrochemical processes and reactors for the abatement of organic water pollutants: a critical review. Chem Rev 115:13362–13407
Scialdone O, Randazzo S, Galia A, Silvestri G (2009) Electrochemical oxidation of organics in water: role of operative parameters in the absence and in the presence of NaCl. Water Res 43:2260–2272
Barhoumi N, Labiadh L, Oturan MA, Oturan N, Gadri A, Ammar S, Brillas E (2015) Electrochemical mineralization of the antibiotic levofloxacin by electro-Fenton-pyrite process. Chemosphere 141:250–257
Indrawirawan S, Sun H, Duan X, Wang S (2015) Low temperature combustion synthesis of nitrogen-doped graphene for metal-free catalytic oxidation. J Mater Chem 3:3432–3440
Cardoso JC, Lizier TM, Zanoni MVB (2010) Highly ordered TiO2 nanotube arrays and photoelectrocatalytic oxidation of aromatic amine. Appl Catal B 99:96–102
Yang L, Yu LE, Ray MB (2008) Degradation of paracetamol in aqueous solutions by TiO2 photocatalysis. Water Res 42:3480–3488
Yang L, Yu LE, Ray MB (2009) Photocatalytic oxidation of paracetamol: dominant reactants, intermediates, and reaction mechanisms. Environ Sci Technol 43:460–465
Acknowledgements
This work was financially supported by Fujian province Science and Technology project Foundation (2017I01010015), Xiamen Technology project Foundation (3502Z20173050, 3502Z20140057, 3502Z20153025, 3502Z20173052), Quanzhou Technology project Foundation (2016Z074, 2018z002).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
All the authors declare there is not any competing financial interest.
Rights and permissions
About this article
Cite this article
Sun, R., Huang, W., Zhang, Q. et al. Facilely Prepared N-Doped Graphene/Pt/TiO2 as an Efficient Anode for Acetaminophen Degradation. Catal Lett 148, 2418–2431 (2018). https://doi.org/10.1007/s10562-018-2466-5
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10562-018-2466-5