Abstract
A novel cryptomelane-Ir (cry-Ir) electrode is prepared for Ir to enter into the cryptomelane (named as cry-Mn) structure and used for aspirin degradation. This catalyst can efficiently reduce the Ir usage from 85 to 34%. Also, the onset potential of cry-Ir is about 1.40 V and the over potential is about 0.34 V at 10 mA cm−2, indicating that cry-Ir has an excellent oxygen evolution reaction (OER) activity to produce oxidizing species and can decrease electrolytic voltage during the electro-oxidation process. So, the electrical efficiency per log order (EE/O) for cry-Ir electrode is only 5% of PbO2 electrode, which is the best electrode for organic degradation. Also, cry-Ir has large tunnel size which favors insertion of aspirin molecule into cry-Ir structure and enhances the contact between reactive intermediates and the contaminant. Using cry-Ir as anode, 100% aspirin removal and 55% chemical oxygen demand (COD) removal could be obtained at 4 V. We also compare cry-Ir electrode with IrO2 and find that IrO2 anode can only eliminate 20% aspirin under the same condition. As a result, cry-Ir is a promising anode material for organic pollutant degradation.
Similar content being viewed by others
References
And SC, Roark JL, ND, Suib SL (1997) Sol-gel route to the tunneled manganese oxide Cryptomelane. Chem Mater 9:750–754
Bound JP, Voulvoulis N (2004) Pharmaceuticals in the aquatic environment--a comparison of risk assessment strategies. Chemosphere 56:1143–1155
Chen R, Huang Y, Liang Y, Tsai D, Chi Y, Kai J (2003) Growth control and characterization of vertically aligned IrO2 nanorods. J Mater Chem 13:2525
Dai Q, Xia Y, Chen J (2015) Mechanism of enhanced electrochemical degradation of highly concentrated aspirin wastewater using a rare earth la-Y co-doped PbO2 electrode. Electrochim Acta 188:871–881
Daughton CG, Ternes TA (1999) Pharmaceuticals and personal care products in the environment: agents of subtle change? Environmental Health Perspectives 107(Suppl 6):907
Fent K, Weston AA, Caminada D (2006) Ecotoxicology of human pharmaceuticals. Aquat Toxicol 76:122–159
Gao T, Glerup M, Krumeich F, Nesper R, Fjellvåg H, Norby P (2008) Microstructures and spectroscopic properties of Cryptomelane-type manganese dioxide Nanofibers. J Phys Chem C 112:13134–13140
Gorlin Y, Jaramillo TF (2010) A bifunctional nonprecious metal catalyst for oxygen reduction and water oxidation. J Am Chem Soc 132:13612–13614
He Y, Huang W, Chen R, Zhang W, Lin H, Li H (2015) Anodic oxidation of aspirin on PbO2, BDD and porous Ti/BDD electrodes: mechanism, kinetics and utilization rate. Sep Purif Technol 156:124–131
Jalife-Jacobo H, Feria-Reyes R, Serrano-Torres O, Gutiérrez-Granados S, Peralta-Hernández JM (2016) Diazo dye Congo red degradation using a boron-doped diamond anode: an experimental study on the effect of supporting electrolytes. J Hazard Mater 319:78–83
Joss A, Zabczynski S, Göbel A, Hoffmann B, Löffler D, Mcardell CS, Ternes TA, Thomsen A, Siegrist H (2006) Biological degradation of pharmaceuticals in municipal wastewater treatment: proposing a classification scheme. Water Res 40:1686–1696
Kasprzyk-Hordern B (2010) ChemInform abstract: pharmacologically active compounds in the environment and their chirality. ChemInform 39:4466–4503
Klavarioti M, Mantzavinos D, Kassinos D (2009) Removal of residual pharmaceuticals from aqueous systems by advanced oxidation processes. Environ Int 35:402–417
Lee Y, Suntivich J, May KJ, Perry EE, Shao-Horn Y (2012) Synthesis and activities of rutile IrO2 and RuO2 nanoparticles for oxygen evolution in acid and alkaline solutions. J Phys Chem Lett 3:399–404
Li W, Nanaboina V, Chen F, Korshin GV (2015) Removal of polycyclic synthetic musks and antineoplastic drugs in ozonated wastewater: quantitation based on the data of differential spectroscopy. J Hazard Mater 304:242–250
Mcclellan K, Halden RU, Ternes T, Gunten UV (2010) Pharmaceuticals and personal care products in archived U.S. biosolids from the 2001 EPA national sewage sludge survey. Water Res 44:658–668
Panizza M, Cerisola G (2009) Direct and mediated anodic oxidation of organic pollutants. Chem Rev 109:6541–6569
Rodarte-Morales AI, Feijoo G, Moreira MT, Lema JM (2011) Degradation of selected pharmaceutical and personal care products (PPCPs) by white-rot fungi. World J Microbiol Biotechnol 27:1839–1846
Sardar K, Petrucco E, Hiley CI, Sharman JDB, Wells PP, Russell AE, Kashtiban RJ, Sloan J, Walton RI (2014) Water-splitting Electrocatalysis in acid conditions using Ruthenate-Iridate Pyrochlores. Angew Chem Int Ed Engl 53:10960–10964
Shan CC, Tsai D, Huang YS, Jian S, Liang CC (2007) Pt−Ir−IrO2NT Thin-Wall Electrocatalysts derived from IrO2 nanotubes and their catalytic activities in methanol oxidation. Chem Mater 19:424–431
Smital T, Luckenbach T, Sauerborn R, Hamdoun AM, Vega RL, Epel D (2004) Emerging contaminants—pesticides, PPCPs, microbial degradation products and natural substances as inhibitors of multixenobiotic defense in aquatic organisms. Mutat Res Fundam Mol Mech Mutagen 552:101–117
Sun W, Song Y, Gong XQ, Cao L, Yang J (2015) An efficiently tuned d-orbital occupation of IrO2 by doping cu for enhancing oxygen evolution reaction activity. Chem Sci 6:4993–4999
Sun W, Cao L, Yang J (2016) Conversion of inert Cryptomelane-type manganese oxide into a highly efficient oxygen evolution catalyst via limited Ir doping. J Mater Chem A 4:12561–12570
Uranga-Flores A, Rosa-Júarez CDL, Gutierrez-Granados S, Moura DCD, Martínez-Huitle CA, Hernández JMP (2015) Electrochemical promotion of strong oxidants to degrade acid red 211: effect of supporting electrolytes. J Electroanal Chem 738:84–91
Wang J, Chu L (2016) Irradiation treatment of pharmaceutical and personal care products (PPCPs) in water and wastewater: an overview. Radiat Phys Chem 125:56–64
Wudarska E, Chrzescijanska E, Kusmierek E, Rynkowski J (2013) Voltammetric studies of acetylsalicylic acid electrooxidation at platinum electrode. Electrochim Acta 93:189–194
Xia Y, Dai Q, Chen J (2015a) Electrochemical degradation of aspirin using a Ni doped PbO 2 electrode. J Electroanal Chem 744:117–125
Xia Y, Dai Q, Weng M, Peng Y, Luo J, Meng X, Luo X, Chen J, Crittenden J (2015b) Fabrication and electrochemical treatment application of an al-doped PbO2Electrode with high oxidation capability, oxygen evolution potential and reusability. J Electrochem Soc 162:258–262
Zhang T, Zhang X, Ng J, Yang H, Liu J, Sun DD (2011) Fabrication of magnetic cryptomelane-type manganese oxide nanowires for water treatment. Chem Commun 47:1890
Zwiener C, Seeger S, Glauner T, Frimmel FH (2002) Metabolites from the biodegradation of pharmaceutical residues of ibuprofen in biofilm reactors and batch experiments. Anal Bioanal Chem 372:569–575
Author information
Authors and Affiliations
Corresponding author
Additional information
Responsible editor: Vítor Pais Vilar
Rights and permissions
About this article
Cite this article
Kang, X., Sun, W., Cao, L. et al. Highly efficient electro-oxidation catalyst under ultra-low voltage for degradation of aspirin. Environ Sci Pollut Res 24, 25881–25888 (2017). https://doi.org/10.1007/s11356-017-0207-8
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-017-0207-8