Carbon Black Oxidized by Air Calcination for Enhanced H2O2 Generation and Effective Organics Degradation

被引:136
作者
Zhang, Haichuan [1 ,2 ,3 ,4 ]
Li, Yingjie [5 ]
Zhao, Yingshuang [1 ,2 ,3 ,4 ]
Li, Guanghe [1 ,2 ,3 ,4 ]
Zhang, Fang [1 ,2 ,3 ,4 ]
机构
[1] Natl Engn Lab Site Remediat Technol, Beijing 100015, Peoples R China
[2] Tsinghua Univ, Minist Educ China, Sch Environm, Beijing 100084, Peoples R China
[3] Tsinghua Univ, Minist Educ China, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China
[4] Tsinghua Univ, Minist Educ China, Key Lab Solid Waste Management & Environm Safety, Beijing 100084, Peoples R China
[5] Peking Univ, Coll Engn, Dept Mat Sci & Engn, Beijing 100871, Peoples R China
基金
中国国家自然科学基金;
关键词
oxidized carbon black; oxygen functional groups; two-electron oxygen reduction reaction; H2O2; production; electrochemical advanced oxidation processes; NITROGEN-DOPED CARBON; OXYGEN REDUCTION REACTION; PT/C CATALYTIC CATHODE; HYDROGEN-PEROXIDE; ELECTROCHEMICAL PROPERTIES; DURABILITY ENHANCEMENT; FUNCTIONAL-GROUPS; ELECTRODES; GRAPHITE; SURFACE;
D O I
10.1021/acsami.9b07765
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Carbon black (CB) has a high conductivity and a large surface area, which are the basis of an excellent electrocatalyst. However, CB itself is usually less active or even inactive toward two-electron oxygen reduction reaction (2e(-) ORR) due to the absence of highly active functional groups with low oxygen content. To activate commercial CB for 2e(-) ORR, oxygen-containing functional groups were introduced onto the CB surface by a simple air calcination method. After the oxidation treatment at 600 degrees C (CB600), the oxygen content increased from the initial 1.17 +/- 0.15 to 4.08 +/- 0.60%, leading to a dramatic increase of the cathodic current from only -8.1 mA (CB) to -117.6 mA (CB600). The air cathode made of CB600 achieved the maximum H2O2 production of 517.7 +/- 2.4 mg L-1 within 30 min, resulting in the removal of similar to 91.1% rhodamine B in 2 min and an effective mineralization of similar to 76.3% in an electro-Fenton reactor. This performance was much better than that obtained using the CB catalyst (65.3 +/- 5.6 mg L-1 H2O2 production, and similar to 20.3% mineralization). This excellent activity of CB600 toward 2e(-) ORR was greatly improved by the introduction of O=C-OH and C-O-C groups. The successful improvement of the 2(e-)ORR activity of CB using air calcination enables its practical application in electrochemical advanced oxidation processes.
引用
收藏
页码:27846 / 27853
页数:8
相关论文
共 44 条
[1]   A comparative study of the electrogeneration of hydrogen peroxide using Vulcan and Printex carbon supports [J].
Assumpcao, M. H. M. T. ;
De Souza, R. F. B. ;
Rascio, D. C. ;
Silva, J. C. M. ;
Calegaro, M. L. ;
Gaubeur, I. ;
Paixao, T. R. L. C. ;
Hammer, P. ;
Lanza, M. R. V. ;
Santos, M. C. .
CARBON, 2011, 49 (08) :2842-2851
[2]   Electro-peroxone treatment of Orange II dye wastewater [J].
Bakheet, Belal ;
Yuan, Shi ;
Li, Zhaoxin ;
Wang, Huijiao ;
Zuo, Jiane ;
Komarneni, Sridhar ;
Wang, Yujue .
WATER RESEARCH, 2013, 47 (16) :6234-6243
[3]   Electrogeneration of hydrogen peroxide in acidic medium using gas diffusion electrodes modified with cobalt (II) phthalocyanine [J].
Barros, Willyam R. P. ;
Reis, Rafael M. ;
Rocha, Robson S. ;
Lanza, Marcos R. V. .
ELECTROCHIMICA ACTA, 2013, 104 :12-18
[4]   Electro-Fenton Process and Related Electrochemical Technologies Based on Fenton's Reaction Chemistry [J].
Brillas, Enric ;
Sires, Ignasi ;
Oturan, Mehmet A. .
CHEMICAL REVIEWS, 2009, 109 (12) :6570-6631
[5]   Chemical oxidation of multiwalled carbon nanotubes [J].
Datsyuk, V. ;
Kalyva, M. ;
Papagelis, K. ;
Parthenios, J. ;
Tasis, D. ;
Siokou, A. ;
Kallitsis, I. ;
Galiotis, C. .
CARBON, 2008, 46 (06) :833-840
[6]   THE OXYGEN ELECTRODE .1. ISOTOPIC INVESTIGATION OF ELECTRODE MECHANISMS [J].
DAVIES, MO ;
CLARK, M ;
YEAGER, E ;
HOVORKA, F .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1959, 106 (01) :56-61
[7]   Mesoporous Nitrogen-Doped Carbon for the Electrocatalytic Synthesis of Hydrogen Peroxide [J].
Fellinger, Tim-Patrick ;
Hasche, Frederic ;
Strasser, Peter ;
Antonietti, Markus .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (09) :4072-4075
[8]   Interpretation of Raman spectra of disordered and amorphous carbon [J].
Ferrari, AC ;
Robertson, J .
PHYSICAL REVIEW B, 2000, 61 (20) :14095-14107
[9]   Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction [J].
Gong, Kuanping ;
Du, Feng ;
Xia, Zhenhai ;
Durstock, Michael ;
Dai, Liming .
SCIENCE, 2009, 323 (5915) :760-764
[10]   Active sites of nitrogen-doped carbon materials for oxygen reduction reaction clarified using model catalysts [J].
Guo, Donghui ;
Shibuya, Riku ;
Akiba, Chisato ;
Saji, Shunsuke ;
Kondo, Takahiro ;
Nakamura, Junji .
SCIENCE, 2016, 351 (6271) :361-365