Janus Electrode of Asymmetric Wettability for H2O2 Production with Highly Efficient O2 Utilization

被引:69
作者
Zhang, Haichuan [1 ,2 ,3 ]
Zhao, Yingshuang [1 ,2 ,3 ]
Li, Yingjie [4 ]
Li, Guanghe [1 ,2 ,3 ]
Li, Juan [5 ]
Zhang, Fang [1 ,2 ,3 ]
机构
[1] Tsinghua Univ, Sch Environm, Beijing 100084, Peoples R China
[2] Tsinghua Univ, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China
[3] Natl Engn Lab Site Remediat Technol, Beijing 100015, Peoples R China
[4] Peking Univ, Dept Mat Sci & Engn, Coll Engn, Beijing 100871, Peoples R China
[5] Beijing Inst Technol, Adv Res Inst Multidisciplinary Sci, Beijing 100081, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
Janus electrode; asymmetric wettability; two-electron oxygen reduction reaction; H2O2; production; oxygen utilization efficiency; GAS-DIFFUSION ELECTRODES; HYDROGEN-PEROXIDE; OXYGEN REDUCTION; CARBON; GENERATION; ELECTROGENERATION; OXIDATION; ELECTROCATALYST; MINERALIZATION; CATHODE;
D O I
10.1021/acsaem.9b01908
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Aeration-based electrochemical systems to produce H2O2 face two major challenges: O-2 mass transfer limitation and low utilization efficiency of sparged oxygen. To mitigate these problems, a Janus electrode (JE) of asymmetric wettability with hydrophobic gas storage layer (GSL) and hydrophilic catalyst layer (CL) was successfully fabricated by substrate hydrophobization and a subsequent catalyst-coating treatment. When O-2 was sparged at 6 mL min(-1), the JE obtained a H2O2 generation rate of 2.8 +/- 0.02 mg h(-1) cm(-2) with oxygen utilization efficiency (OUE) of 5.0 +/- 0.7% at -0.4 V vs Ag/AgCl, much higher than those of hydrophobic electrodes (1.1 +/- 0.3 mg h(-1) cm(-2), OUE of 2.0 +/- 0.5%) and hydrophilic electrodes (0.1 +/- 0.004 mg h (-1) cm(-2), OUE of 0.2 +/- 0.01%). The improved performance with JE was attributed to an adequate oxygen supply from hydrophobic GSL and abundant active sites in hydrophilic CL. With the critical aeration rate of 0.5 mL min(-1), the JE obtained an extremely high OUE of 37.4 +/- 3.7%. With the applied potential increase to -1.0 V vs Ag/AgCl, the H2O2 generation rate of JE consequently improved to 19.5 +/- 0.4 mg h(-1) cm(-2). This asymmetric structure of the Janus electrode successfully mitigated the O-2 mass transport limitation and reduced the O-2 bubble waste for H2O2 production, enabling more energy-efficient and cost-effective electrochemical remediation processes.
引用
收藏
页码:705 / 714
页数:19
相关论文
共 39 条
[1]   Comparative study of hydrogen peroxide electro-generation on gas-diffusion electrodes in undivided and membrane cells [J].
Agladze, G. R. ;
Tsurtsumia, G. S. ;
Jung, B. -I. ;
Kim, J. -S. ;
Gorelishvili, G. .
JOURNAL OF APPLIED ELECTROCHEMISTRY, 2007, 37 (03) :375-383
[2]   In Situ Electrochemical Generation of Hydrogen Peroxide in Alkaline Aqueous Solution by using an Unmodified Gas Diffusion Electrode [J].
Barros, Willyam R. P. ;
Ereno, Thais ;
Tavares, Ana C. ;
Lanza, Marcos R. V. .
CHEMELECTROCHEM, 2015, 2 (05) :714-719
[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]   Mineralization of 2,4-D by advanced electrochemical oxidation processes [J].
Brillas, E ;
Calpe, JC ;
Casado, J .
WATER RESEARCH, 2000, 34 (08) :2253-2262
[5]   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
[6]   Electrochemical durability of gas diffusion layer under simulated proton exchange membrane fuel cell conditions [J].
Chen, Guobao ;
Zhang, Huamin ;
Ma, Haipeng ;
Zhong, Hexiang .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2009, 34 (19) :8185-8192
[7]  
Eddy M.a., 2003, Wastewater Engineering Treatment and Reuse
[8]   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
[9]   Effects of poly-1,5-diaminoanthraquinone morphology on oxygen reduction in acidic solution [J].
Gao, Mingming ;
Yang, Fenglin ;
Zhang, Guoquan ;
Liu, Lifen ;
Wang, Xinhua .
ELECTROCHIMICA ACTA, 2009, 54 (08) :2224-2228
[10]   In-Plane Carbon Lattice-Defect Regulating Electrochemical Oxygen Reduction to Hydrogen Peroxide Production over Nitrogen-Doped Graphene [J].
Han, Lei ;
Sun, Yanyan ;
Li, Shuang ;
Cheng, Chong ;
Halbig, Christian E. ;
Feicht, Patrick ;
Huebner, Jessica Liane ;
Strasser, Peter ;
Eigler, Siegfried .
ACS CATALYSIS, 2019, 9 (02) :1283-1288