Effect of Urine Compounds on the Electrochemical Oxidation of Urea Using a Nickel Cobaltite Catalyst: An Electroanalytical and Spectroscopic Investigation

被引:54
作者
Schranck, Andrew [1 ]
Marks, Randal [1 ]
Yates, Elon [2 ]
Doudrick, Kyle [1 ]
机构
[1] Univ Notre Dame, Dept Civil & Environm Engn & Earth Sci, Notre Dame, IN 46556 USA
[2] Florida A&M, Dept Civil & Environm Engn, Tallahassee, FL 32310 USA
关键词
ELECTROCATALYTIC OXIDATION; PHOSPHATE ADSORPTION; HYDROGEN-PRODUCTION; AQUEOUS-SOLUTIONS; SOURCE SEPARATION; CLOSED-SYSTEM; ELECTROOXIDATION; ELECTROLYSIS; METAL; CREATININE;
D O I
10.1021/acs.est.8b01743
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Cyclic voltammetry (CV) and in situ attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy were used to investigate the effect of major urine compounds on the electro-oxidation activity of urea using a nickel cobaltite (NiCo2O4) catalyst. As a substrate, carbon paper exhibited better benchmark potential and current values compared with stainless steel and fluorine-doped tin oxide glass, which was attributed to its greater active surface area per electrode geometric area. CV analysis of synthetic urine showed that phosphate, creatinine, and gelatin (i.e., proteins) had the greatest negative effect on the electro-oxidation activity of urea, with decreases in peak current up to 80% compared to that of a urea-only solution. Further investigation of the binding mechanisms of the deleterious compounds using in situ ATR-FTIR spectroscopy revealed that urea and phosphate weakly bind to NiCo(2)O(4 )through hydrogen bonding or long-range forces, whereas creatinine interacts strongly, forming deactivating inner-sphere complexes. Phosphate is presumed to disrupt the interaction between urea and NiCo(2)O(4 )by serving as a hydrogen-bond acceptor in place of catalyst sites. The weak binding of urea supports the hypothesis that it is oxidized through an indirect electron transfer. Outcomes of this study contribute to the development of electrolytic systems for treating source-separated urine.
引用
收藏
页码:8638 / 8648
页数:11
相关论文
共 93 条
  • [1] Effects of carbonate on the electrolytic removal of ammonia and urea from urine with thermally prepared IrO2 electrodes
    Amstutz, Veronique
    Katsaounis, Alexandros
    Kapalka, Agnieszka
    Comninellis, Christos
    Udert, Kai M.
    [J]. JOURNAL OF APPLIED ELECTROCHEMISTRY, 2012, 42 (09) : 787 - 795
  • [2] Analysis of phosphate adsorption onto ferrihydrite using the CD-MUSIC model
    Antelo, Juan
    Fiol, Sarah
    Perez, Claudio
    Marino, Silvia
    Arce, Florencio
    Gondar, Dora
    Lopez, Rocio
    [J]. JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2010, 347 (01) : 112 - 119
  • [3] Ethanol electro-oxidation reaction using a polycrystalline nickel electrode in alkaline media: Temperature influence and reaction mechanism
    Barbosa, A. F. B.
    Oliveira, V. L.
    van Drunen, J.
    Tremiliosi-Filho, G.
    [J]. JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2015, 746 : 31 - 38
  • [4] Substrate Selection for Fundamental Studies of Electrocatalysts and Photoelectrodes: Inert Potential Windows in Acidic, Neutral, and Basic Electrolyte
    Benck, Jesse D.
    Pinaud, Blaise A.
    Gorlin, Yelena
    Jaramillo, Thomas F.
    [J]. PLOS ONE, 2014, 9 (10):
  • [5] In situ vibrational study of the initial steps during urea electrochemical oxidation
    Bezerra, ACS
    deSa, EL
    Nart, FC
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (33): : 6443 - 6449
  • [6] Urea electrolysis: direct hydrogen production from urine
    Boggs, Bryan K.
    King, Rebecca L.
    Botte, Gerardine G.
    [J]. CHEMICAL COMMUNICATIONS, 2009, (32) : 4859 - 4861
  • [7] Brad A.J., 2000, Electrochemical Methods: Fundamentals and Applications, V2nd
  • [8] Strong hydrogen bond-mediated complexation of H2PO4- by neutral bis-thiourea hosts
    Buhlmann, P
    Nishizawa, S
    Xiao, KP
    Umezawa, Y
    [J]. TETRAHEDRON, 1997, 53 (05) : 1647 - 1654
  • [9] CREATININE - AN EXAMINATION OF ITS STRUCTURE AND SOME OF ITS REACTIONS BY SYNERGISTIC USE OF MNDO CALCULATIONS AND NUCLEAR MAGNETIC-RESONANCE SPECTROSCOPY
    BUTLER, AR
    GLIDEWELL, C
    [J]. JOURNAL OF THE CHEMICAL SOCIETY-PERKIN TRANSACTIONS 2, 1985, (09): : 1465 - 1467
  • [10] Size Fractionation of Two-Dimensional Sub-Nanometer Thin Manganese Dioxide Crystals towards Superior Urea Electrocatalytic Conversion
    Chen, Sheng
    Duan, Jingjing
    Vasileff, Anthony
    Qiao, Shi Zhang
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2016, 55 (11) : 3804 - 3808