Palladium nanoparticles for catalytic reduction of Cr(VI) using formic acid

被引:181
作者
Omole, Marcells A. [1 ]
K'Owino, Isaac O. [1 ]
Sadik, Omowunmi A. [1 ]
机构
[1] SUNY Binghamton, Dept Chem, Binghamton, NY 13902 USA
基金
美国国家科学基金会;
关键词
pd; nanoparticles; reduction; catalyst; formic acid;
D O I
10.1016/j.apcatb.2007.05.018
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
Cr(VI), a leading contaminant in most hazardous waste sites, is acutely toxic, a proven mutagen and a carcinogen whereas Cr(III) is believed to be an essential element. We describe a one-pot synthesis and characterization of palladium nanoparticles (PdNPs) using transmission electron microscopy (TEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD) and C-13 nuclear magnetic resonance (NMR). The resulting PdNPs were used as catalyst to demonstrate a new concept for the reduction of Cr(VI) to Cr(III) using formic acid as a reducing agent. Percentage decrease in the concentration of Cr(VI) as a function of time was monitored using UV/vis spectroscopy at a fixed wavelength of 350 nm. Results showed that the reduction follows first-order reaction kinetics with respect to initial concentrations of Cr(VI) and HCOOH. The leveling off in reaction rate with respect to PdNPs loading confirms the importance of surface reaction as the rate-controlling step. The rate of Cr(VI) reduction was found to be dependent on temperature, pH, amount of PdNPs and formic acid concentrations, with the optimum at 45 degrees C under acidic conditions. For every 0.1 M increment in formic acid concentration, there was a corresponding 18.4% enhancement in the reduction rate. Consequently, it took 5 min for the PdNPs to catalyze the reduction of a 7.14 mM concentration of Cr(VI) at 99.8% efficiency. Subsequent practical application in environmental samples indicates a complete elimination of Cr(VI) from the tested soil and aqueous media. (C) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:158 / 167
页数:10
相关论文
共 38 条
  • [1] Abass E., 2005, AM J APPL SCI, V2, P1471, DOI DOI 10.3844/AJASSP.2005.1471.1473
  • [2] ANDERSON RA, 1995, NUTRITION, V11, P83
  • [3] Nanostructured polyamic acid membranes as novel electrode materials
    Andreescu, D
    Wanekaya, AK
    Sadik, OA
    Wang, J
    [J]. LANGMUIR, 2005, 21 (15) : 6891 - 6899
  • [4] [Anonymous], 1996, GUIDELINES DRINKING
  • [5] The electro-oxidation of formic acid on Pt-Pd single crystal bimetallic surfaces
    Arenz, M
    Stamenkovic, V
    Schmidt, TJ
    Wandelt, K
    Ross, PN
    Markovic, NM
    [J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2003, 5 (19) : 4242 - 4251
  • [6] Bonding and motional aspects of CO adsorbed on the surface of Pt nanoparticles decorated with Pd
    Babu, PK
    Kim, HS
    Chung, JH
    Oldfield, E
    Wieckowski, A
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (52) : 20228 - 20232
  • [7] Formic acid oxidation on ultrathin Pd films on Au(hkl) and Pt(hkl) electrodes
    Baldauf, M
    Kolb, DM
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (27) : 11375 - 11381
  • [8] BALDI G, 1974, IND ENG CHEM PROC DD, V13, P447, DOI 10.1021/i260052a026
  • [9] In-situ remediation of Cr(VI)-contaminated groundwater using permeable reactive walls: Laboratory studies
    Blowes, DW
    Ptacek, CJ
    Jambor, JL
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1997, 31 (12) : 3348 - 3357
  • [10] Incorporation of metal nanoparticles in photopolymerized organic conducting polymers: A mechanistic insight
    Breimer, MA
    Yevgeny, G
    Sy, S
    Sadik, OA
    [J]. NANO LETTERS, 2001, 1 (06) : 305 - 308