Palladium-indium catalyzed reduction of N-nitrosodimethylamine:: Indium as a promoter metal

被引:57
作者
Davie, Matthew G. [1 ]
Shih, Kaimin [1 ]
Pacheco, Federico A. [1 ]
Leckie, James O. [1 ]
Reinhard, Martin [1 ]
机构
[1] Stanford Univ, Dept Civil & Environm Engn, Stanford, CA 94305 USA
关键词
D O I
10.1021/es7023115
中图分类号
X [环境科学、安全科学];
学科分类号
08 [工学]; 0830 [环境科学与工程];
摘要
An emerging technology for the removal of N-nitrosodimethylamine (NDMA) from drinking and groundwater is reductive destruction using noble metal catalysts and hydrogen gas as a reducing agent. Bimetallic palladium-indium (Pd-In) supported on alumina combines the ability of Into activate NDMA with the hydrogen activating properties of Pd. This study examined the effect of In addition to a commercial 5% Pd by weight on gamma-Al2O3 catalyst on the efficacy of NDMA reduction. The pseudo-first-order rate constant increased proportionately to In loading from 0.057 h(-1) for 0% In to a maximum of 0.25 h(-1) for 1% In and then decreased with additional In loading. Data suggest that hydrogen activation occurred only on Pd surfaces and In activated NDMA 20 times more effectively than Pd on a mass basis. The rate-limiting factor was NDMA activation for In loadings below 1%. The decrease at higher loadings is interpreted as In blocking pore spaces and limiting access to Pd sites, suggesting monatomic hydrogen limitation. The only products detected were dimethylamine and ammonium with carbon and nitrogen balances in excess of 92%, consistent with a mechanism involving reductive N-N bond cleavage. Results from this study serve as a basis for optimizing bimetallic catalysts for treating NDMA contaminated waters.
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收藏
页码:3040 / 3046
页数:7
相关论文
共 41 条
[1]
SOLUBILITY OF HYDROGEN IN SMALL PARTICLES OF PALLADIUM [J].
BOUDART, M ;
HWANG, HS .
JOURNAL OF CATALYSIS, 1975, 39 (01) :44-52
[2]
Boudart M., 2014, KINETICS HETEROGENEO
[3]
*CA DHS, 2006, BRIEF HIST NDMA FIND
[4]
Effects of natural water ions and humic acid on catalytic nitrate reduction kinetics using an alumina supported Pd-Cu catalyst [J].
Chaplin, BP ;
Roundy, E ;
Guy, KA ;
Shapley, JR ;
Werth, CJ .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (09) :3075-3081
[5]
Regeneration of sulfur-fouled bimetallic Pd-based catalysts [J].
Chaplin, Brian P. ;
Shapley, John R. ;
Werth, Charles J. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2007, 41 (15) :5491-5497
[6]
Mechanistic studies of N-nitrosodimethylamine (NDMA) formation in chlorinated drinking water [J].
Choi, J ;
Duirk, SE ;
Valentine, RL .
JOURNAL OF ENVIRONMENTAL MONITORING, 2002, 4 (02) :249-252
[7]
Metal-catalyzed reduction of N-nitrosodimethylamine with hydrogen in water [J].
Davie, Matthew G. ;
Reinhard, Martin ;
Shapley, John R. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (23) :7329-7335
[8]
Reduction of N-nitrosodimethylamine with granular iron and nickel enhanced iron.: 1.: Pathways and kinetics [J].
Gui, L ;
Gillham, RW ;
Odziemkowski, MS .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2000, 34 (16) :3489-3494
[10]
UV photolytic mechanism of N-nitrosodimethylamine in water: Dual pathways to methylamine versus dimethylamine [J].
Lee, C ;
Choi, W ;
Kim, YG ;
Yoon, J .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2005, 39 (07) :2101-2106