Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 131, Issue 40, Pages 14172-+Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja905446t
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Funding
- National Science Foundation [CHE 0718078, CBET 0730050]
- WaterCAMPWS at UIUC [CTS-0120978]
- China Scholarship Council [2008620016]
- U.S. DOE [DE-FG02-07ER46453, DE-FG02-07ER46471]
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New bimetallic heterogeneous catalysts for the reduction of perchlorate in water with dihydrogen have been prepared in two ways: (1) by impregnating 5 wt % Pd on activated carbon powder with one of the complexes trans-[ReO2(py-X)(4)](+) (py-X = 4-substituted pyridine; X = H, Me, OMe, NMe2) or (2) by adsorbing perrhenate onto the Pd/C powder in the presence of the pyridine Ligand under a hydrogen atmosphere. Both sets of catalysts are highly active at pH 2.7-3.0 (HCl), with observed rates increasing with varying X in the order H < Me < C)Me < NMe2, which supports a rate-determining oxygen atom transfer reaction involving the Re(V) centers. However, the materials prepared by method (1) show evidence of facile formation of perrhenate from handling under ambient conditions. A system prepared by method (2) with 2 equiv of dimethylaminopyridine per Re is especially active and stable up to pH 4.5.
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