title: Enhanced activity and selectivity of carbon nanofiber supported Pd catalysts for nitrite reduction.
abstract: Pd-based catalyst treatment represents an emerging technology that shows promise to remove nitrate and nitrite from drinking water. In this work we use vapor-grown carbon nanofiber (CNF) supports in order to explore the effects of Pd nanoparticle size and interior versus exterior loading on nitrite reduction activity and selectivity (i.e., dinitrogen over ammonia production). Results show that nitrite reduction activity increases by 3.1-fold and selectivity decreases by 8.0-fold, with decreasing Pd nanoparticle size from 1.4 to 9.6 nm. Both activity and selectivity are not significantly influenced by Pd interior versus exterior CNF loading. Consequently, turnover frequencies (TOFs) among all CNF catalysts are similar, suggesting nitrite reduction is not sensitive to Pd location on CNFs nor Pd structure. CNF-based catalysts compare favorably to conventional Pd catalysts (i.e., Pd on activated carbon or alumina) with respect to nitrite reduction activity and selectivity, and they maintain activity over multiple reduction cycles. Hence, our results suggest new insights that an optimum Pd nanoparticle size on CNFs balances faster kinetics with lower ammonia production, that catalysts can be tailored at the nanoscale to improve catalytic performance for nitrite, and that CNFs hold promise as highly effective catalyst supports in drinking water treatment.
authors.affiliation: Department of Civil and Environmental Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.
authors.forename: Danmeng
authors.initials: D
authors.lastname: Shuai
authors.forename: Jong Kwon
authors.initials: JK
authors.lastname: Choe
authors.forename: John R
authors.initials: JR
authors.lastname: Shapley
authors.forename: Charles J
authors.initials: CJ
authors.lastname: Werth
mesh_terms: D000641:Ammonia / Q000032:analysis; D002244:Carbon / Q000737:chemistry*; D002384:Catalysis; D004777:Environment; D007700:Kinetics; D057139:Nanofibers / Q000737:chemistry* / Q000648:ultrastructure; D053758:Nanoparticles / Q000737:chemistry / Q000648:ultrastructure; D009573:Nitrites / Q000737:chemistry*; D010084:Oxidation-Reduction; D010165:Palladium / Q000737:chemistry*; D010316:Particle Size; D013010:Sonication
chemical_list: D009573:Nitrites; D010165:Palladium; D002244:Carbon; D000641:Ammonia