Comparing methods to deposit Pd-In catalysts on hydrogen-permeable hollow-fiber membranes for nitrate reduction

Juliana Levi, Sujin Guo, Shalinee Kavadiya, Yihao Luo, Chung Seop Lee, Hunter P. Jacobs, Zachary Holman, Michael S. Wong, Sergi Garcia-Segura, Chen Zhou, Bruce E. Rittmann, Paul Westerhoff

Research output: Contribution to journalArticlepeer-review

Abstract

Catalytic hydrogenation of nitrate in water has been studied primarily using nanoparticle slurries with constant hydrogen-gas (H2) bubbling. Such slurry reactors are impractical in full-scale water treatment applications because 1) unattached catalysts are difficult to be recycled/reused and 2) gas bubbling is inefficient for delivering H2. Membrane Catalyst-film Reactors (MCfR) resolve these limitations by depositing nanocatalysts on the exterior of gas-permeable hollow-fiber membranes that deliver H2 directly to the catalyst-film. The goal of this study was to compare the technical feasibility and benefits of various methods for attaching bimetallic palladium/indium (Pd/In) nanocatalysts for nitrate reduction in water, and subsequently select the most effective method. Four Pd/In deposition methods were evaluated for effectiveness in achieving durable nanocatalyst immobilization on the membranes and repeatable nitrate-reduction activity: (1) In-Situ MCfR-H2, (2) In-Situ Flask-Synthesis, (3) Ex-Situ Aerosol Impaction-Driven Assembly, and (4) Ex-Situ Electrostatic. Although all four deposition methods achieved catalyst-films that reduced nitrate in solution (≥ 1.1 min−1gPd−1), three deposition methods resulted in significant palladium loss (>29%) and an accompanying decline in nitrate reactivity over time. In contrast, the In-Situ MCfR-H2 deposition method had negligible Pd loss and remained active for nitrate reduction over multiple operational cycles. Therefore, In-Situ MCfR-H2 emerged as the superior deposition method and can be utilized to optimize catalyst attachment, nitrate-reduction, and N2 selectivity in future studies with more complex water matrices, longer treatment cycles, and larger reactors.

Original languageEnglish (US)
Article number119877
JournalWater Research
Volume235
DOIs
StatePublished - May 15 2023

Keywords

  • Catalysis
  • Groundwater
  • Hydrogen
  • Nitrogen
  • Water treatment

ASJC Scopus subject areas

  • Environmental Engineering
  • Civil and Structural Engineering
  • Ecological Modeling
  • Water Science and Technology
  • Waste Management and Disposal
  • Pollution

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