Plasma-Catalytic Ammonia Synthesis beyond the Equilibrium Limit

Article

Abstract

We explore the consequences of nonthermal plasma-activation on product yields in catalytic ammonia synthesis, a reaction that is equilibrium-limited at elevated temperatures. We employ a minimal microkinetic model that incorporates the influence of plasma-activation on N2 dissociation rates to predict NH3 yields into and across the equilibrium-limited regime. NH3 yields are predicted to exceed bulk thermodynamic equilibrium limits on materials that are thermal-rate-limited by N2 dissociation. In all cases, yields revert to bulk equilibrium at temperatures at which thermal reaction rates exceed plasma-activated ones. Beyond-equilibrium NH3 yields are observed in a packed bed dielectric barrier discharge reactor and exhibit sensitivity to catalytic material choice in a way consistent with model predictions. The approach and results highlight the opportunity to exploit synergies between nonthermal plasmas and catalysts to affect transformations at conditions inaccessible through thermal routes. KEYWORDS:

Attributes

Attribute NameValues
Creator
  • Prateek Mehta

  • Patrick Barboun

  • Yannick Engelmann

  • David Go

  • Annemie Bogaerts

  • William Schneider

  • Jason Hicks

Journal or Work Title
  • Catalysis

Volume
  • 10

Issue
  • 12

First Page
  • 6726

Last Page
  • 6734

ISSN
  • 21555435

Publication Date
  • 2020-05

Subject
  • Titan TEM

  • X-Ray Diffractometer

Publisher
  • American Chemical Society

Date Created
  • 2020-11-17

Language
  • English

Departments and Units
Record Visibility Public
Content License
  • All rights reserved

Digital Object Identifier

doi:10.1021/acscatal.0c00684

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