open access publication

Article, 2021

Tailored monolith supports for improved ultra-low temperature water-gas shift reaction

Reaction Chemistry & Engineering, ISSN 2058-9883, Volume 6, 11, Pages 2114-2124, 10.1039/d1re00226k

Contributors

Portela, Raquel 0000-0002-1882-4759 [1] Wolf, Patrick 0000-0002-9467-5812 [2] Marinkovic, Jakob Maximilian 0000-0002-0630-5679 [3] Serrano-Lotina, Ana 0000-0001-7498-7491 [1] Riisager, Anders 0000-0002-7086-1143 [3] Haumann, Marco 0000-0002-3896-365X [2]

Affiliations

  1. [1] Spanish National Research Council
  2. [NORA names: Spain; Europe, EU; OECD];
  3. [2] University of Erlangen-Nuremberg
  4. [NORA names: Germany; Europe, EU; OECD];
  5. [3] Technical University of Denmark
  6. [NORA names: DTU Technical University of Denmark; University; Denmark; Europe, EU; Nordic; OECD]

Abstract

A monolithic γ-Al 2 O 3 support is developed to scale up the WGS process using the supported ionic liquid-phase concept in a structured reactor. The support-ionic liquid-catalyst system maximizes loading and mechanical resistance while achieving high activity and selectivity. Supported ionic liquid-phase (SILP) particulate catalysts consisting of Ru-complexes dissolved in an ionic liquid that is dispersed on a γ-alumina porous substrate facilitate the water-gas shift (WGS) reaction at ultra-low temperatures. In this work, a screening of different ceramic support materials was performed to design a suitable monolithic support to disperse the SILP system with the objective of scaling up the WGS process efficiently. γ-Alumina-rich channeled monoliths were developed with the use of natural clays as binders (10 wt% bentonite and 20 wt% sepiolite) with the following properties: i) high volume of mesopores to maximize the catalyst loading and successfully immobilize the ionic liquid-catalyst system via capillary forces, ii) mechanical resistance to withstand the impregnation process and the reaction operating conditions, and iii) surface chemistry compatible with a highly active and selective phase for WGS. The developed monolithic-SILP catalyst demonstrated high stability and long-term WGS performance at 130 °C with an average steady-state CO conversion of around 30% after 190 h time-on-stream (TOS) and a conversion of 23% after 320 h TOS. Interestingly, the catalyst activity proved essentially unaffected by variation in the water partial pressure during operation due to accumulation of water in the monolith, thus making the system highly durable.

Keywords

CO conversion, Ru complexes, SILP, SILP system, WGS, WGS performance, WGS process, accumulation, activity, binder, capillary forces, catalyst, catalyst activity, catalyst loading, ceramic support materials, chemistry, clay, concept, conditions, conversion, force, g-alumina, impregnation, impregnation process, ionic liquid catalyst system, ionic liquids, liquid, load, materials, mechanical resistance, mesopores, monolithic supports, monoliths, natural clay, objective, operating conditions, operation, partial pressure, particulate catalysts, performance, porous substrate, pressure, process, properties, reaction, reaction operating conditions, reactor, resistance, screening, selection, shift reaction, stability, steady-state CO conversion, structured reactors, substrate, support, support material, surface, surface chemistry, system, temperature, time-on-stream, ultra-low temperatures, variation, volume, volume of mesopores, water, water partial pressure, water-gas shift (WGS) reaction, water-gas shift reaction

Funders

  • Spanish National Research Council
  • Bavarian State Ministry of Education Science and the Arts
  • European Commission

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