4.6 Article

Toward High Selectivity Aniline Synthesis Catalysis at Elevated Temperatures

Journal

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
Volume 60, Issue 49, Pages 17917-17927

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.iecr.1c03695

Keywords

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Funding

  1. College of Science and Engineering (GU) [EP/R513222/1, EP/N509668/1]
  2. School of Chemistry (GU) [EP/R513222/1, EP/N509668/1]
  3. Huntsman Polyurethanes [EP/R513222/1, EP/N509668/1]
  4. EPSRC [EP/R513222/1, EP/N509668/1]

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A study on Pd/Al2O3 catalysts for aniline production via nitrobenzene hydrogenation shows that the low loading catalyst is more suitable for enhancing aniline selectivity and avoiding the formation of overhydrogenated products. This is indicated by a volcano-like curve in aniline yield plotted against reaction conditions.
In connection with an initiative to enhance heat recovery from the large-scale operation of a heterogeneously catalyzed nitrobenzene hydrogenation process to produce aniline, it is necessary to operate the process at elevated temperatures (>100 degrees C), a condition that can compromise aniline selectivity. Alumina-supported palladium catalysts are selected as candidate materials that can provide sustained aniline yields at elevated temperatures. Two Pd/Al2O3 catalysts are examined that possess comparable mean Pd particle sizes (similar to 5 nm) for different Pd loading: 5 wt % Pd/Al2O3 and 0.3 wt % Pd/Al2O3. The higher Pd loading sample represents a reference catalyst for which the Pd crystallite morphology has previously been established. The lower Pd loading technical catalyst more closely corresponds to industrial specifications. The morphology of the Pd crystallites of the 0.3 wt % Pd/Al2O3 sample is explored by means of temperature-programmed infrared spectroscopy of chemisorbed CO. Reaction testing over the range of 60-180 degrees C shows effectively complete nitrobenzene conversion for both catalysts but with distinction in their selectivity profiles. The low loading catalyst is favored as it maximizes aniline selectivity and avoids the formation of overhydrogenated products. A plot of aniline yield as a function of WHSV for the 0.3 wt % Pd/Al2O3 catalyst at 100 degrees C yields a volcano like curve, indicating aniline selectivity to be sensitive to residence time. These observations are brought together to provide an indication of an aniline synthesis catalyst specification suited to a unit operation equipped for enhanced heat transfer.

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