Center for Environmentally Beneficial Catalysis
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postdoc working in lab"Revolutionary spray oxidation process for terephthalic acid"

A good target for cleaning up and cutting costs is terephthalic acid—a giant among commodity chemicals. A staggering 100 billion pounds of this white sandy powder are made annually, mostly for use in plastic bottles, easy-care fabrics and food packaging. 

Currently, the standard commercial process for making polymer-grade terephthalic acid requires an extra purification step.  Eliminating the need for this costly step would save energy and cut operating costs.  A novel spray reactor technology being developed at CEBC shows promise at achieving this goal.  Economic assessments show that the spray process has the potential to lower operating costs by 16%.  It also conserves feedstock and solvents by reducing burning in the reactor.  The team is currently adapting the technology to other oxidation processes, such as the one for making 2,5-furandicarboxylic acid, a renewable PET plastic monomer replacement.
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researchers in lab"Novel epoxidation process for light olefins with no CO2 byproduct"

Researchers are developing a process that applies to the manufacture of both ethylene oxide and propylene oxide, two major building-block chemicals. Compared to the commercial process, CEBC's  award-winning, low-temperature ethylene epoxidation process eliminates burning of feed/product and maximizes substrate utilization toward the desired product. The economics are currently on par with the conventional process, and projected to cost 17% less with advances in catalyst durability, peroxide efficiencies, and use of mixed ethylene feedstock. The growing supply of ethylene in the U.S. and strong plastics demand could give a global advantage to U.S.-based companies who license this technology.  Read more:

  • CEBC receives $4.4 million from NSF and EPA to design safer chemical manufacturing processes
  • Ramanathan, A.; Maheswari, R.; Barich, D. H.; Subramaniam, B. "Niobium incorporated mesoporous silicate, Nb-KIT-6: Synthesis and characterization," Micro. Meso. Mat. 2014 190 240-247. (Abstract)
  • Pan, Q.; Ramanathan, A.; Snavely, W.K.; Chaudhari, R.V.; Subramaniam, B. "Synthesis and Dehydration Activity of Novel Lewis Acidic Ordered Mesoporous Silicate: Zr-KIT-6," Ind. Eng. Chem. Res. 2013 52:44 15481-15487. (Abstract)
  • Graduate Student Wins Prestigious Green Chemistry Award
  • Ghanta, M.; Lee, H.-J.; Busch, D.H.; Subramaniam, B. "Highly Selective Homogeneous Ethylene Epoxidation in Gas (Ethylene)-Expanded Liquid: Transport and Kinetic Studies," AIChE J. 2013 59:1 180-187. (Abstract)
  • Ghanta, M.; Ruddy, T.; Fahey, D.; Busch, D.; Subramaniam, B. "Is the Liquid-Phase H2O2-based Ethylene Oxide Process More Economical and Greener Than the Gas-Phase O2-based Silver-Catalyzed Process?" Ind. Eng. Chem. Res. 2013 52:1 18-29. (Abstract)

hydroformylation"Hydroformylation innovations"

Hydroformylation is a common industrial reaction used to produce basic building blocks for all sorts of consumer goods, including pharmaceuticals, detergents, plastics, and many more.

CEBC has several projects underway to improve the hydroformylation process.  For example, the team has discovered that using gas-expanded liquids significantly improves catalyst activity and selectivity to desired products. They're also developing tools for effectively retaining costly rhodium catalysts in the reactor by nanofiltration membranes.  The research is finding new application opportunities, such as 1,4-butanediol ($41B market) from biomass.

A collaboration with computational chemists is helping the team better understand the catalytic mechanism at the molecular level.  The work is proving especially useful at elucidating the impact of phosphine ligand properties on experimentally observed regioselectivity trends. 
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  • Can A Greener Chemical Process Be Economical Too?
  • Xie, Z.; Fang, J.; Subramaniam, B.; Maiti, S.K.; Snavely, W.; Tunge, J. A. "Enhanced hydroformylation by carbon dioxide-expanded media with soluble Rh complexes in nanofiltration membrane reactors," AIChE J. 2013 59:11 4287-4296. (Abstract)
  • Fang, J.; Jana, R.; Tunge, J. A.; Subramaniam, B. "Continuous homogeneous hydroformylation with bulky rhodium catalyst complexes retained by nano-filtration membranes," App. Catal. A 2011 393:1-2 294-301. (Abstract)

"New catalysts for hydrogenolysis of plant-derived polyols"Sample image

Polyols are oxygen-containing compounds that are readily derived from biomass. However, converting them into higher value materials requires replacing those oxygen atoms with hydrogen, a costly process that uses fossil fuel-derived hydrogen. Using a clever design, CEBC researchers are able to produce hydrogen at the  catalytic site and simultaneously use it in the reaction.  These novel catalysts eliminate the need for adding fossil-based hydrogen to the system and could one day lead to a safer, greener and cheaper route to bio-based chemicals.   Read more:

  • Sweeten Up: From Sugars to High-Value Chemicals
  • Lactic Acid Article One of ACS Catalysis Top 10
  • Wan, H.; Vitter, A.; Chaudhari, R. V.; Subramaniam, B. "Kinetic investigations of unusual solvent effects during Ru/C catalyzed hydrogenation of model oxygenates," J. Catal. 2014 309 174-184. (Abstract)
  • Jin, X.; Roy, D.; Thapa, P.S.; Subramaniam, B.; Chaudhari, R.V. "Atom Economical Aqueous-Phase Conversion (APC) of Biopolyols to Lactic Acid, Glycols, and Linear Alcohols Using Supported Metal Catalysts," ACS Sus. Chem. Eng. 2013 1:11 1453-1462. (Abstract)
  • Chaudhari, R.V.; Torres, A.; Jin, X.; Subramaniam, B. "Multiphase Catalytic Hydrogenolysis/Hydrodeoxygenation Processes for Chemicals from Renewable Feedstocks: Kinetics, Mechanism, and Reaction Engineering," Ind. Eng. Chem. Res. 2013 52:44 15226-15243. (Abstract)

"Metal nanocatalysts for biomass conversion"Sample image

Researchers at CEBC are developing novel graphene-based nanocatalysts for converting biomass-derived substrates into valuable chemical intermediates, such as lactic acid and polyethylene glycol.  The team's goal is to design highly active, selective and stable catalysts that function at mild conditions and can be recycled many times. Graphene-supported metal catalysts show promise because of their low-cost, high activity and selectivity, and excellent durability.
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  • Prof. Shenqiang Ren's research website
  • Jin, X.; Dang, L.; Lohrman, J.; Subramaniam, B.; Ren, S.; Chaudhari, R.V. "Lattice-Matched Bimetallic CuPd-Graphene Nanocatalysts for Facile Conversion of Biomass-Derived Polyols to Chemicals," ACS Nano 2013 7:2 1309-1316. (Abstract)

"Rapid screening technique for new photo- and electro-catalysts"Sample image

There is a great need to develop inexpensive, stable and highly active photo- and electro-catalysts. To reach this goal, researchers are utilizing an innovative rapid screening technique called scanning electrochemical microscopy to sift through thousands of combinations of two or more readily abundant metals to find useful catalysts.

The team built its own custom instrument for both screening and electrochemical characterization. It includes a custom-built device that can analyze 64 samples at a time. A 3D printer is used to deposit tiny dots of different materials onto the screening device, and then an electrode is moved across the array of dots to map out which material composites are worth a closer look.

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"Developing novel solid catalysts with large pores for biomass conversions"Researcher by poster

Various materials can serve as supports for metal catalysts.  For example, zeolites--a microporous aluminosilicate mineral--has been used for decades as a support for solid acid catalysts. But these materials are constrained by their tiny pore sizes, which limit their use for acid-catalyzed transformations involving larger molecules such as the fibrous lignin polymers from biomass. CEBC researchers developing selective and stable solid acid catalysts that can accommodate a wide range of substrate sizes (including lignocellulosic molecules) for the growing biomass-based renewable chemicals industry.
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Research presentation"Carbon dioxide splitting with plasma catalysis"

Researchers are constructing and evaluating a plasma catalysis reactor for carbon dioxide splitting into carbon monoxide and oxygen, which could be used as a feedstock for the synthesis of industrially profitable chemicals. The idea is that the plasma will enhance conversion by electron impact dissociation of CO2, and that the highly endothermic reaction could be carried out under low temperature and atmospheric pressure conditions.

Ionic liquids researcher"Innovations with ionic liquids"

CEBC researchers have several projects underway that involve ionic liquids.  These liquid salts  display negligible volatility and therefore promise to be useful replacements for air-polluting volatile organic solvents or as a useful way to solubilize and process biomass cellulose fibers.     
Read more:

  • Minnick, D. L.; Scurto, A. M. "Vapor-liquid equilibrium in the production of the ionic liquid, 1-hexyl-3-methylimidazolium bromide ([HMIm][Br]), in acetone," Fluid Phase Equilibria 2014 365 11-19. (Abstract)
  • Amarasekara, A. S.; Callis, B.; Wiredu, B. "Synthesis and characterization of branched polymeric ionic liquids with imidazolium chloride segments," Polymer Bulletin 2012 68 901-908. (Abstract)
  • Prof. Aaron Scurto's website

researcher"Cheaper, safer, greener route to carbon coupling"

One widely used process for coupling a carbon atom to another carbon during allylation is called “direct displacement of alcohols”. But current methods for this reaction use hazardous and corrosive materials and generate large volumes of waste and byproducts.  The wastes and hazards are so great that the American Chemical Society Green Chemistry Institute ranks this reaction a top priority for improvement.  CEBC researchers are tackling this challenge and working to develop a simpler, safer, cheaper route.
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