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Heterogeneous Catalysis

Our group has made significant contributions in the field of heterogeneous catalysis. We focus on understanding the underlying physical and chemical processes at work in heterogeneous catalytic systems and use this knowledge to guide us in the design of optimal catalysts.

Guiding design of active sites through modeling

Modeling

Our computational work focuses on gaining a better understanding of chemical transformations and catalytic activity using ab initio methods and developing physically transparent models. Alloying allows tuning of the electronic and geometric structure of catalysts to enhance certain reactions or to inhibit side reactions. We have used density functional theory calculations to predict that nickel/tin alloys could limit carbon mobility on the surface thus improving coking tolerance in high-temperature fuel cells. We have also used density functional theory to show that Ag(100) surfaces are more selective toward the partial oxidation of ethylene compared to Ag(111), suggesting that nanostructures dominated by Ag(100) facets could improve selectivity. In both of these cases, we were able to successfully synthesize the appropriate catalytic structures and verify our model predictions.

Experimental Heterogeneous Catalysis

Shape dependendent silver

Much of our experimental work is inspired by modeling which we use to identify the optimal active sites and optimal hybrid catalyst systems for chemical transformations. The next steps involve synthesis, characterization, and study of these catalysts in experimental reactor systems. Our material syntheses have involved perovskite oxides catalysts, ion-conducting solid oxide membranes, nickel-tin alloy nanoparticles, shape and size dependent silver nanoparticles, silver-platinum alloy nanoparticles, and many others. We characterize these materials with X-ray diffraction, Nitrogen physisorption, scanning/transmission electron microscopy, energy-dispersive X-ray spectroscopy, wavelength dispersive X-ray spectroscopy, UV-vis spectroscopy, IR spectroscopy, Raman spectroscopy, and others. We have studied many different heterogeneous reactions including oxidative methane conversion, hydrocarbon steam reforming, carbon monoxide oxidation, ethylene epoxidation, and water-gas shift reaction. Current members working in this area include Valentina Igenegbai and Rawan Almallahi.

Relevant group publications

Analyzing Relationships between Surface Perturbations and Local Reactivity

H. Xin, S. Linic, J. Chem. Phys., 144, 234704, 2016.

A Viewpoint on Direct Methane Conversion to Ethane and Ethylene Using Oxidative
Coupling on Solid Catalysts


B. Farrell, V. Igenegbai, and S. Linic, ACS Catalysis, 6, 4340, 2016.

Oxidative coupling of methane over mixed oxide catalysts designed for solid oxide membrane reactors

B. Farrell, S. Linic, Catalysis Science & Technology, 6, 4370, 2016.

Direct electrochemical oxidation of ethanol on SOFCs: improved carbon tolerance
of Ni anode by alloying


B. Farrell, S. Linic, Applied Catalysis B: Environmental, 183, 386, 2016.

Identifying optimal active sites for heterogeneous catalysis by metal alloys
based on molecular descriptors and electronic structure engineering.


A. Holewinski, H. Xin, E. Nikolla, S. Linic, Current Opinions in Chemical Engineering, 2, 312, 2013.

High Activity Carbide Supported Catalysts for Water Gas Shift

N. Schweitzer, J. Schaidle, E. Obiefune, X. Pan, S. Linic, L. Thompson, JACS, 133, 2378, 2011.

Two-Step Mechanism for Low-Temperature Oxidation of Vacancies in Graphene

J. M. Carlsson, F. Hanke, S. Linic, M. Scheffler, Phys. Rev. Lett., 102, 166104, 2009.

Hydrocarbon steam reforming on Ni alloys at solid oxide fuel cell
operating conditions


E. Nikolla, J. W. Schwank, S. Linic, Catalysis Today, 136, 243, 2008.

Promotion of the long-term stability of reforming Ni catalysts by
surface alloying


E. Nikolla, J. W. Schwank, S. Linic, J. Catal., 250, 85, 2007.

Controlling carbon surface chemistry by alloying: Carbon tolerant reforming catalyst

E. Nikolla, A. Holewinski, J. Schwank, S. Linic, JACS, 128, 11354, 2006.

Synthesis, structure, and reactions of stable oxametallacycles from styrene oxide
on Ag(111)


M. Enever, S. Linic, K. Uffalussy, J. M. Vohs, M. A. Barteau, J. Phys. Chem. B, 109, 2227, 2005.

Selectivity driven design of bimetallic ethylene epoxidation catalysts
from first principles


S. Linic, J. Jankowiak, M. A. Barteau, J. Catal., 224, 489, 2004.

On the mechanism of Cs-promotion in ethylene epoxidation on Ag

S. Linic, M. A. Barteau, JACS, 126, 8086, 2004.

Control of ethylene epoxidation selectivity by surface oxametallacycle

S. Linic, M. A. Barteau, JACS, 125, 4034, 2003.