The Scott group conducts both fundamental and applied research in reactions, surface chemistry, and catalysis. Our goal is to understand the interactions and transformations of molecules at gas-solid and liquid-solid interfaces by creating highly uniform active sites. We use advanced techniques in organometallic and coordination chemistry, surface science, spectroscopy, kinetics, mechanistic analysis and modeling to investigate, design and reengineer heterogeneous catalysts. Our group includes both chemical engineering and chemistry students, working to solve important current problems at the interface of chemistry and reaction engineering.
Designing Self-Activating Catalysts for Olefin Metathesis and Polymerization
Olefin metathesis is the redistribution of hydrocarbon chain lengths by rearranging the substituents on C=C bonds, for example:
It is widely used in manufacturing commodity chemicals, surfactants, polymers, and many specialty chemicals.
Atomically-dispersed catalysts (typically, based on Mo, W, or Re) on oxide supports (typically, silica or alumina) show the remarkable ability to self-activate, offering the prospect of being able to design catalysts that can also reactivate themselves on demand. The active sites are metal carbenes. We are investigating mechanisms of self-activation and deactivation in collaboration with Prof. Al Stiegman (FSU), Dr. Mostafa Taoufik (CPE-Lyon) and Dr. Régis Gauvin (Chimie Paristech).
A significant primary kinetic isotope effect suggests that perrhenate activates by a mechanism involving C-H activation:
Read about our recent work in: J. Am. Chem. Soc. 2018, 129, 8912; ACS Catal. 2018, 8, 1728; ACS Catal. 2017, 7, 7442; J. Am. Chem. Soc. 2016, 129, 8912; J. Phys. Chem. C. 2011, 30, 133; Top. Catal. 2011, 30, 133; J. Am. Chem. Soc. 2007, 129, 8912.
Chlorination of alumina results in a dramatic increase in activity and stability of a grafted CH3ReO3 catalyst:
Isolated strong Lewis sites (i.e., Lewis acid sites remote from hydroxyl groups) are relatively more abundant on amorphous and chlorinated Al2O3. Their presence is linked to the generation of active sites:
Research sponsor: 
Exploring the Spatial Distribution of Active Sites on Surfaces
Hydroxyl groups present on oxide surface terminations are the principal sites of attachment for molecular catalysts. For high surface area amorphous oxides, thermal pretreatment reduces their surface density and allows the formation of stable, isolated active sites. According to X-ray absorption spectroscopy (EXAFS), the absence of metal-metal scattering paths provides evidence of these isolated sites. Or does it? Grafted GaR3 has such paths, showing that site pairing that persists even at very low hydroxyl densities. In collaboration with Prof. Songi Han (UCSB) and Prof. Baron Peters (UIUC), we are investigating the distribution of paramagnetic VCl4 on silica and alumina using electron paramagnetic resonance (EPR) spectroscopy and computational modeling.
The absence of room temperature EPR signals for VCl4/SiO2 (in contrast to VCl4/Al2O3) suggests strong dipolar coupling of V(IV) centers. It implies that hydroxyl grafting sites are co-located. EPR signals emerge at low T, when the rotational motion of the V(IV) centers is frozen.
Read about our recent work in: React. Chem. Eng. 2020, 5, 66; ACS Catal. 2017, 7, 7543; J. Chem. Phys. 2015, 142, 104708; J. Am. Chem. Soc. 2012, 134, 355; J. Am. Chem. Soc. 2011, 133, 4847; Chem. Eur. J. 2011, 17, 4632; Organometallics 2006, 25, 189.
Research sponsor:
Understanding Alkane Dehydrogenation with Operando X-ray Absorption Spectroscopies
An operando spectroscopy involves observing the active sites in real-time, while reactions are taking place. In collaboration with Dr. Simon Bare (SSRL), Prof. Jean-Sabin McEwen (WSU), Dr. Mostafa Taoufik (CPE-Lyon), and Prof. Adam Hock (UIC), we are studying the evolution of gallium sites in the presence of propane, propene and H2 at temperatures up to 550 °C using operando X-ray absorption spectroscopies (XANES and EXAFS) at the Stanford Synchrotron Lightsource.
Read about our recent work in: ACS Catal. 2018, 8, 7566; J. Phys. Chem. C. 2015, 119, 26611; J. Energy Chem. 2013, 22, 1.
Ga K-edge XANES evolution for GaiBu3 on Al2O3 and SiO2, heated from room temperature to 550 °C
SSRL Beamline 2-2, equipped with a goniometer to allow quick EXAFS scans.
Stanford Synchrotron Lightsorces
In-situ cell designed for air-sensitive samples and high temp X-ray experiments.
Research sponsor:
Exploring Catalytic Mechanisms in Upgrading Biomass to Renewable Fuels and Chemicals
Selectively 13C-labeled model compounds such as 2-phenoxy-1-phenyethanol are synthesized to study the mechanisms of catalytic lignin conversion to aromatic monomers. Operando solid-state NMR studies of the reaction progress at elevated temperatures and pressures reveal the evolution of individual species in the reaction network.
Read about our recent work in: Chem. Sci. 2020 (in press); Green. Chem., 2020, 22, 550; J. Am. Chem. Soc. 2019, 141, 17370; ACS Catal., 2019, 9, 7204; ChemCatChem, 2019, 11, 190; J. Phys. Chem. C, 2018, 122, 8209; ACS Catal. 2017, 7, 3489; ACS Catal. 2016, 6, 8286; Catal. Sci. Technol. 2015, 5, 1540; ACS Catal. 2014, 4, 2165; Angew. Chem. Int. Ed. 2013, 52, 10349.
Research sponsor: 
Probing P-Zeolite Catalysts using Advanced Solid-State NMR Methods
P-modified zeolites show high selectivity in acid-catalyzed reactions for biomass upgrading to renewable chemicals, such as the conversion of furanics to butadiene or p-xylene.
With the Catalysis Center for Energy Innovation (CCEI) and Prof. Songi Han (UCSB), we are studying the nature of the P-sites and their dynamic behavior under reaction conditions, using solid-state NMR methods with advanced pulse sequences to distinguish sites with similar chemical shifts, and the enhanced sensitivity of Dynamic Nuclear Polarization (DNP) to reveal spatial correlations.
Research sponsors: 
Tuning Porous Catalysts for Selective Liquid-Phase Reactions
Solid catalysts for the efficient conversion of non-food biomass (lignocellulose) to platform chemicals should selectively adsorb reactants and promote desorption of products. By modulating the surface polarity of an ordered mesoporous silica (SBA-15) using various (organo)silica precursors, we have established that molecular adsorption can indeed be precisely tuned by a judicious combination of surface polarity and solvent. We are exploring the effect on catalytic activity and selectivity in the hydrogenation/hydrogenolysis of lignin model compounds.
Read about our recent work in: Chem. Sci., 2020, Advance Article
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Upcycling Plastic Waste to Value-Added Chemicals
Every year, millions of tons of plastics are used and then quickly discarded as waste, creating a growing environmental burden due to their long lifetimes. Existing mechanical recycling methods generate lower value materials are economically challenging. With the Institute for Cooperative Upcycling of Polymers (iCOUP) and Prof. Mahdi Abu-Omar (UCSB), we are developing new chemical recycling methods could motivate better plastic recovery and reduce inputs to the environment.
Hydrogenolysis of polyethylene gives liquid alkanes, while catalytic pyrolysis yields alkylaromatic liquids directly in high yields under mild conditions. These products have broad applications as surfactants, solvents, and refrigeration fluids.
Read about our recent work in: ACS Sustainable Chem. Eng. 2020, 7, 11004; ACS Cent. Sci. 2019, 5, 11, 1795.
Research sponsor:
Designing Catalysts for Continuous Flow Pharmaceutical Production
Pharmaceutical manufacturing is mostly conducted in batches, generating large amounts of catalyst and solvent waste, and requiring extensive product purification to remove catalyst residues. We are developing solid acid catalysts for more efficient pharmaceutical processes using continuous flow reactions to enhance safety, efficiency, and productivity.
In collaboration with Pfizer, we have found that robust materials such as H-Beta zeolite (HBEA) and amorphous silica-alumina (ASA) are effective solid catalysts for important pharma reactions such as:
- N-Boc deprotection of amines
- direct amidation of esters
- synthesis of N-substituted azacycles
