The core focus of the group is materials chemistry, with the primary application areas in catalysis and separations, as noted above. The group places a significant emphasis on materials synthesis, and we are adept at synthesis of oxides, polymers and various types of hybrid materials. In conjunction with the focus on synthesis, we are wqell-equipped to characterize materials of nearly any type using facilities at GT or elsewhere.
Porous oxides, zeolites
Porous materials are a dominant theme in the group, with numerous projects targeting ordered mesoporous materials, as well as other porous materials such as zeolites. Our group has expertise in the synthesis of several conventional as well as hierarchical zeolites. These are being studied for catalysis and membrane separation applications in collaboration with other groups at Georgia Tech.
82. D.-Y. Hong, S. J. Miller, P. K. Agrawal, C. W. Jones, “Hydrodeoxygenation and Coupling of Aqueous Phenolics over Bifunctional Zeolite-supported Metal Catalysts.” Chem. Commun. (2010) 46, 1038-1040.
140. W. Xu, S.J. Miller, P.K. Agrawal, C.W. Jones, “Zeolite Topology Effects in the Alkylation of Phenol with Propylene.” Appl. Catal. A. Gen. (2013) 459, 114-120.
153. W. Xu, S. J. Miller, P. K. Agrawal, C. W. Jones, “Positive Effect of Water on Zeolite BEA catalyzed Alkylation of Phenol with Propylene.” Catal. Lett. (2014) 144, 434-438.
233. S.-W. Choi, J.-S. So, J. S. Moore, Y. Liu, R. S. Dixit, J. G. Pendergast, C. Sievers, D. S. Sholl, S. Nair, C. W. Jones, “Propane Dehydrogenation Catalyzed by Gallosilicate MFI Zeolites with Perturbed Acidity.” J. Catal. (2017) 345, 114-123.
251. W.-G. Kim, J. So, S. W. Choi, Y. Liu, R. S. Dixit, C. Sievers, D. S. Sholl, S. Nair, C. W. Jones, “Hierarchical Ga-MFI Catalysts for Propane Dehydrogenation.” Chem. Mater. (2017) 29, 7213-7222.
MOFs and COFs
Georgia Tech has numerous groups that focus on MOFs materials and their applications. In many cases, we collaborate with these groups targeting specific separation problems. A major focus has been on the use of MOF materials for direct capture of CO2 from ambient air. We also are exploring COFs and related molecular cage materials in separations and catalysis.
118. S. Choi, T. Watanabe, T.-H. Bae, D. S. Sholl and C. W. Jones, “Modification of Mg/DOBDC MOF with Amines to Enhance CO2Adsorption from Ultra-Dilute Gases.” J. Phys. Chem. Lett. (2012) 3, 1136-1141.
120. J. A. Thompson, C. R. Blad, N. A. Brunelli, M. E. Lydon, R. P. Lively, C. W. Jones, S. Nair, “Hybrid Zeolitic Imidazolate Frameworks: Controlling Framework Porosity and Functionality by Mixed-Linker Synthesis.” Chem. Mater. (2012) 24, 1930-1936
228. L. A. Darunte, A. D. Oetomo, K. S. Walton, D. S. Sholl, C. W. Jones, “Direct Air Capture of CO2 using Amine Functionalized MIL-101(Cr).” ACS Sustain. Chem. Eng. (2016) 4, 5761-5768
245. L. A Darunte, Y. Terada, C. R. Murdock, K. S. Walton, S. Sholl, C. W. Jones, “Monolith Supported Amine Functionalized Mg2(dobpdc) Adsorbents for CO2 Capture.” ACS Appl. Mater. Interf. (2017) 9, 17043-17051
221. G. Zhu, C. D. Hoffman, Y. Liu, S. Bhattacharyya, U. Tumuluri, M. L. Jue, Zili Wu, D. S. Sholl, S. Nair, C. W. Jones, R. P. Lively, “Engineering Porous Organic Cage Crystals with Increased Acid Gas Resistance.” Chem. Eur. J. (2016) 22, 10743-10747
257. G. Zhu, Y. Liu, L. Flores, Z. R. Lee, C. W. Jones, D. A. Dixon, D. S. Sholl, R. P. Lively, “Formation Mechanisms and Defect Engineering of Imine-based Porous Organic Cages.” Chem. Mater. (2018) in press.
Organic-inorganic hybrid materials
The majority of work on supported molecular catalysts and CO2 separations employs organic-inorganic hybrid materials. These include mesoporous oxides functionalized with discrete organic or organometallic molecular entities, as well as MOFs and related materials. In many projects, inorganic hosts are functionalized with low molecular weight polymeric or oligomeric molecules. Functionalization routes may be physical (polymer impregnation) or chemical (covalent tethering or grafting) depending on the targeted application(s). These organic-inorganic hybrid materials are investigated at fundamental physical and chemical levels while advancing the cutting edge of material performance.
17. M. W. McKittrick, C. W. Jones, “Towards Single-Site, Immobilized Molecular Catalysts: Site-Isolated Ti Ethylene Polymerization Catalysts Supported on Porous Silica.” J. Am. Chem. Soc. (2004) 126, 3052-3053.
51. J. M. Richardson, C. W. Jones, “Strong Evidence of Solution Phase Catalysis Associated with Palladium Leaching from Immobilized Thiols during Heck and Suzuki Coupling of Aryl Halides.” J. Catal. (2007) 251, 80-93.
127. N. A. Brunelli, S. A. Didas, K. Venkatasubbaiah, C. W. Jones, “Tuning Cooperativity by Controlling the Linker Length of Silica-Supported Amines in Catalysis and CO2 Capture.” J. Am. Chem. Soc. (2012) 134, 13950-13953.
168. M. Alkhabbaz, P. Bollini, G. S. Foo, C. Sievers, C. W. Jones, “Important Roles of Enthalpic and Entropic Contributions to CO2 Capture from Simulated Flue Gas and Ambient Air using Mesoporous Silica Grafted Amines.” J. Am. Chem. Soc. (2014) 136, 13170-13173.
172. S. A. Didas, M. A. Sakwa-Novak, G. S. Foo, C. Sievers, C. W. Jones, “Effect of Amine Surface Coverage on the Co-Adsorption of CO2 and Water: Spectral Deconvolution of Adsorbed Species.” J. Phys. Chem. Lett. (2014) 5, 4194-4200.
195. A. Holewinski, M. A. Sakwa-Novak, C. W. Jones, “Linking CO2 Sorption Performance to Polymer Morphology in Amino-polymer/Silica Composites through Neutron Scattering.” J. Am. Chem. Soc. (2015) 137, 11749-11759.
253. J. J. Lee, C.-H. Chen, D. Shimon, S. E. Hayes, C. Sievers, C. W. Jones, “Effect of Humidity on the CO2 Adsorption of Tertiary Amine Grafted SBA-15.” J. Phys. Chem. C (2017) 121, 23480-23487.
We are adept at monomer and polymer synthesis, with experience in controlled (ATRP, RAFT) polymerization, olefin metathesis, anionic and cationic polymerization and free radical polymerization. In many projects, we are seeking to develop new, low molecular weight oligomeric materials for use in separations applications as well as catalysis.
47. X. Zheng, C. W. Jones, M. Weck “Unsymmetrical Macrocyclic Oligomeric Co-Salen Complexes Generated via Ring-Expanding Olefin Metathesis: Highly Reactive and Enantioselective Catalysts for Hydrolytic Kinetic Resolution of Terminal Epoxides.” J. Am. Chem. Soc. (2007) 125, 1105-1112.
59. G. G. Qi, M. Nolan, F. J. Schork, C. W. Jones, “Emulsion and Controlled Miniemulsion Polymerization of the Renewable Monomer g-Methyl-a-Methylene-g-Butyrolactone.” J. Polym. Sci. Polym. Chem. (2008) 46, 5929-5944.
74. C. S. Gill, W. Long, C. W. Jones, “Magnetic Nanoparticle Polymer Brush Catalysts: Alternative Hybrid Organic/Inorganic Structures to Obtain High, Local, Catalyst Loadings for Use in Organic Transformations.”Catal. Lett. (2009) 131, 425-431.
231. C. B. Hoyt, L.-C. Lee, A. E. Cohen, M. Weck, C. W. Jones, “Bifunctional Polymer Architectures for Cooperative Catalysis: Tunable Acid-Base Polymers for the Aldol Condensation.” ChemCatChem (2017) 9, 137-143.
255. M. L. Sarazen, C. W. Jones, “Insights into Azetidine Polymerization for the Preparation of Poly(propylenimine)-based CO2 Adsorbents.”Macromolecules (2017) 50, 9135-9143.
MOF-derived carbons and oxides
An emerging topic for the group is the use of solid catalyst derived from MOFs as precursors. The use of MOFs as precursors allows the direct synthesis of carbon or oxide supported metal nanoparticles with controlled metal composition and dispersion.
Supported metals and metal sulfides
A mainstay of our work in heterogeneous catalysis employs supported metal nanoparticles or metal sulfides (e.g. MoS_2). Catalysts are synthesized via traditional impregnation approaches, as well as via in-situ transformation of mixed oxides and other materials to generate well-dispersed catalysts. We perform a variety of ex- and in-situ characterization techniques here at Georgia Tech and with our collaborators to deeply understand the measured catalytic performance of these catalysts in a variety of light hydrocarbon and biomass upgrading reactions.
86. E.W. Ping, R. Wallace, J. Pierson, T. F. Fuller, C. W. Jones, “Highly Dispersed Palladium Nanoparticles on Ultra-porous Silica Mesocellular Foam for the Catalytic Deoxygenation of Stearic Acid.”Micropor. Mesopor. Mater. (2010) 132, 174-180.
238. T. P. Sulmonetti, Bo Hu, Z. P. Ifkovitis, S. Lee, P. K. Agrawal, C. W. Jones, “Vapor Phase Hydrogenolysis of Furanics Utilizing Reduced Cobalt Mixed Metal Oxide Catalysts.” ChemCatChem (2017) 10, 815-823
144. M. R. Morrill, N. T. Thao, H. Shou, R. J. Davis, D. G. Barton, D. Ferrari, P. K. Agrawal, C. W. Jones, “Origins of Unusual Alcohol Selectivities over Mixed MgAl Oxide Supported K/MoS2Catalysts for Higher Alcohol Synthesis from Syngas.”ACS Catal. (2013) 3, 1665-1675.
182. M. Taborga Claure, S.H. Chai, S. Dai, K.A. Unocic, F.M. Alamgir, P.K. Agrawal, C.W. Jones, “Tuning of Higher Alcohol Selectivity and Productivity in CO Hydrogenation Reactions over K/MoS2 Domains Supported on Mesoporous Activated Carbon and Mixed MgAl Oxide.” J. Catal. (2015) 324, 88-97