{"id":13,"date":"2017-07-07T20:21:07","date_gmt":"2017-07-07T20:21:07","guid":{"rendered":"http:\/\/utsaengineer.wpengine.com\/faculty-page-example\/?page_id=13"},"modified":"2025-01-09T17:41:32","modified_gmt":"2025-01-09T23:41:32","slug":"research","status":"publish","type":"page","link":"https:\/\/ceid.utsa.edu\/gjacobs\/research\/","title":{"rendered":"Research"},"content":{"rendered":"

GENERAL OVERVIEW<\/strong><\/p>\n

\u00a0<\/strong>For over 25 years, my research has been directed at the synthesis, characterization, and testing of catalysts for numerous applications related to energy and the environment.\u00a0\u00a0 These include:<\/p>\n

1.\u00a0 the conversion of syngas (COX<\/sub> and H2<\/sub>) derived from natural gas, coal, and biomass to hydrocarbons that are upgraded to transportation fuels and chemicals;
\n2.\u00a0 the production and purification of hydrogen for fuel cells;
\n3.\u00a0 the selective reforming of light alkanes to chemical feedstocks for the petrochemicals industry;
\n4.\u00a0 the hydrodeoxygenation of oxygenates derived from biomass pyrolysis to high octane products.<\/p>\n

My goal is to continue in these areas, and expand to related ones.\u00a0 Ongoing threads are using synchrotron radiation for the characterization of catalysts, promoters, supports, and poisons; applying isotopic tracers to shed light on reaction mechanisms; and practical applications of nanotechnology.<\/p>\n

\"\"
Synchrotron, Canadian Light Source
Saskatoon, Canada<\/figcaption><\/figure>\n
\"\"
Synchrotron, Canadian Light Source
Saskatoon, Canada<\/figcaption><\/figure>\n

Fischer-Tropsch synthesis<\/strong><\/p>\n

\u00a0<\/strong>Texas is a leading producer of natural gas in the country.\u00a0\u00a0\u00a0 Since 2000, shale gas has become the key source of natural gas and production has risen sharply (e.g., 6 time between 2007 and 2013).\u00a0 In Texas, top producing fields include Newark East Barnett Shale (~2 trillion cu. ft per year), Haynesville Shale (~1.5 trillion cu. ft per year), Eagle Ford Formation (~1 trillion cu. ft per year), Carthage (~650 billion cu. ft per year), and Sprayberry (~300 billion cu. ft per year).\u00a0 While the lion’s share of natural gas is used to generate electricity, some is used to power vehicles.\u00a0 The problem is that it has few retail outlets.\u00a0 A better way to monetize natural gas is to first convert it to syngas (CO and H2<\/sub>) using a combination of steam reforming and partial oxidation known as autothermal reforming.\u00a0 Fischer-Tropsch synthesis (FTS) with either cobalt (preferred) or iron\u00a0 catalyst converts the syngas to hydrocarbons:\u00a0 2H2<\/sub> + CO \u2192 -[CH2<\/sub>]n<\/sub>– + H2<\/sub>O (\u0394H = -167 kJ\/mol).<\/p>\n

In general, syngas (CO + H2<\/sub>) can be derived from natural gas, coal, and biomass and converted to hydrocarbons and oxygenates that are upgraded to transportation fuels and chemicals.\u00a0 Often, the terms GTL (gas-to-liquids), CTL (coal-to-liquids), BTL (biomass-to-liquids), and XTL (any resource-to-liquids) are employed.\u00a0 While high temperature FTS relies on fluidized bed reactors and is targeted to gasoline range hydrocarbons, my attention is on the more environmentally benign low temperature process (200 – 230o<\/sup>C), which targets longer chain hydrocarbons with high cetane number (related to ignition delay time).\u00a0 These premium products are upgraded to ultrapure, virtually sulfur-free, diesel and jet fuels, as well as lubricants and food grade waxes.<\/p>\n

There are numerous challenges to be overcome for improving FTS catalyst formulations.\u00a0 Small nanosized cobalt clusters (2 – 4 nm) are especially susceptible to oxidation and encapsulation by the support by intrinsic or externally added\u00a0 steam, and as H2<\/sub>O is a major product, oxidation is typically problematic above 80% conversion for typical catalysts.\u00a0 Oxidized cobalt is active for water-gas shift, CO + H2<\/sub>O \u2192 CO2<\/sub> + H2<\/sub>, which tends to increase CO2<\/sub> and drive up the selectivity of undesired CH4<\/sub>, a greenhouse gas.\u00a0 This is due to enhanced chain termination caused by the higher surface fugacity of hydrogen.\u00a0 Water also accelerates sintering due to surface oxidation-reduction cycles.\u00a0 Other causes of deactivation of FTS catalysts include the buildup of carbonaceous deposits and poisoning by impurities from natural gas (e.g., H2<\/sub>S, COS), coal and biomass (e.g., H2<\/sub>S, NH3<\/sub> and other nitrogen compounds, hydrohalic acids, alkali compounds, and various metals).\u00a0 Therefore, my research is centered on new catalysts to optimize cobalt size and morphology, interactions with the support, reducibility, and resistance to deactivation.<\/p>\n

New small channel and microchannel reactors require new catalyst designs.\u00a0 For example, novel compact heat exchange reactors offer both high single pass conversion (like a fixed bed reactor) with excellent heat management (like a slurry reactor).\u00a0 However, pellets are utilized to prevent a large pressure drop from occurring.\u00a0 One problem with supporting cobalt nanoparticles within the pores of pellets is that hydrogen diffuses more rapidly than CO.\u00a0 This results in higher H2<\/sub>\/CO ratios on the catalyst surface, which in turn drives up selectivity to CH4<\/sub>, a greenhouse gas, at the expense of valuable C5<\/sub>+.\u00a0 My research is focused on new catalysts with optimal pore characteristics for maximizing C5<\/sub>+ selectivity and driving down light gas selectivities that deviate above the ASF kinetics curve.<\/p>\n

Hydrogen production<\/strong><\/p>\n

\u00a0<\/strong>Fuel cells for transportation and portable power applications offer the potential for eliminating line sources of unwanted emissions (CO2<\/sub>, NOX<\/sub>, SOX<\/sub>, particulates, etc.).\u00a0 However, the costs of fuel cell vehicles (one order of magnitude) and hydrogen production (factor of 4) are too high.\u00a0 Syngas produced from natural gas is an attractive route for generating hydrogen, but the catalysts in polymer electrolyte membrane fuel cells are susceptible to poisoning by CO.\u00a0 My research aims at converting CO and generating additional H2<\/sub>, as well as purifying the hydrogen, by using the low temperature water-gas shift and preferential oxidation (PROX) reactions.\u00a0 The catalysis relies on a junction between the metal and active support (e.g., ceria, zirconia, ceria-zirconia, etc.) either through a support-mediated redox mechanism or an associative mechanism.\u00a0 The defects in the oxide provide sites for activating water, while the metal facilitates hydrogen transfer pathways.\u00a0 I have worked extensively with Honda Research Inc. to demonstrate with isotopic tracers that additives such as light alkali promoters (e.g., Na) facilitate scission of the C-H bond in reactive formate intermediates that significantly accelerate the reaction rate.\u00a0 I have recently demonstrated that the catalysts can also be used to accelerate formate decomposition in releasing H2<\/sub> from potential chemical carriers, such as formic acid and methanol.<\/p>\n

Bioethanol may be an important source of hydrogen in the future, and I have a fruitful collaboration with INT in Brazil in this area.\u00a0 The catalysts are comprised of active oxide carriers and metal particles.\u00a0 However, one critical difference is that the metals chosen must have the capability of handling carbon-carbon scission reactions (e.g., supported Co and Ni catalysts).<\/p>\n

CO2<\/sub> conversion<\/strong><\/p>\n

There is growing evidence that anthropogenic CO2<\/sub> is linked to climate change.\u00a0 One way to convert CO2<\/sub> is to first capture it at a point source (e.g., power plant) and then use FTS technology.\u00a0 However, in that case, H2<\/sub> must be from sources that do not generate CO2<\/sub> (e.g., solar or nuclear powered electrolysis, direct methane decomposition, etc.).\u00a0 My research investigates new catalysts that rely on a reactive interface between FTS metals (Co, Fe, Ru) and an active support (e.g., ceria) for converting CO2<\/sub> to useful products, like alcohols and olefins.\u00a0 Here, the catalysis relies on both reverse water gas shift, CO2<\/sub> + H2<\/sub> = CO + H2<\/sub>O and FTS.\u00a0 Defects in the support promote WGS\/RWGS pathways by providing sites for activating water.<\/p>\n

Reforming<\/strong><\/p>\n

I currently have a collaboration in this area with a major oil company in Texas.\u00a0 Aromatization of light alkanes (e.g., C6<\/sub>-C8<\/sub>) to benzene, toluene, xylene, and ethylbenzene is important to provide feedstocks for the chemicals industry.\u00a0 Benzene alone is critically important for making plastics, resins, pharmaceuticals, detergents, and a host of other important products.\u00a0 My research in this area is focused on KL zeolite (uniaxial with 7 angstrom narrow window and 13 angstrom lobes) supported highly dispersed Pt clusters.\u00a0 The isotopic tracer studies have shown that a 1,6 ring closure mechanism likely occurs. \u00a0These catalysts are highly susceptible to poisoning by sulfur.\u00a0 Using a special low energy beamline at the Canadian Light Source, Inc., we found that sulfur poisoning occurs in part by direct adsorption, which breaks up ensembles of platinum required for aromatization, resulting in higher selectivities to the less structurally sensitive dehydrogenation reaction (requires 1 to 2 atoms).\u00a0 My research is focused on nanostructuring techniques (e.g., simplified chemical vapor deposition methods) and promoters that improve the resistance of Pt to sulfur through “gettering” and anchoring.<\/p>\n

\"\"
Synchrotron, Canadian Light Source
Saskatoon, Canada<\/figcaption><\/figure>\n
\"\"
Synchrotron, Canadian Light Source
Saskatoon, Canada<\/figcaption><\/figure>\n

Hydrodeoxygenation<\/strong><\/p>\n

One significant problem with biofuels from pyrolysis is that the molecules contain oxygen.\u00a0 This reduces their heating value (they are essentially partially combusted) and makes them corrosive and unstable for storage.\u00a0 Using phenol as a platform molecule, my research using infrared spectroscopy has provided evidence that oxophilicity of the catalyst support for palladium particles is critically important.\u00a0 Oxophilic supports such as zirconia and niobia tend to adsorb the keto-tautomer of phenol on the surface via the oxygen atom, allowing for hydrogenation of the carbonyl function in lieu of the ring.\u00a0 The dienol molecule formed is readily dehydrated to benzene, the target product of interest.\u00a0 New catalysts are underway that maximize the density of\u00a0 oxophilic sites.\u00a0 This research is in collaboration with INT in Brazil and the University of Oklahoma.<\/p>\n","protected":false},"excerpt":{"rendered":"

GENERAL OVERVIEW \u00a0For over 25 years, my research has been directed at the synthesis, characterization, and testing of catalysts for numerous applications related to energy and the environment.\u00a0\u00a0 These include: 1.\u00a0 the conversion of syngas (COX and H2) derived from natural gas, coal, and biomass to hydrocarbons that are upgraded to transportation fuels and chemicals; … <\/p>\n

Continue reading “Research”<\/span><\/a><\/p>\n","protected":false},"author":2,"featured_media":0,"parent":0,"menu_order":0,"comment_status":"closed","ping_status":"closed","template":"","meta":{"_monsterinsights_skip_tracking":false,"_monsterinsights_sitenote_active":false,"_monsterinsights_sitenote_note":"","_monsterinsights_sitenote_category":0,"footnotes":""},"class_list":["post-13","page","type-page","status-publish","hentry"],"yoast_head":"\nResearch - Gary Jacobs<\/title>\n<meta name=\"robots\" content=\"index, follow, max-snippet:-1, max-image-preview:large, max-video-preview:-1\" \/>\n<link rel=\"canonical\" href=\"https:\/\/ceid.utsa.edu\/gjacobs\/research\/\" \/>\n<meta property=\"og:locale\" content=\"en_US\" \/>\n<meta property=\"og:type\" content=\"article\" \/>\n<meta property=\"og:title\" content=\"Research - Gary Jacobs\" \/>\n<meta property=\"og:description\" content=\"GENERAL OVERVIEW \u00a0For over 25 years, my research has been directed at the synthesis, characterization, and testing of catalysts for numerous applications related to energy and the environment.\u00a0\u00a0 These include: 1.\u00a0 the conversion of syngas (COX and H2) derived from natural gas, coal, and biomass to hydrocarbons that are upgraded to transportation fuels and chemicals; 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