Brian G Trewyn

Colorado School of Mines · Department of Chemistry and Geochemistry

Research on permanently porous nanomaterials has gripped the attention of materials chemists for decades. Mesoporous silica nanoparticles (MSNs) and metal-organic frameworks (MOFs) are two of the most studied classes of materials in this field. Recently, explorations into embedding MOFs within the mesopores of MSNs have aimed to create composites t...

Solid base metal oxide catalysts such as MgO offer utility in a wide variety of syntheses from pharmaceuticals to fuels. The (111) facet of MgO shows enhanced, unique properties relative to the other facets. Carbon coatings have emerged as a promising modification to impart metal oxide catalyst stability. Here, we report the synthesis, characteriza...

Background To reestablish blood flow in vessels occluded by clots, tissue plasminogen activator (tPA) can be used; however, its efficacy is limited by transport to and into a clot and by the depletion of its substrate, plasminogen. Objectives To overcome these rate limitations, a platform was designed to co-deliver tPA and plasminogen based on mic...

Most widely used carbon-based materials feature a bulk framework tolerant of extreme pH and temperature conditions while maintaining physical robustness and inherent electrical conductivity and biological relevance due to its inherent nontoxicity. At the nanoscale, the study of porous carbons has been of interest because of the enhanced accessible...

Fibrinolysis is the enzymatic degradation of fibrin, the biopolymer that gives blood clots their mechanical integrity. To reestablish blood flow in vessels occluded by clots, tissue plasminogen activator (tPA) can be used; however, its efficacy is limited by transport to and into a clot and by the depletion of its substrate, plasminogen. To overcom...

Tandem catalysis research has recently come alive with various methods to design biosynthetic pathways utilizing enzymes and inorganic catalysts in single-pot systems. Clever applications of porous supports have brought about ways for the successful integration of incompatible enzymes and inorganic catalysts into these one-pot systems to enhance th...

The development of new antimicrobial agents that can overcome antibiotic-resistance and possess improved antibacterial activity is of important global need. A one-step process is demonstrated to prepare silver nanoparticle decorated MCM–41 type mesoporous silica nanoparticles (AgMSN, average diameter ~ 200–500 nm) using a novel cationic surfactant...

The microscopic, short-range coordination environments and mesoscopic, long-range structures of Eu³⁺ in contact with tetra-n-octyl diglycolamide (TODGA) confined on ordered mesoporous carbon (OMC) nanoparticles and Amberchrom CG-71 resin were probed using Eu L3-edge extended X-ray absorption fine structure (EXAFS) as well as small-angle and wide-an...

Gas storage via adsorption in microporous crystals, such as zeolites, has the potential to transform both the energy and transportation sectors. This potential results from the highly tunable pore chemistry and geometry of zeolites, which allows for precise control of the chemical environment of the adsorbed gas. However, while strong gas-solid int...

This work investigates the one-electron reduction of Eu(III) to Eu(II) with ordered mesoporous carbon (OMC) in cavity microelectrode (CME) systems. OMC materials with and without tetra-n-octyl diglycolamide (TODGA) functionalization were subjected to voltammetric measurements and compared with commercial carbon black Vulcan® XC-72. The electrochemi...

BACKGROUND Oils derived from plants, animal fats, and algae contain both saturated and unsaturated fatty acids. These fatty acids can be converted into liquid fuels and chemicals in the presence of active solid catalysts. RESULTS Nickel‐based catalysts were supported on mordenite via ion exchange synthesis and evaluated for the deoxygenation of st...

Adjacent lanthanides are among the most challenging elements to separate, to the extent that current separations materials would benefit from transformative improvement. Ordered mesoporous carbon (OMC) materials are excellent candidates, owing to their small mesh size and uniform morphology. Herein, OMC materials were physisorbed with bis-(2-ethylh...

Materials composed of earth abundant first-row transition metalnanoparticles supported upon zeolites serve as both fundamentally interesting and useful nanostructures. Examples such as Cu-functionalized zeolites have shown high activity for partial oxidation of methane to methanol. Currently wet impregnation serves as the most popular method for th...

Materials such as Fe-SBA-15, combining first-row earth abundant transition metals and mesoporous silica are of interest as heterogeneous catalysts. Strategies to incorporate Fe within mesoporous silica SBA-15 involve lowering the acidity of the synthesis gel which detrimentally effects the morphology of the final catalyst. Alternatively, multi-step...

Due to the uniform and stable pore structure, mesoporous silica has attracted increasing research attention as a catalyst support material. As a large family of mesoporous silica supported materials, noble metal nanoparticles supported on mesoporous silica catalysts have demonstrated desirable properties across a broad platform of reactions. In thi...

Nanostructured noble-metal catalysts traditionally suffer from sintering under high operating temperatures, leading to durability issues and process limitations. The encapsulation of nanostructured catalysts to prevent loss of activity through thermal sintering, while maintaining accessibility of active sites, remains a great challenge in the catal...

To establish a new method for tracking the interaction of nanoparticles with chemical cleaving agents, we exploited the optical effects caused by attaching 5-10 nm gold nanoparticles with molecular linkers to large mesoporous silica nanoparticles (MSN). At low levels of gold loading onto MSN, the optical spectra resemble colloidal suspensions of go...

Mesoporous silica nanoparticles (MSN) with enlarged pores were prepared, characterized, and reversibly dissociated subunits of Concanavalin A were entrapped in the mesopores as shown by multiple biochemical and material characterizations. When loaded in the MSN, we demonstrated protein stability from proteases and, upon release, the subunits reasso...

We describe a non-DNA-based system for delivering Cre recombinase protein into maize tissue using gold-plated mesoporous silica nanoparticle (Au-MSN). Cre protein is first loaded into the pores of Au-MSNs and then delivered using the biolistic method to immature embryos of a maize line (Lox-corn), which harbors loxP sites flanking a selection and a...

Energy-efficient and scalable harvesting and lipid extraction processes must be developed in order for the algal biofuels and bioproducts industry to thrive. The major challenge for harvesting is the handling of large volumes of cultivation water to concentrate low amounts of biomass. For lipid extraction, the major energy and cost drivers are asso...

Nickel based metal organic frameworks (Ni-MOFs) were successfully synthesized using new conjugated carboxylic acid linkers. These conjugated carboxylic acid linkers were synthesized using mild Heck coupling that led to the incorporation of functional groups not possible by traditional synthetic methods. Control of linker size allows for porosity tu...

The catalytic fast pyrolysis (CFP) of biomass is a promising technology for producing renewable transportation fuels and chemicals. MFI-type catalysts have shown promise for CFP because they produce gasoline range hydrocarbons from oxygenated pyrolysis compounds; however, rapid catalyst deactivation due to coking is one of the major technical barri...

Metal carbide catalysts are essential to many widely used chemical processes. Fischer-Tropsch synthesis, methane dehydroaromatization, and biomass conversion catalysts are typically prepared in situ from a metal oxide precursor with a carbon-containing gas. The reduction process of the metal oxide affects the final catalyst, as does the carburizati...

We have prepared a series of mesoporous silica nanoparticle (MSN) supported Pd-Au bimetallic catalysts using a newly developed sequential impregnation method. These catalysts were fully characterized by various techniques including nitrogen sorption, powder X-ray diffraction, inductively coupled plasma mass spectrometry (ICP-MS), transmission elect...

Protein therapeutics are promising candidates for disease treatment due to their high specificity and minimal adverse side effects; however, targeted protein delivery to specific sites has proven challenging. Mesoporous silica nanoparticles (MSN) have demonstrated to be ideal candidates for this application, given their high loading capacity, bioco...

We report platinum catalysts for the efficient aerobic oxidation of olefins to form epoxides and/or derived glycol monoethers. The catalysts—diaqua and dichloro PtII complexes supported by the ligand di(2-pyridine)methanesulfonate (dpms)—are most active when they are covalently tethered to mesoporous silica nanoparticles (MSNs). Supporting the mole...

Zeolites are crystalline microporous aluminosilicates that have numerous applications in industry, specifically in catalysis, separation and adsorption. Zeolites catalyze the conversion of biomass-derived pyrolysis vapors into hydrocarbons; however, zeolites frequently suffer from rapid deactivation under pyrolysis conditions. Methanol-to-hydrocarb...

Transition metal carbides and nitrides have received a large amount of attention in chemistry and materials science due to their interesting properties and potential to substitute precious metal catalysts. Earth-abundant early transition metal carbides and nitrides were the primary focus of many efforts, while late transition metal alternatives are...

Low-temperature direct methane fuel cells (DMEFCs) offer the opportunity to substantially improve the efficiency of energy production from natural gas. This study focuses on the development of well-defined platinum organometallic complexes covalently anchored to ordered mesoporous carbon (OMC) for electrochemical oxidation of methane in a proton ex...

Production of value-added furans and phenols from biomass through catalytic fast pyrolysis of pine using molybdenum supported on KIT-5 mesoporous silica support was explored. Catalysts containing different loadings of molybdenum were synthesized and characterized by X-ray diffraction, nitrogen physisorption analysis, various electron microscopic te...

The main objective of NAABB was to combine science, technology, and engineering expertise from across the nation to break down critical technical barriers to commercialization of algae-based biofuels. The approach was to address technology development across the entire value chain of algal biofuels production, from selection of strains to cultivati...

The present invention provides a magnetic mesoporous nanoparticle that includes a mesoporous silicate nanoparticle and iron oxide. The present invention also provides a method of using magnetic mesoporous nanoparticles to sequester microorganisms from a media.

A universal and benign strategy for the surface functionalization of OMCs through lithium-mediated chemistry has been reported. For this purpose, a hard templating method for the facile synthesis of monodispersed ordered mesoporous carbons (OMCs) with well-defined morphology templated from large pore mesoporous silica nanoparticles (l-MSN) has been...

The invention provides an article having a mesoporous silicate matrix, such as a particle, having one or more pores; and one or more releasable caps obstructing one or more of the pores for delivery of one or more agents to plant cells or other chlorophyll containing cells, or fungi.

Mesoporous silica nanoparticles (MSNs) have been repeatedly demonstrated as potential drug delivery devices. The study of biocompatibility and interaction of these materials with the various cell types is of great interest in regards to the development of viable pharmaceutical products. By mimicking the composition of the outer leaflet of a red blo...

Delivery of proteins instead of DNA into plant cells allows for transient presence of the protein or enzyme that can be useful for biochemical analysis or genome modifications. This may be of particular interest for genome editing because it can avoid DNA (transgene) integration into the genome and generate precisely modified "non-transgenic" plant...

The application of organic polymers and inorganic/organic hybrid systems in numerous fields of biotechnology has seen a considerable growth in recent years. Typically, organic polymers with diverse structures, compositional variations and differing molecular weights have been utilized to assemble polymeric nanosystems such as polymeric micelles, po...

The relative rates of the aldol reaction catalyzed by supported primary and secondary amines can be inverted by 2 orders of magnitude, depending on the use of hexane or water as a solvent. Our analyses suggest that this dramatic shift in the catalytic behavior of the supported amines does not involve differences in reaction mechanism, but is caused...

A series of MCM-41-type mesoporous silica nanoparticle (MSN) materials with different morphologies (spherical and tubular) and sizes but similar surface and pore properties were synthesized and characterized. The effect of particle morphology on human red blood cell (RBC) membrane integrity was evaluated using flow cytometry, UV-Vis spectroscopy, c...

Lipid analysis often needs to be specifically optimized for each class of compounds due to its wide variety of chemical and physical properties. It becomes a serious bottleneck in the development of algae-based next generation biofuels when high-throughput analysis becomes essential for the optimization of various process conditions. We propose a h...

Delivery of drugs and molecules to eukaryote animal and plant cells can be enhanced when mediated by mesoporous silica nanoparticle (MSN) materials. This chapter describes, in detail, the synthesis of several different MSN materials used for the transport of various hydrophilic and hydrophobic drug molecules, neurotransmitters, and macromolecules a...

The synthesis and characterization of a gold nanoparticle functionalized mesoporous silica nanoparticle (Au-MSN) platform for codelivery of proteins and plasmid DNA to plant tissues using a biolistic particle delivery system is reported. The in vitro uptake and release profiles of fluorescently labeled bovine serum albumin (BSA) and enhanced green...

The cell wall of plant cells is a physical barrier for nanoparticle uptake that limits nanotechnology development in plant sciences. On page 3576, Brian G. Trewyn, Kan Wang, and co-workers report using gold-plated mesoporous silica nanoparticles, which have increased performance as projectiles through the biolistic method, to co-deliver proteins an...

In this study, we demonstrate how materials science can be combined with the established methods of organic chemistry to find mechanistic bottlenecks and redesign heterogeneous catalysts for improved performance. By using solid-state NMR, infrared spectroscopy, surface and kinetic analysis, we prove the existence of a substrate inhibition in the al...

A controlled release system composed of mesoporous silica nanoparticles with covalently bound dipalmitoyl moieties supporting phosphorylated lipids has been successfully synthesized and characterized. This MSN system demonstrates controlled release of fluorescein molecules under disulfide reducing conditions. Flow cytometry analyses confirm increas...

Recent breakthrough research on mesoporous silica nanoparticle (MSN) materials has illustrated their significant potential in biological applications due to their excellent drug delivery and endocytotic behavior. We set out to determine if MSN, covalently functionalized with conformation specific bioactive molecules (either linear or cyclic RGD lig...

Well-defined and monodispersed rhodium nanoparticles as small as approximately 2 nm were encapsulated in situ and stabilized in a mesoporous silica nanoparticle (MSN) framework during the synthesis of the mesoporous material. Although both the activity and selectivity of MSN-encapsulated rhodium nanoparticles in CO hydrogenation could be improved b...

A series of 2d-hexagonally packed mesoporous silica nanoparticle material with 10 nm pore diameter (MSN-10) covalently functionalized with organic surface modifiers have been synthesized via a post-synthesis grafting method. The material structure has been characterized by powder X-ray diffraction, electron microscopy, and nitrogen sorption analyse...

Applying nanotechnology to plant science requires efficient systems for the delivery of nanoparticles (NPs) to plant cells and tissues. The presence of a cell wall in plant cells makes it challenging to extend the NP delivery methods available for animal research. In this work, research is presented which establishes an efficient NP delivery system...

We report a gold nanoparticle (AuNP)-capped mesoporous silica nanoparticle (Au-MSN) platform for intracellular codelivery of an enzyme and a substrate with retention of bioactivity. As a proof-of-concept demonstration, Au-MSNs are shown to release luciferin from the interior pores of MSN upon AuNP uncapping in response to disulfide-reducing antioxi...

A series of mesoporous silica nanoparticles (MSNs) were synthesized using the co-structure directing method. A non-cytotoxic anionic surfactant, undec-1-en-11-yltetra(ethylene glycol) phosphate monoester surfactant (PMES), was used as a structure directing agent (SDA) together with aminopropyltrimethoxysilane that functioned as a co-structure direc...

The exocytosis of mesoporous silica nanoparticles (MSNs) from mammalian cells is demonstrated for the first time. The differences in the degree of exocytosis of MSNs between healthy and cancer cells are shown to be responsible for the asymmetric transfer of the particles between both cell types. The exocytosis of highly adsorbent magnetic MSNs prov...

Shining light for drug delivery: The anticancer drug doxorubicin (Dox, red ellipses in the graphic) was adsorbed on nitroveratryl carbamate-protected aminopropyl-functionalized mesoporous silica nanoparticles (MSNs). Upon exposure to UV light, positively charged propylammonium moieties were formed on the surface, which caused expulsion of positivel...

A supramolecular assembly for visible light responsive release of cargo molecules is presented. Sulforhodamine 101 was loaded inside the mesopores of mercaptopropyl-functionalized mesoporous silica nanoparticles (MP-MSN) and entrapped by mercaptopropyl-coordinated Ru(bpy)(2)(PPh(3))-moieties. Irradiation with visible light triggers the release of c...

A simple method for the preparation of nanoscale fibers and tubes by the cationic copolymerization of divinylbenzene (DVB) and styrene (ST) is described.

The structural properties of mesoporous silicananoparticles are reviewed. Different strategies for the introduction of functional groups are considered. Based on the architectural features of the material, the functionalization at defined regions of the particles is described, along with the properties emerging from the corresponding site-specific...

The application of nanotechnology in the field of drug delivery has attracted much attention in the latest decades. Recent breakthroughs on the morphology control and surface functionalization of inorganic-based delivery vehicles, such as mesoporous silica nanoparticles (MSNs), have brought new possibilities to this burgeoning area of research. The...

The incorporation of stimuli-responsive properties into nanostructured systems has recently attracted significant attention in the research of intracellular drug/gene delivery. In particular, numerous surface-functionalized, end-capped mesoporous silica nanoparticle (MSN) materials have been designed as efficient stimuli-responsive controlled relea...

Introduction Mesoporous Silica Materials: Synthesis and Properties Incorporation of Organic Moieties within Mesoporous Silica Gated Mesoporous Silica Outlook References

IntroductionImmobilization Strategies of Single-Site Heterogeneous CatalystsDesign of more Efficient Heterogeneous Catalysts with Enhanced Reactivity and SelectivityOther Heterogeneous Catalyst System on Non-Silica SupportConclusion References

A series of urea- and thiourea-functionalized mesoporous silica nanoparticles (MSN) was synthesized. These materials exhibited a superior catalytic reactivity for Diels–Alder reaction than their homogeneous analogues. The reactivity enhancement was attributed to the site isolation effect induced by the heterogenization of individual catalytic group...

IntroductionImmobilization Strategies of Heterogeneous CatalystsEfficient Heterogeneous Catalysts with Enhanced Reactivity and Selectivity with FunctionalityOther Heterogeneous Catalyst Systems on Nonsilica SupportsConclusion References

Bulk gold metal powder, consisting of particles (5-50 microm) much larger than nanoparticles, catalyzes the coupling of carbenes generated from diazoalkanes (R(2)C=N(2)) and 3,3-diphenylcyclopropene (DPCP) to form olefins. It also catalyzes cyclopropanation reactions of these carbene precursors with styrenes. The catalytic activity of the gold powd...

A boronic acid-functionalized mesoporous silica nanoparticle-based drug delivery system (BA-MSN) for glucose-responsive controlled release of both insulin and cyclic adenosine monophosphate (cAMP) was synthesized. Fluorescein isothiocyanate-labeled, gluconic acid-modified insulin (FITC-G-Ins) proteins were immobilized on the exterior surface of BA-...

13C-modified TiO2 was prepared to facilitate study of the dopant atoms and trace their chemical fate throughout the process. In the preannealed material, NMR showed strong evidence of many Ti−O−C bonds. After annealing, surface-bound coke is a major component. NMR also showed that a washing step before annealing led to the generation of orthocarbon...

Both bulk gold powder (~50 [mu]m particle size) and alumina-supported gold (50-150 nm) are highly active catalysts for the aerobic oxidative dehydrogenation of amines (CH-NH) to imines (CN) under the mild conditions of 1 atm O2 and 100[thin space]°C. Reactions using the 5% Au/Al2O3 catalyst make efficient use of the gold metal and offer a practica...

Mesoporous silicananoparticles (MSNs) containing base (primary amine) and sulfonic acid inside the MCM-41 type porous channels were successfully used as compatible catalysts for one-pot reaction cascades.

The unique structural features of mesoporous silica nanoparticles (MSN) have made them very useful in biological applications, such as gene therapy and drug delivery. Flow cytometry, confocal microscopy, and electron microscopy have been used for observing the endocytosis of MSN. However, flow cytometry cannot directly observe the process of endocy...

A MCM-41 types of Mesoporous Silica Nanosphere material (MSN) covalently anchored with a fluorescent dye (Texas Red™) is synthesized. The Texas-Red-doped MSNs is also functionalized with a second organic group, i.e., mercaptopropyl or aminopropyl functionalities. These organic groups of the resulting bifunctional MSNs are utilized as reversible lin...

Two MCM-41 type, fluorescein-labeled mesoporous silica nanomaterials (MSNs) consisting of spherical and tube-shaped particles were synthesized and characterized. Both materials have hexagonally arranged mesopores with high surface area (>950 m²/g) and a narrow distribution of pore diameters. The cellular uptake efficiency and kinetics of both MSNs...

Mesoporous silica nanoparticles (MSNs) are introduced as chemically and thermally stable nanomaterials with well-defined and controllable morphology and porosity. It is shown that these particles possess external and internal surfaces that can be selectively functionalized with multiple organic and inorganic groups. On the basis of these characteri...