Publications by authors named "Jeffrey J Urban"

Electrochemical technologies add a unique dimension for ore refinement, representing tunable methods that can integrate with renewable energy sources and existing downstream process flows. However, the development of electrochemical extraction technologies has been impeded by the technological maturity of hydro- and pyro-metallurgy, as well as the electrical insulating properties of many metal oxide ores. The fabrication and use of carbon/insulating material composite electrodes has been a longstanding method to enable electrochemical activation.

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  • * The authors present a new method for creating MOFs using non-equilibrium flame aerosol synthesis, which allows for the creation of both nano-crystalline and amorphous MOFs.
  • * This innovative synthesis can produce complex MOFs with multiple metal cations and has the potential for high-performance applications, such as using these materials in catalysts for CO oxidation, making it suitable for scalable industrial production.
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  • Developing an efficient and low-cost catalyst for ethanol dehydrogenation is essential, and the study identifies a "complex active site" formed by atomically dispersed Au atoms and oxygen vacancies that enhances catalytic performance.
  • The Au-Vo-Zr catalyst demonstrated a significantly higher hydrogen production rate at 350°C compared to other metal oxide supports, marking a major breakthrough in catalytic efficiency.
  • The research emphasizes the importance of atomic-level design in catalysis, revealing that tailoring the structure of active sites can greatly improve selectivity and activity in chemical reactions.
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  • MXene shows promise as an electrode material due to its layered structure and good electrical conductivity, but its low reversible capacity limits industrial applications.
  • Researchers synthesized a new heterostructure called N-doped graphene-like carbon intercalated TiCT (NGC-TiCT) and tested it in sodium-ion and lithium-ion batteries, achieving significantly higher capacities (305 mAh/g and 400 mAh/g, respectively) compared to traditional TiCT.
  • The NGC-TiCT heterostructure demonstrates both high cycling stability and improved battery performance through enhanced ion adsorption, suggesting a potential advancement in energy storage technologies.
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Layer-by-layer (LbL) assembly of oppositely charged materials has been widely used as an approach to make two-dimensional (2D) nanosheet-based membranes, which often involves 2D nanosheets being alternately deposited with polymer-based polyelectrolytes to obtain an electrostabilized nanosheet-polymer structure. In this study, we hypothesized that using 2D nanosheets with matching physical properties as both polyanions and polycations may result in a more ordered nanostructure with better stability than a nanosheet-polymer structure. To compare the differences between nanosheet-nanosheet vs nanosheet-polymer structures, we assembled negatively charged molybdenum disulfide nanosheets (MoS) with either positively charged graphene oxide (PrGO) nanosheets or positively charged polymer (PDDA).

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  • Diamine-appended Mg(dobpdc) frameworks are effective for carbon capture, showing high selectivity and CO capacity, but traditional mechanisms limit their uptake to roughly 1 molecule of CO per diamine.
  • The newly developed pip2-Mg(dobpdc) framework achieves a higher carbon capture capacity of about 1.5 molecules of CO per diamine through a unique two-step mechanism involving CO insertion and chain formation.
  • Analysis methods, including solid-state NMR and DRIFTS, demonstrate that this framework can outperform existing materials under conditions similar to landfill gas separation, suggesting future possibilities for designing even more effective carbon capture materials.
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Inkjet printing is a more sustainable and scalable fabrication method than spin coating for producing perovskite solar cells (PSCs). Although spin-coated SnO has been intensively studied as an effective electron transport layer (ETL) for PSCs, inkjet-printed SnO ETLs have not been widely reported. Here, we fabricated inkjet-printed, solution-processed SnO ETLs for planar PSCs.

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Nanoporous carbon materials with customized structural features enable sustainable and electrochemical applications through improved performance and efficiency. Carbon spherogels (highly porous carbon aerogel materials consisting of an assembly of hollow carbon nanosphere units with uniform diameters) are desirable candidates as they combine exceptional electrical conductivity, bespoke shell porosity, tunability of the shell thickness, and a high surface area. Herein, we introduce a novel and more environmentally friendly sol-gel synthesis of resorcinol-formaldehyde (RF) templated by polystyrene spheres, forming carbon spherogels in an organic solvent.

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The Hume-Rothery rules governing solid-state miscibility limit the compositional space for new inorganic material discovery. Here, we report a non-equilibrium, one-step, and scalable flame synthesis method to overcome thermodynamic limits and incorporate immiscible elements into single phase ceramic nanoshells. Starting from prototype examples including (NiMg)O, (NiAl)O, and (NiZr)O, we then extend this method to a broad range of Ni-containing ceramic solid solutions, and finally to general binary combinations of elements.

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This study presents a novel approach to developing high-performance lithium-ion battery electrodes by loading titania-carbon hybrid spherogels with sulfur. The resulting hybrid materials combine high charge storage capacity, electrical conductivity, and core-shell morphology, enabling the development of next-generation battery electrodes. We obtained homogeneous carbon spheres caging crystalline titania particles and sulfur using a template-assisted sol-gel route and carefully treated the titania-loaded carbon spherogels with hydrogen sulfide.

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  • Electrochemical-oxidation-driven reconstruction faces challenges like poor conductivity and active-species dissolution, making it less effective for advanced materials.
  • The new hybrid reconstruction method, called electrochemical oxidation with electrochemical polymerization (EOEP), enhances material structure by integrating metal hydroxides with polypyrrole to improve the microenvironment.
  • This approach demonstrates that modifications to metal centers, particularly with manganese, can significantly enhance properties like charge transfer and capacitance, leading to better performance in energy applications.
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In nature, nonheme iron enzymes use dioxygen to generate high-spin iron(IV)=O species for a variety of oxygenation reactions. Although synthetic chemists have long sought to mimic this reactivity, the enzyme-like activation of O to form high-spin iron(IV) = O species remains an unrealized goal. Here, we report a metal-organic framework featuring iron(II) sites with a local structure similar to that in α-ketoglutarate-dependent dioxygenases.

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Methane pyrolysis (MP) is a potential technology for CO-free hydrogen production that generates only solid carbon by-products. However, developing a highly efficient catalyst for stable methane pyrolysis at a moderate temperature has been challenging. We present a new and highly efficient catalyst created by modifying a Ni-Bi liquid alloy with the addition of Mo to produce a ternary NiMo-Bi liquid alloy catalyst (LAC).

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Lithium-ion and sodium-ion batteries (LIBs and SIBs) are crucial in our shift toward sustainable technologies. In this work, the potential of layered boride materials (MoAlB and Mo AlB ) as novel, high-performance electrode materials for LIBs and SIBs, is explored. It is discovered that Mo AlB shows a higher specific capacity than MoAlB when used as an electrode material for LIBs, with a specific capacity of 593 mAh g achieved after 500 cycles at 200 mA g .

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Lithium-excess, cation-disordered rocksalt (DRX) materials have been subject to intense scrutiny and development in recent years as potential cathode materials for Li-ion batteries. Despite their compositional flexibility and high initial capacity, they suffer from poorly understood parasitic degradation reactions at the cathode-electrolyte interface. These interfacial degradation reactions deteriorate both the DRX material and electrolyte, ultimately leading to capacity fade and voltage hysteresis during cycling.

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2-Dimensional (2D) materials are attracting strong interest in printed electronics because of their unique properties and easy processability, enabling the fabrication of devices with low cost and mass scalable methods such as inkjet printing. For the fabrication of fully printed devices, it is of fundamental importance to develop a printable dielectric ink, providing good insulation and the ability to withstand large electric fields. Hexagonal boron nitride (h-BN) is typically used as a dielectric in printed devices.

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The past decade has witnessed the development of layered-hydroxide-based self-supporting electrodes, but the low active mass ratio impedes its all-around energy-storage applications. Herein, the intrinsic limit of layered hydroxides is broken by engineering F-substituted β-Ni(OH) (Ni-F-OH) plates with a sub-micrometer thickness (over 700 nm), producing a superhigh mass loading of 29.8 mg cm on the carbon substrate.

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Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO to high value-added C2 products. In this study, we designed an N,S-codoped Fe-based MIL-88B catalyst with well-defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2-benzisothiazolin-3-one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C H evolution yield of 17.

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  • The study focuses on developing new types of porous polymers (HCPs) to enhance the performance of enzyme-inspired catalysts by modifying the active site environment.
  • Two types of HCPs were created, one with hydroxyl (-OH) groups and the other with hydrophobic methyl (-CH) groups, which influence their catalytic activity differently.
  • The HCP-OH catalysts were found to accelerate hydrogenation reactions involving carbonyl groups, while the HCP-CH catalysts improved activation of other non-H bond substrates, demonstrating the potential for tailored catalytic selectivity.
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Inorganic-organic hybrids, such as Te-PEDOT:PSS core/shell nanowires, have emerged as a class of promising thermoelectric materials with combined attributes of mechanical flexibility and low cost. However, the poorly understood structure-property relationship calls for further investigation for performance enhancement. Here, through precise treatments of focused electron beam irradiation and thermal annealing on individual Te-PEDOT:PSS nanowires, new, nonchemical mechanisms are introduced to specifically engineer the organic phase, and the measured results provide an unprecedented piece of evidence, confirming the dominant role of organic shell in charge transport.

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Metal boride nanostructures have shown significant promise for hydrogen storage applications. However, the synthesis of nanoscale metal boride particles is challenging because of their high surface energy, strong inter- and intraplanar bonding, and difficult-to-control surface termination. Here, it is demonstrated that mechanochemical exfoliation of magnesium diboride in zirconia produces 3-4 nm ultrathin MgB nanosheets (multilayers) in high yield.

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Optical applications of lanthanide-doped nanoparticles require materials with low phonon energies to minimize nonradiative relaxation and promote nonlinear processes like upconversion. Heavy halide hosts offer low phonon energies but are challenging to synthesize as nanocrystals. Here, we demonstrate the size-controlled synthesis of low-phonon-energy KPb X (X=Cl, Br) nanoparticles and the ability to tune nanocrystal phonon energies as low as 128 cm .

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Two-dimensional (2D) materials are uniquely suited for highly anisotropic thermal transport, which is important in thermoelectrics, thermal barrier coatings, and heat spreaders. Solution-processed 2D materials are attractive for simple, low-cost, and large-scale fabrication of devices on, virtually, any substrate. However, to date, there are only few reports with contrasting results on the thermal conductivity of graphene films, while thermal transport has been hardly measured for other types of solution-processed 2D material films.

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  • Researchers have found that 2D anatase titanium dioxide (TiO) has unique properties due to its reactive surfaces, but it's challenging to produce because the bulk crystal isn't layered.
  • They developed a novel, environmentally friendly method to create single crystalline 2D anatase TiO using 1T-TiS, which reveals highly reactive facets.
  • This technique enhances TiO's effectiveness in hydrogen evolution reactions and offers a cost-effective, scalable production method for energy applications.
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Mesoporous silica is a versatile material for energy, environmental, and medical applications. Here, for the first time, we report a flame aerosol synthesis method for a class of mesoporous silica with hollow structure and specific surface area exceeding 1000 m  g . We show its superior performance in water purification, as a drug carrier, and in thermal insulation.

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