Biomedical subjects

Thomas F Jaramillo

Publications and source records attributed to Thomas F Jaramillo.

7 recordsLinked to original sources

PubMed2006

Computational high-throughput screening of electrocatalytic materials for hydrogen evolution.

The pace of materials discovery for heterogeneous catalysts and electrocatalysts could, in principle, be accelerated by the development of efficient computational screening methods. This would require an integrated approach, where the catalytic activity and stability of new materials are evaluated and where predictions are benchmarked by careful synthesis and experimental tests. In this contribution, we present a density functional theory-based, high-throughput screening scheme that successfully uses these strategies to identify a new electrocatalyst for the hydrogen evolution reaction (HER). The activity of over 700 binary surface alloys is evaluated theoretically; the stability of each alloy in electrochemical environments is also estimated. BiPt is found to have a predicted activity comparable to, or even better than, pure Pt, the archetypical HER catalyst. This alloy is synthesized and tested experimentally and shows improved HER performance compared with pure Pt, in agreement with the computational screening results.

Journal Article↗

PubMed2005

Synthesis and characterization of Pt-WO3 as methanol oxidation catalysts for fuel cells.

Several compositions of Pt-WO3 catalysts were synthesized and characterized for the electro-oxidation of methanol and CO. The surface morphologies of the catalysts were found to be dependent on the composition. X-ray energy dispersive spectroscopy and X-ray photoelectron spectroscopy results suggest a surface enrichment of WO3 in the codeposited Pt-WO3 catalysts. Cyclic voltammetry and chronoamperometry in methanol show an improvement in catalytic activity for the Pt-WO3 catalysts. A significant improvement in the poison tolerance toward CO and other organic intermediates was observed in the mixed metal-metal oxide catalyst. The catalytic performance of the different compositions was directly compared by normalization of the current to active sites. CO-stripping voltammetry suggests the involvement of WO3 in the catalytic process as opposed to a mere physical effect as suggested by previous work. A possible mechanism for this improvement is proposed based on the electrochemical data.

Journal Article↗

PubMed2004

Parallel synthesis and characterization of photoelectrochemically and electrochromically active tungsten-molybdenum oxides.

Single phase tungsten-molybdenum mixed oxide films (W(1-x)Mo(x)O(3)) were successfully synthesized by automated parallel electrodeposition, and distinct structural changes were observed as a function of composition. A monoclinic structure (beta-phase) was observed in mixed oxides with less than 90% Mo, and above 90% Mo, orthorhombic structure (alpha-phase) was identified.

Journal Article↗

PubMed2003

Size- and support-dependent electronic and catalytic properties of Au0/Au3+ nanoparticles synthesized from block copolymer micelles.

Supported Au nanoclusters synthesized from diblock copolymer micelles can be reliably prepared with well-controlled sizes and dispersions. For particles with diameters between approximately 1 and 6 nm, the particle size and the support were found to strongly influence the oxygen reactivity, the formation and stabilization of a metal-oxide, and the catalytic activity for electrooxidation of carbon monoxide. The smallest particles studied (1.5 nm) were the most active for electrooxidation of CO and had the largest fraction of oxygen associated with gold at the surface as measured by the Au(3+)/Au(0) X-ray photoemission intensities. Conducting and semiconducting substrates, ITO-coated glass and TiO(2), respectively, were associated with greater stabilization of Au(3+) oxide as compared to insulating, SiO(2), substrates.

Journal Article↗

PubMed2003

Catalytic activity of supported Au nanoparticles deposited from block copolymer micelles.

Quasi-ordered, highly dispersed, gold nanoclusters of tightly controlled particle size were synthesized by dip-coating substrates with gold precursors encapsulated by block-copolymer micelles. By this method, gold particles (4.8 +/- 1.3 nm) were deposited on ITO-coated glass and shown to be catalytically active for electro-oxidation of carbon monoxide. XPS confirmed the catalytically active particles were predominantly Au0; however, a large fraction existed as Au3+. Whereas bulk gold is inert, these results demonstrate that catalytically active Au nanoparticles can be derived from micelle encapsulation.

Journal Article↗

PubMedDate not supplied

High-throughput screening system for catalytic hydrogen-producing materials.

A high-throughput screening system and methodology were developed for libraries of hydrogen (H(2)) producing catalytic materials. The system is based on the chemo-optical properties of WO(3), which give rise to reflectance changes in the presence of H(2). Pd-coated WO(3) sensors were synthesized and examined for their hydrogen sensitivity, wavelength-dependent reflectance, and performance in the presence of water vapor. For high-throughput screening, a polypropylene reactor block was designed and constructed to house 8 x 12 catalyst libraries deposited as thin films. When the library and reactor block are assembled together, 96 independent microreactor units are formed. A large-area Pd/WO(3) sensor film covers and seals all microreactors, forming a 96-element 2-D H(2) sensor array. As H(2) is produced differentially across the library, the reflectance changes of the Pd/WO(3) film are monitored by reflectivity sensors that scan the surface every 30 s. The time-dependent changes in reflectance indicate relative rates of H(2) production. A library of cathode electrocatalysts was synthesized from Ti, Pt, Ni, Au, Pd, Al, Ag, Ge, and mixtures thereof to demonstrate the H(2) high-throughput screening system. The results of the electrolytic screening are in agreement with expected literature trends: mixtures of Ni and samples containing Pt and Pd generated H(2) at the greatest rates, while Ge- and Ti-based materials were the least effective electrocatalysts. A mixture of 80% Al and 20% Pt was found to have the highest rate of H(2) production. This high-throughput screening system is applicable in a variety of catalytic screening applications where hydrogen is the desired product.

Journal Article↗

PubMedDate not supplied

Automated electrochemical synthesis and photoelectrochemical characterization of Zn1-xCo(x)O thin films for solar hydrogen production.

High-throughput electrochemical methods have been developed for the investigation of Zn1-xCo(x)O films for photoelectrochemical hydrogen production from water. A library of 120 samples containing 27 different compositions (0 <or= x <or= 0.068) was synthesized by automated serial electrochemical deposition. High-throughput photoelectrochemical screening revealed improved solar hydrogen production for the cobalt-doped films, with Zn0.956Co0.044O exhibiting a 4-fold improvement over pure ZnO with no external bias. Flat-band potential, bias-dependent photocurrent, and action spectra were also measured automatically with the high-throughput screening system. The 200-nm-thick films were subsequently characterized by numerous techniques, including SEM, XRD, XPS, and UV-vis, which show that the depositions are well-controlled. Zn/Co stoichiometry in the films was controlled by the ratio of the Zn and Co precursors in each deposition bath. All films exhibited the wurtzite structure typical of pure ZnO, and the Co2+ appears to substitute Zn2+, forming a single-phase solid solution. Band gaps of the solid solutions were systematically lower than the 3.2-eV band gap typical of ZnO.

Automation↗