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Opportunity at Naval Research Laboratory (NRL)

Optimizing Metal-Adsorbate and Metal-Support Interactions for Photocatalysis and Plasmonics-Driven Chemistry

Location

Naval Research Laboratory, DC, Chemistry

RO# Location
64.15.15.B6676 Washington, DC 203755321

Advisers

name email phone
Paul Anthony DeSario paul.desario@nrl.navy.mil 202-767-0417

Description

Solar-driven photocatalysis of water splitting (to yield hydrogen) and reduction of carbon dioxide (to yield fuels such as CH4 and CH3OH) are potentially two of the highest payoff pathways to carbon-neutral fuels. The critical variables limiting the performance of heterogeneous photocatalysis are the inefficient absorption of incident light—especially through the visible region of the solar spectrum—and short lifetimes of photogenerated, reactive electron hole pairs. We have demonstrated that nanostructured titania aerogels with incorporated gold nanoparticles (3D Au–TiO2) feature (1) Au surface plasmon resonance (SPR)-sensitized photocatalytic activity that spans a broad portion of the visible spectrum, and (2) enhanced electron–hole lifetimes courtesy of the 3D interconnected oxide network. The Au guest is entrained within the 3D network of covalently bonded oxide nanoparticles: configuring Au||TiO2 interfaces in 3D doubles the rate of visible-light driven photocatalytic water splitting over those produced when Au of the same size and shape is deposited on pre-formed TiO2 aerogels. Fully exploiting these porous nanostructured materials for photocatalysis requires detailed analysis of the plasmonic sensitization mechanism, identification of nanoscale design parameters that control plasmonic-sensitization efficiency, and understanding the effect of the networked oxide on charge tranport and excited state lifetimes.

In this project, we will exploit the design flexibility of composite aerogels to (1) elucidate the multiple visible-light SPR sensitization mechanisms of TiO2 by Au that drive solar fuel-producing photocatalysis; (2) use insights derived from (1) to modify the nanoscale design of 3D Au–TiO2; (3) use 3D networked nanoscale oxides to enhance electron–hole lifetimes; and (4) incorporate the appropriate metal nanoparticles that efficiently catalyze H2O splitting and CO2 reduction, separately or in tandem.

 

References

Panayotov DA, et al: Journal of Physical Chemistry C 117: 15035, 2013

DeSario PA, et al: Nanoscale 5: 8073, 2013

 

Keywords:
Catalysis; Nanoparticle; Supports; Photocatalysis; Plasmonics; Solar fuels;

Eligibility

Citizenship:  Open to U.S. citizens and permanent residents
Level:  Open to Postdoctoral applicants

Stipend

Base Stipend Travel Allotment Supplementation
$87,198.00 $3,000.00
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