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ACS Appl Mater Interfaces ; 12(5): 5901-5908, 2020 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-31971770


Silicon has shown promise for use as a small band gap (1.1 eV) absorber material in photoelectrochemical (PEC) water splitting. However, the limited stability of silicon in acidic electrolyte requires the use of protection strategies coupled with catalysts. Herein, spin coating is used as a versatile method to directly coat silicon photoanodes with an IrOx oxygen evolution reaction (OER) catalyst, reducing the processing complexity compared to conventional fabrication schemes. Biphasic strontium chloride/iridium oxide (SrCl2:IrOx) catalysts are also developed, and both catalysts form photoactive junctions with silicon and demonstrate high photoanode activity. The iridium oxide photoanode displays a photocurrent onset at 1.06 V vs reversible hydrogen electrode (RHE), while the SrCl2:IrOx photoanode onsets earlier at 0.96 V vs RHE. The differing potentials are consistent with the observed photovoltages of 0.43 and 0.53 V for the IrOx and SrCl2:IrOx, respectively. By measuring the oxidation of a reversible redox couple, Fe(CN)63-/4-, we compare the charge carrier extraction of the devices and show that the addition of SrCl2 to the IrOx catalyst improves the silicon-electrolyte interface compared to pure IrOx. However, the durability of the strontium-containing photoanode remains a challenge, with its photocurrent density decreasing by 90% over 4 h. The IrOx photoanode, on the other hand, maintained a stable photocurrent density over this timescale. Characterization of the as-prepared and post-tested material structure via Auger electron spectroscopy identifies catalyst film cracking and delamination as the primary failure modes. We propose that improvements to catalyst adhesion should further the viability of spin coating as a technique for photoanode preparation.

ACS Appl Mater Interfaces ; 11(37): 34059-34066, 2019 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-31442022


Multimetallic Ir-based systems offer significant opportunities for enhanced oxygen evolution electrocatalysis by modifying the electronic and geometric properties of the active catalyst. Herein, a systematic investigation of bimetallic Ir-based thin films was performed to identify activity and stability trends across material systems for the oxygen evolution reaction (OER) in acidic media. Electron beam evaporation was used to co-deposit metallic films of Ir, IrSn2, IrCr, IrTi, and IrNi. The electrocatalytic activity of the electrochemically oxidized alloys was found to increase in the following order: IrTi < IrSn2 < Ir ∼ IrNi < IrCr. The IrCr system demonstrates two times the catalytic activity of Ir at 1.65 V versus RHE. Density functional theory calculations suggest that this enhancement is due to Cr active sites that have improved oxygen binding energetics compared to those of pure Ir oxide. This work identifies IrCr as a promising new catalyst system that facilitates reduced precious metal loadings for acid-based OER catalysis.

Nano Lett ; 17(10): 6040-6046, 2017 10 11.
Artigo em Inglês | MEDLINE | ID: mdl-28945433


Enhanced catalysis for electrochemical oxygen evolution is essential for the efficacy of many renewable energy technologies, including water electrolyzers and metal-air batteries. Recently, Au supports have been shown to enhance the activity of many 3d transition metal-oxide thin films for the oxygen evolution reaction (OER) in alkaline media. Herein, we translate the beneficial impact of Au supports to high surface area, device-ready core-shell nanoparticles consisting of a Au-core and a metal-oxide shell (Au@MxOy where M = Ni, Co, Fe, and CoFe). Through a systematic evaluation, we establish trends in performance and illustrate the universal activity enhancement when employing the Au-core in the 3d transition metal-oxide nanoparticles. The highest activity particles, Au@CoFeOx, demonstrate an overpotential of 328 ± 3 mV over a 2 h stability test at 10 mA cm-2, illustrating that strategically coupling Au support and mixed metal-oxide effects in a core-shell nanoparticle morphology is a promising avenue to achieve device-ready, high-performance OER catalysts.

ChemSusChem ; 8(8): 1472-83, 2015 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-25820199


There is a delicate balance between ion exchange capacity (IEC), conductivity, and dimensional stability in anion exchange membranes as higher charge content can lead to increased water uptake, causing excessive swelling and charge dilution. Using highly-charged benzyltrimethylammonium polysulfone (IEC=2.99 mEq g(-1) ) as a benchmark (which ruptured in water even at room temperature), we report the ability to dramatically decrease water uptake using a semi-interpenetrating network wherein we reinforced the linear polyelectrolyte with a crosslinked poly(styrene-co-divinylbenzene) network. These membranes show enhanced dimensional stability as a result of lower water uptake (75 % vs. 301 % at 25 °C) while maintaining excellent hydroxide conductivity (up to 50 mS cm(-1) at 25 °C). These improvements produced an enhanced alkaline fuel cell capable of generating 236 mW cm(-2) peak power density at 80 °C. This method is easily adaptable and can be a viable strategy for stabilizing existing systems.

Fontes de Energia Elétrica , Membranas Artificiais , Condutividade Elétrica , Eletrodos , Concentração de Íons de Hidrogênio , Hidróxidos/química , Troca Iônica , Cinética , Fenômenos Mecânicos , Polímeros/química , Poliestirenos/química , Sulfonas/química , Temperatura , Água/química