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1.
Angew Chem Int Ed Engl ; 54(43): 12753-7, 2015 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-26314711

RESUMO

Fundamental understanding of non-precious metal catalysts for the oxygen reduction reaction (ORR) is the nub for the successful replacement of noble Pt in fuel cells and, therefore, of central importance for a technological breakthrough. Herein, the degradation mechanisms of a model high-performance Fe-N-C catalyst have been studied with online inductively coupled plasma mass spectrometry (ICP-MS) and differential electrochemical mass spectroscopy (DEMS) coupled to a modified scanning flow cell (SFC) system. We demonstrate that Fe leaching from iron particles occurs at low potential (<0.7 V) without a direct adverse effect on the ORR activity, while carbon oxidation occurs at high potential (>0.9 V) with a destruction of active sites such as FeNx Cy species. Operando techniques combined with identical location-scanning transmission electron spectroscopy (IL-STEM) identify that the latter mechanism leads to a major ORR activity decay, depending on the upper potential limit and electrolyte temperature. Stable operando potential windows and operational strategies are suggested for avoiding degradation of Fe-N-C catalysts in acidic medium.

2.
Angew Chem Int Ed Engl ; 53(51): 14250-4, 2014 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-25354360

RESUMO

The efficiency of polymer electrolyte membrane fuel cells is strongly depending on the electrocatalyst performance, that is, its activity and stability. We have designed a catalyst material that combines both, the high activity for the decisive cathodic oxygen reduction reaction associated with nanoscale Pt alloys, and the excellent durability of an advanced nanostructured support. Owing to the high specific activity and large active surface area, the catalyst shows extraordinary mass activity values of 1.0 A mgPt(-1). Moreover, the material retains its initial active surface area and intrinsic activity during an extended accelerated aging test within the typical operation range. This excellent performance is achieved by confined-space alloying of the nanoparticles in a controlled manner in the pores of the support.

3.
ACS Appl Mater Interfaces ; 7(33): 18273-82, 2015 Aug 26.
Artigo em Inglês | MEDLINE | ID: mdl-26245645

RESUMO

Low-cost solution-processing of highly conductive films is important for the expanding market of printed electronics. For roll-to-roll manufacturing, suitable flexible substrates and compatible postprocessing are essential. Here, custom-developed coated papers are demonstrated to facilitate the inkjet fabrication of high performance copper patterns. The patterns are fabricated in ambient conditions using water-based CuO dispersion and intense pulsed light (IPL) processing. Papers using a porous CaCO3 precoating, combined with an acidic mesoporous absorption coating, improve the effectiveness and reliability of the IPL process. The processing is realizable within 5 ms, using a single pulse of light. A resistivity of 3.1 ± 0.12 µΩ·cm is achieved with 400 µm wide conductors, corresponding to more than 50% of the conductivity of bulk copper. This is higher than previously reported results for IPL-processed copper.

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