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1.
Angew Chem Int Ed Engl ; 52(51): 13794-7, 2013 Dec 16.
Article in English | MEDLINE | ID: mdl-24346953

ABSTRACT

Adding value with membranes: Improved methane aromatization was achieved by using an oxygen-permeable membrane. The resulting membrane reactor shows a superior methane conversion and a higher resistance towards catalyst deactivation.

2.
Anal Chem ; 79(15): 5674-81, 2007 Aug 01.
Article in English | MEDLINE | ID: mdl-17580950

ABSTRACT

The spatially resolved catalytic activity of a catalyst-coated membrane (CCM), which is the essential part of PEM fuel cells, was visualized rapidly without any damage by a distance-controlled scanning mass spectrometer with an improved resolution of 250 microm. Methanol oxidation was identified as a suitable gas-solid probe reaction for the characterization of local catalytic activity. In addition, defects were manually generated in the CCM to simulate inhomogeneous coating and pinholes. The measurements successfully demonstrated that catalytically active and less active regions can be clearly distinguished. Simultaneously, the local topography was recorded, providing additional information on the location of the scratches and pinholes. The catalytic results were highly reproducible due to the constant-distance feedback loop rendering scanning mass spectrometry a promising tool for the quantitative quality control of CCMs.


Subject(s)
Gases/chemistry , Mass Spectrometry/methods , Membranes, Artificial , Methanol/chemistry , Catalysis , Mass Spectrometry/instrumentation , Oxidation-Reduction , Reproducibility of Results , Temperature , Time Factors
4.
Angew Chem Int Ed Engl ; 42(20): 2226-46, 2003 May 25.
Article in English | MEDLINE | ID: mdl-12772152

ABSTRACT

Energized molecules are the essential actors in chemical transformations in solution. As the rearrangement of bonds requires a movement of nuclei, vibrational energy is often the driving force for a reaction. Vibrational energy can be redistributed within the "hot" molecule, or relaxation can occur when molecules interact. Both processes govern the rates, pathways, and quantum yields of chemical transformations in solution. Unfortunately, energy transfer and the breaking, formation, and rearrangement of bonds take place on ultrafast timescales. This Review highlights experimental approaches for the direct, ultrafast measurement of photoinduced femtochemistry and energy flow in solution. In the first part of this Review, we summarize recent experiments on intra- and intermolecular energy transfer. The second part discusses photoinduced decomposition of large organic peroxides, which are used as initiators in free radical polymerization. The mechanisms and timescales of their decarboxylation determine the initial steps of polymerization and the microstructure of the polymer product.

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