A CO2 electrolyzer tandem cell system for CO2-CO co-feed valorization in a Ni-N-C/Cu-catalyzed reaction cascade.

Coupled tandem electrolyzer concepts have been predicted to offer kinetic benefits to sluggish catalytic reactions thanks to their flexibility of reaction environments in each cell. Here we design, assemble, test, and analyze the first complete low-temperature, neutral-pH, cathode precious metal-free tandem CO2 electrolyzer cell chain. The tandem system couples an Ag-free CO2-to-CO2/CO electrolyzer (cell-1) to a CO2/CO-to-C2+ product electrolyzer (cell-2). Cell-1 and cell-2 incorporate selective Ni-N-C-based and Cu-based Gas Diffusion Cathodes, respectively, and operate at sustainable neutral pH conditions. Using our tandem cell system, we report strongly enhanced rates for the production of ethylene (by 50%) and alcohols (by 100%) and a sharply increased C2+ energy efficiency (by 100%) at current densities of up to 700 mA cm-2 compared to the single CO2-to-C2+ electrolyzer cell system approach. This study demonstrates that coupled tandem electrolyzer cell systems can offer kinetic and practical energetic benefits over single-cell designs for the production of value-added C2+ chemicals and fuels directly from CO2 feeds without intermediate separation or purification.

Covalent Organic Framework (COF) Derived Ni-N-C Catalysts for Electrochemical CO2 Reduction: Unraveling Fundamental Kinetic and Structural Parameters of the Active Sites.

Electrochemical CO2 reduction is a potential approach to convert CO2 into valuable chemicals using electricity as feedstock. Abundant and affordable catalyst materials are needed to upscale this process in a sustainable manner. Nickel-nitrogen-doped carbon (Ni-N-C) is an efficient catalyst for CO2 reduction to CO, and the single-site Ni-Nx motif is believed to be the active site. However, critical metrics for its catalytic activity, such as active site density and intrinsic turnover frequency, so far lack systematic discussion. In this work, we prepared a set of covalent organic framework (COF)-derived Ni-N-C catalysts, for which the Ni-Nx content could be adjusted by the pyrolysis temperature. The combination of high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure evidenced the presence of Ni single-sites, and quantitative X-ray photoemission addressed the relation between active site density and turnover frequency.

Multicore fiber with integrated fiber Bragg gratings for background-free Raman sensing.

In the last years a variety of fiber optic Raman probes emerged, which are only partly suited for in vivo applications. The in vivo capability is often limited by the bulkiness of the probes. The size is associated with the required filtering of the probes, which is necessary due to Raman scattering inside the fibers. We employed in-line fiber Bragg gratings (FBG) as notch filter for the collection path and integrated them in a novel type of Raman probe. Multicore singlemode fibers (MCSMF) were designed and drawn integrating 19 singlemode cores to achieve better collection efficiency. A Raman probe was assembled with one excitation fiber and six MCSMF with inscribed FBGs as collection fibers. The probe was characterized regarding Raman background suppression, collection efficiency, and distance dependence. First Raman measurements on brain tissue are presented.

Post-hydrogen-loaded draw tower fiber Bragg gratings and their thermal regeneration.

The idea of Bragg gratings generated during the drawing process of a fiber dates back almost 20 years. The technical improvement of the draw tower grating (DTG) process today results in highly reliable and cost-effective Bragg gratings for versatile application in the optical fiber sensor market. Because of the single-pulse exposure of the fiber, the gratings behave typically like type I gratings with respect to their temperature stability. This means that such gratings only work up to temperatures of about 300 °C. To increase temperature stability, we combined DTG arrays with hydrogen postloading and a thermal regeneration process that enables their use in high-temperature environments. The regenerated draw tower gratings are demonstrated to be suitable for temperatures of more than 800 °C.

Thermal regeneration of fiber Bragg gratings in photosensitive fibers.

We report about a thermal regeneration of fiber Bragg gratings written in photosensitive fibers with nanosecond laser pulses. We observe a regenerative process in a highly photosensitive fiber without hydrogen loading which indicates a secondary grating growth in an optical fiber by thermal activation. This process is more temperature stable than the commonly known gratings produced by color center modifications. The writing conditions of such new type of gratings are investigated and the temperature behavior of these regenerated fiber Bragg gratings is analyzed. The application possibilities are in the field of high temperature sensor systems by making use of the combination of good spectral shape of a Type I grating with a Type II like temperature stability.

Fiber Bragg grating inscription combining DUV sub-picosecond laser pulses and two-beam interferometry.

The combination of fiber Bragg grating inscription with femtosecond laser sources and the usage of the Talbot interferometer setup not only gives access to the fabrication of Bragg gratings in new types of materials but also allows, at the same time, to keep the high flexibility of an interferometric setup in choosing the Bragg grating wavelength. Since the spatial and temporal coherence properties of the femtosecond laser source differ strongly from those of conventional laser sources, specific limits and tolerances in the interferometric setup have to be considered. Such limits are investigated on the basis of an analytical ray tracing model. The results are applied to tolerance measurements of fiber Bragg grating reflections recorded with a DUV sub-picosecond laser source at 262 nm. Additionally we demonstrate the wavelength versatility of the two-beam interferometer setup for femtosecond inscription over a 40 nm wavelength band. Inscription experiments in Al/Yb doped silica glasses are demonstrated as a prove for the access to non-photosensitive fibers.