Impurity Ion Complexation Enhances Carbon Dioxide Reduction Catalysis

Herein, we show that group 11 CO[subscript 2] reduction catalysts are rapidly poisoned by progressive deposition of trace metal ion impurities present in high purity electrolytes. Metal impurity deposition was characterized by XPS and in situ stripping voltammetry and is coincident with loss of catalytic activity and selectivity for CO[subscript 2] reduction, favoring hydrogen evolution on poisoned surfaces. Metal deposition can be suppressed by complexing trace metal ion impurities with ethylenediaminetetraacetic acid or solid-supported iminodiacetate resins. Metal ion complexation allows for reproducible, sustained catalytic activity and selectivity for CO[subscript 2] reduction on Au, Ag, and Cu electrodes. Together, this study establishes the principal mode by which group 11 CO[subscript 2] reduction catalysts are poisoned and lays out a general approach for extending the lifetime of electrocatalysts subject to impurity metal deposition.MIT Energy Initiative (Saudi Aramco, research agreement)United States. Air Force Office of Scientific Research (Award FA9550-15-1-0135)Massachusetts Institute of Technology. Department of Chemistry (Junior Faculty Funds)National Science Foundation (U.S.) (Predoctoral Fellowship)National Science Foundation (U.S.) (MIT MRSEC Program, award number DMR-0819762

An iterative procedure to obtain inverse response functions for thick-target correction of measured charged-particle spectra

A new method for correcting charged-particle spectra for thick target effects is described. Starting with a trial function, inverse response functions are found by an iterative procedure. The variances corresponding to the measured spectrum are treated similiarly and in parallel. Oscillations of the solution are avoided by rebinning the data to finer bins during a correction iteration and back to the original or wider binning after each iteration. This thick-target correction method has been used for data obtained with the MEDLEY facility at the The Svedberg Laboratory, Uppsala, Sweden, and is here presented in detail and demonstrated for two test cases.Comment: 14 pages, 8 figures, submitted to NIM

Human cortical dynamics during full-body heading changes

The retrosplenial complex (RSC) plays a crucial role in spatial orientation by computing heading direction and translating between distinct spatial reference frames based on multi-sensory information. While invasive studies allow investigating heading computation in moving animals, established non-invasive analyses of human brain dynamics are restricted to stationary setups. To investigate the role of the RSC in heading computation of actively moving humans, we used a Mobile Brain/Body Imaging approach synchronizing electroencephalography with motion capture and virtual reality. Data from physically rotating participants were contrasted with rotations based only on visual flow. During physical rotation, varying rotation velocities were accompanied by pronounced wide frequency band synchronization in RSC, the parietal and occipital cortices. In contrast, the visual flow rotation condition was associated with pronounced alpha band desynchronization, replicating previous findings in desktop navigation studies, and notably absent during physical rotation. These results suggest an involvement of the human RSC in heading computation based on visual, vestibular, and proprioceptive input and implicate revisiting traditional findings of alpha desynchronization in areas of the navigation network during spatial orientation in movement-restricted participants.TU Berlin, Open-Access-Mittel – 202

Measurement of the Absolute Differential Cross Section for np Elastic Scattering at 194 MeV

A tagged medium-energy neutron beam has been used in a precise measurement of the absolute differential cross section for np back-scattering. The results resolve significant discrepancies within the np database concerning the angular dependence in this regime. The experiment has determined the absolute normalization with 1.5% uncertainty, suitable to verify constraints of supposedly comparable precision that arise from the rest of the database in partial wave analyses. The analysis procedures, especially those associated with evaluation of systematic errors in the experiment, are described in detail so that systematic uncertainties may be included in a reasonable way in subsequent partial wave analysis fits incorporating the present results.Comment: 22 pages, 21 figures, submitted for publication in Physical Review

Measurement of the Absolute np Scattering Differential Cross Section at 194 MeV

We describe a double-scattering experiment with a novel tagged neutron beam to measure differential cross sections for np back-scattering to better than 2% absolute precision. The measurement focuses on angles and energies where the cross section magnitude and angle-dependence constrain the charged pion-nucleon coupling constant, but existing data show serious discrepancies among themselves and with energy-dependent partial wave analyses (PWA). The present results are in good accord with the PWA, but deviate systematically from other recent measurements.Comment: 4 pages, 4 figure

Light-ion production in the interaction of 96 MeV neutrons with oxygen

Double-differential cross sections for light-ion (p, d, t, He-3 and alpha) production in oxygen, induced by 96 MeV neutrons are reported. Energy spectra are measured at eight laboratory angles from 20 degrees to 160 degrees in steps of 20 degrees. Procedures for data taking and data reduction are presented. Deduced energy-differential and production cross sections are reported. Experimental cross sections are compared to theoretical reaction model calculations and experimental data at lower neutron energies in the literature. The measured proton data agree reasonably well with the results of the model calculations, whereas the agreement for the other particles is less convincing. The measured production cross sections for protons, deuterons, tritons and alpha particles support the trends suggested by data at lower energies.Comment: 21 pages, 13 figures, submitted to Phys. Rev.

Nucleon-induced reactions at intermediate energies: New data at 96 MeV and theoretical status

Double-differential cross sections for light charged particle production (up to A=4) were measured in 96 MeV neutron-induced reactions, at TSL laboratory cyclotron in Uppsala (Sweden). Measurements for three targets, Fe, Pb, and U, were performed using two independent devices, SCANDAL and MEDLEY. The data were recorded with low energy thresholds and for a wide angular range (20-160 degrees). The normalization procedure used to extract the cross sections is based on the np elastic scattering reaction that we measured and for which we present experimental results. A good control of the systematic uncertainties affecting the results is achieved. Calculations using the exciton model are reported. Two different theoretical approches proposed to improve its predictive power regarding the complex particle emission are tested. The capabilities of each approach is illustrated by comparison with the 96 MeV data that we measured, and with other experimental results available in the literature.Comment: 21 pages, 28 figure