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Parahydrogen (pH ) is a convenient and cost-efficient source of spin order to enhance the magnetic resonance signal. Previous work showed that transient interaction of pH with a metal organic complex in a signal amplification by reversible exchange (SABRE) experiment enabled more than 10 % polarization for some N molecules. Here, we analyzed a variant of SABRE, consisting of a magnetic field alternating between a low field of ∼1 μT, where polarization transfer is expected to take place, and a higher field >50 μT (alt-SABRE). These magnetic fields affected the amplitude and frequency of polarization transfer. Deviation of a lower magnetic field from a "perfect" condition of level anti-crossing increases the frequency of polarization transfer that can be exploited for polarization of short-lived transient SABRE complexes. Moreover, the coherences responsible for polarization transfer at a lower field persisted during magnetic field variation and continued their spin evolution at higher field with a frequency of 2.5 kHz at 54 μT. The latter should be taken into consideration for an efficient alt-SABRE. Theoretical and experimental findings were exemplified with Iridium N-heterocyclic carbene SABRE complex and N-acetonitrole, where a 30 % higher N polarization with alt-SABRE compared to common SABRE was reached.
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http://dx.doi.org/10.1002/cphc.202100543 | DOI Listing |
J Chem Theory Comput
December 2024
Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo 315211, P.R. China.
The evolution of photosynthetic reaction centers (RCs) from anoxygenic bacteria to higher-order oxygenic cynobacteria and plants highlights a remarkable journey of structural and functional diversification as an adaptation to environmental conditions. The role of chirality in these centers is important, influencing the arrangement and function of key molecules involved in photosynthesis. Investigating the role of chirality may provide a deeper understanding of photosynthesis and the evolutionary history of life on Earth.
View Article and Find Full Text PDFNanoscale
December 2024
University of Warsaw, Faculty of Physics, Pasteura 5, 02-093 Warsaw, Poland.
Raman spectroscopy is a powerful analytical method widely used in many fields of science and applications. However, one of the inherent issues of this method is a low signal-to-noise ratio for ultrathin and two-dimensional (2D) materials. To overcome this problem, techniques like surface-enhanced Raman spectroscopy (SERS) that rely on nanometer scale metallic particles are commonly employed.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
Department of Biotechnology, College of Life Sciences and Biotechnology, Korea University, Seoul 02841, Republic of Korea.
A biofuel cell is an electrochemical device using exoelectrogen or biocatalysts to transfer electrons from redox reactions to the electrodes. While wild-type microbes and natural enzymes are often employed as exoelectrogen and biocatalysts, genetically engineered or modified organisms have been developed to enhance exoelectrogen activity. Here, we demonstrated a redox-enzyme integrated microbial fuel cell (REI-MFC) design based on an exoelectrogen-enhancing strategy that reinforces the electrogenic activity of MR1 by displaying an extra redox enzyme on the cell surface.
View Article and Find Full Text PDFChemphyschem
December 2024
Ruhr Universität Bochum, Anorganische Chemie I, Universitätsstraße 150, NC 3/26, 44801, Bochum, GERMANY.
The commercialisation of PEM water electrolysis is still hindered by the necessity of using noble metals that are rare, expensive and therefore unsustainable. To replace the benchmark HER catalyst Pt with more abundant materials, promising non-noble catalysts need to be identified and optimal electrode preparation and electrolysis conditions need to be transferred between catalyst materials to reveal their full potential under industrially relevant conditions. This study investigates the optimal ink composition for spray-coating the cathode regarding the effects on electrode structure, performance and catalyst layer composition.
View Article and Find Full Text PDFChemistry
December 2024
Tongji University, School of Chemical Science and Engineering, 1239 Siping Road, Shanghai, CHINA.
Upconverted circularly polarized luminescence (UC-CPL) active organic and organic-inorganic composite materials have garnered increasing attention due to their vast potential applications in areas such as 3D displays, encryptions, spintronics and optoelectronic devices. However, effective methods for fabricating chiral inorganic materials exhibiting UC-CPL remain a challenge. Herein, we propose an approach for the synthesis of UC-CPL active chiral mesostructured CeO2 powders (CMCs) via a hydrothermal growth method, using L/D-aspartic acid as symmetry-breaking and structure-directing agents.
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