Time-resolved surface-enhanced IR-absorption spectroscopy triggered by electrochemical modulation has been performed on cytochrome c oxidase from Rhodobacter sphaeroides. Single bands isolated from a broad band in the amide I region using phase-sensitive detection were attributed to different redox centers. Their absorbances changing on the millisecond timescale could be fitted to a model based on protonation-dependent chemical reaction kinetics established previously. Substantial conformational changes of secondary structures coupled to redox transitions were revealed.
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http://dx.doi.org/10.1016/j.bpj.2013.10.037 | DOI Listing |
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November 2024
National Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu, 610500, China.
Effective electron supply to produce ammonia in photoelectrochemical nitrogen reduction reaction (PEC NRR) remains challenging due to the sluggish multiple proton-coupled electron transfer and unfavorable carrier recombination. Herein, InP quantum dots decorated with sulfur ligands (InP QDs-S) bound to MIL-100(Fe) as a benchmark catalyst for PEC NRR is reported. It is found that MIL-100(Fe) can combined with InP QDs-S via Fe─S bonds as bridge to facilitate the electron transfer by experimental results.
View Article and Find Full Text PDFACS Appl Mater Interfaces
June 2024
Division of Biophysics and Bioengineering, IFM, Linköping University, Linköping 581 83, Sweden.
In the domain of organic mixed ionic-electronic conductors (OMIECs), simultaneous transport and coupling of ionic and electronic charges are crucial for the function of electrochemical devices in organic electronics. Understanding conduction mechanisms and chemical reactions in operational devices is pivotal for performance enhancement and is necessary for the informed and systematic development of more promising materials. Surface-enhanced Raman spectroscopy (SERS) is a potent tool for monitoring electrochemical evolution and dynamic doping in operational devices, offering enhanced sensitivity to subtle spectral changes.
View Article and Find Full Text PDFACS Nano
May 2024
Chair in Hybrid Nanosystems, Nano-Institute Munich, Faculty of Physics, Ludwig-Maximilians-Universtität München, Königinstraße 10, 80539 München, Germany.
Nanophotonic devices excel at confining light into intense hot spots of electromagnetic near fields, creating exceptional opportunities for light-matter coupling and surface-enhanced sensing. Recently, all-dielectric metasurfaces with ultrasharp resonances enabled by photonic bound states in the continuum (BICs) have unlocked additional functionalities for surface-enhanced biospectroscopy by precisely targeting and reading out the molecular absorption signatures of diverse molecular systems. However, BIC-driven molecular spectroscopy has so far focused on end point measurements in dry conditions, neglecting the crucial interaction dynamics of biological systems.
View Article and Find Full Text PDFCommun Chem
March 2024
Department of Physics, Freie Universität Berlin, Arnimallee 14, Berlin, 14195, Germany.
Oxide-derived copper (OD-Cu) materials exhibit extraordinary catalytic activities in the electrochemical carbon dioxide reduction reaction (CORR), which likely relates to non-metallic material constituents formed in transitions between the oxidized and the reduced material. In time-resolved operando experiment, we track the structural dynamics of copper oxide reduction and its re-formation separately in the bulk of the catalyst material and at its surface using X-ray absorption spectroscopy and surface-enhanced Raman spectroscopy. Surface-species transformations progress within seconds whereas the subsurface (bulk) processes unfold within minutes.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2024
Walter Schottky Institute, Technical University of Munich, 85748 Garching, Germany.
Attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) is a powerful method for probing interfacial chemical processes. However, SEIRAS-active nanostructured metallic thin films for the in situ analysis of electrochemical phenomena are often unstable under biased aqueous conditions. In this work, we present a surface-enhancing structure based on etched black Si internal reflection elements with Au-coatings for in situ electrochemical ATR-SEIRAS.
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