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Herein, we demonstrate operando photoelectron photoion coincidence (PEPICO) spectroscopy as a pivotal technique for evidencing unprecedented mechanistic insights by isomer selective radical detection within complex hydrocarbon-functionalization reaction networks, such as those of catalyzed propane oxychlorination and oxybromination. In particular, while the oxychlorination is surface-confined, we show that in oxybromination alkane activation follows a gas-phase reaction mechanism with evolved bromine and bromine radicals, favoring 2-propyl over 1-propyl radical formation, as evidenced by isomer-selective threshold photoelectron analysis. Furthermore, we provide new mechanistic insights into the cracking and coking pathways that are observed in oxybromination. The first entails propargyl radicals formation from consecutive hydrogen abstraction of propyl radicals, ultimately yielding benzene. The second originates from C-C bond cleavage in propane to ethyl and methyl radicals, which produce CH and CH, or undergo chain growth reactions, forming C-C species.
This article was published in the following journal.
Name: The journal of physical chemistry letters
Recent advances on operando-synchrotron-based X-ray techniques are making it possible to address fundamental questions related to complex proton-coupled electron transfer reactions, as for instance th...
The unimolecular dissociation of ionized tetralin was probed by tandem mass spectrometry, imaging photoelectron photoion coincidence (iPEPICO) spectroscopy and theory. The major reactions observed wer...
Hard X-ray photoelectron spectroscopy at multiple photon energies is used to investigate the surface structure of carbon coatings on silicon materials destined for use as negative electrodes in lithiu...
Due to the ability to tightly confine electromagnetic energy, plasmonic nanoantennas have been widely studied for surface-enhanced infrared absorption (SEIRA) spectroscopy, surface-enhanced Raman spec...
The interaction potential characterizing the ground electronic state of MgAr$^+$ has been determined from the photoelectron spectrum recorded from the a$\,^3\Pi_0$ metastable state of MgAr at high res...
Protocol Near infrared spectroscopy liver transplants: comparison of two monitoring of Near infrared spectroscopy in pediatric liver transplant.
RATIONALE: Diagnostic procedures, such as laser spectroscopy, may help find and diagnose breast cancer. PURPOSE: This phase I trial is studying laser spectroscopy to see how well it works...
The main objective of this study is to evaluate the ability of infrared spectroscopy to discriminate simple hepatic steatosis from NASH
The aim of this study is to demonstrate that infrared spectroscopy is able to detect pressure injuries at a very early stage
In order to come as close as possible to the correct diagnosis of CNS tumors, MRI is the long-standing accepted method of choice that can in some cases be supported by the use of CT to dem...
The study of the energy of electrons ejected from matter by the photoelectric effect, i.e., as a direct result of absorption of energy from electromagnetic radiation. As the energies of the electrons are characteristic of a specific element, the measurement of the energy of these electrons is a technique used to determine the chemical composition of surfaces.
A method of differentiating individuals based on the analysis of qualitative or quantitative biological traits or patterns. This process which has applications in forensics and identity theft prevention includes DNA profiles or DNA fingerprints, hand fingerprints, automated facial recognition, iris scan, hand geometry, retinal scan, vascular patterns, automated voice pattern recognition, and ultrasound of fingers.
Spectroscopy technique which measures changes in organic compounds by tracking the spectral energy of absorption of HYDROGEN atoms.
Magnetic resonance spectroscopy involving detection of changes in the resonance of carbon-13 nuclei in organic molecules.
A technique applicable to the wide variety of substances which exhibit paramagnetism because of the magnetic moments of unpaired electrons. The spectra are useful for detection and identification, for determination of electron structure, for study of interactions between molecules, and for measurement of nuclear spins and moments. (From McGraw-Hill Encyclopedia of Science and Technology, 7th edition) Electron nuclear double resonance (ENDOR) spectroscopy is a variant of the technique which can give enhanced resolution. Electron spin resonance analysis can now be used in vivo, including imaging applications such as MAGNETIC RESONANCE IMAGING.