Article
Chemistry, Multidisciplinary
Anaelle Humblot, Tony Chave, Prince N. Amaniampong, Stephane Streiff, Francois Jerome
Summary: With the progressive defossilization of our industry, hydrogen (H-2) has been identified as a central molecule to store renewable electricity. In this context, ammonia (NH3) is now rapidly emerging as a promising hydrogen carrier for the future. This study demonstrates a novel method of cleaving the N-H bond of NH3 within cavitation bubbles, generated by ultrasonic irradiation, leading to the in situ formation of a diimide, which then catalyzes the hydrogenation of alkenes. This work offers a potential solution for hydrogenation reactions using ammonia directly, without the need for transition metals and with N-2 as the sole co-product.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Multidisciplinary Sciences
S. Gurban, A. Sulyok, Miklos Menyhard, E. Baradacs, B. Parditka, C. Cserhati, G. A. Langer, Z. Erdelyi
Summary: The study revealed that interface induced diffusion creates an oxygen concentration gradient and results in oxygen diffusion, leading to the growth of an altered layer from the Al2O3/Si substrate interface. The rate of diffusion and relaxation is strongly temperature dependent, resulting in different altered layer compositions at different temperatures.
SCIENTIFIC REPORTS
(2021)
Article
Chemistry, Analytical
Umesh Chiluwal, Gary A. Eiceman
Summary: Introducing an additional dimension of selectivity through field-induced decomposition of RDX in ion mobility spectrometry enables the selective detection of RDX in the absence of interfering peaks. Quantitative determination of RDX is achieved through sequential ion processing, selective field-induced decomposition, and mobility analysis during a second drift region.
Article
Chemistry, Multidisciplinary
Julien Dieu, Francois Jerome, Catherine Batiot-Dupeyrat
Summary: Non-thermal atmospheric plasma is capable of cleaving the N-H bond of NH3 to form aminium radicals, which then react with ethylene to produce ethylamine with a yield of 17%. This technology can also be applied to n-octene, leading to the formation of 1-octylamine, demonstrating anti-Markovnikov addition of NH3.
REACTION CHEMISTRY & ENGINEERING
(2021)
Article
Chemistry, Organic
Mohammad Z. Abidin, Thangavelu Saravanan, Laura Bothof, Pieter G. Tepper, Andy-Mark W. H. Thunnissen, Gerrit J. Poelarends
Summary: The study presents the asymmetric synthesis of N-arylalkyl-substituted l-aspartic acids using EDDS lyase as a biocatalyst, resulting in products with good enantioselectivity and high yields. This demonstrates that C-N lyases can serve as a powerful synthetic tool for preparing difficult noncanonical amino acids.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2021)
Article
Chemistry, Physical
C. Juillet, Q. Auzoux, F. Datcharry, F. Martin, M. Tupin
Summary: In this study, the permeation process of tritium in nuclear pressurized water reactors was investigated by using deuterium as an isotopic tracer. The results showed that surface recombination reaction in the metal was the rate-limiting step of the permeation process, and stress in the specimens decreased the apparent activation energy of deuterium desorption.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Physical
Daniela Torres-Diaz, Romain Basalgete, Mathieu Bertin, Jean-Hugues Fillion, Xavier Michaut, Lionel Amiaud, Anne Lafosse
Summary: Recent research has found that X-ray irradiation of interstellar ice analogues can induce molecule desorption, potentially explaining the presence of gaseous organics in the coldest regions of the interstellar medium, particularly in protoplanetary disks. The proposed desorption mechanism involves the Auger decay of excited molecules following soft X-ray absorption, known as X-ray induced electron-stimulated desorption (XESD). In this study, pure methanol (CH3OH) ices were irradiated with 505 eV electrons to simulate the Auger electrons, and desorption yields of various organic fragments were quantitatively determined by mass spectrometry, showing remarkable similarity to XESD values.
Article
Chemistry, Multidisciplinary
Karolin Pluschke, Aaron Herrmann, Michael Duerr
Summary: Desorption/ionization induced by neutral clusters (DINeC) is a technique used for the soft transfer of organic and biomolecules from a bulk sample onto a desired substrate. This study demonstrates the qualitative and quantitative analysis of the deposition technique using mass spectrometry and a quartz crystal microbalance, respectively. The prepared samples provide a platform for investigating the reactions of deposited molecules with the surface.
Article
Chemistry, Physical
C. Juillet, M. Tupin, F. Martin, Q. Auzoux, C. Berthinier, F. Gaudier, T. Guilbert, C. Toffolon
Summary: This study identifies and quantifies the rate-limiting steps of the hydrogen desorption process from unoxidized M5 alloy. It reveals that surface molecular recombination and trapping of hydrogen by Nb-rich precipitates are key factors affecting desorption kinetics. The kinetic constant for surface recombination on M5 alloy is found to be identical to that on Zircaloy-4.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Applied
Yuan-Qiang Guo, Kaihua Wang, Ruiguo Wang, Hongjian Song, Yuxiu Liu, Qingmin Wang
Summary: The practical protocol described utilizes visible-light induction for efficient and mild three-component intermolecular trifluoromethyl-alkenylation reactions of unactivated alkenes. It demonstrates good functional group tolerance and a wide substrate scope, allowing for introduction of trifluoromethyl groups, conversion of unactivated alkenes to styrene-based activated alkenes, and late-stage functionalization of pharmaceutical intermediates.
ADVANCED SYNTHESIS & CATALYSIS
(2021)
Article
Materials Science, Multidisciplinary
Yuki Fukaya, Shiro Entani, Seiji Sakai
Summary: Intercalation of Ag and Au atoms in graphene/Co(0001) interface leads to reversible changes in graphene height and Debye temperature, indicating the importance of intercalation on interface structure.
Article
Optics
B. M. Gareev, A. M. Abdrakhmanov, L. R. Yakshembetova, G. L. Sharipov
Summary: In this study, light emission phenomena were observed in the single- and multibubble sonolysis of liquid ammonia and solutions of salts in liquid ammonia. The mechanisms of glow excitation in other liquids with known sonoluminescence were found to be applicable in this case as well. The emission of light in liquid NH3 was caused by the formation of nonequilibrium plasma in the cavitation bubbles under the action of ultrasound. The presence of various additives in the solutions resulted in sonoluminescence of these additives, solvent molecules, or the products of sonochemical reactions.
JOURNAL OF LUMINESCENCE
(2023)
Article
Engineering, Environmental
Mohammad Feizbakhshan, Arman Peyravi, Zaher Hashisho, David Crompton, John H. Phillips, James E. Anderson, Mark Nichols
Summary: This study aims to improve the understanding of heel build-up mechanisms in the presence of oxygen during the desorption of VOCs from adsorbents. The results showed that increasing the desorption temperature in the presence of oxygen reduced the adsorbents' BET surface area and increased oxygen-induced reactions. Among the tested temperatures, the minimum heel formation was observed at 200 degrees C. Activated carbons were found to be more susceptible to oxygen-induced reactions at elevated temperatures compared to zeolite.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Chaorui Ma, Jingyu Shen, Chaofan Qu, Tianju Shao, Shanshan Cao, Yanli Yin, Xiaowei Zhao, Zhiyong Jiang
Summary: Chemodivergent synthesis is achieved in asymmetric photocatalysis using a dual catalyst system consisting of a chiral phosphoric acid and DPZ as a photosensitizer. Different inorganic bases enable the formation of valuable products from the three-component radical tandem transformations. The distinct pKa environment plays a key role in the success of this process.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Chaorui Ma, Jingyu Shen, Chaofan Qu, Tianju Shao, Shanshan Cao, Yanli Yin, Xiaowei Zhao, Zhiyong Jiang
Summary: Chemodivergent synthesis was achieved using asymmetric photocatalysis. By using a dual catalyst system consisting of a chiral phosphoric acid and DPZ as a photosensitizer, different inorganic bases were used to enable the formation of two sets of valuable products from a three-component radical tandem transformation. The key to success was the distinct pK(a) environment, which determined the fate of the radicals formed on the quinoxalin-2(1H)-one rings.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Analytical
Markus Rohdenburg, Johannes E. Froch, Petra Martinovic, Charlene J. Lobo, Petra Swiderek
Article
Chemistry, Physical
Christian Preischl, Markus Rohdenburg, Elif Bilgilisoy, Rene Cartaya, Petra Swiderek, Hubertus Marbach
JOURNAL OF PHYSICAL CHEMISTRY C
(2020)
Article
Chemistry, Multidisciplinary
Fabian Schmidt, Petra Swiderek, Jan H. Bredehoft
Summary: The study monitored the formation of products upon electron irradiation of multilayer adsorbates of CH3OH as a model of cosmic CH3OH ice, revealing the reaction mechanisms and energy dependences of product formation. The formation of products is primarily attributed to reactions of radicals formed by the dissociation of neutral electronically excited states.
ACS EARTH AND SPACE CHEMISTRY
(2021)
Article
Chemistry, Physical
Jozef Lengyel, Andriy Pysanenko, Petra Swiderek, Ueli Heiz, Michal Farnik, Juraj Fedor
Summary: Focused electron beam deposition often requires the use of purification techniques to increase the metal content of the deposit. One promising method is adding H2O vapor during electron irradiation, which can either stabilize ligands against dissociation or enhance decomposition depending on the electron energy range. This study demonstrates the sensitivity of water action on Fe(CO)(5) decomposition and its dependency on hydration degree.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Correction
Optics
Fabian Schmidt, Martin Philipp Mues, Jan Hendrik Bredehoeft, Petra Swiderek
Summary: A correction to the paper has been published.
EUROPEAN PHYSICAL JOURNAL D
(2022)
Article
Optics
Fabian Schmidt, Martin Philipp Mues, Jan Hendrik Bredehoeft, Petra Swiderek
Summary: Chemical reactions in mixed molecular ices relevant to astrochemistry can be initiated by electron-molecule interactions, with dissociative electron attachment (DEA) to CO leading to the formation of HCN, HCOOH, and CH3OCHO in different ice mixtures. The enhancement of product yields at specific electron energies suggests the importance of DEA to CO in electron-induced syntheses in molecular ices. The neutral C fragment insertion into a N-H bond is proposed as a reaction mechanism in the formation of HCN from CO/NH3 ice.
EUROPEAN PHYSICAL JOURNAL D
(2021)
Article
Chemistry, Multidisciplinary
Petra Martinovic, Markus Rohdenburg, Aleksandra Butrymowicz, Selma Sarigul, Paula Huth, Reinhard Denecke, Iwona B. Szymanska, Petra Swiderek
Summary: The study demonstrates that the performance of different Ag(I) complexes in FEBID critically depends on their molecular structure, with Ag(I) carboxylates containing aliphatic side chains being particularly favorable for FEBID.
Article
Chemistry, Multidisciplinary
Hannah Boeckers, Petra Swiderek, Markus Rohdenburg
Summary: Focused Electron Beam Induced Deposition (FEBID) is a tool for producing nanoscale materials, which can be used for humidity or strain sensors. Through post-deposition electron irradiation in the presence of ammonia (NH3), the interaction between the deposits and water can be enhanced, enabling the improvement and tuning of humidity sensors fabricated by FEBID.
Article
Materials Science, Coatings & Films
Petra Martinovic, Lars Barnewitz, Markus Rohdenburg, Petra Swiderek
Summary: Focused electron beam induced deposition (FEBID) is a direct-write method used to produce nanostructures from organometallic precursor molecules. This study aims to suppress thermal chemistry and re-enable it within an area defined by the electron beam. The results show that co-injection of NH3 during FEBID could be a viable strategy to enhance the spatial control of the deposition process.
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A
(2023)
Article
Physics, Atomic, Molecular & Chemical
Fabian Schmidt, Tobias Borrmann, Martin Philipp Mues, Sanna Benter, Petra Swiderek, Jan Hendrik Bredehoeft
Summary: Electron-induced chemistry is relevant to various processes involving ionizing radiation, such as radiation damage, polymer curing, and nanofabrication. It triggers reactions and leads to the formation of larger products. Although the initial interaction is non-thermal, the subsequent reactions follow familiar thermal and radical-driven mechanisms of organic chemistry, influencing the formation of products.
Article
Chemistry, Physical
Markus Rohdenburg, Neha Thakur, Rene Cartaya, Sonia Castellanos, Petra Swiderek
Summary: The electron-induced chemistry of Zn(MA)(TFA) resist material for extreme ultraviolet lithography (EUVL) was studied, with results showing reactions related to EUV absorption and faster reaction rates for salt ligands compared to ligand side chains. The study also revealed the importance of low-energy electrons in the resist material's chemical conversion during electron irradiation.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Fabian Schmidt, Petra Swiderek, Tarek Scheele, Jan H. Bredehoeft
Summary: The formation of methyl formate (CH3OCHO) in mixed ices of carbon monoxide (CO) and methanol (CH3OH) upon electron irradiation is primarily initiated by various electron-molecule interactions that result in the production of CH3O radicals. Dissociative electron attachment (DEA) and neutral dissociation (ND) processes release CH3O radicals which can combine with CO to form methyl formate. Alternately, reactions between DEA to CO and ND in CH3OH can also lead to the formation of CH3O radicals, indicating complex pathways for the formation of methyl formate.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Nanoscience & Nanotechnology
Markus Rohdenburg, Robert Winkler, David Kuhness, Harald Plank, Petra Swiderek
ACS APPLIED NANO MATERIALS
(2020)
Article
Chemistry, Physical
Kai Ahlenhoff, Sascha Koch, Daniel Emmrich, Raphael Dalpke, Armin Goelzhaeuser, Petra Swiderek
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2019)
Article
Chemistry, Physical
Laxman Kankate, Thorben Hamann, Shikun Li, Lyudmila V. Moskaleva, Armin Goelzhaeuser, Andrey Turchanin, Petra Swiderek
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2018)
