
Vladimir I FeldmanLomonosov Moscow State University | MSU · Faculty of Chemistry
Vladimir I Feldman
Professor, D.Sc.
About
222
Publications
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2,696
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Introduction
Additional affiliations
October 1988 - October 1994
January 2001 - present
December 1997 - June 2008
Enokolopov Institute of Synthetic Polymer Materials, Russian Academy of Sciences
Position
- Principal Investigator
Education
November 1979 - December 1982
September 1974 - June 1979
Publications
Publications (222)
1,1,7-Trihydrododecafluoroheptanol is a promising solvent for the development of strontium-selective extractants based on individual stereoisomers of dicyclohexano-18-crown-6 (DCH18C6). In this study the distribution of DCH18C6 between organic and aqueous phases was determined and the effect of macrocycle stereoisomerism was revealed. Extractabilit...
The α-hydroxyethyl radical (CH3·CHOH, ²A) is a key intermediate in ethanol biochemistry, combustion, atmospheric chemistry, radiation chemistry, and astrochemistry. Experimental data on the vibrational spectrum of this radical are crucially important for reliable detection and understanding of the chemical dynamics of this species. This study repre...
The reactive open-shell species play a very important role in the radiation-induced molecular evolution occurring in the cold areas of space and presumably leading to the formation of biologically relevant molecules. This review presents an insight into the mechanism of such processes coming from matrix isolation studies with a main focus on the ex...
Ethanol (C2H5OH) is the second important alcohol molecule in various space media (molecular clouds, star formation regions and, highly likely, interstellar ices), where it can be exposed to light and ionizing radiation leading to complex organic molecules (COMs) and eventually to the biologically important species. In order to better understand the...
The investigation of the reactions of oxygen atoms with fluoroform (CHF3) molecules and products of their degradation present significant interest for better understanding of the impact of chemically inert fluorinated compounds on atmospheric chemistry and may provide a deeper insight into mechanisms of chemical processes occurring under the action...
This paper addresses the basic question of the impact of a chemically inert environment on the radiation-induced transformations of isolated organic molecules in icy media at cryogenic temperatures with possible implications for astrochemical issues. The radicals produced by X-ray irradiation of isolated ethanol molecules (C2H5OH and CH3CD2OH) in s...
In this work we report the first direct evidence for formation of the key simplest molecule with the peptide bond (acetamide) under radiation-induced transformations occurring in the CH3CN∙∙∙H2O complex isolated in an argon matrix at 6 K. The 1:1 CH3CN∙∙∙H2O intermolecular complex was obtained by deposition of CH3CN/H2O/Ar mixtures and characterize...
Gold nanoparticles (AuNPs) stabilized with poly(1-vinyl-1,2,4-triazole) (PVT) have been synthesized via a one-pot manner in irradiated solutions of 1-vinyl-1,2,4-triazole (VT) and Au(III) ions. The transmission electron microscopy examinations have shown that the sizes of nanoparticles formed range from 1 to 11 nm and are affected by the ratio of V...
Acetylene and ammonia are important constituents of the interstellar medium and their coupled chemistry induced by high-energy radiation may be responsible for the formation of a variety of prebiotically important organic-nitrogen compounds. In this work, we first comprehensively characterized the vibrational spectrum of the 1:1 C 2 H 2 ∙∙∙NH 3 com...
The vibrational spectrum of CF2⁺ radical cation was first explicitly characterized by FTIR spectroscopy in an argon matrix. The radical cation was produced from X-ray radiolysis of difluoromethane isolated in solid argon at 6 K in the presence of electron scavengers. The assignment was made on the basis of ab initio calculations at the CCSD(T)/L3a_...
Gold nanoparticles (GNPs) are promising radiosensitizers for cancer radiotherapy. Moreover, they can be used in the same way for radiation processing and sterilization. Such application of GNPs is of practical interest since it may significantly reduce the dose load and expand the application of radiation treatment. In the present study, the high r...
The NH3···CO complex can be considered an important building block for cold synthetic astrochemistry leading to the formation of complex organic molecules, including key prebiotic species. In this work, we have studied the radiation-induced transformations of this complex in Ar, Kr, and Xe matrices using FTIR spectroscopy. On the basis of compariso...
The interpolyelectrolyte complexes (IPECs) are widely used for various applications, ranging from agriculture and medicine to advanced technological processes. In many cases, they are subjected to the action of ionizing radiation or hard UV light, either intentionally (e.g., for fabrication of nanocomposites) or in the course of routine treatment (...
The complexes of 18-crown-6 with alkali-earth metal halides were synthesized to simulate the macrocyclic component of crown-containing extractants selective for radionuclide ⁹⁰Sr and to investigate the effect of cationic and anionic factors on its radiation destruction at low-temperature (77 K) irradiation. The halide anion was found to protect the...
Gold nanoparticles (AuNPs) with average sizes of 1.5 nm and 3 nm and narrow size distribution have been prepared in the irradiated aqueous solutions and suspensions of Au(III)-complexes with units of poly(1-vinyl-1,2,4-triazole) (PVT) and poly(1-vinyl-1,2,4-triazole) – poly(acrylic acid) (PAA) respectively. The formation of AuNPs has been studied u...
In this study we have probed the role of different enhancement mechanisms of the nanosensitizers in the X-ray irradiated oxygen-free model aqueous organic systems containing “bare” gold nanoparticles (AuNPs) using the spin-trapping technique with electron paramagnetic resonance detection. The observed enhancement effect was found to be ca. 1.67 wp⁻...
Acetaldehyde is one of the key small organic molecules involved in astrochemical and atmospheric processes occurring under the action of ionizing and UV radiation. While the UV photochemistry of acetaldehyde is well studied, little is known about the mechanism of processes induced by high-energy radiation. This paper reports the first systematic st...
Difluoromethane is considered among the environment friendly alternatives to the ozone depleting chlorofluorocarbons. Due to its chemical inertness and lack of UV absorption above 200 nm, this compound can easily come to the upper layers forming complexes with widely abundant atmospheric components, such as water. The radiation-induced degradation...
The radiation-induced assembling of the naphthalene molecule was first directly observed under X-ray irradiation of the isolated styrene-acetylene complex in a solid krypton matrix at 6 K using FTIR spectroscopy. The observation of naphthalene radical cation in the presence of electron scavenger suggests a cationic pathway of this reaction. This fi...
Nitriles are important constituents of extraterrestrial media. Nitriles are supposed to play a crucial role in prebiotic chemistry occurring in the interstellar medium. In this work, we have investigated the low-temperature radiation-induced transformations of a 1 : 1 CH4HCN complex as a plausible precursor of the simplest nitriles using the matrix...
In this work we have examined the radiation-induced synthetic chemistry occurring in an astrochemically important C2H2–CO system at the molecular level using a matrix isolation approach. The 1:1 C2H2∙∙∙CO intermolecular complex of linear structure was obtained in the solid low-temperature (5 K) noble gas matrices by deposition of the C2H2/CO/Ng (Ng...
Difluoromethane (CH2F2) is considered as an ecologically friendly alternative to conventionally used chlorofluorocarbons for various applications. Being photochemically inert in the broad UV range, this molecule can be decomposed only through the action of hard vacuum UV or ionizing radiation, while the corresponding mechanisms are poorly studied....
A hydrogen-bonded CHF⋯HF complex was characterized by FTIR matrix isolation spectroscopy and ab initio calculations. Three possible structures of this complex were found at the coupled-cluster with single, double, and perturbative triple excitations [CCSD(T)/L3a_3] level of theory. The comparison between the experiment and theory reveals that the m...
The discovery of carbon-rich species, including polycyclic aromatic hydrocarbons (PAH) and fullerenes, in the space environment is among the most intriguing findings in molecular astrophysics and astrochemistry of the recent decades. The mechanism of their formation remains unclear and the one of the key issues is related to making “first ring”, i....
The nitrogen-containing molecules of general structure C3HxN are important astrochemical species, which occur in interstellar and other extraterrestrial media. In this work, we have first demonstrated the formation of a number of nitriles and isonitriles (C2H3CN, C2H3NC, and C2H5NC) through a direct radiation-induced synthesis from the matrix isola...
Hydrogen cyanide, acetylene and ethylene, as well as the products of their reactions, were found in comets, interstellar space and atmospheres of different planets, for example, in the atmosphere of Titan, the largest satellite of Saturn. These small molecules may be involved in the processes of multistage formation of complex organic compounds and...
This work was aimed at quantitative determination of the absorbed doses under X-ray irradiation of cryogenic deposited films, particularly related to the matrix isolation experiment. The relative absorbed doses in the layers of solid noble gases of different thickness irradiated with an X-ray tube (46.6 kVp) in the specified cryostat geometry were...
Macrocyclic 18-crown-6⋅SrCl2 and 18-crown-6⋅YCl3⋅4.25H2O complexes were synthesized, characterized by FTIR and DSC/TGA analysis and exposed to X-rays irradiation to study their resistance to polyether ring cleavage at early radiolysis stages by using EPR spectroscopy. Yttrium complex was found to be less stable in comparison with that of strontium...
The structure and spectroscopy of hydrogen-bonded complexes of partially fluorinated methanes attract considerable interest from both fundamental and applied points of view. Here we report an experimental and theoretical study on CH2F2⋯CO complex, which represents the first example of difluoromethane complex characterized by matrix isolation vibrat...
The transformations of isolated toluene molecules under X-ray radiolysis in solid noble gas matrices at 6 K were characterized by FTIR spectroscopy. It was found that the efficiency of the radiation-induced decomposition of toluene was generally comparable to that of benzene. Meanwhile, a remarkable matrix effect was observed: toluene is more stabl...
A single-electron reduction of carbon dioxide is an important basic step in various processes, ranging from interstellar chemistry to photocatalytic transformations. In this work we report a FTIR spectroscopic study on the reactions of carbon dioxide (12CO2 and 13CO2) with the radiation-induced excess electrons in deposited cryogenic matrices with...
X-radiolysis of the noble-gas matrices containing both H2O and CO was investigated at 5 K using infrared spectroscopy. It was found that formic acid molecule (HCOOH) could be produced from the matrix-isolated H2O⋯CO complexes, either directly as a result of irradiation or upon the subsequent annealing activating the trans-HOCO + H reaction. The for...
The X-ray-induced transformations of CHF3/CO/Ar and CHF3/CO/Kr systems were investigated by FTIR matrix isolation spectroscopy at 6 K. It was found that addition of CO suppressed decomposition of fluoroform in an Ar matrix probably due to trapping of matrix holes by CO and CHF3…CO complexes. Considerable increase of the CF3/CF2 ratio with increasin...
The generation of metal nanostructures by radiation-induced reduction of copper ions in aqueous dispersions of macromolecular complexes of poly(acrylic acid) and polyvinylimidazolе has been studied in the pH range of 2.3–4.3. It was shown that an effective coordination number of Cu2+ in the complex with polymer units decreased at lower pH, which re...
FKrCF and FXeCF were synthetized in solid krypton and xenon matrices at cryogenic temperatures. These molecules representing a new class of noble-gas compounds are formed as a result of reaction between mobile F atoms and trapped CF fragment in solid Kr and Xe, which occur after X-ray radiolysis of CH2F2 in the corresponding matrices. The assignmen...
Investigations of the low-temperature radiation-induced transformations in the C2H2–H2O system are relevant to the chemistry occurring in interstellar and cometary ices. In this work we applied a matrix isolation technique to study the radiation-driven evolution of this system at molecular level in order to get new mechanistic insight. The 1:1 C2H2...
Development of the physico-chemical basis for applications of nanoradiosensitizers for targeted treatment of tumours is one of the crucial issues of modern radiotherapy. Ceramic nanoparticles (NPs) composed of heavy metal oxides are considered as prospective sensitizers, particularly for X-ray treatment. The present study reports a novel approach t...
1. Isolated benzene molecules demonstrate rather efficient transformation upon irradiation in rigid inert media at cryogenic temperatures. The decomposition yield depends significantly on matrix physical properties.
2. Phenyl radical and fulvene are the major primary products of radiolysis of matrix isolated benzene. The relative yield of phenyl r...
Effects of cation size on relative yields of macrocycle cleavage under irradiation of stereoisomeric dicyclohexano-18-crown-6 complexes with alkaline earth metal chlorides were studied to mimic the radiolysis of the macrocyclic components of metal-loaded extractants applicable for radioactive waste reprocessing. Chloride-anions was found to prevent...
The radiation resistance of aromatic compounds is one of the key concepts of basic and applied radiation chemistry in condensed phases. Usually it is attributed to the intrinsic radiation stability of benzene ring. In this work we have first demonstrated that the isolated benzene molecules undergo rather efficient radiation-induced degradation in r...
Acetonitrile and the species resulting from its dehydrogenation play an important role in the radiation-induced evolution of organic matter in space environment. In this work we report on FTIR spectroscopic studies of the degradation of isolated CH3CN and CD3CN molecules induced by prolonged X-ray irradiation in solid noble gas matrices at 5 K. The...
The composites with localization of copper nanoparticles on the surface of interpolymer films were prepared by X-ray irradiation of poly(1-vinyl-1,2,4-triazole) – poly(acrylic acid) – Cu ²⁺ complexes. The kinetics of radiation-chemical reduction of ions Cu ²⁺ in films of stoichiometric and nonstoichiometric complexes of poly(1-vinyl-1,2,4-triazole)...
The structural and spectroscopic features of the CHF3…H2O complex have been investigated using high-level ab initio calculations and IR matrix isolation spectroscopy. In contrast to previous findings, the computations at the CCSD(T)/L3a_3 and MP2/L3a_3 levels of theory revealed only one structure of the complex stabilized by two C-H…O and O-H…F hyd...
Copper, silver and gold nanoparticles were obtained by reduction of metal ions under X-ray irradiation of “layer-by-layer” (LbL) coatings in a water-alcohol medium. The precursors for metal polymer composites (metallopolymer complexes) were prepared by sorption of metal ions in polyethyleneimine - poly (styrenesulfonic acid) and polyethyleneimine -...
Effects of irradiations of Phage Lambda dry DNA samples at room and cryogenic temperatures with 158 MeV Xe and 48 MeV Ar ions were investigated. These ions primary transfer energy into the electronic subsystem of a target: dE/dx = Se, SeXe = 10.8 keV/nm and SeAr = 3.5 keV/nm. Site-specific enzymes restriction endonucleases were applied to indicate...
The X-ray irradiation of aqueous solutions containing 1-vinyl-1,2,4-triazole (monomer) and gold ions results in simultaneous polymerization and formation of nanoparticles, which provides a single-step preparation of metal-polymeric nanohybrids.
The radiation-chemical synthesis of metal nanoparticles embedded into polymer matrices is an effective tool for preparation of the composite materials with very useful functional properties. This paper presents a review of an original approach to a single-step production of such materials via the radiation-induced reduction of the interpolyelectrol...
We report an experimental and theoretical study on the complex of a noble-gas hydride HKrCCH with carbon dioxide. This species was prepared by the annealing-induced H + Kr + CCH···CO2 reaction in a krypton matrix, the CCH···CO2 complexes being produced by UV photolysis of propiolic acid (HCCCOOH). The HKr stretching mode of the HKrCCH···CO2 comple...
Complexes of 18-crown-6 with BaCl2, Ba(NO3)2 and Ba(NTf2)2 salts were synthesized and irradiated with X-rays to simulate the radiation degradation of a macrocyclic component of extractants based on crown ether solutions in commonly used solvents. Structures and post-irradiation transformations of radical products stabilized in these complexes at 77...
The radiation-induced transformations of acetylene, ethylene and ethane molecules under X-ray radiolysis in cryogenic media (noble gas matrices and neat hydrocarbon ices) at 5 K were characterized by FTIR spectroscopy. The radiation-chemical yields of decomposition of isolated hydrocarbon molecules were estimated in different solid noble gas matric...
Intermolecular complexes between CHF3 and CO have been studied by ab initio calculations and IR matrix isolation spectroscopy. The computations at the MP2 and CCSD(T) levels of theory indicated five minima on the potential energy surface (PES). The most energetically favorable structure is the C(CO)-H(CHF3) coordinated complex (Cs symmetry) with th...
Ionic Liquid/Crown Ether compositions are an attractive alternative to traditional extractants in the processes for spent nuclear fuel and liquid radioactive wastes reprocessing. These compositions are exposed to ionizing radiation, and their radiation stability, especially in the presence of metal salts, is a crucial issue. In the present study, t...
We report on the complex of a noble-gas hydride HXeOH with carbon monoxide. This species is prepared via the annealing-induced H + Xe + OH···CO reaction in a xenon matrix, the OH···CO complexes being produced by VUV photolysis of the H2O···CO complexes. The H-Xe stretching mode of the HXeOH···CO complex absorbs at 1590.3 cm-1 and it is blue-shifted...
We report on the preparation and vibrational characterization of the C2H3⋯CO2 complex, the first example of a stable intermolecular complex involving vinyl radicals. This complex was prepared in Ar and Kr matrices using UV photolysis of propiolic acid (HC3OOH) and subsequent thermal mobilization of H atoms. This preparation procedure provides vinyl...
Structure and spectroscopic features of the CF2⋯HF complexes were studied by ab initio calculations at the CCSD(T) level and matrix isolation FTIR spectroscopy. The calculations predict three stable structures. The most energetically favorable structure corresponds to hydrogen bonding of HF to the lone pair of the C atom (the interaction energy of...
The HCN…CO complex and its X-ray induced transformation to HNC…CO in solid noble gas (Ng) matrices (Ng = Ne, Ar, Kr, Xe) was first characterized by matrix isolation FTIR spectroscopy at 5 K. The HCN…CO complex was obtained by deposition of the HCN/CO/Ng gaseous mixtures. The assignment was based on extensive quantum chemical calculations at the CCS...
The transformations of isolated CH3CN molecules in various solid noble-gas matrices (Ne, Ar, Kr, and Xe) under the action of X-ray irradiation at 5 K were investigated by FTIR spectroscopy. The main products are CH3NC, CH2CNH and CH2NCH molecular isomers as well as CH2CN and CH2NC radicals. The matrix has a strong effect on the distribution of reac...
Conformers of carboxyl radical have been studied by IR spectroscopy in argon and nitrogen matrices. In an argon matrix, only the lower-energy conformer trans-HOCO is observed, whereas both cis and trans conformers are found for deuterated carboxyl radical DOCO. In a nitrogen matrix, both conformers of HOCO and DOCO isotopologues can be prepared, in...
Formyl radical HCO is an important reactive intermediate in combustion, atmospheric and extraterrestrial chemistry. Like in the case of other transients, the lack of knowledge of the absolute IR intensities limits the quantitative spectroscopic studies on this species. We report the first experimental determination of the absorption intensities for...
The X-ray induced transformations in the /Ng systems (Ng=Ne, Ar, Kr or Xe) at 6 K were studied by FTIR spectroscopy. The radiation-induced decomposition of was found to be rather inefficient in solid xenon with low ionization energy, which suggests primary significance of the positive hole transfer from matrix to the fluoroform molecule. , : , and...
The bimetallic nanostructures are of considerable interest for various prospective applications. This paper reports a generation of the Cu/Ag and Cu/Au nanoparticles in the interpolyelectrolyte films irradiated in aqueous media. It was shown that the radiation-induced reduction of (Cu/Ag) or (Cu/Au) ions in the matrix of poly(acrylic acid)-polyethy...
We report on the experimental and theoretical infrared spectrum of the C2H···CO2 complex. This complex was prepared by UV photochemistry of propiolic acid (HC3OOH) in argon and krypton matrices. The experimental bands of C2H in the C2H···CO2 complex are blue-shifted from those of C2H monomer. The calculations of the C2H···CO2 structures were perfor...
Spectroscopic characteristics and X-ray induced transformations of the HCN ⋯CO2 complex in solid Ar and Kr matrices were studied by FTIR spectroscopy and ab initio calculations at the CCSD(T) level. The complex was prepared by deposition of the HCN/CO2/Ng gas mixtures (Ng = Ar or Kr). The comparison of the experiment and calculations prove formatio...
Vacuum ultraviolet (VUV, 130-170 nm) photochemistry of the H2OCO complex is studied by matrix-isolation infrared spectroscopy. The H2OCO complexes in Ne, Ar, Kr, and Xe matrices are generated by ultraviolet (UV, 193 and 250 nm) photolysis of formic acid (HCOOH). VUV photolysis of the H2OCO complexes is found to lead to the formation of the OHCO rad...
The effect of X-ray irradiation on methanol molecules (CH3OH, CD3OH, and (13)CH3OH) isolated in solid noble gas matrices (Ne, Ar, Kr, and Xe) was studied by FTIR spectroscopy at 6 K. CH2OH˙, H2CO, HCO˙ and CO were found to be the main degradation products. Somewhat unexpectedly, the production of CO is quite prominent, even at low doses, and it str...
The X-ray-induced transformations of simple chlorofluorocarbons (CFCl3 and CF2Cl2) in solid noble-gas matrices (Ne, Ar, Kr and Xe) at 7 K were studied in order to elucidate basic mechanisms of the radiation-chemical degradation with possible implications for stratospheric and extraterrestrial ice chemistry. The decomposition of parent molecules and...
Effect of syn/anti-stereoisomerism of the macrocycle on radiation-chemical transformations of dicyclohexano-18-crown-6 complexes with BaCl2 was studied by EPR spectroscopy. It was found that the stereoisomerism affected the composition of radicals produced under radiolysis at 77 K. In addition, it was demonstrated that the yield of post-radiation m...
It has been shown that the RTL curve of n-tetracosane consists of several curves with dissimilar shapes. These curves have been separated. Their behavior depending on radiation dose, time, and bleaching wavelength has been investigated. Mechanisms for the formation of individual curves have been suggested.
Radiothermoluminescence (RTL) curves of mixtures of C20 and C24 n-alkanes have been deconvoluted into the curves of crystalline and disordered regions, and their change depending on the mixture composition has been analyzed. The shape of the total RTL curve of the mixture regardless of the its composition is fundamentally different from that shape...
It has been shown that a radiothermoluminescence curve of polyethylene with extended-chain crystals can be separated into components corresponding to intracrystalline and disordered regions of the polymer by introducing an electron scavenger.
The spectral features and reactions of ion-radical intermediates produced from organic carbonates in low-temperature matrices were investigated by EPR spectroscopy and quantum-chemical calculations. It was shown that radical cations of diethyl carbonate and dimethyl carbonate underwent intramolecular hydrogen transfer to yield alkyl-type species, a...
In this work we report the results of systematic studies on the radiation-induced transformations in HCN/Ng systems (Ng=Ne, Ar, Kr or Xe) at 7 K using a combination of FTIR and EPR spectroscopy. It was shown that HCN underwent efficient decomposition producing H atoms, CN radicals and HNC isomer. The thermally induced reactions of H atoms in differ...
The radiation-induced transformations of small molecules at low temperatures play an important role in the interstellar, planetary and atmospheric chemistry. This work presents a review of our recent model studies on the radiation chemistry of relevant molecules in solid noble gas (Ng) matrices, including some preliminary new results. Among the tri...
The effect of X-ray irradiation on the isolated formic acid molecules (HCOOH) in solid noble gas matrices (Xe, Kr, Ar, and Ne) at very low temperatures (6 K) was first studied by FTIR spectroscopy. Carbon oxides (CO and CO2) and hydrocarboxyl radicals (HOCO) have been detected as the principal degradation products. The formation of HOCO radicals re...
The primary radiation-induced processes in irradiated low-temperature pyrrolidinium- and piperidinium-type ionic liquids were investigated by EPR and optical absorption spectroscopy. A narrow singlet signal in the EPR spectra of irradiated ionic liquids was attributed to the physically stabilized electron. Broad absorption band in visible region wa...
Formation of paramagnetic intermediates in macrocyclic complexes of cis-syn-cis-dicyclohexano-18-crown-6 (DCH18C6) with alkaline earth metal nitrates under X-rays irradiation was studied by EPR spectroscopy. NO32- dianions appear to be predominant intermediate species in the samples irradiated at 77 K at low doses (up to 40 kGy). This result was in...
The structure and conformation of radicals produced by X-ray irradiation of three polymorphic forms of D-mannitol were investigated using EPR spectroscopy. In all the cases, primary species were identified as radicals resulting from hydrogen abstraction from position 3 or 4 of the mannitol molecule. It was found that molecular packing in crystals o...
The strongest vibrational feature of a radical anion produced from the diacetyl molecule under radiolysis in a low-temperature dimethyl ether matrix has been characterized for the first time by the analysis of IR- and EPR-spectroscopic data supported by quantum-chemical calculations.
The formation of copper nanoparticles (Cu-NPs) in irradiated aqueous solutions of star-shaped poly(acrylic acid) (PAA) were studied at two pH values. Transmission electron microscopy (TEM) demonstrates that the star-shaped macromolecules loaded with Cu2+ ions can act as individual nanosized containers and provide a perfect control over the size and...