Organic peroxy radicals (often abbreviated RO2) play a central role in the chemistry of the Earth's lower atmosphere. Formed in the atmospheric oxidation of essentially every organic species emitted, their chemistry is part of the radical cycles that control the oxidative capacity of the atmosphere and lead to the formation of ozone, organic nitrates, organic acids, particulate matter and other so-called secondary pollutants. In this review, laboratory studies of this peroxy radical chemistry are detailed, as they pertain to the chemistry of the atmosphere. First, a brief discussion of methods used to detect the peroxy radicals in the laboratory is presented. Then, the basic reaction pathways – involving RO2 unimolecular reactions and bimolecular reactions with atmospheric constituents such as NO, NO2, NO3, O3, halogen oxides, HO2, and other RO2 species – are discussed. For each of these reaction pathways, basic reaction rates are presented, along with trends in reactivity with radical structure. Focus is placed on recent advances in detection methods and on recent advances in our understanding of radical cycling processes, particularly pertaining to the complex chemistry associated with the atmospheric oxidation of biogenic hydrocarbons.

/pdf/laboratory-studies-of-organic-peroxy-radical-chemistry-an-nxealvo6x4.pdf

Laboratory studies of organic peroxy radical chemistry: an overview with emphasis on recent issues of atmospheric significance

The protein corona spontaneously develops and evolves on the surface of nanoscale materials when they are exposed to biological environments, altering their physiochemical properties and affecting their subsequent interactions with biosystems. In this Review, we provide an overview of the current state of protein corona research in nanomedicine. We next discuss remaining challenges in the research methodology and characterization of the protein corona that slow the development of nanoparticle therapeutics and diagnostics, and we address how artificial intelligence can advance protein corona research as a complement to experimental research efforts. We then review emerging opportunities provided by the protein corona to address major issues in healthcare and environmental sciences. This Review details how mechanistic insights into nanoparticle protein corona formation can broadly address unmet clinical and environmental needs, as well as enhance the safety and efficacy of nanobiotechnology products. 

/pdf/the-protein-corona-from-nanomedicine-to-environmental-2ufumlbw.pdf

The protein corona from nanomedicine to environmental science

The reaction of chlorine atoms with isoprene (2-methyl-1,3-butadiene) may be important in the marine boundary layer. The kinetics and mechanisms of this reaction have been studied at 760 Torr and 298 K using the photolysis of Cl2 as the chlorine atom source. Product studies in air were carried out using 40 m path length FTIR spectrometry. Rate constants were determined in either air or N2 using a relative rate technique and GC-FID to follow the decay of isoprene relative to n-butane. For comparison, the kinetics of the chlorine atom reactions with isoprene-d8, 1,3-butadiene, and 1,3-butadiene-d6 were also studied at 1 atm in air or N2 at 298 K. The rate constant ratios determined with n-butane as the reference compound are as follows:  isoprene (2.16 ± 0.17); isoprene-d8 (1.79 ± 0.22), 1,3-butadiene (2.01 ± 0.11); 1,3-butadiene-d6 (1.85 ± 0.10) (±2σ). The corresponding absolute rate constants, based on a value for n-butane of 2.11 ± 0.18 × 10-10 cm3 molecule-1 s-1, are as follows:  isoprene (4.6 ± 0.5); i...

Kinetics and Mechanism of the Reaction of Cl Atoms with 2-Methyl-1,3-butadiene (Isoprene) at 298 K

The Cl-atom-initiated photooxidation mechanism of CH3Br has been investigated in chamber experiments conducted under conditions applicable to the lower atmosphere. Major carbon-containing products obtained in the presence of O2 and NO, as determined by FTIR absorption spectroscopy, are CH2O and CO. In addition, HC(O)Br is observed in the absence of NO. At low temperature, in the presence of NO, CH2BrO2NO2 was also identified as a reaction product. The results are used to determine the fate of the alkoxy radical, CH2BrO. It is found that unimolecular decomposition of CH2BrO to CH2O + Br is the dominant process in 1 atm of O2 at all temperatures studied (between 228 and 298 K), while reaction with O2, CH2BrO + O2 → HC(O)Br + HO2, and the three-centered elimination of HBr, CH2BrO → HCO + HBr, are found to be minor pathways under these conditions (less than 5% each). Assumption of a rate constant of 6 × 10-14 cm3 molecule-1 s-1 for the reaction of CH2BrO with O2 (DeMore, W. B., et al. NASA JPL Publ. 1994, No....

Atmospheric Oxidation of CH3Br: Chemistry of the CH2BrO Radical

Injectable hydrogels for cartilage and bone tissue regeneration: A review.

Recent advances in polysaccharide-based in situ forming hydrogels.

Mechanistic study of the BrCH2O radical degradation in 700 Torr air

Kinetic and mechanistic studies for reactions of cf3ch2chf2 (hfc-245fa) initiated by h-atom abstraction using atomic chlorine

Product studies of Cl atom initiated oxidation of ClCH2CHO and Br atom initiated oxidation of BrCH2CHO were conducted by FTIR spectroscopy at 297 ± 2 K in 700 Torr of O2/N2 diluent, using reactant partial pressures in both the torr and millitorr ranges. The halogen atoms initiate reaction via hydrogen abstraction from the aldehydic group (CHO), producing haloacetyl radicals, XCH2CO, where X = Cl or Br. In 700 Torr of air, the XCH2CO radicals may react via three channels:  (i) O2-addition, XCH2CO + O2 → XCH2C(O)O2; (ii) unimolecular dissociation by CC bond cleavage, XCH2CO (+M) → XCH2 + CO (+M); and (iii) unimolecular dissociation by CX bond cleavage, XCH2CO (+M) → X + CH2CO (+M). All three channels were observed for BrCH2CO radicals, enabling estimation of the branching ratios, but ClCH2CO reacts only by O2-addition. Subsequent reactions of XCH2C(O)O2 radicals lead to XCH2O radical and CO2 formation. The ClCH2O radical reacts with O2 to produce CHClO and HO2, while the BrCH2O radical mainly eliminates the...

FTIR Spectroscopic Studies of the Mechanisms of the Halogen Atom Initiated Oxidation of Haloacetaldehydes

Applications of reduced graphene oxide (rGO) in many different areas have been gradually increasing owing to its unique physicochemical characteristics, demanding more understanding of their biological impacts. Herein, we assessed the toxicological effects of rGO in mammary epithelial cells. Because the as-synthesized rGO was dissolved in sodium cholate to maintain a stable aqueous dispersion, we hypothesize that changing the cholate concentration in the dispersion may alter the surface property of rGO and subsequently affect its cellular toxicity. Thus, four types of rGO were prepared and compared: rGO dispersed in 4 and 2 mg/mL sodium cholate, labeled as rGO and concentrated-rGO (c-rGO), respectively, and rGO and c-rGO coated with a protein corona through 1 h incubation in culture media, correspondingly named pro-rGO and pro-c-rGO. Notably, c-rGO and pro-c-rGO exhibited higher toxicity than rGO and pro-rGO and also caused higher reactive oxygen species production, more lipid membrane peroxidation, and more significant disruption of mitochondrial-based ATP synthesis. In all toxicological assessments, pro-c-rGO induced more severe adverse impacts than c-rGO. Further examination of the material surface, protein adsorption, and cellular uptake showed that the surface of c-rGO was coated with a lower content of surfactant and adsorbed more proteins, which may result in the higher cellular uptake observed with pro-c-rGO than pro-rGO. Several proteins involved in cellular redox mediation were also more enriched in pro-c-rGO. These results support the strong correlation between dispersant coating and corona formation and their subsequent cellular impacts. Future studies in this direction could reveal a deeper understanding of the correlation and the specific cellular pathways involved and help gain knowledge on how the toxicity of rGO could be modulated through surface modification, guiding the sustainable applications of rGO.

Biological Impacts of Reduced Graphene Oxide Affected by Protein Corona Formation.

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