preferential formation
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2021 ◽  
Author(s):  
Kori Sye ◽  
Clare Leahy ◽  
Josh Vura-Weis

Bridged μ-oxo iron bisporphyrins serve as photocatalysts for oxidative organic transformations, but suffer from low quantum efficiency. We use femtosecond optical and M2,3-edge XANES spectroscopy to investigate the early photodynamics of the μ-oxo iron bisporphyrin, (TPPFe)2O, providing evidence for the preferential formation of an TPPFe(III)+/TPPFe(III)-O- ion pair state instead of the desired TPPFe(II)/TPPFe(IV)=O.


Molecules ◽  
2021 ◽  
Vol 26 (21) ◽  
pp. 6595
Author(s):  
Peter Jonas Wickhorst ◽  
Heiko Ihmels ◽  
Thomas Paululat

Recently, several quadruplex-DNA-forming sequences have been identified in the insulin-linked polymorphic region (ILPR), which is a guanine-rich oligonucleotide sequence in the promoter region of insulin. The formation of this non-canonical quadruplex DNA (G4-DNA) has been shown to be involved in the biological activity of the ILPR, specifically with regard to its interplay with insulin. In this context, this contribution reports on the investigation of the association of the quadruplex-forming ILPR sequence a2 with insulin as well as with the well-known G4-DNA ligand 3,11-difluoro-6,8,13-trimethyl-8H-quino[4,3,2-kl]acridinium (1), also named RHPS4, by optical and NMR spectroscopy. CD- and NMR-spectroscopic measurements confirmed the preferential formation of an antiparallel quadruplex structure of a2 with four stacked guanine quartets. Furthermore, ligand 1 has high affinity toward a2 and binds by terminal π stacking to the G1–G11–G15–G25 quartet. In addition, the spectroscopic studies pointed to an association of insulin to the deoxyribose backbone of the loops of a2.


Materials ◽  
2021 ◽  
Vol 14 (21) ◽  
pp. 6328
Author(s):  
Michał Sobaszek ◽  
Marcin Gnyba ◽  
Sławomir Kulesza ◽  
Mirosław Bramowicz ◽  
Tomasz Klimczuk ◽  
...  

We report a method of growing a boron-doped diamond film by plasma-assisted chemical vapour deposition utilizing a pre-treatment of GaN substrate to give a high density of nucleation. CVD diamond was deposited on GaN substrate grown epitaxially via the molecular-beam epitaxy process. To obtain a continuous diamond film with the presence of well-developed grains, the GaN substrates are exposed to hydrogen plasma prior to deposition. The diamond/GaN heterojunction was deposited in methane ratio, chamber pressure, temperature, and microwave power at 1%, 50 Torr, 500 °C, and 1100 W, respectively. Two samples with different doping were prepared 2000 ppm and 7000 [B/C] in the gas phase. SEM and AFM analyses revealed the presence of well-developed grains with an average size of 100 nm. The epitaxial GaN substrate-induced preferential formation of (111)-facetted diamond was revealed by AFM and XRD. After the deposition process, the signal of the GaN substrate is still visible in Raman spectroscopy (showing three main GaN bands located at 565, 640 and 735 cm−1) as well as in typical XRD patterns. Analysis of the current–voltage characteristics as a function of temperature yielded activation energy equal to 93.8 meV.


2021 ◽  
Vol 9 ◽  
Author(s):  
Prince Ochonma ◽  
Claire Blaudeau ◽  
Rosalie Krasnoff ◽  
Greeshma Gadikota

Rational integration of chemical pathways at the molecular scale to direct thermodynamically favorable enhanced H2 production with inherent carbon removal from low-value substrates can be guided by exploring the thermodynamic limits of feasibility. The substrates of interest are biomass oxygenates that are water-soluble and uneconomical for separation from water. In this study, we investigate the thermodynamic feasibility of recovering H2 with inherent carbon removal from biomass oxygenates such as ethanol, methanol, glycerol, ethylene glycol, acetone, and acetic acid. The influence of biomass oxygenate-to-water ratios, reaction temperature of 150°C–325°C, and CaO or Ca(OH)2 as the alkalinity source on the yields of H2, CH4, CO2, and Ca-carbonate are investigated. By maintaining the fluids in the aqueous phase under pressure, energy needs associated with vaporization are circumvented. The hypothesis that enhanced alkalinity favors the preferential formation of CO (precursor for CO2 formation) over CH4 and aids the formation of calcium carbonate is investigated. The findings from these studies inform the feasibility, design of experiments, and the tuning of reaction conditions for enhanced H2 recovery with inherent carbon removal from biomass oxygenate sources.


Crystals ◽  
2021 ◽  
Vol 11 (8) ◽  
pp. 919
Author(s):  
Sorachon Yoriya ◽  
Phattarathicha Tepsri

This work presents a study of cenosphere separation from lignite high-calcium (~24 wt.%) fly ash by centrifugal method; this is the first report for Mae Moh, Thailand, fly ash with this high calcium content using this technique. The effect of centrifugal parameters on cenosphere yield and properties were investigated. Those properties include physical properties, morphology, chemical composition, and mineral phases. The recovery yields are in the range of 0.34–0.64%, approximately one third of the yield obtained from the general gravity settling method. Density, particle size, and morphology of the collected cenospheres appeared to be independent of sequence of the applied speeds and times. Interrelation of chemical composition and mineral phases was established, with the focus on calcium carbonate formation on cenosphere surface and crystallite size study. The study has revealed the preferential formation of calcite–(104) peak is observed–by cenospheres, with stable growth behavior of crystallite sizes obtained from all the centrifugal conditions. The result was compared to that obtained from the sink-float method for a better insight. The influence and limitation of the centrifugal method, the varied parameters, and the relevant reaction pathways on crystal growth process in terms of important dissolving species (i.e., Ca2+ and CO32−) behavior in the ash suspension were discussed.


Author(s):  
Declan McKearney ◽  
Ryan J. Roberts ◽  
Devon Mitchell ◽  
Jeffrey C. F. Cheung ◽  
Vance E. Williams ◽  
...  

2021 ◽  
Vol 9 (5) ◽  
pp. 479
Author(s):  
Zilin Wei ◽  
Tianfu Xu ◽  
Songhua Shang ◽  
Hailong Tian ◽  
Yuqing Cao ◽  
...  

Authigenic carbonates are widely distributed in marine sediments, microbes, and anaerobic oxidation of methane (AOM) play a key role in their formation. The authigenic carbonates in marine sediments have been affected by weathering and diagenesis for a long time, it is difficult to understand their formation process by analyzing the samples collected in situ. A pore water environment with 10 °C, 6 MPa in the marine sediments was built in a bioreactor to study the stages and characteristics of authigenic carbonates formation induced by microbes. In experiments, FeCO3 is formed preferentially, and then FeCO3-MgCO3 complete isomorphous series and a small part of CaCO3 isomorphous mixture are formed. According to this, it is proposed that the formation of authigenic carbonates performed by AOM and related microbes needs to undergo three stages: the rise of alkalinity, the preferential formation of a carbonate mineral, and the formation of carbonate isomorphous series. This work provides experimental experience and reference basis for further understanding the formation mechanism of authigenic carbonates in marine sediments.


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