scholarly journals Design of Frustrated Lewis Pair in Defective TiO2 for Photocatalytic Non-Oxidative Methane Coupling

2022 ◽  
Author(s):  
Jiayu Ma ◽  
Qingqing Zhang ◽  
Ziyu Chen ◽  
Kai Kang ◽  
Lihan Pan ◽  
...  
Keyword(s):  
Dft Calculation ◽  
Mesoporous Structure ◽  
Electron Excitation ◽  
Lewis Base ◽  
Long Distance ◽  
Frustrated Lewis Pair ◽  
Oxidative Methane Coupling ◽  
Metal Doped ◽  
Hydrogenation Treatment

Abstract The efficient C-H polarization is the prerequisite for the low-temperature photocatalytic CH4 conversion, which however is restricted by the poor stretching ability of short-distanced lattice atoms. Herein, frustrated Lewis pair (FLP) composed of doped ion in TiO2 as Lewis acid (LA) and neighboring Ti-OH as Lewis base (LB) with a long distance (0.31-0.37 nm) were designed through DFT calculation and fabricated by hydrogenation treatment of metal-doped TiO2-SiO2 with macroporous-mesoporous structure. Benefitting from the long LA-LB distance and matched acid-base intensity, hydrogenated Ga-doped composite achieves superior C-H stretching with a high CH4 conversion rate (139 µmol g−1 h−1) to ethane. The photo-irradiation causes the electron excitation from Ga to Ti-OH according to the time-dependent DFT calculation and in situ EPR analysis, which promotes the formation and coupling of ·CH3. This work provides a key underpinning for regulating the characteristics of FLP for C-H activation and C-C coupling via light irradiation.

The high enrichment of Geobacter by TiN nanoarray anode catalyst for efficient microbial fuel cells

2021 ◽  
Vol 9 (12) ◽  
pp. 7726-7735
Author(s):  
Da Liu ◽  
Weicheng Huang ◽  
Qinghuan Chang ◽  
Lu Zhang ◽  
Ruiwen Wang ◽  
...  
Keyword(s):  
Fuel Cells ◽  
Hierarchical Structure ◽  
Microbial Fuel Cells ◽  
Dft Calculation ◽  
Experimental Results ◽  
Carbon Cloth ◽  
Anode Catalyst ◽  
High Enrichment

TiN nanoarrays, in situ grown on carbon cloth gather 97.2% of the model exoelectrogen Geobacter, greatly enhancing the MFCs' performance. The experimental results and DFT calculation certify the importance of the micro–nano-hierarchical structure.

scholarly journals Chromosomal painting of the sandpiper (Actitis macularius) detects several fissions for the Scolopacidae family (Charadriiformes)

2021 ◽  
Vol 21 (1) ◽  
Author(s):  
Melquizedec Luiz Silva Pinheiro ◽  
Cleusa Yoshiko Nagamachi ◽  
Talita Fernanda Augusto Ribas ◽  
Cristovam Guerreiro Diniz ◽  
Patricia Caroline Mary O´Brien ◽  
...  
Keyword(s):  
Chromosome Painting ◽  
Diploid Number ◽  
Chromosomal Evolution ◽  
Long Distance ◽  
Chromosomal Painting ◽  
Cytogenetic Studies ◽  
Burhinus Oedicnemus ◽  
Clear Idea ◽  
First Time

Abstract Background The Scolopacidae family (Suborder Scolopaci, Charadriiformes) is composed of sandpipers and snipes; these birds are long-distance migrants that show great diversity in their behavior and habitat use. Cytogenetic studies in the Scolopacidae family show the highest diploid numbers for order Charadriiformes. This work analyzes for the first time the karyotype of Actitis macularius by classic cytogenetics and chromosome painting. Results The species has a diploid number of 92, composed mostly of telocentric pairs. This high 2n is greater than the proposed 80 for the avian ancestral putative karyotype (a common feature among Scolopaci), suggesting that fission rearrangements have formed smaller macrochromosomes and microchromosomes. Fluorescence in situ hybridization using Burhinus oedicnemus whole chromosome probes confirmed the fissions in pairs 1, 2, 3, 4 and 6 of macrochromosomes. Conclusion Comparative analysis with other species of Charadriiformes studied by chromosome painting together with the molecular phylogenies for the order allowed us to raise hypotheses about the chromosomal evolution in suborder Scolopaci. From this, we can establish a clear idea of how chromosomal evolution occurred in this suborder.

Correlation of Grassy Lake and Cedar Lake ambers using infrared spectroscopy, stable isotopes, and palaeoentomology

2008 ◽  
Vol 45 (9) ◽  
pp. 1061-1082 ◽  
Author(s):  
Ryan C. McKellar ◽  
Alexander P. Wolfe ◽  
Ralf Tappert ◽  
Karlis Muehlenbachs
Keyword(s):  
Stable Isotopes ◽  
Fourier Transform ◽  
Infrared Spectroscopy ◽  
Late Cretaceous ◽  
Western Canada ◽  
Long Distance ◽  
Geochemical Fingerprinting ◽  
Long Distance Transport ◽  
Distance Transport

The Late Cretaceous Grassy Lake and Cedar Lake amber deposits of western Canada are among North America’s most famous amber-producing localities. Although it has been suggested for over a century that Cedar Lake amber from western Manitoba may be a secondary deposit having originated from strata in Alberta, this hypothesis has not been tested explicitly using geochemical fingerprinting coupled to comparative analyses of arthropod faunal content. Although there are many amber-containing horizons associated with Cretaceous coals throughout Alberta, most are thermally mature and brittle, thus lacking the resilience to survive long distance transport while preserving intact biotic inclusions. One of the few exceptions is the amber found in situ at Grassy Lake. We present a suite of new analyses from these and other Late Cretaceous ambers from western Canada, including stable isotopes (H and C), Fourier transform infrared (FTIR) spectra, and an updated faunal compendium for the Grassy and Cedar lakes arthropod assemblages. When combined with amber’s physical properties and stratigraphic constraints, the results of these analyses confirm that Cedar Lake amber is derived directly from the Grassy Lake amber deposit or an immediate correlative equivalent. This enables the palaeoenvironmental context of Grassy Lake amber to be extended to the Cedar Lake deposit, making possible a more inclusive survey of Cretaceous arthropod faunas.

Documenting the Ikpana interrogative system

2021 ◽  
Vol 42 (1) ◽  
pp. 63-100
Author(s):  
Jason Kandybowicz ◽  
Bertille Baron Obi ◽  
Philip T. Duncan ◽  
Hironori Katsuda
Keyword(s):  
Comprehensive Treatment ◽  
Left Periphery ◽  
Long Distance ◽  
Southeastern Part ◽  
Endangered Language ◽  
Research Questions ◽  
Volta Region ◽  
Movement Asymmetry ◽  
Syntactic Properties

Abstract This article provides a comprehensive treatment of the interrogative system of Ikpana (ISO 639-3: lgq), an endangered language spoken in the southeastern part of Ghana’s Volta region. The article features a description and analysis of both the morphosyntax and intonation of questions in the language. Polar questions in Ikpana are associated with dedicated prosodic patterns and may be segmentally marked. As for wh- interrogatives, Ikpana allows for optional wh- movement. Interrogative expressions may appear clause-internally in their base-generated positions or in the left periphery followed by one of two optionally droppable particles with distinct syntactic properties. In this way, wh- movement structures are either focus-marked constructions or cleft structures depending on the accompanying particle. We identify an interesting wh- movement asymmetry – unlike all other wh- movement structures, ‘how’ questions may not be formed via the focus-marked or cleft strategy. We document a number of other attested wh- structures in the language, including long-distance wh- movement, partial wh- movement, long-distance wh- in-situ, and multiple wh- questions. We argue that by allowing our documentation efforts to be shaped and guided by theoretically driven research questions, we reach deeper levels of description than would have been possible if approached from a purely descriptive-documentary perspective.

scholarly journals Comprehensive Evaluation of Transition Metal Doped Ni3N to Construct High-Efficiency Hydrogen Evolution Catalyst

2021 ◽  
Author(s):  
Meng Wang ◽  
Zepeng Lv ◽  
Xuewei Lv ◽  
Qian Li ◽  
Jie Dang
Keyword(s):  
Transition Metal ◽  
Hydrogen Evolution ◽  
Density Functional ◽  
Rational Design ◽  
Dft Calculation ◽  
High Efficiency ◽  
Comprehensive Evaluation ◽  
Low Cost ◽  
Alkaline Electrolyte ◽  
Metal Doped

Abstract Density functional theory (DFT) calculation indicators (ΔG, densities of state, D-band and bader charge) are commonly used to predict and analyze the hydrogen evolution reaction (HER) activity of catalysts, and most studies discuss only one or few of these indicators’ impact on catalysis, but still no report has comprehensively evaluated the influence of all these indicators on catalytic performance. Herein, foreseen by comprehensive consideration first, we report transition metal doped Ni3N nanosheets combined on Ni foam for utra-efficient alkaline hydrogen evolution. For dual transition metals doped Ni3N, Co,V-Ni3N exhibits remarkable HER performance with a significantly low overpotential of only 10 mV in alkaline electrolyte and 41 mV in alkaline seawater electrolyte at 10 mA cm− 2; while for single transition metal doped Ni3N, V-Ni3N exhibits the best performance with an overpotential of 15 mV and a Tafel slope of 37 mV dec− 1. Our work highlights the importance of comprehensive evaluation of DFT calculation indexes, and opens up a new method for the rational design of efficient and low-cost catalysts.

scholarly journals Base-Mediated Generation of Ketenimines from Ynamides: [3+2] Annulation with Azaallyl Anions.

2020 ◽  
Author(s):  
Agathe C. A. D’Hollander ◽  
Eugénie Romero ◽  
Kamsana Vijayakumar ◽  
Camille le Houérou ◽  
Pascal Retailleau ◽  
...  
Keyword(s):  
Dft Calculation ◽  
Reactive Intermediates ◽  
Reaction Conditions ◽  
Stereo Selectivity

Under basic conditions and heat, ynamides can serve as precursor to ketenimines, whose synthetic potential is often hampered by their difficulty of acces. Herein, we report that they can undergo a [3+2] cycloaddition with 2-azaallyl anions, obtained from benzylimines under the same reaction conditions. This reaction between two highly reactive intermediates, both generated in situ from bench stable starting materials, gives access to various nitrogen-rich heterocycles. The reaction usually proceeds with excellent diastereoselectivity, in favor of the cis adduct. Deuteration experiments and DFT calculation helped rationalize the regio and stereo-selectivity of the process as well as the formation of side-products.<br>

scholarly journals Distinct contracted conformations of the Tcra/Tcrd locus during Tcra and Tcrd recombination

2010 ◽  
Vol 207 (9) ◽  
pp. 1835-1841 ◽  
Author(s):  
Han-Yu Shih ◽  
Michael S. Krangel
Keyword(s):  
In Situ Hybridization ◽  
Fluorescence In Situ Hybridization ◽  
Three Dimensional ◽  
Double Negative ◽  
Thymocyte Development ◽  
Double Positive ◽  
Long Distance ◽  
Large Pool ◽  
Antigen Receptor Loci

Studies have suggested that antigen receptor loci adopt contracted conformations to promote long-distance interactions between gene segments during V(D)J recombination. The Tcra/Tcrd locus is unique because it undergoes highly divergent Tcrd and Tcra recombination programs in CD4−CD8− double negative (DN) and CD4+CD8+ double positive (DP) thymocytes, respectively. Using three-dimensional fluorescence in situ hybridization, we asked whether these divergent recombination programs are supported by distinct conformational states of the Tcra/Tcrd locus. We found that the 3′ portion of the locus is contracted in DN and DP thymocytes but not in B cells. Remarkably, the 5′ portion of the locus is contracted in DN thymocytes but is decontracted in DP thymocytes. We propose that the fully contracted conformation in DN thymocytes allows Tcrd rearrangements involving Vδ gene segments distributed over 1 Mb, whereas the unique 3′-contracted, 5′-decontracted conformation in DP thymocytes biases initial Tcra rearrangements to the most 3′ of the available Vα gene segments. This would maintain a large pool of distal 5′ Vα gene segments for subsequent rounds of recombination. Thus, distinct contracted conformations of the Tcra/Tcrd locus may facilitate a transition from a Tcrd to a Tcra mode of recombination during thymocyte development.

Paleoenvironments revealed by rare-earth element systematics in vertebrate bioapatite from the Lower Devonian of Svalbard

2016 ◽  
Vol 53 (8) ◽  
pp. 788-794
Author(s):  
Živilė Žigaitė ◽  
Alexandre Fadel ◽  
Alberto Pérez-Huerta ◽  
Teresa Jeffries ◽  
Daniel Goujet ◽  
...  
Keyword(s):  
Rare Earth ◽  
Rare Earth Element ◽  
Lower Devonian ◽  
Depositional Environment ◽  
Earth Element ◽  
Long Distance ◽  
Dental Tissues ◽  
Abundance Patterns ◽  
The Eu

In situ rare-earth element (REE) compositions have been measured in early vertebrate microremains from the Lower Devonian basin of Andrée Land (Svalbard), with the aim of obtaining information about their early depositional environment and potential reworking. Vertebrate microremains with different histology were used for the analyses, sourced from two different localities of marginal marine to freshwater sediments from geographically distant parts of the Grey Hœk Formation (Skamdalen and Tavlefjellet members). We selected thelodont and undescribed ?chondrichthyan scales, which allowed us to define potential taxonomic, histological, and taphonomic variables of the REE uptake. Results showed REE concentrations to be relatively uniform within the scales of each taxon, but apparent discrepancies were visible between the studied localities and separate taxa. The compilation of REE abundance patterns as well as REE ratios have revealed that thelodont and ?chondrichthyan originating from the same locality must have had different burial and early diagenetic histories. The shapes of the REE profiles, together with the presence and absence of the Eu and Ce anomalies, equally suggested different depositional and diagenetic environments for these two sympatric taxa resulting from either stratigraphical or long-distance reworking. The REE concentrations appear to have visible differences between separate dental tissues, particularly between enameloid and dentine of thelodonts, emphasizing the importance of in situ measurements in microfossil biomineral geochemistry.

Colonization of depopulated crinoids by symbionts: who comes from the bottom and who from the water column?

2015 ◽  
Vol 95 (8) ◽  
pp. 1607-1612 ◽  
Author(s):  
E.S. Mekhova ◽  
P.Y. Dgebuadze ◽  
V.N. Mikheev ◽  
T.A. Britayev
Keyword(s):  
Water Column ◽  
Field Experiments ◽  
Dispersal Ability ◽  
Long Distance ◽  
Sandy Substrate ◽  
Limited Dispersal ◽  
Set Up ◽  
Almost All ◽  
High Degree

Previous experiments with the comatulid Himerometra robustipinna (Carpenter, 1881) demonstrated intensive host-to-host migration processes for almost all symbiotic species both within host aggregations and among hosts separated by several metres. The aim of this study was to check the ability of symbionts to complete long-distance migrations, by means of two in situ experiments which depopulated the crinoid host. Two different sets of field experiments were set up: exposure of depopulated crinoids (set 1) on stony ‘islands’ isolated from native crinoid assemblages by sandy substrate, and (set 2) in cages suspended in the water column. Hosts from set 1 were exposed for 1, 2, 3 and 4 weeks to assess whether substrate has an influence on the symbionts' long-distance migrations. In set 2 cages were exposed for 10–11 days, aiming to check whether symbionts were able to disperse through the water column with currents. These experiments allow the conclusion that post-settled symbionts can actively migrate among their hosts. Symbionts are able to reach their hosts by employing two different ‘transport corridors’, by drifting or swimming in water column, and by moving on the bottom. Comparison of experimental results allows the division of symbionts into two conventional groups according to the dispersal ability of their post-settled stages: (1) species able to complete long-distance migrations, (2) species unable to migrate or having limited dispersal ability. The finding of the free-living shrimp Periclimenes diversipes Kemp, 1922 in set 2 raises the question about the factors that affect such a high degree of specialization of crinoid assemblages.

Phloem long-distance transport of CmNACP mRNA: implications for supracellular regulation in plants

Development ◽  
1999 ◽  
Vol 126 (20) ◽  
pp. 4405-4419 ◽  
Author(s):  
R. Ruiz-Medrano ◽  
B. Xoconostle-Cazares ◽  
W.J. Lucas
Keyword(s):  
Higher Plants ◽  
Phloem Transport ◽  
The Body ◽  
Pcr Analysis ◽  
Rt Pcr ◽  
Long Distance ◽  
Rna Molecules ◽  
Long Distance Transport ◽  
Meristem Development

Direct support for the concept that RNA molecules circulate throughout the plant, via the phloem, is provided through the characterisation of mRNA from phloem sap of mature pumpkin (Cucurbita maxima) leaves and stems. One of these mRNAs, CmNACP, is a member of the NAC domain gene family, some of whose members have been shown to be involved in apical meristem development. In situ RT-PCR analysis revealed the presence of CmNACP RNA in the companion cell-sieve element complex of leaf, stem and root phloem. Longitudinal and transverse sections showed continuity of transcript distribution between meristems and sieve elements of the protophloem, suggesting CmNACP mRNA transport over long distances and accumulation in vegetative, root and floral meristems. In situ hybridization studies conducted on CmNACP confirmed the results obtained using in situ RT-PCR. Phloem transport of CmNACP mRNA was proved directly by heterograft studies between pumpkin and cucumber plants, in which CmNACP transcripts were shown to accumulate in cucumber scion phloem and apical tissues. Similar experiments were conducted with 7 additional phloem-related transcripts. Collectively, these studies established the existence of a system for the delivery of specific mRNA transcripts from the body of the plant to the shoot apex. These findings provide insight into the presence of a novel mechanism likely used by higher plants to integrate developmental and physiological processes on a whole-plant basis.

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