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1.
Adv Sci (Weinh) ; : e2202352, 2022 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-36109171

RESUMO

In this work, unique Co3 O4 /N-doped reduced graphene oxide (Co3 O4 /N-rGO) composites as favorable sulfur immobilizers and promoters for lithium-sulfur (Li-S) batteries are developed. The prepared Co3 O4  nanopolyhedrons (Co3 O4 -NP) and Co3 O4  nanocubes mainly expose (112) and (001) surfaces, respectively, with different atomic configurations of Co2+ /Co3+ sites. Experiments and theoretical calculations confirm that the octahedral coordination Co3+ (Co3+ Oh ) sites with different oxidation states from tetrahedral coordination Co2+ sites optimize the adsorption and catalytic conversion of lithium polysulfides. Specially, the Co3 O4 -NP crystals loaded on N-rGO expose (112) planes with ample Co3+ Oh active sites, exhibiting stronger adsorbability and superior catalytic activity for polysulfides, thus inhibiting the shuttle effect. Therefore, the S@Co3 O4 -NP/N-rGO cathodes deliver excellent electrochemical properties, for example, stable cyclability at 1 C with a low capacity decay rate of 0.058% over 500 cycles, superb rate capability up to 3 C, and high areal capacity of 4.1 mAh cm-2 . This catalyst's design incorporating crystal surface engineering and oxidation state regulation strategies also provides new approaches for addressing the complicated issues of Li-S batteries.

2.
Blood Cells Mol Dis ; 97: 102697, 2022 11.
Artigo em Inglês | MEDLINE | ID: mdl-35872110

RESUMO

MicroRNAs are known to regulate cell proliferation, differentiation, and apoptosis. However, the immunological mechanism and role of microRNA9-3 (miR9-3) are unknown. This study used CRISPR/cas9 technology to knock out miR9-3 to modulate its expression level. FACS results showed that the absolute number of total B cells declined in miR9-3-deficiency in the spleen (Sp), bone marrow (BM), and lymph node (LN) to different levels compared to the wild-type. Also, the absolute numbers of Fo, T1, and T2 cells decreased both in Sp and LN. The absolute numbers of total T cells in Sp and LN declined sharply; CD4+ and CD8+ T cells showed a dramatic decrease in Sp, LN, and Th (thymus) of the miR9-3- group. In BM, the cells number of immature B cells, pro-pre-B cells, pro-B cells, and pre-B cells reduced to different levels, while mature B cells were comparable to wild-type. These data illustrated that miR9-3-deficiency impaired the development of B cells in BM. Also, the development of T cells was severely impaired. In Th, the numbers of DN and DP cells were remarkably reduced in the miR9-3 mutant mice. Also, the numbers of DN-1, DN-3, and DN-4 cells decreased. The absolute number of cells in the hematopoietic stem cell (HSC) system such as LT-HSC (long-term HSC), ST-HSC (short-term HSC), MPP (multipotent progenitor), GMP (granulocyte-macrophage progenitor), CMP (common myeloid progenitors), MEP (megakaryocyte-erythroid progenitor), and CLP (common lymphoid progenitor) all were decreased in miR9-3 deficient mice. These results showed that miR9-3 deficiency initiated the damage to the entire hematopoietic system. Moreover, the absolute number of myeloid cells in both Sp and BM decreased in mutant mice. The cells number of NK cells showed a sharp reduction in Sp whereas the change was not significant in BM. The above results suggest that miR9-3 participates in the immune regulation of B cells, T cells, and the HSC system, highlighting its regulatory roles.


Assuntos
Linfócitos B , Linfócitos T CD4-Positivos , Linfócitos T CD8-Positivos , Células-Tronco Hematopoéticas , MicroRNAs , Animais , Medula Óssea/patologia , Células da Medula Óssea , Diferenciação Celular , Células-Tronco Hematopoéticas/metabolismo , Camundongos , Camundongos Endogâmicos C57BL , MicroRNAs/imunologia
3.
Phys Chem Chem Phys ; 24(26): 16244-16262, 2022 Jul 06.
Artigo em Inglês | MEDLINE | ID: mdl-35758314

RESUMO

Hydration free energy (HFE) as the most important solvation parameter is often targeted in ion model development, even though the reported values differ by dozens of kcal mol-1 mainly due to the experimentally undetermined HFE of the proton ΔG°(H+). The choice of ΔG°(H+) obviously affects the hydration of single ions and the relative HFE between the ions with different (magnitude or sign) charges, and the impacts of targeted HFEs on the ion solvation and ion-ion interactions are largely unrevealed. Here we designed point charge models of K+, Mg2+, Al3+, and Cl- ions targeting a variety of HFE references and then investigated the HFE influences on the simulations of dilute and concentrated ion solutions and of the salt ion pairs in gas, liquid, and solid phases. Targeting one more property of ion-water oxygen distances (IOD) leaves the ion-water binding distance invariant, while the binding strength increases with the decreasing (more negative) HFE of ions as a result of a decrease in ΔG°(H+) for the cation and an increase in ΔG°(H+) for the anion. The increase in ΔG°(H+) leads to strengthened cation-anion interactions and thus to close ion-ion contacts, low osmotic pressures, and small activity derivatives in concentrated ion solutions as well as too stable ion pairs of the salts in different phases. The ion diffusivity and water exchange rates around the ions are simply not HFE dependent but rather more complex. Targeting both the aqueous IOD and salt crystal properties of KCl was also attempted and the comparison between different models indicates the complexity and challenge in obtaining a balanced performance between different phases using classical force fields. Our results also support that a real ΔG°(H+) value of -259.8 kcal mol-1 recommended by Hünenberger and Reif guides ion models to reproduce ion-water and ion-ion interactions reasonably at relatively low salt concentrations. Simulations of a metalloprotein show that a relatively more positive ΔG°(H+) for Mg2+ model is better for a reasonable description of the metal binding network.


Assuntos
Cloreto de Sódio , Água , Íons , Termodinâmica , Água/química
4.
Front Microbiol ; 13: 805606, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35250927

RESUMO

Foot-and-mouth disease virus (FMDV) is a highly contagious viral disease that mainly infects cloven-hoofed animals. Propagation of FMDV by cell culture is an important method to preserve viral biological and antigenic characteristics, which is crucial in FMD monitoring and vaccine production. However, only a few cell lines are sensitive to FMDV, and there is still a lot of room for improvement. Acetylation is an important post-translational modification, which is dynamically regulated by histone acetyltransferases (HATs) and histone deacetylases (HDACs). However, the study of the relationship between FMDV and HDACs is still unclear. HDAC9 belongs to the class II of HDACs family; in this study, HDAC9 knockout (KO) BHK-21 cells were successfully established using CRISPR/cas9 technology. The results of karyotype analysis, growth curve analysis, and morphological observation showed that the HDAC9 knockout cell line was stable in growth and morphological characteristics. After infection with FMDV, the expression of viral RNA and protein, viral titers, and the copies of viral RNA in HDAC9-KO cells were significantly higher than those in NC cells. Meanwhile, RNA-seq technology was used to sequence HDAC9-KO cells and NC cells infected and uninfected with FMDV. It was found that the differentially expressed innate immune factors containing NFKBIA, SOD2, IL2RG, BCL2L1, CXCL1/2/3, and IL1RAP have significantly enriched in the Jak-STAT, NOD-like receptor, Toll-like receptor, NF-κB, and MAPK signaling pathway. RT-qPCR was performed to detect the expression level of differentially expressed genes and showed consistency with the RNA-seq data. These results preliminarily reveal the role of HDAC9 in host antiviral innate immune response, and the HDAC9-KO cell line could also serve as a useful tool for FMDV research.

5.
ACS Omega ; 7(9): 8115-8127, 2022 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-35284766

RESUMO

Isoflavone compounds are potent inhibitors against mitochondrial aldehyde dehydrogenase (ALDH2) for the treatment of alcoholism and drug addiction, and an in-depth understanding of the underlying structural basis helps design new inhibitors for enhanced binding. Here, we investigated the binding poses and strengths of eight isoflavone analogues (including CVT-10216 and daidzin) with ALDH2 via computational methods of molecular docking, molecular dynamics (MD) simulation, molecular mechanics Poisson-Boltzmann surface area (MM-PBSA), steered MD, and umbrella sampling. Neither the Vina scoring of docked and MD-sampled complexes nor the nonbonded protein-inhibitor interaction energy from MD simulations is able to reproduce the relative binding strength of the inhibitors compared to experimental IC50 values. Considering the solvation contribution, MM-PBSA and relatively expensive umbrella sampling yield good performance for the relative binding (free) energies. The isoflavone skeleton prefers to form π-π stacking, π-sulfur, and π-alkyl interactions with planar (Phe and Trp) or sulfur-containing (Cys and Met) residues. The enhanced inhibition of CVT-10216 originates from both end groups of the isoflavone skeleton offering strong van der Waals contacts and from the methylsulfonamide group at the 4' position by hydrogen bonding (HB) with neighboring receptor residues. These results indicate that the hydrophobic binding tunnel of ALDH2 is larger than the isoflavone skeleton in length and thus an extended hydrophobic core is likely a premise for potent inhibitors.

6.
Nanomaterials (Basel) ; 12(5)2022 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-35269373

RESUMO

The advantages of high energy density and low cost make lithium-sulfur batteries one of the most promising candidates for next-generation energy storage systems. However, the electrical insulativity of sulfur and the serious shuttle effect of lithium polysulfides (LiPSs) still impedes its further development. In this regard, a uniform hollow mesoporous Ni(OH)2@CNT microsphere was developed to address these issues. The SEM images show the Ni(OH)2 delivers an average size of about 5 µm, which is composed of nanosheets. The designed Ni(OH)2@CNT contains transition metal cations and interlayer anions, featuring the unique 3D spheroidal flower structure, decent porosity, and large surface area, which is highly conducive to conversion systems and electrochemical energy storage. As a result, the as-fabricated Li-S battery delivers the reversible capacity of 652 mAh g-1 after 400 cycles, demonstrating excellent capacity retention with a low average capacity loss of only 0.081% per cycle at 1 C. This work has shown that the Ni(OH)2@CNT sulfur host prepared by hydrothermal embraces delivers strong physical absorption as well as chemical affinity.

7.
Front Microbiol ; 13: 832275, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35154063

RESUMO

Phosphorylation is a widespread posttranslational modification that regulates numerous biological processes. Viruses can alter the physiological activities of host cells to promote virus particle replication, and manipulating phosphorylation is one of the mechanisms. Senecavirus A (SVA) is the causative agent of porcine idiopathic vesicular disease. Although numerous studies on SVA have been performed, comprehensive phosphoproteomics analysis of SVA infection is lacking. The present study performed a quantitative mass spectrometry-based phosphoproteomics survey of SVA infection in Instituto Biologico-Rim Suino-2 (IBRS-2) cells. Three parallel experiments were performed, and 4,520 phosphosites were quantified on 2,084 proteins. Gene Ontology (GO) functional enrichment and Kyoto Encyclopedia of Genes and Genomes (KEGG) pathway enrichment analyses showed that many phosphorylated proteins were involved in apoptosis and spliceosome pathways, and subcellular structure localization analysis revealed that more than half were located in the nucleus. Motif analysis of proteins with differentially regulated phosphosites showed that proline, aspartic acid, and glutamic acid were the most abundant residues in the serine motif, while proline and arginine were the most abundant in the threonine motif. Forty phosphosites on 27 proteins were validated by parallel reaction monitoring (PRM) phosphoproteomics, and 30 phosphosites in 21 proteins were verified. Nine proteins with significantly altered phosphosites were further discussed, and eight [SRRM2, CDK13, DDX20, DDX21, BAD, ELAVL1, PDZ-binding kinase (PBK), and STAT3] may play a role in SVA infection. Finally, kinase activity prediction showed 10 kinases' activity was reversed following SVA infection. It is the first phosphoproteomics analysis of SVA infection of IBRS-2 cells, and the results greatly expand our knowledge of SVA infection. The findings provide a basis for studying the interactions of other picornaviruses and their mammalian host cells.

8.
Adv Mater ; 34(2): e2105541, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34613619

RESUMO

Lithium-sulfur (Li-S) batteries are considered as one of the most promising next-generation rechargeable batteries owing to their high energy density and cost-effectiveness. However, the sluggish kinetics of the sulfur reduction reaction process, which is so far insufficiently explored, still impedes its practical application. Metal-organic frameworks (MOFs) are widely investigated as a sulfur immobilizer, but the interactions and catalytic activity of lithium polysulfides (LiPs) on metal nodes are weak due to the presence of organic ligands. Herein, a strategy to design quasi-MOF nanospheres, which contain a transition-state structure between the MOF and the metal oxide via controlled ligand exchange strategy, to serve as sulfur electrocatalyst, is presented. The quasi-MOF not only inherits the porous structure of the MOF, but also exposes abundant metal nodes to act as active sites, rendering strong LiPs absorbability. The reversible deligandation/ligandation of the quasi-MOF and its impact on the durability of the catalyst over the course of the electrochemical process is acknowledged, which confers a remarkable catalytic activity. Attributed to these structural advantages, the quasi-MOF delivers a decent discharge capacity and low capacity-fading rate over long-term cycling. This work not only offers insight into the rational design of quasi-MOF-based composites but also provides guidance for application in Li-S batteries.

9.
J Colloid Interface Sci ; 610: 527-537, 2022 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-34863545

RESUMO

The polysulfides shuttling and slow redox kinetics of sulfur-based cathodes have severely hindered the commercialization of lithium-sulfur (Li-S) batteries. Herein, distinctive three-dimensional microspheres composed of boron nitride (BN) nanosheets and reduced graphene oxide (rGO) were applied to act as efficient sulfur cathode hosts for the first time using in a spray-drying process. Using this construction, the robust microsphere structure could shorten ion diffusion pathways and supply sufficient spaces to alleviate the volumetric expansion of sulfur during lithiation. Besides, the synergistic effect between BN and rGO significantly enhanced polysulfides adsorption capability and accelerated their conversion, verified by the density functional theory (DFT) calculations and adsorption experiments. Consequently, the S-BN@rGO cathode could manifest the high initial capacity (1137 mAh g-1 at 0.2 C) and remarkable cycling/stability performance (572 mAh g-1 at 1 C after 500 cycles). These results shed light on a design concept of high-performance sulfur cathode host materials.

10.
J Phys Chem B ; 125(49): 13502-13518, 2021 12 16.
Artigo em Inglês | MEDLINE | ID: mdl-34860517

RESUMO

Ions are of central importance in nature, and a variety of potential models was proposed to model ions in different phases for an in-depth exploration of ion-related systems. Here, we developed point charge models of 14 monovalent ions with the traditional 12-6 Lennard-Jones (LJ) potential for use in conjunction with 11 water models of TIP3P, OPC3, SPC/E, SPC/Eb, TIP3P-FB, a99SB-disp, TIP4P-Ew, OPC, TIP4P/2005, TIP4P-D, and TIP4P-FB. The designed models reproduced the real hydration free energy (HFE) of ions and the ion-oxygen distance (IOD) in the first hydration shell accurately and simultaneously, a performance similar to the previously reported 12-6-4 LJ-type ion models (12-6 LJ plus an attractive C4 term for cations or a repulsive one for anions). This work, along with our previous work on di-, tri-, and tetravalent metal cations (J. Chem. Inf. Model. 2021, 61, 4031-4044; J. Chem. Inf. Model. 2021, 61, 4613-4629), demonstrates the feasibility of the simple 12-6 LJ potential in ion modeling. In order for the 12-6 LJ potential to reproduce both the HFE and IOD, the LJ R parameters need to be close to Shannon's ionic radii for the highly charged cations and to the Stokes's van der Waals (vdW) radii for the monovalent ions. With an additional C4 term, the R parameters of 12-6-4 LJ ion models agree well with the Stokes's vdW radii and have a more physical meaning. It appears that the C4 term can be merged into the 12-6 LJ potential by a rational tuning of R and the LJ well depth. Simulations of the osmotic coefficients of alkali chloride solutions and the properties of gaseous and solid alkali halides indicate the necessity of further optimizing ion-ion interactions via, for instance, targeting more properties or using a more physical (polarizable) model.


Assuntos
Metais , Água , Cátions , Entropia , Íons , Termodinâmica
11.
ACS Appl Mater Interfaces ; 13(47): 56085-56094, 2021 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-34783521

RESUMO

Lithium-sulfur (Li-S) batteries have attracted much attention attributed to their high theoretical energy density, whereas the parasitic shuttling behavior of lithium polysulfides (LiPS) hinders this technology from yielding practically competitive performance. Targeting this critical challenge, we develop an advanced polysulfide barrier by modifying the conventional separator with CNTs-interspersed V2C/V2O5 nanosheets to alleviate the shuttle effect. The partial oxidization of V2C MXene constructs the V2C/V2O5 composite with V2O5 nanoparticles uniformly dispersed on few-layered V2C nanosheets, which synergistically and concurrently improves the sulfur confinement and redox reaction kinetics. Moreover, the interstacking between the 1D CNTs and the 2D V2C/V2O5 not only prevents the agglomeration of nanosheets for efficient exposure of active interfaces but also constructs a robust conductive network for fast charge and mass transfers. The Li-S cells with V2C/V2O5/CNTs-modified separator realize a high initial capacity (1240.4 mAh g-1 at 0.2 C), decent capacity retention (82.6% over 500 cycles), and favorable areal capacity (5.9 mAh cm-2) at a raised sulfur loading (6.0 mg cm-2). This work affords a unique multifunctional separator design toward durable and efficient sulfur electrochemistry, holding great promise for improving the electrochemical properties of Li-S batteries.

12.
ACS Nano ; 15(12): 19457-19467, 2021 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-34723476

RESUMO

Lithium-sulfur (Li-S) batteries hold great promise for next-generation electronics owing to their high theoretical energy density, low cost, and eco-friendliness. Nevertheless, the practical implementation of Li-S batteries is hindered by the shuttle effect and sluggish reaction kinetics of polysulfides. Herein, the spray drying and chemical etching strategies are implemented to fabricate hierarchically porous MXene microspheres as a multifunctional sulfur electrocatalyst. The interconnected skeleton offers uniform sulfur distribution and prevents the restacking of MXene sheets, while the abundant edges endow the nanosheet-like Ti3C2 with rich active sites and regulated a d-band center of Ti atoms, leading to strong lithium polysulfide (LiPS) adsorption. The unsaturated Ti on edge sites can further act as multifunctional sites for chemically anchoring LiPS and lowering Li-ion migration barriers, accelerating LiPS conversion. Owing to these structural advantages, excellent cycling and rate performances of the sulfur cathode can be obtained, even under a raised sulfur loading and lean electrolyte content.

13.
Nanotechnology ; 33(11)2021 Dec 23.
Artigo em Inglês | MEDLINE | ID: mdl-34740208

RESUMO

The development of efficient sulfur host materials to address the shuttle effect issues of lithium polysulfides (LiPSs) is crucial in the lithium-sulfur (Li-S) batteries but still challenging. In the present study, a novel yolk shell structured MgCo-LDH/ZIF-67 composite is designed as Li-S battery cathode. In this composite, the shell layer is MgCo layered double hydroxide constructed by partially etching ZIF-67 nanoparticle by Mg2+, and the core is the unreacted ZIF-67 particle. The unique yolk shell structure not only provides abundant pores for sulfur accommodation, but also facilitates the electrolyte penetration and ion transport. The ZIF-67 core exhibits strong polar adsorption to LiPSs through the Lewis acid-base interactions, and the micropores/mesoporous can further trap LiPSs. Meanwhile, the MgCo-LDH shell exposes enough sulfur-philic sites for enhancing chemisorption and catalyzes LiPSs conversion. As a result, when MgCo-LDH/ZIF-67 is used as sulfur host in the cathode, the cell achieves a high discharge capacity of 1121 mAh g-1at 0.2 C, and an areal capacity of 5.0 mAh cm-2under high sulfur loading of 5.8 mg cm-2. The S/MgCo-LDH/ZIF-67 electrode holds a promising potential for the development of Li-S batteries.

14.
Plant Phenomics ; 2021: 9895241, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34557676

RESUMO

Plant growth rhythm in structural traits is important for better understanding plant response to the ever-changing environment. Terrestrial laser scanning (TLS) is a well-suited tool to study structural rhythm under field conditions. Recent studies have used TLS to describe the structural rhythm of trees, but no consistent patterns have been drawn. Meanwhile, whether TLS can capture structural rhythm in crops is unclear. Here, we aim to explore the seasonal and circadian rhythms in maize structural traits at both the plant and leaf levels from time-series TLS. The seasonal rhythm was studied using TLS data collected at four key growth periods, including jointing, bell-mouthed, heading, and maturity periods. Circadian rhythms were explored by using TLS data acquired around every 2 hours in a whole day under standard and cold stress conditions. Results showed that TLS can quantify the seasonal and circadian rhythm in structural traits at both plant and leaf levels. (1) Leaf inclination angle decreased significantly between the jointing stage and bell-mouthed stage. Leaf azimuth was stable after the jointing stage. (2) Some individual-level structural rhythms (e.g., azimuth and projected leaf area/PLA) were consistent with leaf-level structural rhythms. (3) The circadian rhythms of some traits (e.g., PLA) were not consistent under standard and cold stress conditions. (4) Environmental factors showed better correlations with leaf traits under cold stress than standard conditions. Temperature was the most important factor that significantly correlated with all leaf traits except leaf azimuth. This study highlights the potential of time-series TLS in studying outdoor agricultural chronobiology.

15.
Science ; 373(6562): eabg7484, 2021 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-34554812

RESUMO

Our study suggests that the global CO2 fertilization effect (CFE) on vegetation photosynthesis has declined during the past four decades. The Comments suggest that the temporal inconsistency in AVHRR data and the attribution method undermine the results' robustness. Here, we provide additional evidence that these arguments did not affect our finding and that the global decline in CFE is robust.


Assuntos
Dióxido de Carbono , Fotossíntese , Fertilização
16.
J Chem Inf Model ; 61(9): 4613-4629, 2021 09 27.
Artigo em Inglês | MEDLINE | ID: mdl-34467756

RESUMO

Here, we developed nonbonded point charge models using a simple Lennard-Jones (LJ) 12-6 potential for highly charged metal cations (18 trivalent and 6 tetravalent ions) for use with 11 water models of TIP3P, OPC3, SPC/E, SPC/Eb, TIP3P-FB, a99SB-disp, TIP4P-Ew, OPC, TIP4P/2005, TIP4P-D, and TIP4P-FB. The designed models simultaneously reproduce the hydration free energy (HFE) and ion-oxygen distance (IOD) in the first hydration shell with an error within 1 kcal/mol and 0.01 Å on average, respectively, and yield reasonable coordination numbers for most cations. Such performance is equivalent to the previously reported point charge models using a more complex 12-6-4 LJ-type potential, while the LJ R parameters of our models are much close to Shannon's revised effective ion radii than that of the 12-6-4 models. Our designed models overestimate the diffusion constants of several trivalent ions by 5-68%. The performance in predicting osmotic coefficients of trivalent chlorides in aqueous solution depends on the salt type. A calibration of cation-anion interacting LJ parameters reproduces the experimental osmotic coefficients of an AlCl3 solution at 0.2-3.0 mol/L. The effectiveness of our new models is further demonstrated by simulating a metalloprotein system with four force field/water combinations. This work facilitates accurate modeling of metal-containing systems by a variety of force fields and water models in aqueous solution.


Assuntos
Metais , Água , Cátions , Entropia , Termodinâmica
17.
Angew Chem Int Ed Engl ; 60(51): 26622-26629, 2021 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-34463010

RESUMO

Lithium-sulfur (Li-S) batteries are regarded as a promising next-generation system for advanced energy storage owing to a high theoretical energy density of 2600 Wh kg-1 . However, the practical implementation of Li-S batteries has been thwarted by the detrimental shuttling behavior of polysulfides, and the sluggish kinetics in electrochemical processes. Herein, a novel single atom (SA) catalyst with oversaturated Fe-N5 coordination structure (Fe-N5 -C) is precisely synthesized by an absorption-pyrolysis strategy and introduced as an effective sulfur host material. The experimental characterizations and theoretical calculations reveal synergism between atomically dispersed Fe-N5 active sites and the unique carbon support. The results exhibit that the sulfur composite cathode built on the Fe-N5 -C can not only adsorb polysulfides via chemical interaction, but also boost the redox reaction kinetics, thus mitigating the shuttle effect. Meanwhile, the robust three-dimensional nitrogen doped carbon nanofiber with large surface area, and high porosity enables strong physical confinement and fast electron/ion transfer process. Attributed to such unique features, Li-S batteries with S/Fe-N5 -C composite cathode realize outstanding cyclability and rate capability, as well as high areal capacities under raised sulfur loading, which demonstrates great potential in developing advanced Li-S batteries.

18.
Nat Plants ; 7(8): 998-1009, 2021 08.
Artigo em Inglês | MEDLINE | ID: mdl-34373605

RESUMO

For decades, the dynamic nature of chlorophyll a fluorescence (ChlaF) has provided insight into the biophysics and ecophysiology of the light reactions of photosynthesis from the subcellular to leaf scales. Recent advances in remote sensing methods enable detection of ChlaF induced by sunlight across a range of larger scales, from using instruments mounted on towers above plant canopies to Earth-orbiting satellites. This signal is referred to as solar-induced fluorescence (SIF) and its application promises to overcome spatial constraints on studies of photosynthesis, opening new research directions and opportunities in ecology, ecophysiology, biogeochemistry, agriculture and forestry. However, to unleash the full potential of SIF, intensive cross-disciplinary work is required to harmonize these new advances with the rich history of biophysical and ecophysiological studies of ChlaF, fostering the development of next-generation plant physiological and Earth-system models. Here, we introduce the scale-dependent link between SIF and photosynthesis, with an emphasis on seven remaining scientific challenges, and present a roadmap to facilitate future collaborative research towards new applications of SIF.


Assuntos
Clorofila A/fisiologia , Ciências da Terra , Fluorescência , Biologia Molecular , Fotossíntese/fisiologia , Folhas de Planta/fisiologia , Tecnologia de Sensoriamento Remoto/métodos
19.
J Chem Inf Model ; 61(8): 4031-4044, 2021 08 23.
Artigo em Inglês | MEDLINE | ID: mdl-34313132

RESUMO

Exploring a metal-involved biochemical process at a molecular level often requires a reliable description of metal properties in aqueous solution by classical nonbonded models. An additional C4 term for considering ion-induced dipole interactions was previously proposed to supplement the widely used Lennard-Jones 12-6 potential (known as the 12-6-4 LJ-type model) with good accuracy. Here, we demonstrate an alternative to modeling divalent metal cations (M2+) with the traditional 12-6 LJ potential by developing nonbonded point charge models for use with 11 water models: TIP3P, SPC/E, SPC/Eb, TIP4P-Ew, TIP4P-D, and TIP4P/2005 and the more recent OPC3, TIP3P-FB, OPC, TIP4P-FB, and a99SB-disp. Our designed models simultaneously reproduce the experimental hydration free energy, ion-oxygen distance, and coordination number in the first hydration shell accurately for most of the metal cations, an accuracy equivalent to that of the complex 12-6-4 LJ-type and double exponential potential models. A systematic comparison with the existing M2+ models is presented as well in terms of effective ion radii, diffusion constants, water exchange rates, and ion-water interactions. Molecular dynamics simulations of metal substitution in Escherichia coli glyoxalase I variants show the great potential of our new models for metalloproteins.


Assuntos
Metais , Simulação de Dinâmica Molecular , Cátions , Entropia , Água
20.
Sci Adv ; 7(27)2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-34193415

RESUMO

Industrial emissions play a major role in the global methane budget. The Permian basin is thought to be responsible for almost half of the methane emissions from all U.S. oil- and gas-producing regions, but little is known about individual contributors, a prerequisite for mitigation. We use a new class of satellite measurements acquired during several days in 2019 and 2020 to perform the first regional-scale and high-resolution survey of methane sources in the Permian. We find an unexpectedly large number of extreme point sources (37 plumes with emission rates >500 kg hour-1), which account for a range between 31 and 53% of the estimated emissions in the sampled area. Our analysis reveals that new facilities are major emitters in the area, often due to inefficient flaring operations (20% of detections). These results put current practices into question and are relevant to guide emission reduction efforts.

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