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1.
Biopolymers ; : e23620, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39109846

RESUMO

Welan gum (WG) has a wide range of applications, but it is not yet suitable for applications such as oil recovery profile control that have complex requirements for viscosity, gelation properties, and so forth. Grafting modification is an important strategy for improving the property of WG, but there are few reports on controllable modification of WG to customize it for specific application. Acrylamide (AM) dosage was identified as the key factor affecting the grafting ratio of AM onto WG by a uniform experimental design. The grafting ratio can be directly adjusted between 99% and 378% based on the positive correlation with dosage of AM, and viscosity can be adjusted between 206 and 327 mPa s based on the negative correlation with grafting ratio. The 50% weight loss temperature of W11 with a grafting ratio of 110% raised from 314 to 336°C after grafting. The viscosity of the hydrogel formed with WG11 reached 15,654 mPa s, nearly nine times higher than that of unmodified WG. In addition, the gelation time can be controlled within 5 days, so that it can be injected to the optimal area in oilfield profile, avoiding pipeline blockage. This study enables adjusting viscosity of WG grafted with AM by controlling the grafting rate, and enhances gelation performance and thermal stability of WG, which will expand the application of WG in oil recovery and other fields.

2.
Angew Chem Int Ed Engl ; : e202413670, 2024 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-39295281

RESUMO

All-solid-state Li-S batteries (ASSLSBs) due to high theoretical energy density and exceptional safety are highly desirable for electric aircraft. However, as the flight altitude rises, the low-temperature performance is hampered by inadequate practical capacity. Here, we discover that low-temperature sulfur utilization is constrained by the multi-step endothermic conversion reaction. By introducing multi-chalcogen to modulate the local entropy, a short-chain molecule cathode is designed to shorten the reduction pathways and enhance low-temperature discharge capacity. Furthermore, the mismatched lithiation lattice of the short-chain cathode reduces the decomposition energy barriers, thus enhancing low-temperature charge/discharge reversibility. The designed short-chain cathode exhibits high cathode utilization (99.4%) and cycling stability (400 cycles, 92.2% retention) at room temperature, as well as delivers excellent discharge capacity (579.6 mAh g-1, -40 °C) and cycling performance (100 cycles, 98.4% retention, 394.9 Wh kg-1electrode, -20 °C) at low temperature. This study presents new opportunities to stimulate the development of low-temperature ASSLSBs.

3.
Angew Chem Int Ed Engl ; 63(17): e202319529, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38443734

RESUMO

Limited triple-phase boundaries arising from the accumulation of solid discharge product(s) in solid-state cathodes (SSCs) pose a challenge to high-property solid-state lithium-oxygen batteries (SSLOBs). Light-assisted SSLOBs have been gradually explored as an ingenious system; however, the fundamental mechanisms of the SSCs interface behavior remain unclear. Here, we discovered that light assistance can enhance the fast inner-sphere charge transfer in SSCs and regulate the discharge products with spherical particles generated via the surface growth model. Moreover, the high photoelectron excitation and transportation capabilities of SSCs can retard cathodic catalytic decay by avoiding structural degradation of the cathode with a reduced charge voltage. The light-induced SSLOBs exhibited excellent stability (170 cycles) with a low discharge-charge polarization overpotential (0.27 V). Furthermore, transparent SSLOBs with exceptional flexibility, mechanical stability, and multiform shapes were fabricated for theory-to-practical applications in sunlight-induced batteries. Our study opens new opportunities for the introduction of solar energy into energy storage systems.

4.
J Am Chem Soc ; 145(47): 25632-25642, 2023 Nov 29.
Artigo em Inglês | MEDLINE | ID: mdl-37943571

RESUMO

Owing to high ionic conductivity and mechanical strength, poly(vinylidene fluoride) (PVDF) electrolytes have attracted increasing attention for solid-state lithium batteries, but highly reactive residual solvents severely plague cycling stability. Herein, we report a free-solvent-capturing strategy triggered by reinforced ion-dipole interactions between Li+ and residual solvent molecules. Lithium difluoro(oxalato)borate (LiDFOB) salt additive with electron-withdrawing capability serves as a redistributor of the Li+ electropositive state, which offers more binding sites for residual solvents. Benefiting from the modified coordination environment, the kinetically stable anion-derived interphases are preferentially formed, effectively mitigating the interfacial side reactions between the electrodes and electrolytes. As a result, the assembled solid-state battery shows a lifetime of over 2000 cycles with an average Coulombic efficiency of 99.9% and capacity retention of 80%. Our discovery sheds fresh light on the targeted regulation of the reactive residual solvent to extend the cycle life of solid-state batteries.

5.
J Am Chem Soc ; 145(3): 1728-1739, 2023 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-36640116

RESUMO

Single-atom catalysts have been paid more attention to improving sluggish reaction kinetics and anchoring polysulfide for lithium-sulfur (Li-S) batteries. It has been demonstrated that d-block single-atom elements in the fourth period can chemically interact with the local environment, leading to effective adsorption and catalytic activity toward lithium polysulfides. Enlightened by theoretical screening, for the first time, we design novel single-atom Nb catalysts toward improved sulfur immobilization and catalyzation. Calculations reveal that Nb-N4 active moiety possesses abundant unfilled antibonding orbitals, which promotes d-p hybridization and enhances anchoring capability toward lithium polysulfides via a "trapping-coupling-conversion" mechanism. The Nb-SAs@NC cell exhibits a high capacity retention of over 85% after 1000 cycles, a superior rate performance of 740 mA h g-1 at 7 C, and a competitive areal capacity of 5.2 mAh cm-2 (5.6 mg cm-2). Our work provides a new perspective to extend cathodes enabling high-energy-density Li-S batteries.

6.
Angew Chem Int Ed Engl ; 61(42): e202207524, 2022 Oct 17.
Artigo em Inglês | MEDLINE | ID: mdl-36038511

RESUMO

Single atom tailored metal nanoparticles represent a new type of catalysts. Herein, we demonstrate a single atom-cavity coupling strategy to regulate performance of single atom tailored nano-catalysts. Selective atomic layer deposition (ALD) was conducted to deposit Ru single atoms on the surface concavities of PtNi nanoparticles (Ru-ca-PtNi). Ru-ca-PtNi exhibits a record-high activity for methanol oxidation reaction (MOR) with 2.01 A mg-1 Pt . Also, Ru-ca-PtNi showcases a significant durability with only 16 % activity loss. Operando electrochemical Fourier transform infrared spectroscopy (FTIR) and theoretical calculations demonstrate Ru single atoms coupled to cavities accelerate the CO removal by regulating d-band center position. Further, the high diffusion barrier of Ru single atoms in concavities accounts for excellent stability. The developed Ru-ca-PtNi via single atom-cavity coupling opens an encouraging pathway to design highly efficient single atom-based (electro)catalysts.

7.
Langmuir ; 37(40): 11931-11938, 2021 Oct 12.
Artigo em Inglês | MEDLINE | ID: mdl-34570495

RESUMO

Frost accretion occurs ubiquitously in various industrial applications and causes tremendous energy and economic loss, as manifested by the Texas power crisis that impacted millions of people over a vast area in 2021. To date, extensive efforts have been made on frost removal by micro-engineering surfaces with superhydrophobicity or lubricity. On such surfaces, air or oil cushions are introduced to suspend the frost layer and promote the rapid frost sliding off, which, although promising, faces the instability of the cushions under extreme frosting conditions. Most existing hydrophilic surfaces, characterized by large interfacial adhesion, have long been deemed unfavorable for frost shedding. Here, we demonstrated that a hydrophilic and slippery surface can achieve efficient defrosting. On such a surface, the hydrophilicity gave rise to a highly interconnected basal frost layer that boosted the substrate-to-frost heat transfer; then, the resulting melted frost readily slid off the surface due to the superb slipperiness. Notably, on our surface, the retained meltwater coverage after frost sliding off was only 2%. In comparison to two control surfaces, for example, surfaces lacking either hydrophilicity or slipperiness, the defrosting efficiency was 13 and 19 times higher and the energy consumption was 2.3 and 6.2 times lower, respectively. Our study highlights the use of a hydrophilic surface for the pronounced defrosting in a broad range of industrial applications.

8.
BMC Nurs ; 20(1): 144, 2021 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-34389005

RESUMO

BACKGROUND: Nursing work is associated with great pressure, and nurses are often overwhelmed. Therefore, correct emotional regulation is essential to improve nurses' job well-being and promote better engagement in nursing work. The purpose of this study was to establish a structural model to estimate the impact of Chinese clinical nurses' emotional intelligence on job well-being, using multiple intermediaries to explain the internal mechanisms underlying the relationship. METHODS: This was a cross-sectional study of 1475 registered nurses from a Chinese hospital who provided responses to emotional intelligence, empathy, communication satisfaction, and job well-being scales. Path analysis using a multiple mediation model was performed using AMOS 23.0. RESULTS: Among all clinical nurses who participated in the survey, 1475 (98.33 %) completed the questionnaire. The nurses' job well-being score was 83.61 ± 12.63. There was a significant positive correlation between job well-being and communication satisfaction, emotional intelligence, and empathy ability (r = 0.346-0.570, P < 0.001). Empathy and communication satisfaction partially mediated the relationship between emotional intelligence and job well-being, with effect sizes of 0.047 and 0.227, respectively. The chain mediating effect of empathy and communication satisfaction had a value of 0.045. CONCLUSIONS: It is recommended that hospital managers take actions to improve nurses' emotional intelligence level, and conduct professional psychological training to improve nurses' empathy and communication satisfaction, and ultimately improve their job well-being.

9.
J Nat Prod ; 82(5): 1114-1119, 2019 05 24.
Artigo em Inglês | MEDLINE | ID: mdl-31013087

RESUMO

Two new p-terphenyls, strepantibins A and B (1 and 2), along with the first representative of a naturally occurring bisphenyltropone, strepantibin C (3), were characterized from a Streptomyces sp. associated with the larvae of the mud dauber wasp Sceliphron madraspatanum. Their structures were determined by high-resolution electrospray ionization mass spectrometry, NMR, and X-ray crystallography data interpretation. Strepantibins A-C inhibited hexokinase II (HK2) activity and displayed antiproliferative activity against hepatoma carcinoma cells HepG-2, SMMC-7721 and plc-prf-5. In SMMC-7721 cells treated with strepantibin A, the morphological characteristics of apoptosis were observed.


Assuntos
Antineoplásicos/isolamento & purificação , Inibidores Enzimáticos/isolamento & purificação , Hexoquinase/antagonistas & inibidores , Streptomyces/química , Vespas/microbiologia , Animais , Antineoplásicos/química , Antineoplásicos/farmacologia , Inibidores Enzimáticos/química , Inibidores Enzimáticos/farmacologia , Células Hep G2 , Humanos , Espectroscopia de Ressonância Magnética , Espectrometria de Massas por Ionização por Electrospray
10.
Int J Biol Macromol ; 271(Pt 1): 132625, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38795884

RESUMO

Graft copolymerization is an effective approach to improve performance of polysaccharide. However, selecting the most suitable modification strategy can be challenging due to the intricate molecular structure. Rational design through computer aided molecular dynamics (MD) simulations requires substantial computational resources. This study designed a simplified MD simulation strategy and suggested that grafting acrylamide (AM) could effectively adjust the molecular conformation of xanthan gum (XG) and its derivatives, thus regulating its viscosity and gelation properties. To rationally modify XG, a uniform experimental design was applied to tune the grafting ratios ranging from 72 % to 360 %, resulting in XG-AM solutions with viscosity ranging from 9 to 104 mPa•s at a concentration of 0.3 %. XG-AM was crosslinked by acid phenolic resin to generate gel with the viscosity of 7890 mPa·s in 3 days, which was 13 times the viscosity of unmodified XG. The controllable gelation will enhance the efficacy of XG-AM in oil recovery. By integrating rational selection of grafting strategies based on simplified MD simulation of polysaccharide derivatives and controllable grafting modification with specified grafting rates, customized production of polysaccharide derivatives can meet the requirements of a diverse range of applications.


Assuntos
Simulação de Dinâmica Molecular , Polissacarídeos Bacterianos , Polissacarídeos Bacterianos/química , Viscosidade , Acrilamida/química , Polimerização
11.
Environ Int ; 186: 108632, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38583296

RESUMO

Plastic fragments are widely found in the soil profile of terrestrial ecosystems, forming plastic footprint and posing increasing threat to soil functionality and carbon (C) footprint. It is unclear how plastic footprint affects C cycling, and in particularly permanent C sequestration. Integrated field observations (including 13C labelling) were made using polyethylene and polylactic acid plastic fragments (low-, medium- and high-concentrations as intensifying footprint) landfilling in soil, to track C flow along soil-plant-atmosphere continuum (SPAC). The result indicated that increased plastic fragments substantially reduced photosynthetic C assimilation (p < 0.05), regardless of fragment degradability. Besides reducing C sink strength, relative intensity of C emission increased significantly, displaying elevated C source. Moreover, root C fixation declined significantly from 21.95 to 19.2 mg m-2, and simultaneously root length density, root weight density, specific root length and root diameter and surface area were clearly reduced. Similar trends were observed in the two types of plastic fragments (p > 0.05). Particularly, soil aggregate stability was significantly lowered as affected by plastic fragments, which accelerated the decomposition rate of newly sequestered C (p < 0.05). More importantly, net C rhizodeposition declined averagely from 39.77 to 29.41 mg m-2, which directly led to significant decline of permanent C sequestration in soil. Therefore, increasing plastic footprint considerably worsened C footprint regardless of polythene and biodegradable fragments. The findings unveiled the serious effects of plastic residues on permanent C sequestration across SPAC, implying that current C assessment methods clearly overlook plastic footprint and their global impact effects.


Assuntos
Pegada de Carbono , Plásticos , Solo , Solo/química , Carbono/análise , Atmosfera/química , Ciclo do Carbono , Ecossistema , Plantas , Sequestro de Carbono , Monitoramento Ambiental/métodos
12.
Chemosphere ; 345: 140342, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37783355

RESUMO

Co-combustion of sewage sludge (SS) and coal slime (CS) could improve the combustion properties of the two materials, however, high levels of trace elements (TEs) can be released from the two wastes, resulting in secondary pollution. The migration and transformation behavior of As, Cr, Pb, Zn, and Mn during co-combustion is explored in current research. The results showed co-combustion could inhibit the emission of Zn, As, Pb, and Mn, and the effect was more pronounced for Zn, As and Mn. Meanwhile, minerals like kaolinite and gypsum were found to generated in the ash from co-combustion but not solo-combustion. Model experiments demonstrated that kaolinite captured As, Pb and Mn, while gypsum captured Zn, As and Mn but facilitated the emission of Pb and Cr. This well explained the distinct TEs emission characteristics between co-combustion and solo combustion. As the temperature elevated, kaolinite in co-combustion ash decomposed and the generation of gypsum was promoted. In this way, the emission ratios of Zn, As, and Mn initially increased but subsequently decreased between 700 and 1300 °C, whereas Pb and Cr emission ratios increased by twofold within the same temperature range. Leaching characteristics and risk assessment code on co-combustion ashes were also conducted in this study. The results indicated a marginal elevation in the risk associated with trace elements (TEs) following co-combustion, provided that all five TEs remained within the limits of national standards.


Assuntos
Esgotos , Oligoelementos , Esgotos/análise , Incineração , Sulfato de Cálcio , Carvão Mineral/análise , Caulim , Chumbo , Cinza de Carvão
13.
Front Endocrinol (Lausanne) ; 13: 1065263, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36714578

RESUMO

Overweight and obesity have become a world-wide problem. However, effective intervention approaches are limited. Brown adipose tissue, which helps maintain body temperature and contributes to thermogenesis, is dependent on uncoupling protein1. Over the last decade, an in-creasing number of studies have found that activating brown adipose tissue and browning of white adipose tissue can protect against obesity and obesity-related metabolic disease. Brown adipose tissue has gradually become an appealing therapeutic target for the prevention and re-versal of obesity. However, some important issues remain unresolved. It is not certain whether increasing brown adipose tissue activity is the cause or effect of body weight loss or what the risks might be for sympathetic nervous system-dependent non-shivering thermogenesis. In this review, we comprehensively summarize approaches to activating brown adipose tissue and/or browning white adipose tissue, such as cold exposure, exercise, and small-molecule treatment. We highlight the functional mechanisms of small-molecule treatment and brown adipose tissue transplantation using batokine, sympathetic nervous system and/or gut microbiome. Finally, we discuss the causality between body weight loss induced by bariatric surgery, exercise, and brown adipose tissue activity.


Assuntos
Tecido Adiposo Marrom , Obesidade , Humanos , Tecido Adiposo Marrom/metabolismo , Obesidade/terapia , Obesidade/metabolismo , Tecido Adiposo Branco/metabolismo , Sistema Nervoso Simpático/metabolismo , Redução de Peso
14.
Adv Sci (Weinh) ; 9(4): e2103964, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34821481

RESUMO

Soluble redox mediators (RMs), an alternative to conventional solid catalysts, have been considered an effective countermeasure to ameliorate sluggish kinetics in the cathode of a lithium-oxygen battery recently. Nevertheless, the high mobility of RMs leads to serious redox shuttling, which induces an undesired lithium-metal degeneration and RM decomposition during trade-off catalysis against the sustainable operation of batteries. Here, a novel carbon family of graphdiyne matrix is first proposed to decouple the charge-carrying redox property of ferrocene and the shuttle effects. It is demonstrated that a ferrocene-anchored graphdiyne framework can function as stationary RM, not only preserving the redox-mediating capability of ferrocene, but also promoting the local orientated three-dimensional (3D) growth of Li2 O2 . As a result, the RM-assisted catalysis in lithium-oxygen battery remains of remarkable efficiency and stability without the depletion of oxidized RMs or lithium degradation, resulting in a significantly enhanced electrochemical performance.

15.
Sci Adv ; 8(35): eabq6261, 2022 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-36054349

RESUMO

Solid-state Li-O2 batteries (SSLOBs) have attracted considerable attention because of their high energy density and superior safety. However, their sluggish kinetics have severely impeded their practical application. Despite efforts to design highly efficient catalysts, efficient oxygen reaction evolution at gas-solid interfaces and fast transport pathways in solid-state electrodes remain challenging. Here, we develop a dual electronic-ionic microenvironment to substantially enhance oxygen electrolysis in solid-state batteries. By designing a lithium-decorative catalyst with an engineering crystal structure, the coordinatively unsaturated sites and high concentration of defects alleviate the limitations of electronic-ionic transport in solid interfaces and create a balanced gas-solid microenvironment for solid-state oxygen electrolysis. This strategy facilitates oxygen reduction reaction, mediates the transport of reaction species, and promotes the decomposition of the discharge products, contributing to a high specific capacity with a stable cycling life. Our work provides previously unknown insight into structure-property relationships in solid-state electrolysis for SSLOBs.

16.
Nat Prod Res ; 35(11): 1869-1873, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-31305144

RESUMO

In the course of searching for cytotoxic metabolites from insects associated actinomyces, two new natural p-terphenyl glycosides, strepantibin D (1) and strepantibin E (2), along with terferol (3), actinomycin D (4), actinomycin V (5) and actinomycin V0ß (6), were identified from the fermentation medium of a Streptomyces sp. which was obtained from the larva body of mud dauber wasp. Strepantibin D (1), previously reported as a synthetic derivative of terfestatin A, is firstly isolated as a natural p-terphenyl in this research. Strepantibin D (1) and terferol (3) showed medium cytotoxic activity against breast cancer cells MCF-7, MDA-MB-231 and BT-474. Actinomycins (4-6), especially actinomycin V (5), displayed remarkable cytotoxicity against breast cancer cells, with IC50 values ranging from 0.83 nM to 369.90 nM.


Assuntos
Dactinomicina/farmacologia , Streptomyces/química , Compostos de Terfenil/farmacologia , Vespas/microbiologia , Animais , Antineoplásicos/farmacologia , Espectroscopia de Ressonância Magnética Nuclear de Carbono-13 , Morte Celular/efeitos dos fármacos , Linhagem Celular Tumoral , Proliferação de Células/efeitos dos fármacos , Dactinomicina/química , Humanos , Larva/microbiologia , Compostos de Terfenil/química
17.
Chemistry ; 16(47): 14181-9, 2010 Dec 17.
Artigo em Inglês | MEDLINE | ID: mdl-20967899

RESUMO

DNA condensing agents play a critical role in gene therapy. A tetranuclear nickel(II) complex, [Ni(II)(4)(L-2H)(H(2)O)(6)(CH(3)CH(2)OH)(2)]·6NO(3) (L=3,3',5,5'-tetrakis{[(2-hydroxyethyl)(pyridin-2-ylmethyl)amino]methyl}biphenyl-4,4'-diol), has been synthesized as a nonviral vector to induce DNA condensation. X-ray crystallographic data indicate that the complex crystallizes in the monoclinic system with space group P2(1)/n, a=10.291(9), b=24.15(2), c=13.896(11) Å, and ß=98.175(13)°. The DNA condensation induced by the complex has been investigated by means of UV/Vis spectroscopy, fluorescence spectroscopy, circular dichroism spectroscopy, dynamic light scattering, atomic force microscopy, gel electrophoresis assay, and zeta potential analysis. The complex interacts strongly with DNA through electrostatic attraction and induces its condensation into globular nanoparticles at low concentration. The release of DNA from its compact state has been achieved using the chelator ethylenediaminetetraacetic acid (EDTA) for the first time. Other essential properties, such as DNA cleavage inactivity and biocompatibility, have also been examined in vitro. In general, the complex satisfies the requirements of a gene vector in all of these respects.


Assuntos
DNA/química , Vetores Genéticos/química , Níquel/química , Compostos Organometálicos/química , Animais , Cristalografia por Raios X , Clivagem do DNA , Eletroquímica , Ligantes , Estrutura Molecular , Espectrofotometria Ultravioleta
18.
ACS Appl Mater Interfaces ; 9(49): 42742-42750, 2017 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-29182850

RESUMO

Transition-metal sulfides (TMSs) are suggested as promising electrode materials for electrochemical pseudocapacitors and lithium- and sodium-ion batteries; however, they typically involve mixed composites or conventionally stoichiometric TMSs (such as NiCo2S4 and Ni2CoS4). Herein we demonstrate a preparation of solid-solution sulfide (Ni0.7Co0.3)S2 supported on three-dimensional graphene aerogel (3DGA) via a sulfuration of NiCo-layered double hydroxide (NiCo-LDH) precursor/3DGA. The electrochemical tests show that the (Ni0.7Co0.3)S2/3DGA electrode exhibits a capacitance of 2165 F g-1 at 1 A g-1, 2055 F g-1 at 2 A g-1, and 1478 F g-1 at 10 A g-1; preserves 78.5% capacitance retention upon 1000 cycles for pseudocapacitors; and in particular, possesses a relatively high charge capacity of 388.7 mA h g-1 after 50 cycles at 100 mA g-1 as anode nanomaterials for sodium-ion batteries. Furthermore, the electrochemical performances are readily tuned by varying the cationic type of the tunable LDH precursors to prepare different solid-solution sulfides, such as (Ni0.7Fe0.3)S2/3DGA and (Co0.7Fe0.3)S2/3DGA. Our results show that engineering LDH precursors can offer an alternative for preparing diverse transition-metal sulfides for energy storage.

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