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1.
Small ; 20(15): e2307357, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38012538

RESUMO

Hydrogen reduction reaction (HER) and corrosion limit the long-life cycle of zinc-ion batteries. However, hydrophilic separators are unable to prevent direct contact between water and electrodes, and hydrophobic separators have difficulty in transporting electrolytes. In this work, an inorganic oxide-based "hydrophobic-hydrophilic-hydrophobic" self-assembled separator system is proposed. The hydrophobic layer consists of a porous structure, which can isolate a large amount of free water to avoid HER and corrosion reactions, and can transport electrolyte by binding water. The middle hydrophilic layer acts as a storage layer consisting of the GF separator, storing large amounts of electrolyte for proper circulation. By using this structure separator, Zn||Zn symmetric cell achieve 2200 h stable cycle life at 5 mA cm-2 and 1mAh cm-2 and still shows a long life of 1800 h at 10 mA cm-2 and 1mAh cm-2. The assembled Zn||VO2 full cell displays high specific capacity and excellent long-term durability of 60.4% capacity retention after 1000 cycles at 2C. The assembled Zn||VO2 pouch full cell displays high specific capacity of 172.5mAh g-1 after 40 cycles at 0.5C. Changing the inorganic oxide materials, the hydrophobic-hydrophilic-hydrophobic structure of the separators still has excellent performance. This work provides a new idea for the engineering of water-based battery separators.

2.
Small ; : e2402422, 2024 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-39077964

RESUMO

Graphene oxide (GO)-based all-solid-state supercapacitors (SCs) provide an important complement to liquid- and gel-electrolyte-based SCs in a variety of applications, including flexible electronics. Still, their mediocre capacitance and complex fabrication methods hold back the realization of their full potential. Here, a simple fabrication of all-solid-state SCs with layered GO as a solid electrolyte and MXene as electrodes is demonstrated. The resultant SCs show excellent energy storage capacitance comparable to other MXene-based SCs using liquid electrolytes. The outperformance is attributed to extra interlayer spacing expansion and improved ion transport kinetics thanks to a synergistic water-absorbing effect due to the hydrophilicity of both MXene and GO in combination, which interestingly satisfies the intrinsic surface-dominated pseudocapacitive behavior of MXene. The application of this SC in humidity sensing has also been demonstrated to be fast responsive. The findings describe in this work provide a means of improving the capacitance performance using GO as a solid electrolyte with MXene as the electrodes and exploit the potential application as electronic elements for smart devices.

3.
Small ; : e2406926, 2024 Sep 29.
Artigo em Inglês | MEDLINE | ID: mdl-39344215

RESUMO

Transition metal dichalcogenides, particularly MoS2, are acknowledged as a promising cathode material for aqueous rechargeable zinc metal batteries (ARZMBs). Nevertheless, its lack of hydrophilicity, poor electrical conductivity, significant restacking, and restricted interlayer spacing translate into inadequate capacity and rate performance. Herein, the unique porous structure and additional functional groups present in holey graphene oxide (hGO) are taken advantage of to dictate the vertical growth pattern of oxygen-doped MoS2 nanowalls (O-MoS2/NW) over the hGO surface. Compared to conventional graphene oxide (GO), the presence of nano-pores in hGO facilitates the homogeneous dispersion of Mo precursors and provides stronger interaction sites, promoting the uniform vertical alignment of O-MoS2/NW. The synergistic interaction between O-MoS2-NW and hGO translates to enhanced electron conductivity, efficient electrolyte penetration, enhanced interlayer spacing, reduced restacking, and enhanced surface area. As a consequence of precise control of various factors that decide the overall battery performance, a high discharge capacity (227 mAh g-1 at 100 mA g-1) cathode material with significantly lower charge transfer resistance (66 Ω) compared to pristine O-MoS2 (153 Ω) is developed. These findings underscore the potential of hGO as a multifunctional platform for nanoengineering high-performance cathode materials for the next generation of efficient and durable ARZMBs.

4.
Mol Pharm ; 21(10): 5041-5052, 2024 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-39208298

RESUMO

Polysorbate 80 (PS80) is widely used in pharmaceutical formulations, and its commercial grades exhibit certain levels of structural heterogeneity. The objective of this study was to apply coarse-grained molecular dynamics simulations to better understand the effect of PS80 heterogeneity on micelle self-assembly, the loading of hydrophobic small molecules into the micelle core, and the interactions between PS80 and a protein, bovine serum albumin (BSA). Four representative PS80 variants with different head and tail structures were studied. Our simulations found that PS80 structural heterogeneity could affect blank micelle properties such as solvent-accessible surface area, aggregation number, and micelle aspect ratio. It was also found that hydrophobic small molecules such as ethinyl estradiol preferentially partitioned into the PS80 micelle core and PS80 dioleates formed a more hydrophobic core compared to PS80 monooleates. Furthermore, multiple PS80 molecules could bind to BSA, and PS80 heterogeneity profoundly changed the binding ratio as well as the surfactant-protein contact area.


Assuntos
Interações Hidrofóbicas e Hidrofílicas , Micelas , Simulação de Dinâmica Molecular , Polissorbatos , Soroalbumina Bovina , Tensoativos , Polissorbatos/química , Tensoativos/química , Soroalbumina Bovina/química
5.
J Periodontal Res ; 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38828886

RESUMO

AIMS: To test whether titanium surface roughness disparity might be used to specifically guide the behavior of gingiva fibroblasts and keratinocytes, thereby improving the quality of soft tissue (ST) integration around abutments. METHODS: Titanium discs resembling the roughness of enamel (M) or cementum (MA) were created with normal or increased hydrophilicity and used as substrates for human fibroblasts and keratinocytes. Adhesion and proliferation assays were performed to assess cell-type specific responses upon encountering the different surfaces. Additionally, immunofluorescence and qPCR analyses were performed to study more in depth the behavior of fibroblasts and keratinocytes on MA and M surfaces, respectively. RESULTS: While enamel-like M surfaces supported adhesion, growth and a normal differentiation potential of keratinocytes, cementum-emulating MA surfaces specifically impaired the growth of keratinocytes. Vice versa, MA surfaces sustained regular adhesion and proliferation of fibroblasts. Yet, a more intimate adhesion between fibroblasts and titanium was achieved by an increased hydrophilicity of MA surfaces, which was associated with an increased expression of elastin. CONCLUSION: The optimal titanium implant abutment might be achieved by a bimodal roughness design, mimicking the roughness of enamel (M) and cementum with increased hydrophilicity (hMA), respectively. These surfaces can selectively elicit cell responses favoring proper ST barrier by impairing epithelial downgrowth and promoting firm adhesion of fibroblasts.

6.
J Pept Sci ; 30(5): e3558, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38115215

RESUMO

The engineering of intracellular delivery systems with the goal of achieving personalized medicine has been encouraged by advances in nanomaterial science as well as a greater understanding of diseases and of the biochemical pathways implicated in many disorders. The development of vectors able to transport the drug to a target location and release it only on demand is undoubtedly the primary issue. From a molecular perspective, the topography of drug carrier surfaces is directly related to the design of an effective drug carrier because it provides a physical hint to modifying its interactions with biological systems. For instance, the initial ratio of hydrophilic to hydrophobic surfaces and the changes brought about by external factors enable the release or encapsulation of a therapeutic molecule and the ability of the nanosystem to cross biological barriers and reach its target without causing systemic toxicity. The first step in creating new materials with enhanced functionality is to comprehend and characterize the interplay between hydrophilic and hydrophobic molecules at the molecular level. Therefore, the focus of this review is on the function of hydrophobicity, which is essential for matching the complexity of biological environments with the intended functionality.


Assuntos
Portadores de Fármacos , Sistemas de Liberação de Medicamentos , Interações Hidrofóbicas e Hidrofílicas , Portadores de Fármacos/química
7.
Macromol Rapid Commun ; 45(5): e2300606, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38087799

RESUMO

Recent advancements in bioengineering and medical devices have been greatly influenced and dominated by synthetic polymers, particularly polyurethanes (PUs). PUs offer customizable mechanical properties and long-term stability, but their inherent hydrophobic nature poses challenges in practically biological application processes, such as interface high friction, strong protein adsorption, and thrombosis. To address these issues, surface modifications of PUs for generating functionally hydrophilic layers have received widespread attention, but the durability of generated surface functionality is poor due to irreversible mechanical wear or biodegradation. As a result, numerous researchers have investigated bulk modification techniques to incorporate zwitterionic polymers or groups onto the main or side chains of PUs, thereby improving their hydrophilicity and biocompatibility. This comprehensive review presents an extensive overview of notable zwitterionic PUs (ZPUs), including those based on phosphorylcholine, sulfobetaine, and carboxybetaine. The review explores their wide range of biomedical applications, from blood-contacting devices to antibacterial coatings, fouling-resistant marine coatings, separation membranes, lubricated surfaces, and shape memory and self-healing materials. Lastly, the review summarizes the challenges and future prospects of ZPUs in biological applications.


Assuntos
Polímeros , Poliuretanos , Humanos , Poliuretanos/química , Propriedades de Superfície , Polímeros/química , Interações Hidrofóbicas e Hidrofílicas , Supuração
8.
Environ Res ; 244: 117897, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38103782

RESUMO

Microplastics (MPs) and pharmaceuticals and personal care products (PPCPs) are two types of emerging contaminants widely present in the global aquatic ecosystem. The ecological risks associated with the coexistence of these two contaminants have garnered increasing attention from researchers. In this study, we selected 15 typical hydrophilic PPCPs, including Sulfacetamide (SA), Thiamphenicol, Florfenicol, Chloramphenicol (CHL), Ampicillin, Cephalexin, Ofloxacin, Fluorouracil, Phenytoin, Theophylline, Cimetidine, Methylparaben, Diethyltoluamide, Benzophenone-2 (BP-2), and Benzophenone-4, as adsorbates. We evaluated the adsorption potential of five traditional plastics (TPs), namely Polyamide 6 (PA6), Polystyrene (PS), Polyethylene terephthalate (PET), Polyvinyl chloride (PVC), and Polyurethane (TPU), as well as three biodegradable plastics (BDPs), including Polylactic acid (PLA), Polybutylene succinate (PBS), and Poly (ε-caprolactone) (PCL), for these adsorbates. Out of the 120 combinations of MPs and PPCPs tested, only 24 exhibited significant adsorption behavior. Notably, the adsorption performance of the three BDPs was stronger than that of the three typical TPs (PS, PET, and PVC). Based on their adsorption potential, PA6, BDPs, phenytoin, and BP-2 were identified as potential sources of high ecological risk. To further explore the adsorption mechanism, we investigated the adsorption behaviors of SA, BP-2, and CHL on PA6. The conclusions were as follows: SA, BP-2, and CHL all reached adsorption equilibrium within 24 h, with the partition coefficient (Kd) following this order: BP-2 (8.051) â‰« SA (0.052) > CHL (0.018). The primary forces of adsorption were electrostatic interactions, intermolecular hydrogen bonding, and hydrophobic interaction, respectively. Additionally, weak electrostatic effects were observed in the adsorption of CHL and BP-2. The effects of pH, ionic strength, and fulvic acid on adsorption capacity varied. These results highlight a complex adsorption mechanism between MPs and hydrophilic contaminants in the aquatic environment. This study provides a basis for further evaluating the ecological risks of MPs and PPCPs combined pollution.


Assuntos
Cosméticos , Poluentes Químicos da Água , Plásticos , Microplásticos , Adsorção , Ecossistema , Fenitoína , Poliestirenos/química , Interações Hidrofóbicas e Hidrofílicas , Preparações Farmacêuticas , Poluentes Químicos da Água/análise
9.
BMC Nephrol ; 25(1): 220, 2024 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-38987671

RESUMO

BACKGROUND: Hemodialyzers should efficiently eliminate small and middle molecular uremic toxins and possess exceptional hemocompatibility to improve well-being of patients with end-stage kidney disease. However, performance and hemocompatibility get compromised during treatment due to adsorption of plasma proteins to the dialyzer membrane. Increased membrane hydrophilicity reduces protein adsorption to the membrane and was implemented in the novel FX CorAL dialyzer. The present randomized controlled trial compares performance and hemocompatibility profiles of the FX CorAL dialyzer to other commonly used dialyzers applied in hemodiafiltration treatments. METHODS: This prospective, open, controlled, multicentric, interventional, crossover study randomized stable patients on post-dilution online hemodiafiltration (HDF) to FX CorAL 600, FX CorDiax 600 (both Fresenius Medical Care) and xevonta Hi 15 (B. Braun) each for 4 weeks. Primary outcome was ß2-microglobulin removal rate (ß2-m RR). Non-inferiority and superiority of FX CorAL versus comparators were tested. Secondary endpoints were RR and/or clearance of small and middle molecules, and intra- and interdialytic profiles of hemocompatibility markers, with regards to complement activation, cell activation/inflammation, platelet activation and oxidative stress. Further endpoints were patient reported outcomes (PROs) and clinical safety. RESULTS: 82 patients were included and 76 analyzed as intention-to-treat (ITT) population. FX CorAL showed the highest ß2-m RR (76.28%), followed by FX CorDiax (75.69%) and xevonta (74.48%). Non-inferiority to both comparators and superiority to xevonta were statistically significant. Secondary endpoints related to middle molecules corroborated these results; performance for small molecules was comparable between dialyzers. Regarding intradialytic hemocompatibility, FX CorAL showed lower complement, white blood cell, and platelet activation. There were no differences in interdialytic hemocompatibility, PROs, or clinical safety. CONCLUSIONS: The novel FX CorAL with increased membrane hydrophilicity showed strong performance and a favorable hemocompatibility profile as compared to other commonly used dialyzers in clinical practice. Further long-term investigations should examine whether the benefits of FX CorAL will translate into improved cardiovascular and mortality endpoints. TRIAL REGISTRATION: eMPORA III registration on 19/01/2021 at ClinicalTrials.gov (NCT04714281).


Assuntos
Estudos Cross-Over , Hemodiafiltração , Interações Hidrofóbicas e Hidrofílicas , Membranas Artificiais , Humanos , Masculino , Feminino , Pessoa de Meia-Idade , Idoso , Hemodiafiltração/instrumentação , Hemodiafiltração/métodos , Estudos Prospectivos , Microglobulina beta-2/sangue , Falência Renal Crônica/terapia
10.
Int J Mol Sci ; 25(16)2024 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-39201280

RESUMO

The medical device market is a high-growth sector expected to sustain an annual growth rate of over 5%, even in developed countries. Daily, numerous patients have medical devices implanted or inserted within their bodies. While medical devices have significantly improved patient outcomes, as foreign objects, their wider use can lead to an increase in device-related infections, thereby imposing a burden on healthcare systems. Multiple materials with significant societal impact have evolved over time: the 19th century was the age of iron, the 20th century was dominated by silicon, and the 21st century is often referred to as the era of carbon. In particular, the development of nanocarbon materials and their potential applications in medicine are being explored, although the scope of these applications remains limited. Technological innovations in carbon materials are remarkable, and their application in medicine is expected to advance greatly. For example, diamond-like carbon (DLC) has garnered considerable attention for the development of antimicrobial surfaces. Both DLC itself and its derivatives have been reported to exhibit anti-microbial properties. This review discusses the current state of DLC-based antimicrobial surface development.


Assuntos
Anti-Infecciosos , Humanos , Anti-Infecciosos/farmacologia , Anti-Infecciosos/química , Materiais Revestidos Biocompatíveis/química , Materiais Revestidos Biocompatíveis/farmacologia , Diamante/química , Carbono/química , Propriedades de Superfície
11.
J Environ Manage ; 367: 122089, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39102785

RESUMO

Bioleaching and Fenton technology are commonly used preconditioning techniques for sludge dewatering. This study compared the dewatering mechanisms of different conditioning technologies. The results showed that bound water, specific resistance to filtration (SRF), and capillary suction time decreased from 3.95 g/g, 6.16 × 1012 m/kg, and 130.6 s to 3.15 g/g, 2.81 × 1011 m/kg, and 33 s, respectively, under combined treatment condition. Moreover, the free radicals, including ·OH, O2-·and Fe (Ⅳ), further damaged the cell structure, thus increasing the concentration of DNA in the S-EPS layer. This intense degradation sludge particle size decreased by 15.6% and significantly increased zeta potential. Under the combined technology, the α-helix and ß-sheet decreased by 42.2% and 56.5%, respectively, destabilizing the spatial structure of proteins and promoting the release of bound water. In addition, the combined technology decreased (Ala/Lys) ratio in the TB-EPS layer by 67.6%, indicating the weakening of protein water-holding capacity. Moreover, the conversion of oxygen-containing compounds to nonpolar hydrocarbons increased the hydrophobicity of the sludge under a combined treatment, thus enhancing dewatering performance.


Assuntos
Interações Hidrofóbicas e Hidrofílicas , Esgotos , Esgotos/química , Eliminação de Resíduos Líquidos/métodos , Tamanho da Partícula , Ferro/química , Filtração , Água/química
12.
Molecules ; 29(17)2024 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-39274995

RESUMO

The microstructure and chemical properties of the corona discharge process could provide an effective method for predicting the performance of high-voltage cable insulation materials. In this work, the depth profile of the microstructure and chemical characteristics of corona discharge-treated PE were extensively investigated using Doppler broadening of position annihilation spectroscopy accompanied with positron annihilation lifetime spectroscopy, attenuated total reflectance Fourier transform infrared spectra, Raman spectra and contact angle measurement. By increasing corona discharge duration, the oxygen-containing polar groups, including hydroxyl, carbonyl and ester groups, strongly contribute to the deterioration of hydrophobicity and the enhancement of hydrophilicity. And the mean free volume size, with a broadening distribution, decreases slightly. The line shape S parameter decreases because of the decrease in free volume elements and the appearance of oxygen-containing groups. Also, the thickness of the degradation layer, determined from the S parameter with positron injection depth, increases and diffuses into the PE matrix. A linear S-W plot within the degradation layer of different corona treatment duration samples indicates the defect type does not change. The S parameter decreases and the W parameter increases with an increasing corona duration. Using a slow positron beam, the nondestructive probe can be used to profile the microstructure and chemical environment across the corona discharge damage depth, which is beneficial for investigating the surface and interfacial insulation materials.

13.
Molecules ; 29(19)2024 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-39407522

RESUMO

In this work, the structure of silica thin films synthesized with three different SiO2 precursors and obtained by the sol-gel method and dip coating technique was studied. Additionally, the influence of Ag addition on the obtained silica sols and then gel structure was investigated. Silica coatings show antireflective properties and high thermal resistance, as well as hydrophobic or hydrophilic properties. Three different silica precursors, TEOS (tetraethylorthosilicate), DDS (dimethyldietoxysilane) and AerosilTM, were selected for the synthesis. DDS added to silica sol act as a pore size modifier, while Ag atoms are known for their antibacterial activity. Coatings were deposited on two different substrates: steel and titanium, dried and annealed at 500 °C in air (steel substrate) and in argon (titanium substrate). For all synthesized films, IR (infrared) spectroscopic studies were performed together with GID and XRD (Grazing Incidence Diffraction, X-ray Diffraction) measurements. The topography and morphology of the surface were traced by SEM and AFM microscopic methods, providing information on the samples' roughness, particle sizes and thickness of the particular layers. The wetting angle values were also measured. GID and XRD measurements pointed to the distinct contribution of an amorphous phase in the samples, allowing us to recognize the crystalline phases and calculate the silver crystallite sizes. The FTIR spectra gave information on the first coordination sphere of the studied samples.

14.
Waste Manag Res ; 42(8): 595-607, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38366790

RESUMO

This study introduces an innovative approach for enhancing oil-water emulsion separation using a polyethersulfone (PES) membrane embedded with a nanocomposite of graphene oxide (GO) and silver oxide (AgO). The composite membrane, incorporating PES and polyvinyl chloride (PVC), demonstrates improved hydrophilicity, structural integrity and resistance to fouling. Physicochemical characterization confirms successful integration of GO and AgO, leading to increased tensile strength, porosity and hydrophilicity. Filtration tests reveal substantial improvements in separating various oils from contaminated wastewater, with the composite membrane exhibiting superior efficiency and reusability compared to pristine PES membranes. This research contributes to the development of environmentally friendly oil-water separation methods with broad industrial applications.


Assuntos
Emulsões , Filtração , Grafite , Membranas Artificiais , Nanocompostos , Polímeros , Sulfonas , Grafite/química , Nanocompostos/química , Sulfonas/química , Polímeros/química , Filtração/métodos , Compostos de Prata/química , Óleos/química , Águas Residuárias/química , Água/química , Interações Hidrofóbicas e Hidrofílicas , Óxidos
15.
Sheng Wu Yi Xue Gong Cheng Xue Za Zhi ; 41(4): 848-853, 2024 Aug 25.
Artigo em Chinês | MEDLINE | ID: mdl-39218613

RESUMO

Hydrogel is a kind of degradable hydrophilic polymer, but excessive hydrophilicity leads to larger volume, lower elastic modulus and looser structure, which further affect its use. Especially in the field of biomedical engineering, excessive swelling of the hydrogel can compress the nerves and improve degradation rate resulting in mismatch of tissue growth and released ions. Therefore, anti-swelling hydrogel has been a research hotspot in recent years. This paper reviews the recent research progress on anti-swelling hydrogel, and expounds the application mechanism and preparation method of hydrogel in biomedical engineering, aiming to provide some references for researchers in the field of anti-swelling hydrogel.


Assuntos
Materiais Biocompatíveis , Hidrogéis , Hidrogéis/química , Materiais Biocompatíveis/química , Engenharia Tecidual/métodos , Engenharia Biomédica , Interações Hidrofóbicas e Hidrofílicas , Polímeros/química , Módulo de Elasticidade , Humanos
16.
Sheng Wu Yi Xue Gong Cheng Xue Za Zhi ; 41(3): 604-611, 2024 Jun 25.
Artigo em Chinês | MEDLINE | ID: mdl-38932548

RESUMO

The surface morphology of titanium metal is an important factor affecting its hydrophilicity and biocompatibility, and exploring the surface treatment strategy of titanium metal is an important way to improve its biocompatibility . In this study , titanium (TA4) was firstly treated by large particle sand blasting and acid etching (SLA) technology, and then the obtained SLA-TA4 was treated by single surface treatments such as alkali-heat, ultraviolet light and plasma bombardment. According to the experimental results, alkali-heat treatment is the best treatment method to improve and maintain surface hydrophilicity of titanium. Then, the nanowire network morphology of titanium surface and its biological property, formed by further surface treatments on the basis of alkali-heat treatment, were investigated. Through the cell adhesion experiment of mouse embryonic osteoblast cells (MC3T3-E1), the ability of titanium material to support cell adhesion and cell spreading was investigated after different surface treatments. The mechanism of biological activity difference of titanium surface formed by different surface treatments was investigated according to the contact angle, pit depth and roughness of the titanium sheet surface. The results showed that the SLA-TA4 titanium sheet after a treatment of alkali heat for 10 h and ultraviolet irradiation for 1 h has the best biological activity and stability. From the perspective of improving surface bioactivity of medical devices, this study has important reference value for relevant researches on surface treatment of titanium implantable medical devices.


Assuntos
Materiais Biocompatíveis , Adesão Celular , Osteoblastos , Próteses e Implantes , Propriedades de Superfície , Titânio , Titânio/química , Animais , Camundongos , Osteoblastos/citologia , Teste de Materiais , Linhagem Celular , Raios Ultravioleta , Interações Hidrofóbicas e Hidrofílicas
17.
Angew Chem Int Ed Engl ; : e202413348, 2024 Aug 26.
Artigo em Inglês | MEDLINE | ID: mdl-39185626

RESUMO

Inevitable leaching and corrosion under anodic oxidative environment greatly restrict the lifespan of most catalysts with excellent primitive activity for oxygen production. Here, based on Fick' s Law, we present a surface cladding strategy to mitigate Ni dissolution and stabilize lattice oxygen triggering by directional flow of interfacial electrons and strong electronic interactions via constructing elaborately cladding-type NiO/NiS heterostructure with controlled surface thickness. Multiple in situ characterization technologies indicated that this strategy can effectively prevent the irreversible Ni ions leaching and inhibit lattice oxygen from participating in anodic reaction. Combined with density functional theory calculations, we reveal that the stable interfacial O-Ni-S arrangement can facilitate the accumulation of electrons on surficial NiO side and weaken its Ni-O covalency. This would suppress the overoxidation of Ni and simultaneously fixing the lattice oxygen, thus enabling catalysts with boosted corrosion resistance without sacrificing its activity. Consequently, this cladding-type NiO/NiS heterostructure exhibits excellent performance with a low overpotential of 256 mV after 500 h. Based on Fick's law, this work demonstrates the positive effect of surface modification through precisely adjusting of the oxygen-sulfur exchange process, which has paved an innovative and effective way to solve the instability problem of anodic oxidation.

18.
Small ; : e2306827, 2023 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-38054756

RESUMO

Zinc metal is a promising candidate for anodes in zinc-ion batteries (ZIBs), but its widespread implementation is hindered by dendrite growth in aqueous electrolytes. Dendrites lead to undesirable side reactions, such as hydrogen evolution, passivation, and corrosion, causing reduced capacity during prolonged cycling. In this study, an approach is explored to address this challenge by directly growing 1D zinc oxide (ZnO) nanorods (NRs) and 2D ZnO nanoflakes (NFs) on Zn anodes, forming artificial layers to enhance ZIB performance. The incorporation of ZnO on the anode offers both chemical and thermal stability and leverages its n-type semiconductor nature to facilitate the formation of ohmic contacts. This results in efficient electron transport during Zn ion plating and stripping processes. Consequently, the ZnO NFs-coated Zn anodes demonstrate significantly improved charge storage performance, achieving 348 mAh g-1 , as compared to ZnO NRs (250 mAh g-1 ) and pristine Zn (160 mAh g-1 ) anodes when evaluated in full cells with V2 O5 cathodes. One significant advantage of ZnO NFs lies in their highly polar surfaces, promoting strong interactions with water molecules and rendering them exceptionally hydrophilic. This characteristic enhances the ability of ZnO NFs to desolvate Zn2+ ions, leading to improved charge storage performance.

19.
Small ; 19(45): e2302629, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37431237

RESUMO

Tailor-made carbonaceous-based cathodes with zincophilicity and hydrophilicity are highly desirable for Zn-ion storage applications, but it remains a great challenge to achieve both advantages in the synthesis. In this work, a template electrospinning strategy is developed to synthesize nitrogen and phosphorous co-doped hollow porous carbon nanofibers (N, P-HPCNFs), which deliver a high capacity of 230.7 mAh g-1 at 0.2 A g-1 , superior rate capability of 131.0 mAh g-1 at 20 A g-1 , and a maximum energy density of 196.10 Wh kg-1 at the power density of 155.53 W kg-1 . Density functional theory calculations (DFT) reveal that the introduced P dopants regulate the distribution of local charge density of carbon materials and therefore facilitate the adsorption of Zn ions due to the increased electronegativity of pyridinic-N. Ab initio molecular dynamics (AIMD) simulations indicate that the doped P species induce a series of polar sites and create a hydrophilic microenvironment, which decreases the impedance between the electrode and the electrolyte and therefore accelerates the reaction kinetics. The marriage of ex situ/in situ experimental analyses and theoretical simulations uncovers the origin of the enhanced zincophilicity and hydrophilicity of N, P-HPCNFs for energy storage, which accounts for the faster ion migration and electrochemical processes.

20.
Environ Sci Technol ; 57(30): 11056-11066, 2023 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-37467155

RESUMO

Because of its favorable thermodynamics and fast kinetics, heterogeneous solid nucleation on membranes triggers early-stage mineral scaling. Iron (hydr)oxide, a typical membrane scale, initially forms as nanoparticles that interact with surface functional groups on membranes, but these nanoscale phenomena are difficult to observe in real time. In this study, we utilized in situ grazing incidence small angle X-ray scattering and ex situ atomic force microscopy to examine the heterogeneous nucleation of iron (hydr)oxide on surface functional groups commonly used in membranes, including hydroxyl (OH), carboxyl (COOH), and fluoro (F) groups. We found that, compared to nucleation on hydrophilic OH- and COOH-surfaces, the high hydrophobicity of an F-modified surface significantly reduced the extents of both heterogeneously and homogeneously formed iron (hydr)oxide nucleation. Moreover, on the OH-surface, the high functional group density of 0.76 nmol/cm2 caused faster heterogeneous nucleation than that on a COOH-surface, with a density of 0.28 ± 0.04 nmol/cm2. The F-surface also had the highest heterogeneous nucleation energy barrier (26 ± 0.6 kJ/mol), followed by COOH- (23 ± 0.8 kJ/mol) and OH- (20 ± 0.9 kJ/mol) surfaces. The kinetic and thermodynamic information provided here will help us better predict the rates and extents of early-stage scaling of iron (hydr)oxide nanoparticles in membrane processes.

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