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1.
J Am Chem Soc ; 146(18): 12556-12564, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38660792

RESUMO

Transition metal nitride (TMN)-based nanostructures have emerged as promising materials for diverse applications in electronics, photonics, energy storage, and catalysis due to their highly desirable physicochemical properties. However, synthesizing TMN-based nanostructures with designed compositions and morphologies poses challenges, especially in the solution phase. The cation exchange reaction (CER) stands out as a versatile postsynthetic strategy for preparing nanostructures that are otherwise inaccessible through direct synthesis. Nevertheless, exploration of the CER in TMNs lags behind that in metal chalcogenides and metal phosphides. Here, we demonstrate cation exchange in colloidal metal nitride nanocrystals, employing Cu3N nanocrystals as starting materials to synthesize Ni4N and CoN nanocrystals. By controlling the reaction conditions, Cu3N@Ni4N and Cu3N@CoN core@shell heterostructures with tunable compositions can also be obtained. The Ni4N and CoN nanocrystals are evaluated as catalysts for the electrochemical oxygen evolution reaction (OER). Remarkably, CoN nanocrystals demonstrate superior OER performance with a low overpotential of 286 mV at 10 mA·cm-2, a small Tafel slope of 89 mV·dec-1, and long-term stability. Our CER approach in colloidal TMNs offers a new strategy for preparing other metal nitride nanocrystals and their heterostructures, paving the way for prospective applications.

2.
Angew Chem Int Ed Engl ; 63(17): e202401507, 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38407548

RESUMO

Rechargeable aqueous zinc batteries are promising but hindered by unfavorable dendrite growth and side reactions on zinc anodes. In this study, we demonstrate a fast melting-solidification approach for effectively converting commercial Zn foils into single (002)-textured Zn featuring millimeter-sized grains. The melting process eliminates initial texture, residual stress, and grain size variations in diverse commercial Zn foils, guaranteeing the uniformity of commercial Zn foils into single (002)-textured Zn. The single (002)-texture ensures large-scale epitaxial and dense Zn deposition, while the reduction in grain boundaries significantly minimizes intergranular reactions. These features enable large grain single (002)-textured Zn shows planar and dense Zn deposition under harsh conditions (100 mA cm-2, 100 mAh cm-2), impressive reversibility in Zn||Zn symmetric cell (3280 h under 1 mA cm-2, 830 h under 10 mAh cm-2), and long cycling stability over 180 h with a high depth of discharge value of 75 %. This study successfully addresses the issue of uncontrollable texture formation in Zn foils following routine annealing treatments with temperatures below the Zn melting point. The findings of this study establish a highly efficient strategy for fabricating highly reversible single (002)-textured Zn anodes.

3.
Angew Chem Int Ed Engl ; 62(30): e202304121, 2023 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-37226711

RESUMO

The practical implementation of high-voltage lithium-rich manganese oxide (LRMO) cathode is limited by the unanticipated electrolyte decomposition and dissolution of transition metal ions. The present study proposes a bi-affinity electrolyte formulation, wherein the sulfonyl group of ethyl vinyl sulfone (EVS) imparts a highly adsorptive nature to LRMO, while fluoroethylene carbonate (FEC) exhibits a reductive nature towards Li metal. This interface modulation strategy involves the synergistic use of EVS and FEC as additives to form robust interphase layers on the electrode. As-formed S-endorsed but LiF-assisted configuration cathode electrolyte interphase with a more dominant -SO2 - component may promote the interface transport kinetics and prevent the dissolution of transition metal ions. Furthermore, the incorporation of S component into the solid electrolyte interphase and the reduction of its poorly conducting component can effectively inhibit the growth of lithium dendrites. Therefore, a 4.8 V LRMO/Li cell with optimized electrolyte may demonstrate a remarkable retention capacity of 97 % even after undergoing 300 cycles at 1 C.

4.
Angew Chem Int Ed Engl ; 60(13): 7213-7219, 2021 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-33381887

RESUMO

The reversibility of metal anode is a fundamental challenge to the lifetime of rechargeable batteries. Though being widely employed in aqueous energy storage systems, metallic zinc suffers from dendrite formation that severely hinders its applications. Here we report texturing Zn as an effective way to address the issue of zinc dendrite. An in-plane oriented Zn texture with preferentially exposed (002) basal plane is demonstrated via a sulfonate anion-induced electrodeposition, noting no solid report on (002) textured Zn till now. Anion-induced reconstruction of zinc coordination is revealed to be responsible for the texture formation. Benchmarking against its (101) textured-counterpart by the conventional sulphate-based electrolyte, the Zn (002) texture enables highly reversible stripping/plating at a high current density of 10 mA cm-2 , showing its dendrite-free characteristics. The Zn (002) texture-based aqueous zinc battery exhibits excellent cycling stability. The developed anion texturing approach provides a pathway towards exploring zinc chemistry and prospering aqueous rechargeable batteries.

5.
Small ; 16(38): e2003321, 2020 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-32812393

RESUMO

With good operation flexibility and scalability, vanadium redox-flow batteries (VRBs) stand out from various electrochemical energy storage (EES) technologies. However, traditional electrodes in VRBs, such as carbon and graphite felt with low electrochemical activities, impede the interfacial charge transfer processes and generate considerable overpotential loss, which significantly decrease the energy and voltage efficiencies of VRBs. Herein, by using a facile electrodeposition technique, Prussian blue/carbon felt (PB/CF) composite electrodes with high electrochemical activity for VRBs are successfully fabricated. The PB/CF electrode exhibits excellent electrochemical activity toward VO2+ /VO2 + redox couple in VRB with an average cell voltage efficiency (VE) of 90% and an energy efficiency (EE) of 88% at 100 mA cm-2 . In addition, due to the uniformly distributed PB particles that are strongly bound to the surface of carbon fibers in CF, VRBs with the PB/CF electrodes show much better long-term stabilities compared with the pristine CF-based battery due to the redox-mediated catalysis. A VRB stack consisting of three single cells (16 cm2 ) is also constructed to assess the reliability of the redox-mediated PB/CF electrodes for large-scale application. The facile technique for the high-performance electrode with redox-mediated reaction is expected to shed new light on commercial electrode design for VRBs.

6.
Proc Natl Acad Sci U S A ; 113(19): 5239-44, 2016 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-27114521

RESUMO

Evidence suggests that light and circadian rhythms profoundly influence the physiologic capacity with which an organism responds to stress. However, the ramifications of light spectrum on the course of critical illness remain to be determined. Here, we show that acute exposure to bright blue spectrum light reduces organ injury by comparison with bright red spectrum or ambient white fluorescent light in two murine models of sterile insult: warm liver ischemia/reperfusion (I/R) and unilateral renal I/R. Exposure to bright blue light before I/R reduced hepatocellular injury and necrosis and reduced acute kidney injury and necrosis. In both models, blue light reduced neutrophil influx, as evidenced by reduced myeloperoxidase (MPO) within each organ, and reduced the release of high-mobility group box 1 (HMGB1), a neutrophil chemotactant and key mediator in the pathogenesis of I/R injury. The protective mechanism appeared to involve an optic pathway and was mediated, in part, by a sympathetic (ß3 adrenergic) pathway that functioned independent of significant alterations in melatonin or corticosterone concentrations to regulate neutrophil recruitment. These data suggest that modifying the spectrum of light may offer therapeutic utility in sterile forms of cellular injury.


Assuntos
Cromoterapia/métodos , Cor , Corticosterona/sangue , Traumatismo por Reperfusão/prevenção & controle , Traumatismo por Reperfusão/fisiopatologia , Animais , Relação Dose-Resposta à Radiação , Proteína HMGB1/sangue , Testes de Função Renal , Testes de Função Hepática , Masculino , Melatonina/sangue , Camundongos , Camundongos Endogâmicos C57BL , Peroxidase/sangue , Doses de Radiação , Traumatismo por Reperfusão/diagnóstico , Índice de Gravidade de Doença , Resultado do Tratamento
7.
Crit Care Med ; 46(8): e779-e787, 2018 08.
Artigo em Inglês | MEDLINE | ID: mdl-29727369

RESUMO

OBJECTIVES: The physiology of nearly all mammalian organisms are entrained by light and exhibit circadian rhythm. The data derived from animal studies show that light influences immunity, and these neurophysiologic pathways are maximally entrained by the blue spectrum. Here, we hypothesize that bright blue light reduces acute kidney injury by comparison with either bright red or standard, white fluorescent light in mice subjected to sepsis. To further translational relevance, we performed a pilot clinical trial of blue light therapy in human subjects with appendicitis. DESIGN: Laboratory animal research, pilot human feasibility trial. SETTING: University basic science laboratory and tertiary care hospital. SUBJECTS: Male C57BL/6J mice, adult (> 17 yr) patients with acute appendicitis. INTERVENTIONS: Mice underwent cecal ligation and puncture and were randomly assigned to a 24-hour photoperiod of bright blue, bright red, or ambient white fluorescent light. Subjects with appendicitis were randomized to receive postoperatively standard care or standard care plus high-illuminance blue light. MEASUREMENTS AND MAIN RESULTS: Exposure to bright blue light enhanced bacterial clearance from the peritoneum, reduced bacteremia and systemic inflammation, and attenuated the degree of acute kidney injury. The mechanism involved an elevation in cholinergic tone that augmented tissue expression of the nuclear orphan receptor REV-ERBα and occurred independent of alterations in melatonin or corticosterone concentrations. Clinically, exposure to blue light after appendectomy was feasible and reduced serum interleukin-6 and interleukin-10 concentrations. CONCLUSIONS: Modifying the spectrum of light may offer therapeutic utility in sepsis.


Assuntos
Injúria Renal Aguda/etiologia , Injúria Renal Aguda/terapia , Apendicite/terapia , Fototerapia/métodos , Sepse/complicações , Adulto , Animais , Citocinas/biossíntese , Feminino , Humanos , Hidrocortisona/sangue , Mediadores da Inflamação/metabolismo , Masculino , Camundongos , Camundongos Endogâmicos C57BL , Técnicas Microbiológicas , Pessoa de Meia-Idade , Escores de Disfunção Orgânica , Distribuição Aleatória
8.
FASEB J ; 31(10): 4382-4395, 2017 10.
Artigo em Inglês | MEDLINE | ID: mdl-28615325

RESUMO

During sepsis and shock states, mitochondrial dysfunction occurs. Consequently, adaptive mechanisms, such as fission, fusion, and mitophagy, are induced to eliminate damaged portions or entire dysfunctional mitochondria. The regulatory PINK1/Parkin and DJ-1 pathways are strongly induced by mitochondrial depolarization, although a direct link between loss of mitochondrial membrane potential (ΔΨ) and mitophagy has not been identified. Mitochondria also buffer Ca2+, and their buffering capacity is dependent on ΔΨ Here, we characterize a role for calcium/calmodulin-dependent protein kinase (CaMK) I in the regulation of these mechanisms. Loss of ΔΨ with either pharmacologic depolarization or LPS leads to Ca2+-dependent mitochondrial recruitment and activation of CaMKI that precedes the colocalization of PINK1/Parkin and DJ-1. CaMKI is required and serves as both a PINK1 and Parkin kinase. The mechanisms operate in both immune and nonimmune cells and are induced in in vivo models of endotoxemia, sepsis, and hemorrhagic shock. These data support the idea that CaMKI links mitochondrial stress with the PINK1/Parkin and DJ-1 mechanisms of mitophagy.-Zhang, X., Yuan, D., Sun, Q., Xu, L., Lee, E., Lewis, A. J., Zuckerbraun, B. S., Rosengart, M. R. Calcium/calmodulin-dependent protein kinase regulates the PINK1/Parkin and DJ-1 pathways of mitophagy during sepsis.


Assuntos
Proteínas Quinases Dependentes de Cálcio-Calmodulina/metabolismo , Mitocôndrias/metabolismo , Proteína Desglicase DJ-1/metabolismo , Proteínas Quinases/metabolismo , Sepse/metabolismo , Animais , Modelos Animais de Doenças , Lipopolissacarídeos/farmacologia , Masculino , Potencial da Membrana Mitocondrial/efeitos dos fármacos , Camundongos Endogâmicos C57BL , Mitofagia/efeitos dos fármacos , Proteínas Serina-Treonina Quinases/metabolismo , Transporte Proteico/efeitos dos fármacos
9.
Crit Care Med ; 44(6): e420-31, 2016 06.
Artigo em Inglês | MEDLINE | ID: mdl-26862708

RESUMO

OBJECTIVES: Murine models of critical illness are commonly used to test new therapeutic interventions. However, these interventions are often administered at fixed time intervals after the insult, perhaps ignoring the inherent variability in magnitude and temporality of the host response. We propose to use wireless biotelemetry monitoring to define and validate criteria for acute deterioration and generate a physiology-based murine cecal ligation and puncture model that is more similar to the conduct of human trials of sepsis. DESIGN: Laboratory and animal research. SETTING: University basic science laboratory. SUBJECTS: Male C57BL/6 mice. INTERVENTIONS: Mice underwent cecal ligation and puncture, and an HD-X11 wireless telemetry monitor (Data Sciences International) was implanted that enabled continuous, real-time measurement of heart rate, core temperature, and mobility. We performed a population-based analysis to determine threshold criteria that met face validity for acute physiologic deterioration. We assessed construct validity by temporally matching mice that met these acute physiologic deterioration thresholds with mice that had not yet met deterioration threshold. We analyzed matched blood samples for blood gas, inflammatory cytokine concentration, cystatin C, and alanine aminotransferase. MEASUREMENTS AND MAIN RESULTS: We observed that a 10% reduction in both heart rate and temperature sustained for greater than or equal to 10 minutes defined acute physiologic deterioration. There was significant variability in the time to reach acute deterioration threshold across mice, ranging from 339 to 529 minutes after cecal ligation and puncture. We found adequate construct validity, as mice that met criteria for acute deterioration had significantly worse shock, systemic inflammation (elevated tumor necrosis factor-α, p = 0.003; interleukin-6, p = 0.01; interleukin-10, p = 0.005), and acute kidney injury when compared with mice that had not yet met acute deterioration criteria. CONCLUSIONS: We defined a murine threshold for acute physiologic deterioration after cecal ligation and puncture that has adequate face and construct validity. This model may enable a more physiology-based model for evaluation of novel therapeutics in critical illness.


Assuntos
Citocinas/sangue , Modelos Animais de Doenças , Monitorização Fisiológica/métodos , Sepse/fisiopatologia , Telemetria , Injúria Renal Aguda/etiologia , Injúria Renal Aguda/fisiopatologia , Alanina Transaminase/sangue , Animais , Gasometria , Temperatura Corporal , Ceco , Cistatina C/sangue , Frequência Cardíaca , Interleucina-10/sangue , Interleucina-6/sangue , Ligadura , Masculino , Camundongos , Camundongos Endogâmicos C57BL , Movimento , Punções , Sepse/complicações , Fator de Necrose Tumoral alfa/sangue , Tecnologia sem Fio
10.
Langmuir ; 31(8): 2321-33, 2015 Mar 03.
Artigo em Inglês | MEDLINE | ID: mdl-25661108

RESUMO

A series of pH-responsive amphiphilic poly(N,N-dimethylaminoethyl methacrylate)-block-poly(D-lactic acid)-block-poly(N,N-dimethylaminoethyl methacrylate) conjugated with poly(ethylene glycol) (D-PDLA-D@PEG) and D-PLLA-D@PEG copolymers were synthesized using a combination of ring-opening polymerization and atom-transfer radical polymerization followed by sequential quaternization of PDMAEMA chains and azide-alkyne click reaction with alkyne-end PEG. Gel permeation chromatography, nuclear magnetic resonance, and Fourier transform infrared spectroscopy results demonstrate the successful synthesis of the copolymers, and the conjugated PEG percentages in the copolymers can be tuned by the feeding ratios in the quaternization reaction. Conjugating PEG onto the PDMAEMA segments also successfully facilitated the D-PDLA-D@PEG, D-PLLA-D@PEG, and its corresponding 1:1 D/L mixtures to be dissolved directly in aqueous solution at the desired concentration range without using any organic solvents unlike the copolymers without PEG conjugation (D-PDLA-D and D-PLLA-D). We demonstrate control over micellar size, charge, and stability via three different preparation pathways, i.e., solution pH, percentages of PEG conjugation in the copolymers, and formation of PLA stereocomplex in micellar core. Static and dynamic light scattering studies demonstrate that the size of the core-shell micelles increases when the solution pH is reduced due to the protonation of the PDMAEMA segments that caused the osmotic pressure within the micelle to increase until the micelles reached a maximum size. It is interesting to note that the micelles formed by 1:1 D/L mixtures have larger swelling ratios as well as aggregation number and hydrodynamic radius that do not change significantly with pH and dilution, respectively, as compared to micelles formed from individual D or L forms of the copolymers. The enhanced stability of the pH-responsive micelles prepared by direct dissolution of the 1:1 D/L mixtures of the PEG conjugated PLA-based polyelectrolytes in aqueous medium is attributed to the stereocomplex formation between PLLA and PDLA in the micellar core as confirmed by wide-angle X-ray scattering measurements.


Assuntos
Poliésteres/química , Polietilenoglicóis/química , Eletrólitos/química , Concentração de Íons de Hidrogênio , Estrutura Molecular , Estereoisomerismo
11.
Biochim Biophys Acta Mol Basis Dis ; 1870(3): 167022, 2024 03.
Artigo em Inglês | MEDLINE | ID: mdl-38216068

RESUMO

BACKGROUND: CAMK1 has been shown to be involved in human disease progression via regulating mitochondrial dynamics. However, whether CAMK1 mediates mitochondrial dynamics to regulate diabetic nephropathy (DN) process remains unclear. METHODS: Mice were injected with streptozotocin (STZ) to mimic diabetic mice models in vivo, and mice with proximal tubule-specific knockout of CAMK1 (CAMK1-KO) were generated. HK-2 cells were treated with high-glucose (HG) to mimic DN cell model in vitro. Histopathological analysis was performed to confirm kidney injury in mice. ROS production and apoptosis were assessed by DHE staining and TUNEL staining. Mitochondria morphology was observed and analyzed by electron microscopy. Mitochondrial membrane potential was detected by JC-1 staining, and cell proliferation was measured by EdU assay. The mRNA and protein expression were examined by qRT-PCR, western blot and immunostaining. RNA interaction was confirmed by RIP assay and dual-luciferase reporter assay. The mRNA stability was tested by actinomycin D treatment, and m6A level was examined by MeRIP assay. RESULTS: CAMK1 was reduced in DN patients and STZ-induced diabetic mice. Conditional deletion of CAMK1 aggravated kidney injury and promoted mitochondrial fission in diabetic mice. CAMK1 overexpression inhibited mitochondrial fission to alleviate HG-induced HK-2 cell apoptosis. IGF2BP3 promoted the stability of CAMK1 mRNA by m6A modification. IGF2BP3 inhibited mitochondrial fission to repress cell apoptosis in vitro and kidney injury in vivo by increasing CAMK1 expression. CONCLUSION: IGF2BP3-mediated CAMK1 mRNA stability alleviated DN progression by inhibiting mitochondria fission.


Assuntos
Diabetes Mellitus Experimental , Nefropatias Diabéticas , Animais , Humanos , Camundongos , Proteína Quinase Tipo 1 Dependente de Cálcio-Calmodulina/metabolismo , Diabetes Mellitus Experimental/complicações , Diabetes Mellitus Experimental/genética , Diabetes Mellitus Experimental/metabolismo , Nefropatias Diabéticas/patologia , Túbulos Renais/patologia , Dinâmica Mitocondrial/fisiologia , RNA Mensageiro/metabolismo
12.
Langmuir ; 29(46): 14307-13, 2013 Nov 19.
Artigo em Inglês | MEDLINE | ID: mdl-24144302

RESUMO

Amphiphilic conetworks (APCNs), consisting of hydrophilic poly[poly(ethylene glycol) methyl ester acrylate] (PPEGMEA) and hydrophobic stereocomplex of poly(L-lactide) (PLLA) and poly(D-lactide) (PDLA), were prepared by free radical copolymerization of PEGMEA with acrylate macromonomer of the PLA stereocomplex. The effects of stereocomplexation and the amount of PLA stereocomplex on the rheology properties of APCNs were investigated. The results indicated that the APCNs was stronger in the presence of stereocomplexation compared with the that of nonstereocomplex system, and the strength of the APCNs increased with the increasing of the amount of PLA stereocomplex. The storage modulus of the APCNs could be easily tuned from 1200 to 4300 Pa by incorporating 2-10% of stereocomplex PLA. On the other hand, the swelling behavior of APCNs decreased with the increasing content of hydrophobic PLA cross-linker.


Assuntos
Interações Hidrofóbicas e Hidrofílicas , Metacrilatos/química , Poliésteres/química , Polietilenoglicóis/química , Géis , Estereoisomerismo
13.
Langmuir ; 29(23): 7087-95, 2013 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-23721059

RESUMO

Polymer nanocomposite (NC) hydrogels exhibiting both dynamic restructuring and unusual adhesive properties in wet and dry states have been prepared in an efficient and straightforward way via free radical polymerization of poly(ethylene glycol) methyl ether acrylate (PEG) in the presence of silane-modified sodium montmorillonite (NaMMT). The dynamic restructuring of the NC gel has been demonstrated by almost instant recovery of mechanical properties, such as storage modulus, loss modulus, and damping tan δ (at 0.025 strain) by 60-110% after being stressed to the point of gel failure. Furthermore, the dry NC gel showed exceptional thermal and mechanical stability during a heating and cooling cycle between 25 and 110 °C, with only slightly decreases followed by at least 30% increases in both moduli, while tan δ remained nearly unchanged. The NC gel in dry state could repeatedly adhere to various surfaces such as steel, glass, plastic, etc., and detach from the surface without being broken and leaving little contamination behind. This unique adhesive characteristic was characterized by high storage modulus, loss modulus (kPa), and tan δ (>0.6) corresponding to high cohesive, adhesive, and tacking properties of pressure-sensitive adhesives (PSAs). Finally, a reversible network structure formed by PEO interpenetrating within 3-dimentional (3-D) silica network was proposed to be responsible for the dynamic restructuring and the unique adhesive behaviors observed in the NC gel, and the 3-D network structure was investigated by XRD, FTIR, and DSC measurements. For this 3-D network structure, we suggest that the flexibility of PEO could allow PEO side chains to contact with various surfaces by either PEO segments or methoxy end groups via weak physical interactions, such as van der Waals interactions or hydrogen bonding, whereas the reversible network structure contributes to the recovery of strength and shape after the gel failure.


Assuntos
Hidrogéis/química , Nanocompostos/química , Polímeros/química , Termodinâmica , Modelos Moleculares
14.
Phys Chem Chem Phys ; 15(35): 14689-95, 2013 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-23900140

RESUMO

Iron oxide nanocrystals are ideal building blocks for the construction of flexible nanodevices whose performance can be modulated by controlling the morphology of isolated particles and their organizational form. This work demonstrates the fabrication of high quality Langmuir-Blodgett (LB) nanocrystal assemblies with limited overlapping and higher coverage by systemically and combinatorially optimizing the parameters of compression pressure and quantity of spread nanocrystals. Monodispersed iron oxide nanocrystals with a diameter of 11.8 nm were synthesized by thermal decomposition of Fe(CO)5 in trioctylamine with the presence of oleic acid. Multilayer nanocrystal assemblies were obtained through a layer-by-layer (LBL) process by repeating the transfer procedure after their hydrophilicity had been improved via treatment in a UV-ozone oven. The quality of nanocrystal assemblies was investigated by UV-vis spectrometry and scanning electron microscopy. The nanomagnetism for the nanostructures of different combination manners was studied systemically by a superconducting quantum interference device (SQUID). A lower superparamagnetic blocking temperature was found in the monolayer Fe3O4 nanocrystal assembly. The superparamagnetic blocking temperature in magnetic nanocrystal assemblies could be tuned through modifying the interparticle interactions among the interlayer and intralayers by controlling the layer number of the assemblies.

15.
Sci Total Environ ; 855: 158880, 2023 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-36130629

RESUMO

Lead dioxide (PbO2) materials have been widely employed in various fields such as batteries, electrochemical engineering, and more recently environmental engineering as anode materials, due to their unique physicochemical properties. Key performances of PbO2 electrodes, such as energy efficiency and space-time yield, are influenced by morphological as well as compositional factors. Micro-nano structure regulation and decoration of metal/non-metal on PbO2 is an outstanding technique to revamp its electrocatalytic activities and enhance environmental engineering efficiency. The aim of this review is to comprehensively summarize the recent research progress in the morphology control, the structure constructions, and the element doping of PbO2 materials, further with many environmental application cases evaluated. Concerning electrochemical environmental engineering, the lead dioxide employed in chemical oxygen demand detection, ozone generators, and wastewater treatment has been comprehensively reviewed. In addition, the future research perspectives, challenges and the opportunities on PbO2 materials for environmental applications are proposed.


Assuntos
Poluentes Químicos da Água , Poluentes Químicos da Água/análise , Titânio/química , Oxirredução , Óxidos/química , Eletrodos
16.
Chem Asian J ; 18(11): e202300360, 2023 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-37144454

RESUMO

This Special Collection highlights the latest developments in the field of gel electrolytes. In this Editorial, guest editors Haitao Zhang, Du Yuan, Jin Zhao, Xiaoyan Ji, and Yi-Zhou Zhang briefly introduced the research focusing on chemistry and applications of gel electrolytes in this special collection.

17.
Chem Asian J ; 18(4): e202201280, 2023 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-36632721

RESUMO

Gel electrolytes are being intensively explored for aqueous rechargeable zinc-ion batteries, especially towards high performance and multi-functionalities. Water plays a central role on the fundamental properties, interface reaction/interaction, and performance of the gel-type zinc electrolyte. In this review, the influence of water on the physiochemical properties of gel electrolytes is focused on. The correlation between water activity and the fundamental properties of zinc electrolytes is presented. Current approaches and challenges in manipulating water activity and the consequent influence on the electrochemical stability, transport, and interface kinetics of gel electrolytes are summarized. An outlook on approaches to tuning and investigating water activity is provided to shed light on the design of advanced gel electrolytes.

18.
Adv Sci (Weinh) ; 10(8): e2206469, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36646504

RESUMO

Novel electrolyte is being pursued toward exploring Zn chemistry in zinc ion batteries. Here, a fluorine-free liquid crystal (LC) ionomer-type zinc electrolyte is presented, achieving simultaneous regulated water activity and long-range ordering of conduction channels and SEI. Distinct from water network or local ordering in current advances, long-range ordering of layered water channels is realized. Via manipulating water activity, conductivities range from ≈0.34 to 15 mS cm-1 , and electrochemical window can be tuned from ≈2.3-4.3 V. The Zn|Zn symmetric cell with LC gel exhibits highly reversible Zn stripping/plating at 5 mA cm-2 and 5 mAh cm-2 for 800 h, with retained ordering of water channels. The capability of gel for inducing in situ formation of long-range ordered layer SEI associated with alkylbenzene sulfonate anion is uncovered. V2 O5 /Zn cell with the gel shows much improved cycling stability comparing to conventional zinc electrolytes, where the preserved structure of V2 O5 is associated with the efficiently stabilized Zn anode by the gel. Via long-range ordering-induced regulation on ion transport, electrochemical stability, and interfacial reaction, the development of LC electrolyte provides a pathway toward advancing aqueous rechargeable batteries.

19.
Polymers (Basel) ; 13(5)2021 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-33807945

RESUMO

Slopes with carbonaceous mudstone (CM) are widely distributed in the southwest of China and have experienced numerous geological disasters in special climate, especially in rainfall conditions. Therefore, novel materials to stabilize CM slopes have attracted increasing interests. However, developing ultra-stable and cost-effective additives for CM slopes is still a great challenge. Herein, a hydrophobic polymeric material (polyvinylidene fluoride, PVDF) is investigated as an additive to enhance the mechanical strength and long-time stability of CM slopes. The PVDF is uniformly dispersed in CM matrix via interfacial interaction. The contact angle of the PVDF-modified carbonaceous mudstone (PVDF-MCM) can reach as high as 103.95°, indicating an excellent hydrophobicity. The unconfined compressive strength (UCS) and tensile strength (TS) of PVDF-MCM have been intensively enhanced to 4.07 MPa and 1.96 MPa, respectively, compared with ~0 MPa of pristine CM. Moreover, the UCS and TS of PVDF-MCM remain at 3.24 MPa and 1.03 MPa even after curing for 28 days in high humidity conditions. Our findings show that the PVDF can improve the hydrophobicity of CM significantly, which leads to super mechanical stability of PVDF-MCM. The excellent performance makes PVDF a promising additive for the development of ultra-stable, long-lifetime and cost-effective carbonaceous mudstone slopes.

20.
iScience ; 24(10): 103157, 2021 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-34646992

RESUMO

Energy storage systems are crucial in the deployment of renewable energies. As one of the most promising solutions, redox flow batteries (RFBs) are still hindered for practical applications by low energy density, high cost, and environmental concerns. To breakthrough the fundamental solubility limit that restricts boosting energy density of the cell, we here demonstrate a new RFB system employing polysulfide and high concentrated ferricyanide (up to 1.6 M) species as reactants. The RFB cell exhibits high cell performances with capacity retention of 96.9% after 1,500 cycles and low reactant cost of $32.47/kWh. Moreover, neutral aqueous electrolytes are environmentally benign and cost-effective. A cell stack is assembled and exhibits low capacity fade rate of 0.021% per cycle over 642 charging-discharging steps (spans 60 days). This neutral polysulfide/ferricyanide RFB technology with high safety, long-duration, low cost, and feasibility of scale-up is an innovative design for storing massive energy.

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