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1.
Bioconjug Chem ; 35(9): 1450-1458, 2024 09 18.
Artigo em Inglês | MEDLINE | ID: mdl-39213480

RESUMO

A porphyrin-containing nanoscale covalent organic polymer (COP) was fabricated from 5,10,15,20-tetra(4-carboxyphenyl)porphyrin (TCPP) and cystamine via an acylation reaction. On the one hand, TCPP can induce tumor cell death by laser irradiation. Due to the presence of disulfide bonds of cystamine which can react with glutathione, it exhibits depletion of glutathione and accumulation of peroxides in tumor cells. Ultimately by the hyaluronic acid to encapsulate the COP to get S-COP@HA, the nanoparticle with a size of 168.6 nm also exhibits good tumor accumulation and biosafety. Significant inhibition of tumor cell growth was observed after two consecutive doses of S-COP@HA at relatively low laser densities. This combination therapy was proved to reduce the level of reduced glutathione in tumor cells, where ferroptosis occurs after photodynamic treatment. Overall, this study presents a potent, good therapeutic option for the effective enhancement of photodynamic therapy by glutathione depletion.


Assuntos
Ferroptose , Glutationa , Fotoquimioterapia , Porfirinas , Glutationa/metabolismo , Fotoquimioterapia/métodos , Porfirinas/química , Porfirinas/farmacologia , Ferroptose/efeitos dos fármacos , Humanos , Animais , Nanopartículas/química , Polímeros/química , Linhagem Celular Tumoral , Camundongos , Fármacos Fotossensibilizantes/farmacologia , Fármacos Fotossensibilizantes/química , Ácido Hialurônico/química
2.
Molecules ; 29(13)2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38998968

RESUMO

The steric interference of proximal dialkyl amino and acyl groups at the peri (1,8) positions of naphthalene affects the intramolecular charge transfer fluorescence. Previous studies indicate that acyl and freely rotating dimethyl amino groups twist toward coplanarity with the naphthalene ring in the excited state. The present study examines the effect of constraining the amino group in a ring. The photophysical properties of 2,2-dimethyl-1-(1-methyl-1,2,3,4-tetrahydrobenzo[h]quinolin-10-yl)propan-1-one (4), ethyl 1-methyl-1,2,3,4-tetrahydrobenzo[h]quinoline-10-carboxylate (5), and 1-methyl-1,2,3,4-tetrahydrobenzo[h]quinoline-10-carbaldehyde (6) are compared with the dimethyl amino derivatives 2 and 3. Crystal structures of 4-6 show that the amine ring adopts a chair conformation, where the N-methyl group is axial. Computational results suggest that the pyramidal amino group planarizes and twists together with the acyl toward coplanarity in the excited state. The ring structure does not thwart the formation of a planar intramolecular charge transfer (PICT) state.

3.
EPMA J ; 15(2): 375-404, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38841623

RESUMO

Background: DNA methylation is an important mechanism in epigenetics, which can change the transcription ability of genes and is closely related to the pathogenesis of ovarian cancer (OC). We hypothesize that DNA methylation is significantly different in OCs compared to controls. Specific DNA methylation status can be used as a biomarker of OC, and targeted drugs targeting these methylation patterns and DNA methyltransferase may have better therapeutic effects. Studying the key DNA methylation sites of immune-related genes (IRGs) in OC patients and studying the effects of these methylation sites on the immune microenvironment may provide a new method for further exploring the pathogenesis of OC, realizing early detection and effective monitoring of OC, identifying effective biomarkers of DNA methylation subtypes and drug targets, improving the efficacy of targeted drugs or overcoming drug resistance, and better applying it to predictive diagnosis, prevention, and personalized medicine (PPPM; 3PM) of OC. Method: Hypermethylated subtypes (cluster 1) and hypomethylated subtypes (cluster 2) were established in OCs based on the abundance of different methylation sites in IRGs. The differences in immune score, immune checkpoints, immune cells, and overall survival were analyzed between different methylation subtypes in OC samples. The significant pathways, gene ontology (GO), and protein-protein interaction (PPI) network of the identified methylation sites in IRGs were enriched. In addition, the immune-related methylation signature was constructed with multiple regression analysis. A methylation site model based on IRGs was constructed and verified. Results: A total of 120 IRGs with 142 differentially methylated sites (DMSs) were identified. The DMSs were clustered into a high-level methylation group (cluster 1) and a low-level methylation group (cluster 2). The significant pathways and GO analysis showed many immune-related and cancer-associated enrichments. A methylation site signature based on IRGs was constructed, including RORC|cg25112191, S100A13|cg14467840, TNF|cg04425624, RLN2|cg03679581, and IL1RL2|cg22797169. The methylation sites of all five genes showed hypomethylation in OC, and there were statistically significant differences among RORC|cg25112191, S100A13|cg14467840, and TNF|cg04425624 (p < 0.05). This prognostic model based on low-level methylation and high-level methylation groups was significantly linked to the immune microenvironment as well as overall survival in OC. Conclusions: This study provided different methylation subtypes for OC patients according to the methylation sites of IRGs. In addition, it helps establish a relationship between methylation and the immune microenvironment, which showed specific differences in biological signaling pathways, genomic changes, and immune mechanisms within the two subgroups. These data provide ones to deeply understand the mechanism of immune-related methylation genes on the occurrence and development of OC. The methylation-site signature is also to establish new possibilities for OC therapy. These data are a precious resource for stratification and targeted treatment of OC patients toward an advanced 3PM approach. Supplementary Information: The online version contains supplementary material available at 10.1007/s13167-024-00359-3.

4.
Huan Jing Ke Xue ; 45(5): 3098-3106, 2024 May 08.
Artigo em Chinês | MEDLINE | ID: mdl-38629570

RESUMO

In recent years, the environmental pollution of microplastics in Poyang Lake has received increasing attention. Baisha Lake of Poyang Lake was selected as the study area, and samples of water and sediments of Baisha Lake and the microplastics therein were collected, and the polymer types of microplastics were identified as polyethylene (PE), polyester (PET), polypropylene (PP), and polystyrene (PS) using Fourier infrared spectroscopy. We also analyzed the structural composition of bacterial communities in water, in sediments, and on microplastic surfaces using 16S high-throughput sequencing. The species richness and diversity of bacteria on the microplastic surfaces were lower than those in the surrounding water and sediments. The results of NMDS analysis showed that the bacterial community structures on the microplastic surfaces differed greatly from those in the surrounding sediments and water. The bacterial community composition in water and sediment differed from that on the microplastic surfaces, and the dominant bacterial phyla on the microplastic surfaces were Proteobacteria and Bacteroidota, and their relative abundance on the microplastic surfaces was higher than that in sediment. The relative abundance of Proteobacteria was higher than that in water. The relative abundances of Bacteroidota and Actinobacteriota were significantly lower than that of water. Massilia and Pseudomonas were the dominant genera on the microplastic surfaces, and their relative abundances were significantly higher than those in the surrounding water and sediments. BugBase phenotype prediction revealed that the relative abundance of contains mobile elements, biofilm formation, potential pathogenicity, and stress tolerance phenotypes of microplastic bacterial communities were significantly higher than those of the surrounding water and sediments. The results revealed that microplastics may have contributed to the spread of harmful bacteria, including pathogenic bacteria, and increased the potential pathogenicity of bacterial communities. Additionally, microplastic surface bacterial communities had higher phenotypes of mobile gene element content. Revealing the potential harm of microplastic pollution to wetland ecology at the micro level may provide a scientific reference for maintaining the ecological stability of wetlands.


Assuntos
Microplásticos , Poluentes Químicos da Água , Plásticos/análise , Lagos/química , Monitoramento Ambiental , Água/análise , Bactérias/genética , Proteobactérias , China , Poluentes Químicos da Água/análise , Sedimentos Geológicos/química
5.
RSC Adv ; 14(17): 12030-12037, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38623294

RESUMO

Ti3C2 MXenes are emerging 2D materials and have attracted increasing attention in sodium metal anode fabrication because of their high conductivity, multifunctional groups and excellent mechanical performances. However, the severe self-restacking of Ti3C2 MXenes is not conducive to dispersing Na+ and limits the function of regulating sodium deposition. Herein, an alkalized MXene/carbon nanotube (CNT) composite (named A-M-C) is introduced to regulate Na deposition behavior, which consists of Na3Ti5O12 microspheres, Ti3C2 MXene nanosheets and CNTs. Ti3C2 MXene nanosheets with large interlayer spaces and "sodiophilic" functional groups can provide abundant active sites for uniform nucleation and deposition of Na. Plenty of nanosheets are grown on the surface of the microsphere, thereby reducing the local current density, which can guide initial Na nucleation and promote Na dendrite-free growth. Furthermore, CNTs increase the electrical conductivity of the composite and achieve fast Na+ transport, improving the cycling stability of Na metal batteries. As a result, at a capacity of 1 mA h cm-2, the A-M-C electrode achieves a high average coulombic efficiency (CE) of 99.9% after 300 cycles at 2 mA cm-2. The symmetric cells of A-M-C/Na provide a long cycling life of more than 1400 h at 1 mA cm-2 with a minimal overpotential of 19 mV at an areal capacity of 1 mA h cm-2. The A-M-C/Na//NVP@C full cell presents a high coulombic efficiency of 98% with 100 mA g-1 in the first cycle. The strategy in this work provides new insights into fabricating novel MXene-based anode materials for dendrite-free sodium deposition.

6.
J Colloid Interface Sci ; 664: 790-800, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38492380

RESUMO

Deleterious volumetric expansion and poor electrical conductivity seriously hinder the application of Si-based anode materials in lithium-ion batteries (LIBs). Herein, boron-doped three-dimensional (3D) porous carbon framework/carbon shell encapsulated silicon (B-3DCF/Si@C) hybrid composites are successfully prepared by two coating and thermal treatment processes. The presence of 3D porous carbon skeleton and carbon shell effectively improves the mechanical properties of the B-3DCF/Si@C electrode during the cycling process, ensures the stability of the electrical contacts of the silicon particles and stabilizes the solid electrolyte interface (SEI) layer, thus enhancing the electronic conductivity and ion migration efficiency of the anode. The developed B-3DCF/Si@C anode has a high reversible capacity, excellent cycling stability and outstanding rate performance. A reversible capacity of 1288.5 mAh/g is maintained after 600 cycles at a current density of 400 mA g-1. The improved electrochemical performance is demonstrated in a full cell using a LiFePO4-based cathode. This study presents a novel approach that not only mitigates the large volume expansion effects in LIB anode materials, but also provides a reference model for the preparation of porous composites with various functionalities.

7.
Carbohydr Polym ; 326: 121580, 2024 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-38142066

RESUMO

Developing naturally-derived wound dressing materials with intrinsic therapeutic effects is desirable for the clinical applications. Recently, guanosine-based supramolecular G-quadruplex (G4) hydrogel exhibited great potential in preparing biological materials due to its simple fabrication method and responsive gel networks. However, the weak mechanical properties and the consequent burst release of bioactive molecules restrict its clinical applications. Herein, we found that konjac glucomannan (KGM) with immunoregulatory effect did not affect the self-assembly of G-quadruplexes and thus effectively enhancing the mechanical properties of G4 hydrogel. Aloin, as a model drug, was in situ loaded into gel networks, finally obtaining the G4/Aloin-KGM hydrogel. This hydrogel exhibited porous morphology, swelling ability and hemostatic capability. Boronate bonds in G4 networks and aloin collectively endowed the hydrogel with excellent antioxidant performance. Meanwhile, aloin also provided outstanding in vitro and in vivo bactericidal ability. The wounds treated with this biocompatible hydrogel demonstrated faster regeneration of epithelial and dermal tissues, and the whole wound healing stages were accelerated by promoting collagen deposition, facilitating macrophage polarization towards M2 phenotype, down-regulating the expression level of IL-6, and up-regulating the expression level of IL-10, CD31 and α-SMA.


Assuntos
Hidrogéis , Lesões dos Tecidos Moles , Humanos , Hidrogéis/farmacologia , Hidrogéis/química , Cicatrização , Antioxidantes/farmacologia , Antibacterianos/farmacologia , Antibacterianos/química
8.
Front Chem ; 11: 1238424, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37711316

RESUMO

Phytoremediation techniques have been widely used in the treatment of heavy metal contaminated soils in recent years, but there is no effective post-treatment method for plant tissues containing heavy metals after remediation. Elsholtzia Harchowensis is a copper hyperaccumulator, commonly distributed in copper mining areas and often used for soil remediation of mine tailings. Moreover, copper-based catalysts are widely used in electrocatalytic reduction of carbon dioxide, which aims to convert carbon dioxide into useful fuels or chemicals. In this study, copper-modified biochar was prepared from Elsholtzia Harchowensis. Its specific surface area can reach as high as 1202.9 m2/g, with a certain porous structure and even distribution of copper on the amorphous carbon. Various products (such as carbon monoxide, methane, ethanol, and formic acid) could be obtained from the electrolytic reduction of carbon dioxide by using the as-prepared catalyst. Instantaneous current density of up to 15.3 mA/cm2 were achieved in 1.0 M KHCO3 solution at a potential of -0.82 V (vs. RHE). Electrolysis at a potential of -0.32 V (vs. RHE) for 8 h resulted in a stable current of about 0.25 mA/cm2, and the Faraday efficiency (FE) of carbon monoxide can reach as high as 74.6%. In addition, electrolysis at a potential of -0.52 V (vs. RHE) for 8 h led to a stable current of about 2.2 mA/cm2 and a FE of 8.7% for the C2 product. The rich variety of elements in plants leads to catalysts with complex structural and elemental characteristics as well, which facilitates the electrolytic reduction of carbon dioxide with a variety of useful products.

9.
Int J Biol Macromol ; 253(Pt 3): 126848, 2023 Dec 31.
Artigo em Inglês | MEDLINE | ID: mdl-37699465

RESUMO

Skin wound management faces significant clinical challenges, including continuous bacterial infection and inflammation. Therefore, developing removable hydrogel dressings with intrinsic multifunctional properties is highly desirable. In this study, a body temperature-induced adhesive and removable hydrogel was designed to treat skin defect wounds. The HA/Gel-R-Ag hybrid gel was prepared by incorporating a silver ion-crosslinked sulfhydryl hyaluronate/gelatin-based polymeric gel network into a supramolecular rhein gel network, thereby significantly enhancing its mechanical properties. Temperature-responsive gelatin chains give the hybrid gel reversible tissue adhesiveness and detachment, thus avoiding secondary injury to wounds when changing the hydrogels. The hybrid gel exhibited excellent bactericidal ability owing to the antibacterial capacity of the silver ions and rhein. Moreover, both HA and rhein endowed the hybrid gel with immunoregulatory effects by promoting macrophage polarization from pro-inflammatory M1 phenotype to anti-inflammatory M2 phenotype. In a full-thickness skin defect mouse mode, this porous, degradable, and biocompatible HA/Gel-R-Ag hybrid gel boosted skin regeneration by inhibiting inflammation and promoting collagen deposition and angiogenesis. It is thus a simple method for widening the application range of mechanically weak rhein gels and providing a promising wound dressing material with multiple intrinsic functions for treating skin wounds.


Assuntos
Gelatina , Hidrogéis , Animais , Camundongos , Hidrogéis/farmacologia , Gelatina/farmacologia , Adesivos , Temperatura Corporal , Prata , Bandagens , Antibacterianos , Inflamação
10.
Huan Jing Ke Xue ; 44(9): 5063-5070, 2023 Sep 08.
Artigo em Chinês | MEDLINE | ID: mdl-37699824

RESUMO

Plastic particles smaller than 5 mm in size are known as microplastics which are widespread in the environment and can cause several negative effects. Moreover, only a few studies have focused on the relationship between microplastics and microbes in the natural wetland ecosystem. In this study, microplastics were collected from sediment, water, and sediment flooded and non-flooded conditions in the lake wetland of Poyang Lake as the study area. The structural distribution of bacterial community on sediment, water, and microplastics were analyzed using 16S high-throughput sequencing. The results of the α-diversity analysis showed that the bacterial abundance and diversity on the surface of microplastics were significantly different from those in the environment and were lower than those in the surrounding environment in both flooded and non-flooded conditions. The results of the principal co-ordinates analysis indicated that the bacterial community on the surface of microplastics was more influenced by the sediment in non-flooded conditions and by the water in flooded conditions. The structure of the bacterial community on the microplastic surface also showed significant differences from the surrounding environment, with the sediment mainly consisting of several other bacterial genera with <1% abundance, whereas the bacterial community on the microplastics had clearly dominant species. The relative abundance of Proteobacteria on the microplastic surfaces increased significantly in the non-flooded condition compared to that in the water and sediment samples, whereas the relative abundance of Bacteroidota on the microplastic surface increased in the flooded condition. The genus Flavobacterium, Massilia, and Pseudomonas were the most abundant in the non-flooded state, and the genus Flavobacterium was the most abundant in the flooded state. In this study, Pseudomonas spp. was the focus of future research on plastic biodegradation. This study can further improve the understanding of microplastic pollution in wetland ecosystems and provide a theoretical basis for lake environmental management.


Assuntos
Microplásticos , Áreas Alagadas , Plásticos , Ecossistema , Lagos , Biodegradação Ambiental , Pseudomonas , Água
11.
Adv Healthc Mater ; 12(26): e2300962, 2023 10.
Artigo em Inglês | MEDLINE | ID: mdl-37499265

RESUMO

This study reports a facile and green synthesis of a new multifunctional nanotheranostic probe for the synergistic therapy of rheumatoid arthritis (RA) and in situ assessment of therapeutic response. The probe is synthesized through a one-step self-assembly of two exquisitely designed peptide-amphiphilic block copolymers (PEG-DTIPA-KGPLGVRK-MTX and Pal-GGGGHHHHD-TCZ) under mild conditions, requiring minimal energy input. The resultant probe demonstrates excellent biocompatibility, water solubility, and colloidal stability. It exhibits a strong IL-6R targeting ability toward inflamed joints, and releases drugs in an MMP-2-responsive manner. The co-loading of methotrexate(MTX) and tocilizumab (TCZ) into the probe enables synergistic RA therapy with improved efficacy by simultaneously decreasing the activity of adenosine synthetase and interfering with the binding of IL-6 to its receptor. In addition, the resultant probe exhibits a high r1 relaxation rate (7.00 mm-1  s-1 ) and X-ray absorption capability (69.04 Hu mm-1 ), enabling sensitive MR and CT dual-modal imaging for simultaneous evaluation of synovial thickness and bone erosion. Both in vitro experiments using lipopolysaccharide-treated RAW264.7 cells and in vivo experiments using collagen-induced arthritis mice demonstrate the probe's high effectiveness in synergistically inhibiting inflammation. This study provides new insights into RA theranostics, therapeutic monitoring, the design of multifunctional theranostic probes, and beyond.


Assuntos
Antirreumáticos , Artrite Reumatoide , Camundongos , Animais , Antirreumáticos/farmacologia , Antirreumáticos/uso terapêutico , Metaloproteinase 2 da Matriz , Nanomedicina Teranóstica , Artrite Reumatoide/diagnóstico por imagem , Artrite Reumatoide/tratamento farmacológico , Metotrexato/farmacologia , Metotrexato/uso terapêutico , Tomografia Computadorizada por Raios X
12.
Bioresour Technol ; 382: 129207, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37217148

RESUMO

A side-stream tank which was in parallel with the anoxic tank was used to improve the performance of an Anaerobic-Anoxic-Oxic process. The partial mixtures from the anaerobic tank were injected into the side-stream tank with the initial nitrite nitrogen (NO2--N) concentrations of 10 mg/L and 20 mg/L. When the initial NO2--N concentration in the tank was 20 mg/L, total nitrogen and total phosphorus removal efficiencies of the A2/O process increased from 72% and 48% to 90% and 89%, respectively. 2.23 mg/L of nitric oxide (NO) were observed in the side-stream tank. The abundance of Nitrosomonas sp. and Nitrospira sp. were varied from 0.98% and 6.13% to 2.04% and 1.13%, respectively. The abundances of Pseudomonas sp. and Acinetobacter sp. were increased from 0.81% and 0.74% to 6.69% and 5.48%, respectively. NO plays an important role for improving the nutrients removal of the A2/O process in the side-stream nitrite-enhanced strategy.


Assuntos
Nitritos , Eliminação de Resíduos Líquidos , Óxido Nítrico , Anaerobiose , Rios , Dióxido de Nitrogênio , Reatores Biológicos , Fósforo , Nitrogênio , Nutrientes , Esgotos , Desnitrificação
13.
J Colloid Interface Sci ; 646: 538-546, 2023 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-37210901

RESUMO

Silicon (Si) is considered as one of the most promising candidates for next-generation lithium-ion battery (LIB) anode due to its high theoretical capacity. However, the drastic volume change of Si anodes during lithiation/delithiation processes leads to rapid capacity fade. Herein, a three-dimensional Si anode with multiple protection strategy is proposed, including citric acid-modification of Si particles (CA@Si), GaInSn ternary liquid metal (LM) addition, and porous copper foam (CF) based electrode. The CA modified supports strong adhesive attraction of Si particles with binder and LM penetration maintains good electrical contact of the composite. The CF substrate constructs a stable hierarchical conductive framework, which could accommodate the volume expansion to retain integrity of the electrode during cycling. As a result, the obtained Si composite anode (CF-LM-CA@Si) demonstrates a discharge capacity of 3.14 mAh cm-2 after 100 cycles at 0.4 A g-1, corresponding to 76.1% capacity retention rate based on the initial discharge capacity and delivers comparable performance in full cells. The present study provides an applicable prototype of high-energy density electrodes for LIBs.

14.
J Colloid Interface Sci ; 640: 829-838, 2023 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-36905892

RESUMO

Transition metal oxide (TMO)-based electrodes exhibit increased capacities, yet the mechanism behind the true cause of capacity in such materials remains unclear. Herein, hierarchical porous and hollow Co-CoO@NC spheres assembled by nanorods with refined nanoparticles and amorphous carbon have been synthesized by a two-step annealing approach. A temperature gradient-driven mechanism is revealed for the evolution of the hollow structure. Compared with the solid CoO@NC spheres, the novel hierarchical of Co-CoO@NC can fully utilize the interior active material by exposing both ends of each nanorod into electrolyte. The hollow interior provides extra space for the volume variation, leading to an up-trend capacity of 919.3 mAh g-1 at 200 mA g-1 over 200 cycles. Differential capacity curves disclose that solid electrolyte interface (SEI) films reactivation partly contributes to increasing reversible capacity. The introduction of nanosized Co particles benefits the process by participating in the transformation of SEI components. This study provides a guide for constructing anodic material with exceptional electrochemical performance.

15.
J Colloid Interface Sci ; 638: 99-108, 2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-36736122

RESUMO

Anodes based on silicon/carbon composites promise their commercial prospects for next-generation lithium ion batteries owing to their merits of high specific capacity, enhanced ionic and electronic conductivity, and excellent compatibility. Herein, a series of carbonaceous framework/Si composites are designed and prepared by rational waste utilization. N, P codoped foam-like porous carbon/Si composites (FPC@Si) and N, P codoped carbon coated Si composites (NPC@Si) are fabricated by utilizing expired milk powder as a carbon source with facile treatment methods. The results indicate that the porous carbon skeleton and carbon shell can improve the conductivity of Si and stabilize the solid electrolyte interfaces to avoid direct contact between active material and electrolyte. Moreover, the influence of drastic volume expansion of Si on the anode can be efficiently alleviated during charge/discharge processes. Therefore, the Si/C composite electrodes present excellent long-term cycling stability and rate capability. The electrochemical performance shows that the reversible capacity of FPC@Si and NPC@Si can be respectively maintained at 587.3 and 731.2 mAh g-1 after 1000 charge/discharge cycles under 400 mA g-1. Most significantly, the optimized Si/C composite electrodes exhibit outstanding performance in the full cell tests, promising them great potential for practical applications. This study not only provides a valuable guidance for recycling of waste resources, but also supports a rational design strategy of advanced composite materials for high-performance energy storage devices.


Assuntos
Lítio , Leite , Animais , Emulsões , Pós , Íons , Carbono , Eletrodos
16.
J Colloid Interface Sci ; 631(Pt A): 112-121, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36370494

RESUMO

The rapid capacity decay severely limits the commercial applications of metal oxide-based electrodes. Exploring innovative materials with enhanced lithium storage performance is urgent and challenging. Herein, we propose a strategy for the synthesis of NiCo-NiCoO2@C composites using layered double hydroxide (LDH) precursors. When used as the anode materials, the composites deliver enhanced capacity throughout the continuous charge-discharge process. In our design, the electrochemically active NiCoO2 nanoparticles pulverize the NiCo phases via a conversion reaction. The NiCo phases can increase capacity by reacting with the Li2O yielded from the conversion of NiCoO2 and participating in the reversible transformation of solid-electrolyte interface (SEI) films, thus ensuring fast charge transfer. Voids that appear with the consumption of NiCo phases can provide abundant channels for Li+ transportation. Carbon matrices can effectively alleviate the stress generated during repeated cycles of expansion and shrinkage. Benefiting from these features, NiCo-NiCoO2@C anode delivers a highly enhanced reversible capacity of 961.6 mAh g-1 after 300 cycles at 200 mA g-1. This LDH-based strategy may be extended to the design and synthesis of various enhanced anode materials for lithium-ion batteries (LIBs).

17.
J Colloid Interface Sci ; 625: 373-382, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35717851

RESUMO

Capacity retention is one of the key factors affecting the performance of silicon (Si)-based lithium-ion batteries and other energy storage devices. Herein, a three dimension (3D) network self-healing binder (denoted as PVA + LB) consisting of polyvinyl alcohol (PVA) and lithium metaborate (LiBO2) solution is proposed to improve the cycle stability of Si-based lithium-ion batteries. The reversible capacity of the silicon electrode is maintained at 1767.3 mAh g-1 after 180 cycles when employing PVA + LB as the binder, exhibiting excellent cycling stability. In addition, the silicon/carbon (Si/C) anode with the PVA + LB binder presents superior electrochemical performance, achieving a stable cycle life with a capacity retention of 73.7% (858.3 mAh g-1) after 800 cycles at a current density of 1 A g-1. The high viscosity and flexibility, 3D network structure, and self-healing characteristics of the PVA + LB binder are the main reasons to improve the stability of the Si or Si/C contained electrodes. The novel self-healing binder shows great potential in designing the new generation of silicon-based lithium-ion batteries and even electrochemical energy storage devices.

18.
J Environ Manage ; 316: 115237, 2022 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-35568014

RESUMO

NO and N2O as important greenhouse gases andtheir production mechanisms during nitrification are not completely understood. This study aimed to analyze the effect of hydroxylamine (NH2OH) on NO and N2O produced by nitrifying bacteria from activated sludge in a sequencing batch reactor (SBR). Experimental results showed that when nitrite (NO2-) accumulated during aerobic ammonia (NH4+) oxidation, N2O was the main product. The total amount of NO and N2O produced by NH2OH oxidation was positively correlated with dissolved oxygen (DO) levels. The imbalance of NH4+ oxidation caused by NH2OH addition was more conducive to the generation of NO and N2O under high DO conditions. When NH2OH was added into the reactor with NO2- as the substrate, the production of NO and N2O under high DO levels was mainly related to NH2OH oxidation. Under low DO conditions, NO and N2O from the biotic/abiotic hybrid pathways were more significant in the reactor of the coexistence of NO2- and NH2OH, which could be mainly caused by the pathways of nitrifier denitrification and abiotic reaction. Besides, limited amount of NO and N2O was generated by heterotrophic denitrification pathway during autotrophic nitrification. The implications for the above results are important for understanding the production of NO and N2O under NH2OH stress in nitrifying sludge reactor.


Assuntos
Reatores Biológicos , Esgotos , Reatores Biológicos/microbiologia , Desnitrificação , Hidroxilamina/metabolismo , Hidroxilaminas , Nitrificação , Dióxido de Nitrogênio , Óxido Nitroso/análise , Oxirredução , Oxigênio , Esgotos/microbiologia
19.
Bioresour Technol ; 355: 127271, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35526711

RESUMO

The inhibitory roles of hydroxylamine (NH2OH) and hydrazine (N2H4) on nitrite-oxidizing bacteria were investigated in a comparative study. The results showed that nitrite accumulation was achieved by adding 5 mg-N/L NH2OH or N2H4 to two parallel sequencing batch reactors, with nitrite accumulation rate reaching 95.83% and 86.58% within 15 days after adopting aeration time control, respectively. Correspondingly, the maximum level of NO in typical cycles caused by NH2OH addition was 0.18 mg-N/L, which was higher than obtained for N2H4. NH2OH or N2H4 showed strong inhibition on Nitrospira and promoted the enrichment of Nitrosomonas, with the effects of NH2OH being more significant. However, nitritation began to deteriorate after the cessation of inhibitors addition. In conclusion, NH2OH was a better inhibitor than N2H4 for Nitrospira. The inhibitory role of NH2OH was primarily related to NO toxicity, while for N2H4 it was attributed to its own toxicity, with NO playing a smaller role.


Assuntos
Nitrificação , Nitritos , Amônia , Bactérias , Reatores Biológicos/microbiologia , Hidrazinas , Hidroxilamina/farmacologia , Hidroxilaminas , Oxirredução
20.
J Colloid Interface Sci ; 606(Pt 1): 577-587, 2022 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-34416452

RESUMO

Advanced anode materials with high theoretical capacity and rate capability are urgently required for next generation lithium ion batteries (LIBs). In this study, hierarchical N, P codoped porous 3D-carbon framework@TiO2 nanoparticle hybrid (N, PC@TiO2) is synthesized by using pollen as biomass precursor through a facile template assisted sol-gel methode and exhibits hierarchical porous hollow structure with plenty of redox active sites and enhanced specific surface area. Compared with N, P codoped porous micro-carbon sphere framework and TiO2 porous hollow microspheres anodes, the N, PC@TiO2 anode shows superior reversible capacity of 687.3 mAh g-1 at 0.1 A g-1 after 200 cycles and 440.5 mAh g-1 after 1000 cycles at 1 A g-1. The excellent performance can be attributed to the rational hierarchical porous hollow structure and the synergetic contributions from the N, P codoped-carbon and TiO2 components, which enhance Li+ storage capability, accelerate the reaction kinetics and stabilize the electrode structure and interface during charge/discharge process. This study suggests a practical strategy to prepare novel anode material with abundant natural resource and facile synthetic route, and the optimized hybrid anode with outstanding Li+ storage properties provides hopeful application prospect in advanced LIBs and other energy storage devices.

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