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1.
Nano Lett ; 22(12): 4879-4887, 2022 Jun 22.
Artículo en Inglés | MEDLINE | ID: mdl-35640090

RESUMEN

Preparing advanced electrocatalysts via solid-phase reactions encounters the challenge of low controllability for multiconstituent hybridization and microstructure modulation. Herein, a hydrothermal-mimicking solid-phase system is established to fabricate novel Fe2O3/Fe5C2/Fe-N-C composites consisting of Fe2O3/Fe5C2 nanoparticles and Fe,N-doped carbon species with varying morphologies. The evolution mechanism featuring a competitive growth of different carbon sources in a closed hypoxic space is elucidated for a series of Fe2O3/Fe5C2/Fe-N-C composites. The size and dispersity of Fe2O3/Fe5C2 nanoparticles, the graphitization degree of the carbonaceous matrix, and their diverse hybridization states lead to disparate electrocatalytic behaviors for the oxygen reduction reaction (ORR). Among them, microspherical Fe2O3/Fe5C2/Fe-N-C-3 exhibits an optimal ORR performance and the as-assembled zinc-air battery shows all-round superiority to the Pt/C counterpart. This work presents a mild solid-phase fabrication technique for obtaining a variety of nanocomposites with effective control over composition hybridization and microstructural modulation, which is significantly important for the design and optimization of advanced electrocatalysts.

2.
Angew Chem Int Ed Engl ; 62(49): e202314124, 2023 Dec 04.
Artículo en Inglés | MEDLINE | ID: mdl-37872117

RESUMEN

Constructing atom-clusters (ACs) with in situ modulation of coordination environment and simultaneously hollowing carbon support are critical yet challenging for improving electrocatalytic efficiency of atomically dispersed catalysts (ADCs). Herein, a general diffusion-controlled strategy based on spatial confining and Kirkendall effect is proposed to construct metallic ACs in N,P,S triply-doped hollow carbon matrix (MACs /NPS-HC, M=Mn, Fe, Co, Ni, Cu). Thereinto, FeACs /NPS-HC with the best catalytic activity for oxygen reduction reaction (ORR) is thoroughly investigated. Unlike the benchmark sample of symmetrical N-surrounded iron single-atoms in N-doped carbon (FeSAs /N-C), FeACs /NPS-HC comprises bi-/tri-atomic Fe centers with engineered S/N coordination. Theoretical calculation reveals that proper Fe gathering and coordination modulation could mildly delocalize the electron distribution and optimize the free energy pathways of ORR. In addition, the triple doping and hollow structure of carbon matrix could further regulate the local environment and allow sufficient exposure of active sites, resulting in more enhanced ORR kinetics on FeACs /NPS-HC. The zinc-air battery assembled with FeACs /NPS-HC as cathodic catalyst exhibits all-round superiority to Pt/C and most Fe-based ADCs. This work provides an exemplary method for establishing atomic-cluster catalysts with engineered S-dominated coordination and hollowed carbon matrix, which paves a new avenue for the fabrication and optimization of advanced ADCs.

3.
Chembiochem ; 22(1): 124-128, 2021 01 05.
Artículo en Inglés | MEDLINE | ID: mdl-32789939

RESUMEN

Optically active ß-amino alcohols are very useful chiral intermediates frequently used in the preparation of pharmaceutically active substances. Here, a novel cyclohexylamine oxidase (ArCHAO) was identified from the genome sequence of Arthrobacter sp. TYUT010-15 with the R-stereoselective deamination activity of ß-amino alcohol. ArCHAO was cloned and successfully expressed in E. coli BL21, purified and characterized. Substrate-specific analysis revealed that ArCHAO has high activity (4.15 to 6.34 U mg-1 protein) and excellent enantioselectivity toward the tested ß-amino alcohols. By using purified ArCHAO, a wide range of racemic ß-amino alcohols were resolved, (S)-ß-amino alcohols were obtained in >99 % ee. Deracemization of racemic ß-amino alcohols was conducted by ArCHAO-catalyzed enantioselective deamination and transaminase-catalyzed enantioselective amination to afford (S)-ß-amino alcohols in excellent conversion (78-94 %) and enantiomeric excess (>99 %). Preparative-scale deracemization was carried out with 50 mM (6.859 g L-1 ) racemic 2-amino-2-phenylethanol, (S)-2-amino-2-phenylethanol was obtained in 75 % isolated yield and >99 % ee.


Asunto(s)
Amino Alcoholes/metabolismo , Oxidorreductasas actuantes sobre Donantes de Grupo CH-NH/metabolismo , Transaminasas/metabolismo , Amino Alcoholes/química , Arthrobacter/enzimología , Biocatálisis , Estructura Molecular , Oxidorreductasas actuantes sobre Donantes de Grupo CH-NH/genética , Estereoisomerismo , Transaminasas/genética
4.
Cancer Sci ; 111(5): 1514-1527, 2020 May.
Artículo en Inglés | MEDLINE | ID: mdl-32030850

RESUMEN

Estrogen-related receptor-α (ERRα) is a nuclear receptor of transcription factor that binds to estrogen responsive elements and estrogen-related responsive elements. Estrogen-related receptor-α is involved in metabolic processes and implicated in the progression and growth of several human malignancies. However, the biologic role and clinical significance of ERRα in gallbladder cancer (GBC) remains to be clarified. Here, we reported that ERRα protein expression was notably higher in GBC tissues than in cholecystitis tissues, and that the aberrantly higher ERRα expression was positively correlated with advanced TNM stage and indicated dismal prognosis of GBC (P < .01). In GBC cell lines NOZ and OCUG, the targeted depletion of ERRα retarded the growth and suppressed the migration and invasive capabilities of GBC cells, and inhibited epithelial-mesenchymal transition by decreasing the expression of mesenchymal markers and elevating the expression of epithelial markers. Moreover, ERRα knockdown inhibited tumor growth in nude mice and led to decreased expression levels of Nectin-4, p-PI3K p85α, and p-AKT. Overexpression of ERRα in the GBC-SD cell line showed exactly the opposite effect. The targeted inhibition of Nectin-4 antagonized GBC cell proliferation and invasion, which were induced by ERRα upregulation. Moreover, Nectin-4 depletion inhibited the ERRα-induced activation of the PI3K/AKT pathway. Chromatin immunoprecipitation analysis and dual-luciferase reporter gene assays showed that ERRα enhanced the transcription of Nectin-4 by binding to the promoter of Nectin-4. In conclusion, our data indicated that ERRα could be a potential target for the genetic treatment of GBC.


Asunto(s)
Moléculas de Adhesión Celular/genética , Neoplasias de la Vesícula Biliar/patología , Receptores de Estrógenos/metabolismo , Transcripción Genética , Animales , Línea Celular Tumoral , Movimiento Celular , Proliferación Celular , Transformación Celular Neoplásica , Transición Epitelial-Mesenquimal/genética , Femenino , Neoplasias de la Vesícula Biliar/genética , Neoplasias de la Vesícula Biliar/metabolismo , Neoplasias de la Vesícula Biliar/mortalidad , Expresión Génica , Regulación Neoplásica de la Expresión Génica , Humanos , Masculino , Ratones , Ratones Desnudos , Persona de Mediana Edad , Fosfatidilinositol 3-Quinasas/metabolismo , Pronóstico , Proteínas Proto-Oncogénicas c-akt/metabolismo , Receptores de Estrógenos/genética , Transducción de Señal , Receptor Relacionado con Estrógeno ERRalfa
5.
Biotechnol Lett ; 42(8): 1501-1511, 2020 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-32219689

RESUMEN

OBJECTIVES: To screening of bacteria with cyclic amino alcohol deamination activity for enantioselective synthesis of chiral cyclic ß-amino alcohols. RESULTS: A new strain named Arthrobacter sp. TYUT010-15 with the (R)-selective deamination activity of cyclic ß-amino alcohol has been isolated from nature via a high throughput solid-phase screening method. The reaction conditions of TYUT010-15 were optimized. Using the resting cell of TYUT010-15 as the catalyst, kinetic resolution of trans-2-aminocyclopentanol, trans-2-aminocyclohexanol and cis-1-amino-2-indanol was carried out to afford (1S, 2S)-trans-2-aminocyclopentanol, (1S, 2S)-trans-2-aminocyclohexanol and (1R, 2S)-cis-1-amino-2-indanol in > 99% ee and 49.6-50% conversion. Four aromatic ß-amino alcohols and two amines were also resolved, (S)-ß-amino alcohols and (R)-amines were obtained in > 99% ee. Preparation experiment was conducted with 200 mM (23.2 g L-1) racemic trans-2-aminocyclohexanol, yielding the desired (1S, 2S)-trans-2-aminocyclohexanol in 40% isolated yield, > 99% ee and 5.8 g L-1 d-1 space time yields. CONCLUSIONS: This study provides a high throughput solid-phase method for screening of bacteria with cyclic amino alcohol deamination activity and a first example for practical preparation of chiral cyclic ß-amino alcohol by Arthrobacter sp. TYUT010-15.


Asunto(s)
Amino Alcoholes , Bacterias/metabolismo , Ensayos Analíticos de Alto Rendimiento/métodos , Aminas/análisis , Aminas/química , Aminas/metabolismo , Amino Alcoholes/análisis , Amino Alcoholes/química , Amino Alcoholes/metabolismo , Arthrobacter/genética , Arthrobacter/metabolismo , Bacterias/genética , Colorimetría , Desaminación , Cinética , Estereoisomerismo , Especificidad por Sustrato
6.
Small ; 15(8): e1804855, 2019 02.
Artículo en Inglés | MEDLINE | ID: mdl-30632276

RESUMEN

Natural chloroplasts containing big amounts of chlorophylls (magnesium porphyrin, Mg-Chl) are employed both as template and porphyrin source to synthesize biomorphic CoNC/CoOx composite as electrocatalyst for the oxygen reduction reaction (ORR). Cobalt-substituted chlorophyll derivative (Co-Chl) in chloroplasts is first obtained by successively rinsing in hydrochloric acid and cobalt acetate solutions. After calcining in nitrogen to 800 °C, Co-Chl is transferred to CoNC; while other parts of chloroplasts adsorbed with Co ions are transferred to CoOx retaining the microarchitecture of chloroplasts. The abundant active CoNC sites are protected by circumjacent biocarbon and CoOx to avoid leakage and agglomeration, and at the same time can overcome the poor conductivity weakness of CoOx by directly transporting electrons to the carbonaceous skeleton. This unique synergistic effect, together with efficient bioarchitecture, leads to good electrocatalytical performance for the ORR. The onset and half-wave potentials are 0.89 and 0.82 V versus reversible hydrogen electrode, respectively, with better durability and methanol tolerance than that of commercial Pt/C. Different from the traditional concept of biomorphic materials which simply utilize bioarchitectures, this work provides a new example of coupling bioderivative components with bioarchitectures into one integrated system to achieve good comprehensive performance for electrocatalysts.

7.
J Nanosci Nanotechnol ; 19(9): 5871-5877, 2019 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-30961752

RESUMEN

MnO2/C composite with ordered submicron pore array structure was obtained by using Atrophaneura horishana butterfly wings as template and carbon source for high performance supercapacitor electrode. Micro/nanostructured carbon substrate was firstly constructed by calcining the wing specimen under nitrogen atmosphere. Then, amorphous MnO2 was formed on the structure via surface solution reaction. The as-prepared composite shows a high specific capacitance of 1342 F g-1 at 1 A g-1 with good rate capability and stability. The excellent charge-discharge performance should be attributed to the coupling effect of pseudocapacitive amorphous MnO2 and robust porous carbon. The pore array structured substrate not only provides high specific surface area for sufficient active sites, but also exhibits good connectivity for efficient charge and mass transport.

8.
Arch Environ Contam Toxicol ; 67(1): 78-86, 2014 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-24823680

RESUMEN

Numerous studies have reported polychlorinated biphenyl (PCB) concentrations in soil, root, and aerial parts of vegetables. However, few studies have measured the contribution of PCBs bound to particles in air in relation to uptake by vegetables. In the present study, PCB concentrations were measured in five types of vegetables, soil, and settled air particle samples from two sites (at a domestic waste incinerator and at 20 km away from the incinerator) in Guangzhou, South China. ∑PCB concentrations in rhizosphere soil samples from the two sites ranged from 17.2-77.7 to 5.48-25.57 ng/g, respectively. ∑PCB concentrations in aerial parts of vegetables were greater than those in rhizosphere soils and roots with median values of 108 and 47.08 ng/g, respectively. Among the five types of vegetables studied, the highest concentration of PCBs was found in bitter lettuce. No significant correlation between PCBs in soil and roots or aerial parts of vegetables was observed. However, principal component analysis indicated that settled air particles were the dominant source of PCBs in the aerial parts of vegetables. In addition, similar PCB congener profiles were found in the aerial parts of vegetables and settled air particles. This suggests that foliar uptake of PCBs is an important pathway. Risk assessment indicated that human exposure to PCBs by way of dietary intake of vegetables from incinerator sites would result in high risk.


Asunto(s)
Incineración , Bifenilos Policlorados/análisis , Contaminantes del Suelo/análisis , Verduras/química , Instalaciones de Eliminación de Residuos , China , Monitoreo del Ambiente , Medición de Riesgo
9.
ACS Appl Mater Interfaces ; 16(13): 16399-16407, 2024 Apr 03.
Artículo en Inglés | MEDLINE | ID: mdl-38527861

RESUMEN

Composition screening and structure optimization are two critical factors in improving the electrocatalytic performance of hybrid materials. Herein, we present a straightforward hydrothermal hydrolyzation-topological transformation strategy for the synthesis of a range of Ni-Co bimetallic compounds with a hollow nanoflower structure. Among these Ni-Co compounds, Ni2P/Co2P hollow nanoflowers (HNFs) exhibit the most impressive electrocatalytic activity for the hydrogen evolution reaction (HER), necessitating only an 153 mV overpotential to achieve a current density of 10 mA cm-2 under alkaline conditions. Importantly, this performance remains stable for over 48 h, indicating exceptional durability. The exceptional catalytic performance of Ni2P/Co2P HNFs arises from the synergy between the hybrid Ni2P/Co2P components and the hollow nanoflower structure. The former provides abundant catalytic sites, while electron rearrangement at the heterointerfaces enhances the adsorption/desorption of active species and facilitates electron transfer. The latter contributes to the exposure of catalytic sites, shortening mass and charge transfer routes, and bolstering structural stability during prolonged electrocatalysis. This research offers valuable insights into the screening and optimization of advanced hybrid electrocatalysts, holding significant promise for applications in the emerging field of new energy technologies.

10.
J Colloid Interface Sci ; 670: 364-372, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-38768549

RESUMEN

Improving the conductivity of the electrocatalyst itself is essential for enhancing its performance. In this work, N, S-rich 6-thioguanine (TG) is selected as the ligand to synthesize a Fe, Ni bimetallic porous coordination polymer (PCP), which is then derived to fabricate N,S codoped carbon (NSC)-coated (Fe,Ni)9S8/Ni3S2 bridged nanowires. The (Fe,Ni)9S8/Ni3S2@NSC bridged nanowires obtained through bimetallic synergistic catalysis and self-sulfurization processes not only introduced additional electrocatalytic active sites but also significantly enhance the overall conductivity of the catalyst due to the interconnected nanowire structure. The resulting (Fe,Ni)9S8/Ni3S2@NSC demonstrates remarkable oxygen evolution reaction (OER) performance, exhibiting an overpotential as low as 252 mV at a current density of 10 mA cm-2. This work proposes a novel strategy for enhancing the overall conductivity of catalysts by growing bridged nanowires, providing valuable insights and inspiration for the design and preparation of advanced transition metal sulfide electrocatalysts.

11.
Int J Surg Pathol ; : 10668969231217632, 2024 Jan 03.
Artículo en Inglés | MEDLINE | ID: mdl-38173283

RESUMEN

Background. Pigmented microcystic chromophobe renal cell carcinoma (RCC) is a subtype of chromophobe RCC. Its distinct histopathologic features are microcystic and microtubular pattern, pigmentation, and microcalcifications. Pigmented microcystic chromophobe RCC has ultrastructure, immunophenotypic structure, and molecular results similar to chromophobe RCC. Methods. We report five tumors of pigmented microcystic chromophobe RCC. Morphological observation and immunohistochemical examination were performed, and clinical and molecular features were analyzed. Results. Microscopically, all five tumors showed brown pigmentation, microcystic, and tubular cystic structures, one tumor presented microscopic calcifications. All tumors were positive for EMA, AE1/AE3, PAX8, KRT7, KIT (CD117), claudin 7, KRT8, and E-cadherin, and three tumors expressed P504S. All tumors were negative for vimentin, CA9, KRT20, TFE3, TFEB, Melan-A, HMB45, FH, SDHB, and GATA3. Ki-67 index varied from less than 1% to 2%. In three tumors, next-generation sequencing of the 688 gene was performed, the results found gene variants with potential clinical significance such as JMJD1C, MYCL, TP53, PI3KCA, KRAS, APC, GLI1, LRRK2, and gene variants with unclear clinical significance such as NTRK1 and RAD50; All patients remained alive over a follow-up period of 8-46 months without tumor recurrence and sarcomatoid transformation. Conclusions. Pigmented microcystic chromophobe RCC has a relatively benign biological behavior, and distant metastases and sarcomatoid transformation are rare. This overview of five additional tumors of pigmented microcystic chromophobe RCC offers further insight into this special subtype of chromophobe RCC.

12.
Int J Surg Pathol ; 31(6): 1041-1047, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-36253711

RESUMEN

Introduction. Five cases of non-small cell lung carcinoma (NSCLC) with diffuse coexpression of TTF1 and p40 in the same tumor cells (hereafter referred to as TTF1/P40-NSCLC) have been reported since 2015. It was considered a new entity of NSCLC occurred in aged male smokers with poorly differentiated carcinomas and a similar molecular signature harboring a TP53 mutation. Methods. We report an extremely rare tumor of TTF1/P40-NSCLC. Morphological observation and immunohistochemical examination were performed, clinical and molecular features were summarized, and a review of the relevant literature was provided. Results. The tumor showed a solid growth pattern with patchy necrosis, and glandular and squamous pattern were not obvious. The tumor cells proliferated within the bronchial epithelium. Spreading through air spaces of tumor cells were observed. A peculiar immunohistochemical phenotype of diffuse and strong positivity for TTF1 (8G7G3/1) and p40 in the same tumor cells was detected. Additionally, the tumor cells were positive for KRT7 and KRT20, while negative for PD-L1 (22C3). Negative P53 (null) Immunohistochemistry (IHC) staining indicated mutational status and the Ki67 index was 80%. Molecular investigation was performed using whole exome sequencing, and TP53, NOTCH2, and STK11 mutations were detected. The patient remained alive over a follow-up period of 22 months without tumor recurrence or metastasis. Conclusions. We describe an unusual tumor of TTF1/P40-NSCLC harboring TP53, NOTCH2 and STK11 mutations. These gene mutations may be helpful in providing additional therapeutic possibilities. Our report offers further insight into this rare tumor.


Asunto(s)
Carcinoma de Pulmón de Células no Pequeñas , Neoplasias Pulmonares , Masculino , Humanos , Carcinoma de Pulmón de Células no Pequeñas/patología , Neoplasias Pulmonares/patología , Recurrencia Local de Neoplasia , Inmunohistoquímica , Mutación , Biomarcadores de Tumor/genética , Proteína p53 Supresora de Tumor/genética , Quinasas de la Proteína-Quinasa Activada por el AMP , Receptor Notch2/genética , Proteínas de Unión al ADN/genética , Factores de Transcripción/genética , Factores de Transcripción/metabolismo
13.
Chemosphere ; 292: 133544, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-34998848

RESUMEN

Fe-MCM-41 had been widely used as ozonation catalyst, however, the existence of large amount of hydrophilic silanol hindered its interfacial reaction with O3 and pollutants. To solve this problem, F-Fe-MCM-41 was synthesized by co-doping F and Fe into the framework of MCM-41 to replace silanol with Si-F groups through a one-step hydrothermal method. F introduced hydrophobic sites which contributed to more ibuprofen (IBP) chemisorption on the surface of F-Fe-MCM-41. Moreover, doping F also enhanced the acidity, which accelerated O3 decomposition into •OH. F-Fe-MCM-41/O3 exhibited notably activity with 96.6% IBP removal efficiency within 120 min, while only 78.5% and 80.9% in O3 alone and Fe-MCM-41/O3, respectively. Surface Lewis acid sites and metal hydroxyl groups were considered as important factors for O3 activation and •OH generation. F-Fe-MCM-41 exhibited excellent catalytic performance under acidic and alkaline conditions. Comparative experiments revealed that F doping improved the interfacial reaction, especially the interfacial electron transfer, which resulted in the high catalytic activity of F-Fe-MCM-41. F-Fe-MCM-41 possessed good stability and reusability, with only 5.7% decline for IBP removal in five successive cycles. Furthermore, the possible degradation path of IBP was proposed according to DFT calculation and GC-MS analysis.


Asunto(s)
Ozono , Contaminantes Químicos del Agua , Catálisis , Flúor , Hierro , Ácidos de Lewis , Dióxido de Silicio , Contaminantes Químicos del Agua/análisis
14.
Chem Commun (Camb) ; 57(81): 10580-10583, 2021 Oct 12.
Artículo en Inglés | MEDLINE | ID: mdl-34558580

RESUMEN

Dual-confined porous Si@c-ZIF@carbon nanofibers (Si@c-ZIF@CNFs) are fabricated that possess excellent antioxidant capacity, high surface area and abundant pores, which enhances conductivity, relieves volume expansion and facilitates electrolyte penetration during cycling. When evaluated as self-supporting anodes for lithium-ion batteries, the Si@c-ZIF@CNFs exhibit excellent cycling and rate performance.

15.
Nanoscale ; 12(7): 4374-4382, 2020 Feb 20.
Artículo en Inglés | MEDLINE | ID: mdl-32049080

RESUMEN

Streptococcus thermophilus, a Gram-positive (G+) bacterium featuring a teichoic acid-rich cell wall, has been employed as both a phosphorus source and template to synthesize a biomorphic Co2P-Co3O4/rGO/C composite as an efficient electrocatalyst for the oxygen reduction reaction (ORR). Different from the conventional method for the synthesis of phosphides, bio-derivative phosphorus vapor was emitted from the inside out, which facilitated the in situ transformation of the chemically adsorbed Co precursor on the bacteria into Co2P-Co3O4 heterogeneous nanoparticles, which featured a Co2P-rich body and Co3O4-rich surface. Besides, reduced graphene oxide (rGO) was also introduced in the synthetic process to keep Co2P-Co3O4 scattered and further promote the electron transport efficiency. All the Co2P-Co3O4 nanoparticles and rGO sheets were supported on the bacteria-derived carbon substrate with submicron-spherical morphology. The as-obtained Co2P-Co3O4/rGO/C composite exhibited excellent electrocatalytic performance for ORR with onset and half-wave potentials of 0.91 and 0.80 V vs. RHE, respectively. Furthermore, its long-term stability and methanol tolerance were better than those of commercial Pt/C. Thus, this work presents a new strategy of using an interior bio-phosphorus source to obtain heterojunction particles featuring a phosphide-rich body and oxide-rich surface, which may provide some insights for the construction of efficient heterogeneous electrocatalysts.

16.
J Nanosci Nanotechnol ; 20(5): 2728-2735, 2020 05 01.
Artículo en Inglés | MEDLINE | ID: mdl-31635608

RESUMEN

Biomass-derived porous carbons are considered as one of the most promising electrode materials for supercapacitors due to their low-cost and natural abundance. In this work, pinecone is used to fabricate biomass N, S, O-doped porous carbon via one-step carbonization process with KOH activation. By optimizing the additive amount of KOH and calcination temperature, the asprepared product shows a high specific surface area and pore volume up to 1593.8 m² g-1 and 0.8582 cm³ g-1, respectively. As an electric double-layer capacitor (EDLC) electrode, the N, S, O-doped porous carbon exhibits a high specific capacitance of 285 F g-1 at 0.5 A g-1 and good rate performance with a capacitance retention of 78.6% from 0.5 to 20 A g-1. Furthermore, the as-assembled symmetric supercapacitor with 6 mol L-1 KOH as electrolyte possesses a promising energy density of 6.34 Wh kg-1 and a power density of 250 W kg-1. Outstanding cycling stability was also demonstrated with 94.4% capacitance retention after 10,000 charge/discharge cycles at 1 A g-1.

17.
J Nanosci Nanotechnol ; 20(2): 949-956, 2020 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-31383091

RESUMEN

To improve lithium storage performances of Si anode for lithium-ion batteries, Si nanoparticles encapsulated into porous N-doped carbon (Si@PNC) was devised and prepared by metal nitrate accelerated polymer blowing process. The Si@PNC composites have large specific surface area of 221.7 m² g-1 and possess a great deal of mesopores and micropores, which are attributed to the carbonization of PVP and etching metallic nanoparticles. As anode for lithium ion battery, the initial discharge capacity of Si@PNC composites is high to 1626 mA h g-1, and the specific capacity still retains 1030 mA h g-1 after 200 cycles at 200 mA g-1. Meanwhile, remarkably improved rate capability is achieved with an excellent reversible specific capacity of 375 mA h g-1 at 5.0 A g-1. The excellent lithium storage performances benefit from the unique porous core-shell structure of Si@PNC composites, which improve electroconductivity, reduce volume dilatation and accelerate lithium ion transmission.

18.
ACS Appl Mater Interfaces ; 11(23): 21126-21136, 2019 Jun 12.
Artículo en Inglés | MEDLINE | ID: mdl-31117427

RESUMEN

This work reports a new approach for the synthesis of a zeolitic imidazolate framework (ZIF-8) composite. It employs the direct growth of the crystalline ZIF-8 on a mixed-metal oxide support TiO2-SiO2 (TSO), which mimics the porous structure of Populus nigra. Using the natural leaf as a template, the TSO support was prepared using a sol-gel method. The growth of the ZIF-8 layer on the TSO support was carried out by the seeds and second growth method. This method facilitates the homogeneous dispersion of ZIF-8 crystals at the surface of the TSO composite. The ZIF-8@TSO composite adsorbs methanol selectively, mainly due to the hierarchical porous structure of the mixed oxide support. As compared with the as-synthesized ZIF-8, a 50% methanol uptake is achieved in the ZIF-8@TSO composite, with only 25 wt % ZIF-8 loading. IAST simulations show that the ZIF-8@TSO composite has a preferential adsorption toward methanol when using an equimolar methanol-ethanol mixture. An opposite behavior is observed for the as-synthesized ZIF-8. The results show that combining MOFs and mixed-oxide supports with bioinspired structures opens opportunities for synthesizing new materials with unique and enhanced adsorption and separation properties.

19.
ACS Omega ; 4(27): 22325-22331, 2019 Dec 31.
Artículo en Inglés | MEDLINE | ID: mdl-31909315

RESUMEN

Oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are important reactions of energy storage and conversion devices. Therefore, it is highly desirable to design efficient and dual electrocatalysts for replacing the traditional noble-metal-based catalysts. Herein, we have developed a high-efficiency and low-cost MnCo2O4-rGO nanocomposite derived from bimetal-organic frameworks. For OER, MnCo2O4-rGO showed an onset potential of 1.56 V (vs reversible hydrogen electrode (RHE)) and a current density of 14.16 mA/cm2 at 1.83 V, being better than both pure MnCo2O4 and Pt/C. For ORR, MnCo2O4-rGO exhibited a half-wave potential (E 1/2) of 0.77 V (vs RHE), a current density of 3.33 mA/cm2 at 0.36 V, a high electron transfer number n (3.80), and long-term stability, being close to the performance of Pt/C. The high activity of MnCo2O4-rGO was attributed to the synergistic effect among rGO, manganese, and cobalt oxide. As a result, the resultant MnCo2O4-rGO has a great potential to be applied as a high-efficiency ORR and OER electrocatalyst.

20.
Environ Sci Pollut Res Int ; 25(6): 5514-5520, 2018 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-29218575

RESUMEN

The leaching characteristics of hazardous materials from Ni-Cd batteries immersed in four typical water samples, i.e., water with NaCl, river water, tap water, and deionized water, were investigated to evaluate the potential environmental harm of spent Ni-Cd batteries in the water surroundings. It is shown that four water surroundings all could leach hazardous materials from the Ni-Cd batteries. The water with NaCl concentration of 66.7 mg L-1 had the highest leaching ability, the hazardous materials were leached after only approximately 50 days (average time, with a standard deviation of 4.1), while less than 100 days were needed in the others. An electrochemical corrosion is considered to be the main leaching mechanism leading to battery breakage, while the dissolution-deposition process and the powder route result in the leakage and transference of nickel and cadmium materials from the electrodes. The anions, i.e., SO42- and Cl-, and dissolved oxygen in water were demonstrated to be the vital factors that influence the leaching processes. Thus, it is proposed that spent Ni-Cd batteries must be treated properly to avoid potential danger to the environment.


Asunto(s)
Cadmio/química , Suministros de Energía Eléctrica , Sustancias Peligrosas/química , Níquel/química , Contaminantes del Agua/química , Electrodos
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