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1.
J Colloid Interface Sci ; 659: 799-810, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38218084

RESUMO

The catalytic activity improvement of Fe-based active sites derived from metal organic frameworks toward oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) remains a major challenge. In this study, the growth of strontium decorated 2-methylimidazole zinc salt (Sr/ZIF-8) is prepared as a carrier to vapor deposited iron formation Sr doped Fe-based nitrogen-doped carbon framework (named as Sr/FeNC). After high-temperature pyrolysis and vapor deposition, strontium carbonate nanocrystals are evenly dispersed on the shrunk dodecahedron carbon frame and multitudinous Fe-based active catalytic sites are embedded in carbon skeleton. The optimal Sr/FeNC-2 catalyst demonstrates the outstanding ORR performance in terms of a half-wave potential of 0.851 V and an onset potential of 0.90 V, while Sr/FeNC-2 exhibits a high current density of 18.2 mA cm-2 and a lower Tafel slope of 21 mV dec-1 in MOR. The exceptional catalytic activity could be ascribed to the synergistic coupling effect of strontium compounds with Fe-based catalytic sites (Fe-Nx, Fe, and iron oxide). In particular, the formation of SrCO3 affects the bonding configuration of the iron species sites, leading to an optimization of the electronic structure within the multihole carbon matrix. The synthetic approach presents a prospective strategy for future endeavors in developing innovative and advanced bifunctional catalysts for ORR and MOR.

2.
J Colloid Interface Sci ; 624: 88-99, 2022 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-35660914

RESUMO

Designing highly efficient, long-lasting, and cost-effective cathodic and anodic functional materials as a bifunctional electrocatalyst is essential for overcoming the bottleneck in fuel cell development. Herein, a novel two-step synthesis strategy is developed to synthesize metal-organic framework (MOF) derived nitrogen-doped carbon (NC) with improved spatial isolation and a higher loading amount of cobalt (Co) and nickel carbide (Ni3C) nanocrystal decorated on graphene (denoted as Co@NC-Ni3C/G). Benefiting from multiple active sites of high N-doping level, uniform dispersion of Co and Ni3C nanocrystals, and a large active area of graphene, the Co@NC-Ni3C/G hybrids exhibit excellent methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR) efficiency in an alkaline environment. For MOR, the optimized Co@NC-Ni3C/G-350 catalyst achieved a current density of 44.8 mA cm-2 at an applied potential of 1.47 V (V vs. RHE), which is significantly higher than Co@NC-Ni3C (42.07 mA cm-2) and Co@NC (24.1 mA cm-2) in 0.5 M methanol + 1.0 M KOH solutions. In addition, during the CO retention test, the Co@NC-Ni3C/G-350 catalyst exhibits excellent CO tolerance capacity. Excitingly, the as-prepared Co@NC-Ni3C/G-350 hybrid exhibits significantly improved ORR catalytic efficiency in terms of positive onset and half-wave potential (Eonset = 0.90 V, E1/2 = 0.830 V vs. RHE), small Tafel slope (34 mV dec-1) and excellent durability (only reduced 0.016 V after 5000 s test). This work provides new insights into MOF-derived functional nanomaterials for anode and cathode co-catalysts for methanol fuel cells.

3.
J Colloid Interface Sci ; 590: 164-174, 2021 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-33548600

RESUMO

Interaction of multi-active components can effectively maximize the overall catalytic ability of alcohol fuel cells. Herein, the self-assembled nitrogen doped carbon nanotubes (NCNTs) containing Co-MnO composite (Co-MnO/NCNTs) are successfully synthesized using dihydrodiamine as carbon and nitrogen source through one-step synthesis. In order to further improve the catalytic activity of Co-MnO/NCNTs for alcohol oxidation, small amounts of platinum quantum dots are uniformly loaded on Co-MnO/NCNTs formation of quaternary hybrid (named Pt/Co-MnO/NCNTs) during microwave reduction stage. Notably, the prepared Pt/Co-MnO/NCNTs hybrids possess the excellent methanol and ethanol oxidation mass current density of 1775.4 and 1112.8 mA mg-1 in alkaline condition, which are 3.6 and 2.25 times higher than that of Pt/C catalysts, respectively. The current density of ethanol catalytic oxidation is lower than that of methanol, which may be due to the partial oxidation of acetyl (the intermediate product of ethanol) on the Pt (1 1 1) crystal surface. More importantly, CO oxidation experiments reveal that strong electronic synergistic effect between MnO and Pt quantum dot can greatly improve the CO anti-poisoning ability. Another significant advantage of Pt/Co-MnO/NCNTs is that low platinum loading leads to low cost effective, which demonstrates that the modification non-noble metal catalysts with a few noble metals quantum dots is a promising choice to mass produce high performance catalyst with remarkably boosting electrocatalytic activity for alcohol oxidation.

4.
Bioorg Med Chem Lett ; 29(15): 1943-1947, 2019 08 01.
Artigo em Inglês | MEDLINE | ID: mdl-31130266

RESUMO

The G-quadruplex aptamer is a high-order structure formed by folding of guanine-rich DNA or RNA. The recognition and assembly of G-quadruplex and compounds are important to find biocompatible drugs. Herein, triphenylamine conjugated 4, 4-difluoro-4-bora-3a, 4a-diaza-s-indacene (BODIPY) compound (BPTPA) was synthesized, and the interaction of BPTPA with G4 DNA was studied. It is found that BPTPA selectively binds with G3T3 G4 DNA forming a water-compatible nanocomplex (BPTPA-G3T3). BPTPA-G3T3 can image mitochondria and inhibit the expression of TrxR2. Cytotoxicity results indicate BPTPA-G3T3 can decrease the membrane potential of mitochondria and inhibit the proliferation of BGC-823 cancer cells. Therefore, BPTPA-G3T3 can be the biocompatible attenuator of mitochondria for cancer image and chemotherapy.


Assuntos
Quadruplex G , Mitocôndrias/metabolismo , Humanos , Estrutura Molecular
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