RESUMO
Fabricating high-efficiency catalysts of Pt nanoparticles coupled with single-atom sites (MNC) attracts intensive attention to accelerate the oxygen reduction reaction (ORR). Here we rationally design the low-Pt hybrid catalyst containing fine Pt nanoparticles coupled with Co-Nx moieties via a microwave-assisted heating process. The well-dispersed Pt nanoparticles are anchored by CoNC supports because of the metal-support interaction. Furthermore, the Co-Nx moiety acts as an electron donor to regulate the electronic structure of Pt through the electron synergistic effect, moderating the adsorption energy of oxygen intermediates on Pt sites, and then increasing the intrinsic activity of Pt. In addition, the overflow effect from CoNC to Pt facilitates a nearly four-electron process and enhances the kinetics of ORR. In acid media, the optimized 10% Pt/CoNC hybrid catalysts with Pt nanoparticles size (2.18 nm) exhibit improved ORR activity and robust durability, delivering a half-wave potential (E1/2) of 0.886 V and negligible loss after accelerated durability test, exceeding the best-in-class commercial Pt/C. The finding of the synergy between CoNC supports and Pt nanoparticles offers a novel ideation to construct various low-loading Pt-based hybrid catalysts.
Assuntos
Nanopartículas , Oxigênio , Catálise , Domínio CatalíticoRESUMO
The ß-defensins are important components of the vertebrate innate immune system. While mammalian ß-defensins have wide-ranging antibacterial and immunomodulatory activities, those of amphibians remain largely uncharacterised. In this study, ß-defensin cDNA was identified from the skin transcriptome of the Chinese spiny frog Quasipaa spinosa. This ß-defensin (QS-BD) consists of a signal and a mature peptide. Sequence alignments with other amphibian ß-defensins showed conservation of the functional mature peptide and that its closest relative is ß-defensin from Zhangixalus puerensis. Synthetic QS-BD showed antibacterial activity against Vibrio vulnificus, Vibrio harveyi, Streptococcus iniae, and Aeromonas hydrophila. QS-BD showed bactericidal activity by destroying the cell membrane integrity, but did not hydrolyse genomic DNA. QS-BD treatment promoted respiratory bursts and upregulated the expression of interleukin-1ß and tumour necrosis factor-α in the murine leukemic monocyte/macrophage cell line RAW264.7. This is the first demonstration of immunomodulatory activity by an amphibian ß-defensin.
Assuntos
beta-Defensinas , Animais , Antibacterianos/metabolismo , Anuros/metabolismo , China , Mamíferos , Camundongos , Ranidae/genética , beta-Defensinas/genética , beta-Defensinas/metabolismoRESUMO
The catalyst in the oxygen electrode is the core component of the aqueous metal-air battery, which plays a vital role in the determination of the open circuit potential, energy density, and cycle life of the battery. For rechargeable aqueous metal-air batteries, the catalyst should have both good oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalytic performance. Compared with precious metal catalysts, non-precious metal materials have more advantages in terms of abundant resource reserves and low prices. Over the past few years, great efforts have been made in the development of non-precious metal bifunctional catalysts. This review selectively evaluates the advantages, disadvantages and development status of recent advanced materials including pure carbon materials, carbon-based metal materials and carbon-free materials as bifunctional oxygen catalysts. Preliminary improvement strategies are formulated to make up for the deficiency of each material. The development prospects and challenges facing bifunctional catalysts in the future are also discussed.
RESUMO
Tri-and hexavalent chromium have different chemical properties, and their levels of toxicity to plants are different. However, there is no limit set by the soil environmental quality risk control standard for Cr(â ¢) or Cr(â ¥). Therefore, studying the ecological toxicity of Cr has important implications for protecting the environment. Based on the dynamics of the Cr(â ¢) and Cr(â ¥) levels in soil solution collected from eight soils, the toxicity thresholds of the two Cr forms to barley roots were investigated through model calculation and correlation analysis under different soil properties. The results showed that both Cr forms and the soil properties had significant effects on the root length of barley. The effective concentrations of Cr(â ¢) added to the soils that led to 10% inhibition (EC10), 50% inhibition (EC50), and no-observed-effect concentrations (NOEC) were significantly higher than those of Cr(â ¥). The EC50 of Cr(â ¢) ranged from 298.8 to 2014.1 mg·kg-1 (6.7-fold variation); the EC50 of Cr(â ¥) ranged from 8.0 to 126.6 mg·kg-1 (15.8-fold variation). Under the same soil conditions, the EC50 of Cr(â ¢) was 2.8 to 101.7 times higher than that of Cr(â ¥), suggesting the higher phytotoxicity of Cr(â ¥) than Cr(â ¢). Correlation analysis showed that the pH and soil organic matter were the main factors that influenced the Cr toxicity thresholds, as indicated by the root length of barley. The concentration of chromium in the soil solution was below the detection limit of the TAS-990 when Cr(â ¢) was applied at 1280 mg·kg-1 (or less) to soils, whereas for Cr(â ¥), the level was 40 mg·kg-1 (or less). Cr(â ¢) adsorption to the soil was significantly stronger than that of Cr(â ¥). The toxicity of Cr(â ¥) was significantly higher than that of Cr(â ¢), which was also influenced by soil properties.
Assuntos
Poluentes do Solo/análise , Solo , Cromo , Hordeum , Raízes de Plantas/químicaRESUMO
Non-noble metal materials are regarded as the most promising catalysts for the oxygen reduction reaction (ORR) to overcome the inherent defects of Pt-based catalysts, like high cost, limited availability and insufficient stability. Here, we fabricate sandwich-like Co encapsulated nitrogen doped carbon polyhedron/graphene (s-Co@NCP/rGO) via a facile and scalable strategy by loading Co-based zeolitic imidazolate framework (ZIF-67) and graphene oxide (GO) layers individually on a polyurethane (PU) sponge template. The 3D sandwich structure is maintained with the assistance of the sponge template, which promotes the uniform dispersion of ZIF-67-derived Co embedded nitrogen doped carbon polyhedra (Co@NCP) and prevents the graphene plates from agglomerating during the annealing process. The final product demonstrates considerable catalytic performance for the ORR with a half-wave potential of 0.85 V, preferable stability and increased poisoning tolerance by comparison to 20 wt% Pt/C, which stems from the 3D sandwich-like structure, N/Co-doping effect, large accessible surface area and hierarchical porous structures. The excellent ORR performance of the catalysts means that they can be utilised in a Zn-air battery as cathode catalysts. During such a demonstration, s-Co@NCP/rGO shows a high open-circuit voltage of 1.466 V, remarkable long-term durability and an outstanding peak power density of 186 mV cm-2, which shows its high potential as a prospective alternative for widespread practical application in the field of non-noble metal ORR catalysts.
RESUMO
The oxygen reduction reaction (ORR) in a cathode is an essential component of many electrochemical energy storage and conversion systems. Two-dimensional materials are beneficial for electron conduction and mass transport with high density, showing prominent electrochemical catalytic performance towards the ORR. Herein, a simple NaCl-assisted method to synthesize cobalt-nitrogen-doped carbon materials (CoNC), which present prominent performance towards the ORR in alkaline media, is described. The utilization of the NaCl template endows the product with a large specific surface area of 556.4â m2 g-1 , as well as good dispersion of cobalt nanoparticles. CoNC-800@NaCl (800 indicates the calcination temperature in °C) displays an excellent onset potential of 0.94â V (vs. a reversible hydrogen electrode), which is close to that of commercial Pt/C. Additionally, CoNC-800@NaCl also exhibits better long-term durability and methanol tolerance than that of Pt/C. The high-performance CoNC-800@NaCl catalyst provides a hopeful alternative to noble-metal catalysts for the ORR in practical applications.
RESUMO
A batch sorption study was carried out to investigate the sorption behaviors of DDT onto JiaoZhou Bay sediment in the presence of an anionic surfactant sodium dodecylbenzene sulfonate (SDBS), and a cationic surfactant, cetyltrimethylammonium bromide (CTAB) with low concentrations. The results indicated that the sorption process followed the pseudo-second-order model and the sorption systems could be well described by the Freundlich type. Within the investigated concentrations of CTAB and SDBS, both SDBS and CTAB increased the sorption of DDT to sediment. The sorption rate and capacity increased with increasing SDBS and CTAB concentrations, and CTAB showed a significant impact. Take p ,p'-DDT as an example, the sorption rate constant increased from 1.232 x 10(-2) g x (microg x min)(-1) to 4.193 x 10(-2) g x (microg x min)(-1) and the Freundlich coefficient increased from 2.866 (microg x g(-1)) (L x microg(-1))(1/n) to 7.932 (microg x g(-1)) (L x microg(-1))(1/n) when the SDBS concentration was 10 mg x L(-1). The influence of temperature on sorption of DDT in the presence of SDBS was also studied. Within the temperature range of 283-308 K, lower temperature had a positive effect on the sorption. The thermodynamic parameters showed that the sorption was spontaneous and exothermic, and the randomness was increased during the process. Furthermore, the presence of SDBS caused lower deltaG0, deltaH0 and deltaS0 values. This study provided theoretical foundation for migration, transformation and fate of DDT in Jiaozhou Bay sediment.