Unique Octupolar 2D-Polymer Frameworks as Mixed Conductors and Metal-Free Catalysts for Dual-Promoted Li and S Electrochemistry: Multi-regulation Role of Ethoxylation Chemistry

Here, we for the first time introduce ethoxylation chemistry to develop a new octupolar cyano-vinylene-linked 2D polymer framework (Cyano-OCF-EO) capable of acting as efficient mixed electron/ion conductors and metal-free sulfur evolution catalysts for dual-promoted Li and S electrochemistry. Our strategy creates a unique interconnected network of strongly-coupled donor 3-(acceptor-core) octupoles in Cyano-OCF-EO, affording enhanced intramolecular charge transfer, substantial active sites and crowded open channels. This enables Cyano-OCF-EO as a new versatile separator modifier, which endows the modified separator with superior catalytic activity for sulfur conversion and rapid Li ion conduction with the high Li⁺ transference number up to 0.94. Thus, the incorporation of Cyano-OCF-EO can concurrently regulate sulfur redox reactions and Li-ion flux in Li−S cells, attaining boosted bidirectional redox kinetics, inhibited polysulfide shuttle and dendrite-free Li anodes. The Cyano-OCF-EO-involved Li−S cell is endowed with excellent overall electrochemical performance especially large areal capacity of 7.5 mAh cm⁻² at high sulfur loading of 8.7 mg cm⁻². Mechanistic studies unveil the dominant multi-promoting effect of the triethoxylation on electron and ion conduction, polysulfide adsorption and catalytic conversion as well as previously-unexplored −CN/C−O dual-site synergistic effect for enhanced polysulfide adsorption and reduced energy barrier toward Li₂S conversion.     

Non-Interacting Ni and Fe Dual-Atom Pair Sites in N-Doped Carbon Catalysts for Efficient Concentrating Solar-Driven Photothermal CO2 Reduction

Solar-to-chemical energy conversion under weak solar irradiation is generally difficult to meet the heat demand of CO₂ reduction. Herein, a new concentrated solar-driven photothermal system coupling a dual-metal single-atom catalyst (DSAC) with adjacent Ni−N₄ and Fe−N₄ pair sites is designed for boosting gas-solid CO₂ reduction with H₂O under simulated solar irradiation, even under ambient sunlight. As expected, the (Ni, Fe)−N−C DSAC exhibits a superior photothermal catalytic performance for CO₂ reduction to CO (86.16 μmol g⁻¹ h⁻¹), CH₄ (135.35 μmol g⁻¹ h⁻¹) and CH₃OH (59.81 μmol g⁻¹ h⁻¹), which are equivalent to 1.70-fold, 1.27-fold and 1.23-fold higher than those of the Fe−N−C catalyst, respectively. Based on theoretical simulations, the Fermi level and d-band center of Fe atom is efficiently regulated in non-interacting Ni and Fe dual-atom pair sites with electronic interaction through electron orbital hybridization on (Ni, Fe)−N−C DSAC. Crucially, the distance between adjacent Ni and Fe atoms of the Ni−N−N−Fe configuration means that the additional Ni atom as a new active site contributes to the main *COOH and *HCO₃ dissociation to optimize the corresponding energy barriers in the reaction process, leading to specific dual reaction pathways (COOH and HCO₃ pathways) for solar-driven photothermal CO₂ reduction to initial CO production.     

An Injectable Integration of Autologous Bioactive Concentrated Growth Factor and Gelatin Methacrylate Hydrogel with Efficient Growth Factor Release and 3D Spatial Structure for Accelerated Wound Healing

Growth factors are essential for wound healing owing to their multiple reparative effects. Concentrated growth factor (CGF) is a third-generation platelet extract containing various endogenous growth factors. Herein, a CGF extract solution is combined with gelatin methacrylate (GM) by physical blending to produce GM@CGF hydrogels for wound repair. The GM@CGF hydrogels show no immune rejection during autologous transplantation. Compared to CGF, GM@CGF hydrogels not only exhibit excellent plasticity and adhesivity but also prevent rapid release and degradation of growth factors. The GM@CGF hydrogels display good injectability, self-healing, swelling, and degradability along with outstanding cytocompatibility, angiogenic functions, chemotactic functions, and cell migration-promoting capabilities in vitro. The GM@CGF hydrogel can release various effective molecules to rapidly initiate wound repair, stimulate the expressions of type I collagen, transform growth factor β1, epidermal growth factor, and vascular endothelial growth factor, promote the production of granulation tissues, vascular regeneration and reconstruction, collagen deposition, and epidermal cell migration, as well as prevent excessive scar formation. In conclusion, the injectable GM@CGF hydrogel can release various growth factors and provide a 3D spatial structure to accelerate wound repair, thereby providing a foundation for the clinical application and translation of CGF.     

病原微生物感染的蛋白质组学研究

基于质谱的蛋白质组学在近20年有巨大的发展。在其应用中,病原微生物和与感染相关的蛋白质组学具有重要科学意义,体系复杂度又相对较小,一直受到广泛关注并有较快发展。本文从感染中病原微生物和宿主的蛋白质组学两方面入手,简要综述应用蛋白质组学研究感染过程的相关工作,着重介绍该领域近几年的主要进展,并对其发展做出展望。     

均四嗪衍生物结构、生成焓及爆轰性能的理论研究

运用DFT-w B97/6-31+G**方法对23种1,2,4,5-四嗪衍生物的几何结构、自然键轨道(NBO)和生成焓(EOF)进行研究,并在此基础上运用Kamlet-Jacobs方程估算衍生物的爆轰性能,得到其爆速在6.69~9.37 km/s之间;基于统计热力学,求得部分标题化合物在200~800 K温度范围内的热力学性质,随温度T升高,热容Cp、熵Sm及焓Hm逐渐增大。根据最小键级理论,C-R(取代基)键和N-R键可能是1,2,4,5-四嗪衍生物高温裂解的热引发键。综合分析,基团-NO2、-N3和-N=N-有助于提高四嗪衍生物的生成焓和爆轰性能,3,6-二硝基-1,2,4,5-四嗪和3,6-二偶氮基-二硝基-1,2,4,5-四嗪从能量、爆轰性能上可以作为高能量密度材料候选物。     

Improving the luminous efficiency of quantum dot-converted LEDs by doping boron nitride nanoparticles

Optical Review - Quantum dot-converted LEDs (QCLEDs) are a new type of LED device. However, the low luminous efficiency of the QCLED cannot meet the requirements for practical applications. In this...     

新型吡唑肟衍生物的设计、合成与杀虫活性研究

为寻找高效与低毒的吡唑肟活性物质,设计合成了9个未见文献报道的新型吡唑肟化合物,通过¹H NMR、¹³C NMR及元素分析等方法确证了其目标物的结构。初步生物活性测试数据显示,在500µg/mL浓度下,目标化合物6a~6i对粘虫均有较好的杀虫效果,其杀死率均为100%,与对照药啶虫丙醚的防效相当,值得进一步深入研究。     

ZIF-derived mesoporous carbon materials prepared by activation via Na2SiO3 for supercapacitor

Metal organic frameworks (MOFs) derived carbonaceous materials have a wide range of applications in the fields of energy storage, catalysis, adsorption and separation, etc. Especially, zeolitic imidazolate framework-8 (ZIF-8) is an excellent candidate to synthesize porous carbon due to the large surface area and high nitrogen content. However, the dominated microporous structure of ZIF-8-derived carbon significantly hinders ionic mass transfer, limiting the improvement of performance. Herein, MOF-derived mesoporous carbon was prepared using ZIF-8 as carbon precursor and cheap sodium silicate (Na₂SiO₃) as activator. The introduction of Na₂SiO₃ created rich mesoporous structure and increased specific surface area, as well as the effects of pyrolysis temperature and Na₂SiO₃ dosage on performance was also investigated. The obtained ZIF-derived porous carbon exhibits good electrochemical performance with specific capacitance of 263 F/g at 1 A/g and excellent cycle life (96.07% after 10,000 GCD cycles) in supercapacitor. The use of cheap Na₂SiO₃ activator provides a new orientation for the preparation of MOF-derived carbons with rich pores, high surface area, and facilitates the large-scale application of MOF-derived carbons.     

Built-in piezoelectric field improved photocatalytic performance of nanoflower-like Bi2WO6 using low-power white LEDs

Photocatalysis technology has been proved to be a potential strategy for removal of organic dyes, however high-power light sources are generally necessary to initiate photocatalytic reaction. In this work, we employed an excellent photocatalyst of Bi₂WO₆ with visible light harvest and meanwhile an intrinsic ferroelectricity, which realized the efficient degradation of organic dye via the synergetic photopiezocatalysis. Through coupling the illumination by a low-power (9 W) LED and the ultrasonic vibration (120 W) by an ultrasonic cleaner, the nanoflower-like Bi₂WO₆ composed of ultrathin nanosheets showed a much more enhanced photopiezocatalysis performance for purification of organic dye than the individual photocatalysis and piezocatalysis. Furthermore, the high mineralization efficiency and the good durability of the Bi₂WO₆ catalyst were demonstrated. The possible mechanism of photopiezocatalysis was finally proposed, where the ultrasound-induced piezoelectric field in Bi₂WO₆ drove photo-generated electrons and holes to diffuse along opposite directions, consequently promoting the separation efficiency of charge carriers. This work indicates that the synergetic photopiezocatalysis by coupling irradiation and ultrasonic vibration is a promising strategy to purify organic pollutants in wastewater.