摘要：MXene具有丰富的高电负性末端原子、较大的比表面积和较小的原子厚度等优点,已被用作前驱体制备多种纳米材料.然而,目前已报道的用于衍生金属有机框架(MOF)的MXene仅限于V_(2)CT_(x).因此,通过增加MXene和有机配体的种类,合理设计和合成新型MOF,并进一步深入探索其合成机理仍是目前面临的重要挑战.本文采用金属离子辅助转化策略,以二维Ti_(3)C_(2)T_(x)为前驱体,合成了具有非互穿SrSi2(srs)框架的基于儿茶酚的三维(3D)TiCu-HHTP(HHTP=2,3,6,7,10,11-六羟基三苯)MOF.该策略表现出了良好的普适性,Ti3C2和辅助Cu^(2+)离子可以扩展到V2C MXene和其他辅助金属离子Mn^(+)(M=Ni^(2+)、Co^(2+),Mn^(2+)和Zn^(2+)).转化机制包括从Ti3C2纳米片到辅助金属离子的电荷转移、Ti-C键断裂促进释放Ti^(4+)离子以及Ti^(4+)/Mn^(+)与HHTP之间的强螯合配位协同促进TiCu-HHTP的形成.独特的3D导电网络和丰富的氧化还原位点赋予了TiCu-HHTP-7/PPy复合柔性透明电极快速的离子/电子传输和可逆的法拉第反应.在0.02 mA cm^(-2)电流密度下,TiCu-HHTP/PPy透明电极的面积比电容值达到3.63 mF cm^(-2),明显高于纯PPy电极的面积电容值(1.79 mF cm^(-2)).TiCu-HHTP/PPy透明电容器在0.75μW cm^(-2)的功率密度下,能量密度为0.042μWh cm^(-2).

摘要：Natural anisotropic nanostructures occurring in several organisms have gained more and more attention because of their obvious advantages in sensitivity, stability, security, miniaturization, portability, online use, and remote monitoring. Due to the development of research on nature-inspired bionic structures and the demand for highly efficient, low-cost microfabrication techniques, an understanding of and the ability to replicate the mechanism of structural coloration have become increasingly significant. These sophisticated structures have many unique functions and are used in many applications. Many sensors have been proposed based on their novel structures and unique optical properties. Several of these bio-inspired sensors have been used for infrared radiation/thermal, pH, and vapor techniques, among others, and have been discussed in detail, with an intense focus on several biomedical applications. However, many applications have yet to be discovered. In this review, we will describe these nanostructured materials based on their sources in nature and various structures, such as layered, hierarchical, and helical structures. In addition, we discuss the functions endowed by these structures, such as superhydrophobicity, adhesion, and high strength, enabling them to be employed in a number of applications in biomedical fields, including cell cultivation, biosensors, and tissue engineering.

摘要：A novel metal/semiconductor photocatalyst,Cu nanoparticles(NPs)modified TiO2 hollow spheres(Cu/TiO2),was designed for efficient photocatalytic overall water splitting(POWS)under both ultraviolet(UV)and visible(Vis)*** Cu/TiO2 photocatalyst possesses excellent POWS performance under Vis light at the highest level among the reported TiO2-based ***,the metal/semiconductor junction formed between Cu and TiO2 enables controlled water-oxidation product selectivity(H2O2 or O2)via different reaction pathways regulated by irradiation *** UV light,the electrons excited in TiO2 are captured by Cu NPs through the Cu/TiO2 Schottky interface for H2 production,with the photoholes in TiO2 producing H2O2 through a two-electron process;whilst under Vis light,Cu NPs act as plasmon to inject hot electrons to TiO2 for H2 production,while O2 is produced by hot holes on Cu NPs via a four-electron *** rational design of function-switchable metal/semiconductor junction may be helpful to understand the mechanisms for POWS with desired gas/liquid water-oxidation products.

摘要：Binuclear ruthenium complexes bearing the2,2'‐bipyridine‐6,6'‐dicarboxylate(bda)ligand have been demonstrated to be highly active catalysts towards water oxidation with CeIV as an ***,the catalytic properties of ruthenium dimers have not yet been explored for visible light‐driven water ***,the photocatalytic performance of a dipyridyl propane‐bridged ruthenium dimer2was investigated in comparison with its monomeric precursor,[Ru(bda)(pic)2](1),in CH3CN/phosphate buffer mixed solvent in a three‐component system including a photosensitizer and a sacrificial electron *** results showed that the activity of each catalyst was strongly dependent on the content of CH3CN in the phosphate buffer,which not only affected the driving force for water oxidation,but also altered the kinetics of the reaction,probably through different mechanisms associated with the O–O bond *** a result,dimer2showedsignificantly higher activity than monomer1in the solvent containing a low content of CH3CN,and comparable activities were attained with a high content of CH3CN in the *** the optimal conditions,complex2achieved a turnover number of638for photocatalytic O2evolution.

摘要：金属有机骨架(MOFs)衍生的Co基催化剂用于芳香硝基化合物选择加氢引起了广泛的关注,但催化剂合成过程中使用大量溶剂,且对催化剂中活性中心的认识存在争议.本文开发了一种固相合成策略,在不使用任何溶剂的情况下获得MOF前体材料,经发泡和热解处理获得Co@NC催化剂.研究发现,800℃热解所得的催化剂中Co纳米颗粒被氮掺杂石墨烯壳层包裹,在3-硝基苯乙烯的加氢过程中表现出~100%的转化率,3-乙烯基苯胺的选择性大于99%,同时,该催化剂具有良好的循环稳定性和底物普适性.表征和实验结果证明该催化剂中Co–N物种为活性中心,其含量可通过热解温度进行调变,且催化性能与Co–N物种的含量存在正相关关系.本工作为设计用于选择加氢反应的高效Co基催化剂提供了一种新的绿色合成策略.

摘要：通过电催化氧化葡萄糖等可再生生物质生产高附加值化学品为实现碳中和目标提供了一条有效途径.目前用于电催化生物质氧化反应的电催化剂主要分为贵金属基催化剂和非贵金属基催化剂.对于贵金属基电催化剂,文献报道了铂基催化剂的氧化态随电势变化,进而调控电催化葡萄糖氧化的活性和选择性.对于非贵金属基催化剂,钴基和镍基氧化物和氢氧化物被广泛应用于电催化生物质氧化反应,但铜基催化剂直到最近才引起关注.最近,金属铜、氧化亚铜和氢氧化铜在内的铜基材料被证实是一类有应用前景的电催化生物质氧化催化剂,但在电化学条件下的真实活性位结构仍难以鉴定.本文针对电催化葡萄糖等生物质平台分子的氧化反应,证明了氧化铜的催化活性相随电压升高从氢氧化铜演变为羟基氧化铜,阐明了结构和反应活性及选择性的构效关系,该工作加深了对铜基催化剂活性位动态重构的理解,有助于电催化生物质转化的催化剂理性设计,促进可再生资源利用和碳中和目标的实现.

摘要：Developing efficient electrocatalysts for the oxygen evolution reaction(OER)under neutral conditions is important for microbial electrolysis cells(MECs).However,the OER kinetics in neutral electrolytes at present are extremely sluggish,resulting in high overpotentials that greatly limit the energy conversion efficiencies of *** studies failed to probe the adsorbates on surface metal sites of catalysts at the atomic scale and elucidate their influence on the catalytic activities,which has impeded the rational design of efficient neutral OER catalysts with optimal surface ***,using in situ transmission electron microscopy(TEM),in situ X-ray photoelectron spectroscopy(XPS)and in situ low-energy ion scattering studies,we have identified,for the first time,that the electrochemically activated adsorbates on surface metal sites play a critical role in boosting the neutral OER activities of Ru-Ir binary oxide(RuxIryO2)*** adsorbate-activated RuxIryO2on a glassy carbon electrode achieved a low overpotential of 324 m V at10 m A cm-2in neutral electrolyte,with a 36-fold improvement in turnover frequency compared with that of Ir *** application in an MEC system,the resulting full cell showed a decreased voltage of 1.8 V,200 m V lower than the best value reported to date,facilitating efficient synthesis of poly(3-hydroxybutyrate)from bioelectrochemical *** functional theory(DFT)studies revealed that the enhanced OER activity of RuxIryO2catalyst arose from local structural distortion of adjacent adsorbate-covered Ru octahedra at the catalyst surface and the consequently decreased adsorption energies of OER intermediates on Ir active center.

摘要：Photocatalytic hydrogen production coupled with selective oxidation of organic substrates to produce highvalue-added fine chemicals has drawn increasing ***,we report a noble metal-free photocatalyst for the highly efficient and simultaneous generation of hydrogen and the selective oxidation of benzyl alcohol into benzaldehyde over Cd S@Mo S2 heterostructures under visible *** the need for a sacrificial agent,Cd S@Mo S2 displayed an excellent hydrogen production rate of 4233μmol g^-1h^-1with0.3 mmol benzyl alcohol,which is approximately 53 times higher than that of bare Cd S nanorods(80μmol g^-1h^-1).The reaction system was highly selective for the oxidation of benzyl alcohol into *** the amount of benzyl alcohol increased to 1.0 mmol,the hydrogen production reached9033μmol g^-1h^-*** electron microscopy and transmission electron microscopy images revealed that p-type Mo S2 sheets with a flower-like structure closely adhered to n-type semiconductor Cd S nanorods through the formation of a p-n *** a potential Z-scheme photocatalyst,the Cd S@Mo S2 heterostructure effectively produces and separates electron-hole pairs under visible ***,the electrons are used for reduction to generate hydrogen,and the holes oxidize benzyl alcohol into ***,a mechanism of photogenerated charge transfer and separation was proposed and verified by photoluminescence,electrochemical impedance spectroscopy,photocurrent and Mott-Schottky *** results reveal that the Cd S@Mo S2 heterojunctions have rapid and efficient charge separation and transfer,thereby greatly improving benzyl alcohol *** work provides insight into the rational design of high-performance Z-scheme photocatalysts and the use of holes and electrons to obtain two valuable chemicals simultaneously.

摘要：Although dielectric elastomer(DE)with substantial actuated strain(AS)has been reported 20 years ago,its scientific understanding remains *** most accepted theory of DE,which is proposed in 2000,holds the view that AS of DE is induced by the Maxwell *** to this theory,materials have similar ratios of permittivity and Young’s modulus should have similar AS,while the experimental results are on contrary to this theory,and the experimental AS has no relationship with ideal ***,a new dipole-conformation-actuated strain cross-scale model is proposed,which can be generally applied to explain the AS of DE without *** to this model,several characteristics of an ideal DE are listed in this work and a new DE based on polyphosphazene(PPZ)is *** AS of PPZ can reach 84%without any *** last,a PPZ-based all soft artificial heart(ASAH)is built,which works in the similar way with natural myocardium,indicating that this material has great application potential and possibility in the construction of an ASAH for heart failure(HF)patients.

摘要：The antibacterial properties of nano-metal oxides （ZnO, CuO） are based on the formation of reactive oxygen species （ROS）. This work reveals that the antibacterial properties of these nano-metal oxides are strongly dependent on their crystalline structure. The antibacterial activity of the nanooxides was tested against four types of bacteria that commonly cause nosocomial infections. The sonochemical method was applied not only for synthesis of nanooxides but also to their coating on textiles. The antibacterial properties of textiles coated with commercial and sonochemically prepared nano-metal oxides were evaluated and compared. The toxicity was evaluated on human lung cells and amphibian embryos, as representative models for inhalation and aquatic toxicology. The sonochemically prepared metal nanooxides are better antimicrobials than commercially available metal oxides with the same particle size range. It was found that the crystallites which have more defects and less organized structure are more toxic. The formation of ROS was studied by electron spin resonance （ESR） measurements for both the sonochemically prepared and commercial samples of ZnO/CuO nanoparticles. A significant increase in the production of radical species was found in the more defective, sonochemically prepared samples, as compared to the commercial ones. Since modulation of the nanoparticle defects influenced their toxicity, the possibility of engineering safer nano-antibacterials is indicated.