摘要：The interest in curtailing environmental pollution issues through physical separation processes has inspired an extensive search for novel nanoporous materials with exceptional adsorption *** triazine frameworks(CTFs),emerged as a class of crystalline covalent organic frameworks(COFs),have been widely examined for various separation applications,owing to their large porosity,high stability,and rich nitrogen(N)*** development of CTFs for efficient adsorption of mercury(Ⅱ)(Hg^(2+))is of great importance for the field,whereas it is rarely attempted,on account of limited synthetic strategies and unknown structural-property relations of conventional CTFs derived from ionothermal ***,we report rational synthesis of a crystalline CTF with methylthio pendant arms for efficient removal of Hg^(2+)with an exceptional capacity of 751 mg·g^(-1),ranking at the top among previously-reported *** work may open up new possibility in the synthesis of COFs for various separations.

摘要：铂(Pt)是质子交换膜燃料电池(PEMFCs)阳极氢氧化反应(HOR)中最先进的电催化剂.然而,Pt催化剂对CO(工业低成本氢燃料中的杂质)极度敏感从而中毒,这会引起器件性能的急剧衰退,导致器件运行成本高.因此,提高Pt催化剂的CO耐受性对PEMFCs的商业化推广至关重要.在此,我们设计合成了一种独特的PtNiW@WO_(x)核壳纳米线来提高Pt基催化剂对CO的耐受能力.机理研究表明,表面无定形的WO_(x)壳层可以作为分子围栏,在动力学上阻碍CO扩散到达Pt位点.在热力学上,Ni和W元素合金化产生的电子效应可以使Pt的d带中心降低,减弱CO在Pt位点上的化学吸附.此外,亲氧W元素可以加速水的解离,提供更多OH活性物种,促进CO的氧化脱附.因此,在1000ppm CO/H_(2)条件下,所设计的PtNiW@WO_(x)核壳纳米线催化剂表现出优异的HOR抗CO中毒性能,在4000 s后仍能保持超过90%的HOR电流密度,超过了原始的PtNi纳米线和目前报道的绝大多数Pt基催化剂.

摘要：聚合物基固态电解质得益于其易加工性,最有希望应用于下一代固态锂金属电池.目前,聚合物基态电解质的离子电导率提升策略多为加入导锂陶瓷以构建离子传输通道,其提升程度有限.电场在锂离子输运过程中存在重要影响,目前研究中有关电场对锂离子传输的影响机制尚不明确.本文将兼具高离子电导率和高介电常数的铌酸锂嵌入聚偏氟乙烯基体中,设计了一种新型复合固态电解质.铌酸锂颗粒有效调节电解质内部电场结构,增强了离子输运方向电场强度,实现了离子电导率的大幅提升(7.39×10^(-4)S cm^(-1),25℃).该电解质匹配高镍正极和锂金属负极的固态电池可稳定循环1000次以上,容量保持率为72%.该研究为设计下一代固态锂电池用高离子电导复合固态电解质提供了新的策略.

摘要：高活性MOF基催化剂的设计和合成为促进动力学不利的氧还原反应(ORR)过程开辟了新的途径.本研究通过在ZIF-8前驱体表面涂覆二茂铁甲酸,然后进行两步炭化工艺,设计和制备了一种具有新型结构的高效电催化剂,以提高ORR性能.两步炭化过程对于将热解Fe_(3)C纳米颗粒封装到碳纳米管(CNTs)中以及将Fe单原子隔离到N掺杂碳(NC)基体上至关重要.此外,Fe元素的相对含量对优化催化剂的ORR性能至关重要.所制得Fe_(3)C@CNTs/NC-M催化剂结构先进,在碱性溶液中表现出良好的长期稳定性和电催化ORR性能,其半波电位和极限电流分别达到0.941 V和6.31 mA cm^(-2).此外,该电催化剂在甲醇溶液中具有较强的耐受性和良好的稳定性.Fe_(3)C@CNTs/NC-M锌空气电池(ZAB)具有1.525 V的开路电位,420 mA cm^(-2)时的峰值功率密度为348 mW cm^(-2),10 mA cm^(-2)时的最大容量为843 mA h g_(Zn)^(-1).因此,这种合成策略为构建具有有效和稳定的ORR性能的MOF基电催化材料提供了一条有效途径.

摘要：矸石胶结充填开采是一种重要的充填开采方法,然而,酸性矿井水会严重影响矸石胶结充填体的强度。在本研究中,将矸石胶结充填体试件分别置于不同环境(空气、水、硫酸溶液、硫酸与荷载耦合)中,测试了不同龄期试件的抗压强度、电阻率及超声波波速,监测了加载过程中试件的声发射能量数值,同时结合扫描电镜和X衍射分析不同龄期充填体的微观结构。结果表明,1)空气中与水中养护的充填体抗压强度的增长趋势随龄期的增加而逐渐减缓。硫酸溶液中的充填体强度在前90天大于空气及水中养护的充填体强度。硫酸溶液与荷载耦合作用下充填体的强度随龄期的下降速率比单一硫酸溶液作用的较为缓慢;2)不同龄期矸石胶结充填体电阻率与超声波波速与强度有较好的对应关系。受侵蚀后矸石胶结充填体的破坏形式较为多样,且在加载不同阶段表现出不同的声发射能量特征,可以将声发射能量激增作为充填体的破坏前兆;3)侵蚀产物前期填充充填体内部孔隙,提高了其强度,后期会导致充填体膨胀开裂,强度降低。施加40%应力强度比的荷载会抵抗硫酸溶液的侵蚀。本文研究结果可以为充填体的耐侵蚀设计提供参考。

摘要：Three-dimensional(3D)printing has attracted increasing research interest as an emerging manufacturing technology for devel-oping sophisticated and exquisite architecture through hierarchical *** has also been employed in various advanced industrial *** development of intelligent biomedical engineering has raised the requirements for 3D printing,such as flexible manufacturing processes and technologies,biocompatible constituents,and alternative ***,state-of-the-art 3D printing mainly involves inorganics or polymers and generally focuses on traditional industrial fields,thus severely limiting applications demanding biocompatibility and *** this regard,peptide architectonics,which are self-assembled by programmed amino acid sequences that can be flexibly functionalized,have shown promising potential as bioinspired inks for 3D ***,the combination of 3D printing and peptide self-assembly poten-tially opens up an alternative avenue of 3D bioprinting for diverse advanced ***,a small but innovative nation,has significantly contributed to 3D bioprinting in terms of scientific studies,marketization,and peptide architectonics,including modulations and applications,and ranks as a leading area in the 3D bioprinting *** review summarizes the recent progress in 3D bioprinting in Israel,focusing on scientific studies on printable components,soft devices,and tissue *** paper further delves into the manufacture of industrial products,such as artificial meats and bioinspired supramolecular architectures,and the mechanisms,physicochemical properties,and applications of peptide ***,Israel contributes significantly to the field of 3D bioprinting and should thus be appropriately recognized.

摘要：局部电荷的强离域和强偶极矩是影响共价有机框架(COFs)基光催化剂催化析氢性能的两个关键因素.然而,基于精确的调控结构模型来系统研究这种构效关系的报告相对较少.本研究提出了一种新的策略,通过合理的设计,制备了三种三芴酮基COFs,通过在分子水平上调控单体的结构和偶极来提高局部电荷离域指数.我们重点研究这三种三芴酮基COF的局部电荷离域与光催化性能之间的构效关系.在不同三芴酮基COF中,1,3,5-三(对甲酰基苯基)苯基COF(TeTpb-COF)展现出21.6 mmol g^(-1)h^(-1)的最高析氢速率,与2,4,6-三(4-醛基苯基)-1,3,5-三嗪基COF(TeTt-COF,0.2mmol g^(-1)h^(-1))相比,光催化析氢性能提高了108倍.这种性能的增强可归因于其强大的分子内置电场提高了供体-受体嵌段单元中光生电荷的有效分离效率.这项工作证实了调整构建块可以极大增强三芴酮基COFs中的局部偶极矩,从而显著改善光催化析氢性能.构建模块的调控策略为创建高效的新型COF基光催化析氢平台提供了新机会.

摘要：Photocatalytic CO_(2)reduction to sustainably product of fuels is a potential route to achieve clean energy ***,the sluggish charge transport dynamics and poor CO_(2)activation performance result in a low CO_(2)conversion ***,we develop a multidimensional In_(2)O_(3)/In_(2)S_(3)(IO/IS)heterojunction with abundant lattice distortion structure and high concentration of oxygen *** close contact interfaces between the junction of the two phases ensure undisturbed transmission of electrons with high‐*** increased free electron concentration promotes the adsorption and activation of CO2 on the catalyst surface,leaving the key intermediate*COOH at a lower energy *** perfect combination of the band matching oxide and sulfide effectively reduces the internal energy barrier of the CO2 reduction ***,the lattice distortion structure not only provides additional active sites,but also optimizes the kinetics of the reaction through microstructural ***,the optimal IO/IS heterojunction exhibits superior CO_(2)reduction performance with CO evolution rate of 12.22μmol g^(−1)h^(−1),achieving about 4 times compared to that of In_(2)O_(3)and In2S3,*** work emphasizes the importance of tight interfaces of heterojunction in improving the performance of CO_(2)photoreduction,and provides an effective strategy for construction of heterojunction photocatalysts.

摘要：High-temperature proton exchange membrane(HT-PEM)fuel cells offer more advantages than low-temperature PEM fuel *** ideal characteristics of HT-PEMs are high conductivities,low-humidity operation conditions,adequate mechanical properties,and competitive *** molecular moieties,such as benzimidazole,benzothiazole,imide,and ether ether ketone,have been introduced to polymer chain backbones to satisfy the application requirements for *** most common sulfonated polymers based on the main chain backbones have been employed to improve the *** group/chain engineering,including the introduction of SO_(3)^(-) on the side chain,grafting,branching,and crosslinking,has been widely applied to HTPEMs to further improve their proton conductivity,thermal stability,and mechanical ***,phosphoric acid-doped polybenzimidazole is the most successful polymer material for application in *** compositing/blending modification methods of polymers are effective in obtaining high PA-doping levels and superior mechanical *** this review,the current progress of various membrane materials used for HT-PEMs is *** synthesis and performance characteristics of polymers containing specific moieties in the chain backbones applied to HT-PEMs are discussed *** modification approaches and their deficiencies associated with HT-PEMs are analyzed and *** and future challenges are also presented.

摘要：Based on the boron-containing thermally activated delayed fuorescence(TADF)compound p-AC(AC:acridine)5,9-dioxa-13 b-boranaphtho[3,2,1-de]anthracene(a),a series of new TADF molecules b1-b4 were designed via adding two nitrogen atoms at the AC donor *** functional theory and time-dependent density functional theory calculations were performed on the frontier orbital energy levels,emission spectra,singlet-triplet states energy gaps(?EST),reverse intersystem crossing(RISC)rate constant(kRISC)for compounds a and *** calculation results show that the maximum emission wavelengths of b1-b4 are significantly blue-shifted by47-125 nm compared with that of *** b1 and b3 exhibit dark-blue emission,while molecules b2 and b4 display light-blue emission,indicating that these four derivatives could be potential organic light-emitting diode(OLED)candidates with blue-light ***,we found the RISC processes in a,b2,and b4 can occur not only from T_(1) state to S_(1) state,but also from T_(2) state to S_(1) state significantly,while the RISC processes in b1 and b3 mainly take place via the T_(2)→S_(1) hot exciton ***,the T_(1)→S_(1) kRISC values of b2 and b4 are predicted to be two to three times of that of a,indicating enhanced TADF *** results not only provide two promising boron-based TADF candidates(b2 and b4),but also offer useful theoretical basis for the design of blue OLED materials.