摘要：The special electronic characteristics and high atom usage efficiency of metal-nitrogen-carbon(M-N-C)materials have made them extremely attractive for oxygen reduction reactions(ORRs).However,it is inevitable that hydrogen peroxide(H_(2)O_(2))will be formed via the two-electron pathway in ***,the Cu nanoparticles(NPs)have been encapsulated into Ni doped hollow mesoporous carbon spheres(Ni-HMCS)to reduce the generation of H_(2)O_(2)in *** tests confirm that the introduction of Cu NPs improves the ORR performance *** obtained Cu/Ni-HMCS exhibits a half-wave potential of 0.82 V *** hydrogen electrode and a limited current density of 5.5 mA cm^(-2),which is comparable with the commercial Pt/***,Cu/Ni-HMCS has been used in Zn-air battery,demonstrating a high power density of 161 mW cm^(-2)and a long-term recharge capability(50 h at 5 mA cm^(-2)).The theoretical calculation proposes a tandem catalysis pathway for Cu/Ni multi-sites catalysis,that is,H_(2)O_(2)released from the Ni-N_(4)and Cu-N_(4)sites migrates to the Cu(111)face,on which the captive H_(2)O_(2)is further reduced to H_(2)*** work demonstrates an interesting tandem catalytic pathway of dual-metal multi-sites for ORR,which provides an insight into the development of effective fuel cell electrocatalysts.

摘要：作为细胞中的主要运输系统,天然囊泡在物质的定点输运过程中具有至关重要的作用.高分子囊泡是与之结构相似的一种人工囊泡,具有优异的膜稳定性和胶体稳定性、高药物负载率、低膜穿透性、优异的可修饰性和长循环时间等优势,在生物医用领域具有广泛的应用前景.然而,目前该领域尚面临一系列重要挑战,如合成和制备方法较为复杂、生物相容性较难预测、功能和递送途径有限等,限制了其临床转化之路.本文从囊泡的构建模块合成、自组装技术和潜在的生物医学应用等角度,提出了设计和制备下一代高分子囊泡需要解决的五个关键科学问题,指出了未来面临的重要挑战和发展方向,例如简化设计和合成过程,优化和规范自组装过程,拓展潜在的应用前景.

摘要：对超低浓度盐溶液响应产生大尺度形变的功能水凝胶在海水渗透能收集、刺激响应分离材料、智能传感和致动器等方面具有广阔的应用前景.本文结合聚电解质和两性离子聚合物开发了一种盐度超敏感离子水凝胶.以稀盐作为分散介质时,水凝胶体积缩小为原来1/60.本文研究了盐响应水凝胶的溶胀、形态和力学性能,并基于拉曼光谱对聚合物网络盐响应重构行为进行了表征.此外,利用毛细管和盐响应水凝胶成功设计了一种可视化、便携离子检测计,可媲美商用水质监测计.同时开发了具有传感和致动功能的智能液阀,用于自动感应调节液体的流出和输送.该盐敏感水凝胶在淡水监测和调控、海水渗透能收集、刺激响应分离材料、智能软机器人和电子穿戴等方面具有很大的应用潜力.

摘要：过渡金属氧化物具有丰富的功能性,但其错综复杂的内部自由度对相图绘制和结构设计提出了挑战.本文中,我们引入了描述相图物理起源的轨道能级序(ELO),并通过对La_(0.67)Sr_(0.33)MnO_(3)(LSMO)氧化物的研究证明了其在相图预测中的有效性.结合DFT计算和实验,我们构建了氧含量和应变关联的LSMO相图,结果表明LSMO结构稳定性与ELO密切相关.据此发现了一种由ELO演化而产生的四倍氧有序相.最后,我们提出了描述轨道分裂程度的轨道弹性定律,阐明了ELO演化的起源,助力功能氧化物的设计.这项研究拓宽了材料科学领域的性能调控手段,并为从轨道角度预测相图提供了思路.

摘要：石墨炔(GYs)是一种新型碳同素异形体,由sp和sp^(2)杂化碳原子组成.其中,石墨双炔(GDY)是目前研究和关注度最广泛的材料.其独特的sp杂化、均匀的孔隙和高度共轭的结构带来了优良的电子、光学和力学特性,其被广泛应用于电子器件、储能和转换、催化、气体分离、海水淡化等领域.然而,GDY材料仍然面临着诸多挑战,包括高结晶GDY的合成和快速无损的表征方法.本文就高结晶度GDY的设计、合成和结构表征进行了综述.本文还描述了GDY在各个领域的应用,为高度均匀的单晶GDY材料带来新的机遇.

摘要：在柔性设备和静态储能电网应用中,可充电水性锌离子电池展现出巨大的潜力.但其发展受到界面不稳定性引起的副反应及枝晶生长的阻碍.本研究中,我们采用了一种新颖的电解液设计,通过含大量孤电子对的亲锌葫芦[7]超分子来应对这一挑战.这些超分子因其独特的分子结构,能够在电化学循环中有效地吸纳和固定Zn离子,从而有效避免了Zn离子的无序迁移和枝晶的形成.超分子中丰富的孤对电子提供的Lewis碱性位点(如叔胺和羰基氧)作为Zn离子的供电子成核位点,促进了紧密成核.这些超分子与Zn离子之间的强烈相互作用,不仅提高了系统的稳定性,还显著抑制了不良副反应.因此,我们组装的对称电池和Zn//V_(2)O_(5)全电池均展示了长效的循环稳定性和卓越的库仑效率.

摘要：磁场触发的催化剂轨道电子自旋排列已成为促进析氧反应的一种有趣而可行的策略.然而,具有强d-d库仑相互作用的高熵合金(HEAs)催化剂中的磁场增强机制尚未得到充分挖掘.在此,我们设计了具有优异软磁性的高熵合金金属片,在微小磁场下表现出显著的磁场增强催化作用,其磁导率可作为评估磁场增强的描述因子.具体地,仅施加50 mT的磁场,(FeCoNi)_(82.5)Cr_(17.5)HEAs的过电位下降就超过了36mV@10 mA cm^(-2).此外,过电位的降低与HEA的磁导率呈线性关系.原位拉曼光谱与理论计算结果表明,施加磁场可显著提高自旋密度,改善催化剂的3d电子与*O自由基的2p轨道之间的自旋相互作用,从而有效降低速率决定步骤(*O→*OOH)的能量障碍,进而促进O-O的形成.

摘要：V_(2)O_(5),which has multicolor and energy storage properties,is a promising electrochromic material for multifunctional electrochromic devices,but its practical application is limited by its poor lifespan and long switching *** this work,high-performance V_(2)O_(5)/TiO_(2)films were fabricated by spraying a V_(2)O_(5)solution on in situ-grown TiO_(2)*** to the porous structure formed between the TiO_(2)nanorods and the remarkable electron transfer performance of TiO_(2),the switching time of the V_(2)O_(5)/TiO_(2)films ***,the strong adhesion between the TiO_(2)nanorods and F-doped tin oxide(FTO)glass and the increased surface roughness of the substrates significantly improved the cycling stability of the V_(2)O_(5)/TiO_(2)*** a large transmittance modulation(47.8%at 668 nm),fast response speed(τ_(c)=5.1 s,τ_(b)=4.2 s),and long lifespan,V_(2)O_(5)/TiO_(2)films were used as electrodes for the electrochromic energy storage device(EESD),which switched in six colors through color overlay:dark orange,sandy yellow,green-yellow,yellow-green,dark green,and dark *** by pixel displays,EESDs were designed by segmenting V_(2)O_(5)films to stagger the display of the electrochromic and ion storage layers,which presented 11 types of information based on different combinations of *** work provides inspiration for developing multifunctional electrochromic devices,especially for camouflage and information displays.

摘要：The accumulation of excessive nitrate in the atmosphere not only jeopardizes human health but also disrupts the balance of the nitrogen cycle in the *** various nitrate removal technologies,electrocatalytic nitrate reduction reaction(eNO_(3)RR)has been widely studied for its advantages of being eco-friendly,easy to operate,and controllable under environmental conditions with renewable energy as the driving *** metal-based catalysts(TMCs)have been widely used in electrocatalysis due to their abundant reserves,low costs,easy-to-regulate electronic structure and considerable electrochemical *** addition,TMCs have been extensively studied in terms of the kinetics of the nitrate reduction reaction,the moderate adsorption energy of nitrogen-containing species and the active hydrogen supply *** on this,this review firstly discusses the mechanism as well as analyzes the two main reduction products(N_(2)and NH_(3))of eNO_(3)RR,and reveals the basic guidelines for the design of efficient nitrate catalysts from the perspective of the reaction ***,this review mainly focuses on the recent advances in the direction of eNO_(3RR)with four types of TMCs,Fe,Co,Ni and Cu,and unveils the interfacial modulation strategies of Fe,Co,Ni and Cu catalysts for the activity,reaction pathway and ***,reasonable suggestions and opportunities are proposed for the challenges and future development of eNO_(3)*** review provides far-reaching implications for exploring cost-effective TMCs to replace high-cost noble metal catalysts(NMCs)for eNO_(3)RR.

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.