摘要：Wearable bioelectronic devices have the capacity for real-time human health monitoring,the provision of tailored services,and natural interaction with smart ***,these wearable bioelectronic devices rely on conventional rigid batteries that are frequently charged or replaced and are incompatible with the skin,leading to a discontinuity in complex therapeutic tasks related to human health monitoring and human-machine *** triboelectric nanogenerator(TENG)is a high-efficiency energy harvesting technology that converts mechanical into electrical energy,effectively powering wearable bioelectronic *** study comprehensively overviews recent advances in stretchable TENG for use in wearable bioelectronic *** working mechanism of stretchable TENG is initially explained.A comprehensive discussion presents the approaches for fabricating stretchable TENG,including the design of stretchable structures and the selection of stretchable ***,applications of wearable bioelectronic devices based on stretchable TENG in human health monitoring(body movements,pulse,and respiration)and human-machine interaction(touch panels,machine control,and virtual reality)are ***,the challenges and developmental trends regarding wearable bioelectronic devices based on stretchable TENG are elaborated.

摘要：环保型CuInSe_(2)量子点具有高消光系数和宽光谱吸收范围,在光电化学催化应用中展现了良好的发展前景.然而,CuInSe_(2)量子点较低的载流子分离能力和严重的界面电荷复合降低了其光电化学性能,制约了其应用.因此,我们设计并合成了具有Ⅱ型能带排列的CuInSe_(2)/CuInS_(2)核/壳结构量子点,以促进载流子分离、减少界面缺陷;进一步通过调节In/Cu前驱体的摩尔比,产生铜空位.光物理性质研究表明,导带电子-铜空位捕获的空穴之间的辐射复合成为主要的复合方式,有效延长了载流子寿命,促进了载流子分离.因此,基于富铜空位的CuInSe_(2)/CuInS_(2)核壳量子点的光阳极获得了~8.0 mA cm^(-2)的最大饱和光电流密度,该性能是当前报道的CISe基量子点光电化学电池中的最高值之一.本工作提供了一种通过表面或内在缺陷的调控来促进光电化学应用中的电荷载流子分离和传输的有效方法.

摘要：应用3D打印技术制备准固态微型超级电容器(MSCs)在可编程结构设计和高质量负载电极制造方面具有固有的优势.然而,缺乏高性能的可打印墨水和厚电极内缓慢的离子传输,对其实际电荷存储能力提出了重大挑战.本文成功开发了一种具有优异流变性能的新型NiCo_(2)S_(4)基纳米复合墨水,并结合直墨书写的3D打印技术合理设计了准固态MSCs的三维结构.得益于牢固锚定在还原氧化石墨烯(rGO)表面的NiCo_(2)S_(4)纳米颗粒和有序的三维微孔,锯齿状厚电极提供了丰富的反应位点并增强了离子传输.因此,三层锯齿状MSCs的面电容高达416.7 mF cm^(-2).在1 mA cm^(-2)的电流密度下,单层、双层和三层电极的锯齿状MSCs的面电容与相对应的网格状MSCs相比,分别增加了127.1%、349.8%和585.9%.本工作为高面电容MSCs的材料和电极结构的跨尺度设计提供了新见解,推动了MSCs在柔性便携式电子设备中的集成应用研究.

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：二维过渡金属硫族化合物(TMDCs)材料被认为是拓展摩尔定律的极具前景的候选材料.然而,该材料的低光致发光效率严重限制了其实际应用,其本质源于材料制备中不可避免引入的缺陷.在本文中,我们报道了一种Sr掺杂单层MoS_(2)的有效缺陷工程策略,该策略在实验上通过简便的化学气相沉积(CVD)一步法成功实现.所制备的具有亚毫米(~324μm)级的大尺寸样品的光致发光可实现高达两个数量级的增强,并伴随着载流子寿命的显著增强.这一现象主要归因于Sr掺杂后MoS_(2)体系中其三激子向激子转换.与此同时,掺杂样品的辐射质量和稳定性也显著提升.第一性原理计算进一步阐明了其调控机制,即在MoS_(2)中引入适当互补缺陷能级与其自身的缺陷能级协同,从而可调节其载流子组分,以实现光致发光的显著增强.此外,我们的缺陷工程策略也适用于其他掺杂剂,如钙掺杂剂.我们的工作报告了一种可以显著提升单层MoS_(2)的荧光性能的有效缺陷工程策略,这为设计和调控二维TMDCs的光电特性提供一种极具前途的方法.

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：Due to their tunable acidity,shape selectivity,and excellent stability,zeolites are of great importance as solid acid materials in industrial *** the properties of the acid sites in zeolites allows for the rational design and fabrication of catalysts for target *** ether(DME)carbonylation,a critical chain-growth reaction for C1 resource utilization,is selectively catalyzed by the Brønsted acid sites within the eight-membered rings(8-MRs)of mordenite(MOR).It is anticipated that strengthening the Brønsted acidity—particularly in 8-MRs—will improve the catalytic performance of *** this work,density functional theory(DFT)calculations are first employed and the results used to design a modified MOR with stannum(Sn)and to predict the corresponding changes in *** by the theoretical studies,a series of Sn-modified MOR are synthesized via a defect-engineering and subsequent heteroatom-substitution *** partial desilication,isolated tetrahedral Sn species in an open configuration are successfully synthesized for the first time,within which tetrahedrally coordinated Al sites are *** acidic characterization is used to confirm that the acidity of the Brønsted acid sites is enhanced by the introduction of the Sn species;as a result,the sample exhibits excellent activity in DME carbonylation *** and DFT studies reveal that this strengthened acidity facilitates the adsorption of DME and reduces the activation barriers of DME dissociation and acetyl formation,accounting for the improved *** work demonstrates mechanistic insights into the promoting effects of strong acidity on DME carbonylation and offers a promising strategy to precisely control the acidic strength of zeolites.

摘要：Aqueous zinc-ion batteries(AZIBs)are attracting worldwide attention due to their multiple merits such as extreme safety,low cost,feasible assembly,and environmentally friendly enabled by water-based *** present,AZIBs have experienced systematic advances in battery components including cathode,anode,and electrolyte,whereas research involving separators is *** separator is the crucial component of AZIBs through providing ion transport,forming contact with electrodes,serving as a container for electrolyte,and ensuring the efficient battery *** this great yet ignored significance,it is timely to present the latest advances in design strategies,the systematic classification and summary of *** summarize the separator optimization strategies mainly along two approaches including the modification of the frequently used glass fiber and the exploitation of new *** advantages and disadvantages of the two strategies are analyzed from the material types and the characteristics of different *** effects and mechanisms of various materials on regulating the uniform migration and deposition of Zn2+,balancing the excessively concentrated nucleation points,inhibiting the growth of dendrites,and the occurrence of side reactions were discussed using confinement,electric field regulation,ion interaction force,desolvation,***,potential directions for further improvement and development of AZIBs separators are proposed,aiming at providing helpful guidance for this booming field.

摘要：调控金属活性位点的电子结构来发展高活性的选择性加氢反应催化剂对于可持续有机合成非常重要.但时至今日,这仍然是非常具有挑战性的课题.在本文中,我们将具有电子结构调节特性的超细PtRu合金纳米颗粒负载在CdS纳米棒上,成功构建了PtRu/CdS复合催化剂并研究了其光催化芳香族硝基化合物氢化还原性能.我们发现当以水为质子源时,所得复合催化剂表现出高效的光催化加氢活性.超快光谱研究和密度泛函理论计算揭示了合金的形成促进了光生载流子的分离并降低了氢化还原反应中决速步的能垒,从而显著提高了加氢活性.本研究通过合金化效应调节助催化剂的电子结构,为高活性助催化剂/光催化剂体系的理性设计开辟了一条新途径.

摘要：高效光电探测器在监控、热成像、光通信和环境监测等领域具有广泛、迫切的应用需求.优化光电探测器参数如微型化、高量子效率、超快响应速度等,仍然是一项艰巨的任务.我们提出了一种由顶部/底部MoTe_(2)和中间Ta_(2)NiSe_(5)层组成的双范德华异质结.利用双异质结界面增强光收集效率和产生两个对立的内置电场,使得器件具有400到1550 nm的宽光谱响应,并表现出优异的性能,包括82.9%的外量子效率和3.5/4.2μs的快速响应速度.此外,利用二维Ta_(2)NiSe_(5)纳米片的面内各向异性,我们实现了在635和1550 nm波长下的极化灵敏度,分别为16.3和8.1.这项研究为开发高性能和多功能光电探测器提供了平台,为先进光电器件的设计和应用提供了新的方向.