Insights into the efficient charge separation over Nb2O5/2D-C3N4 heterostructure for exceptional visible-light driven H2 evolution

Two-dimensional carbon nitride(2 D-C₃ N₄)nanosheets are promising materials in photocatalytic water splitting,but still suffer from easy agglomeration and fast photogene rated electron-hole pairs recombination.To tackle this issue,herein,a hierarchical Nb₂ O₅/2 D-C₃ N₄ heterostructure is precisely constructed and the built-in electric field between Nb₂O₅ and 2 D-C₃ N₄ can provide the driving force to separate/transfer the charge carriers efficiently.Moreover,the strongly Lewis acidic Nb₂O₅ can adsorb TEOA molecules on its surface at locally high concentrations to facilitate the oxidation reaction kinetics under irradiation,resulting in efficient photogene rated electrons-holes separation and exceptional photocatalytic hydrogen evolution.As expected,the champion Nb₂O₅/2 D-C₃N₄ heterostructure achieves an exceptional H2 evolution rate of 31.6 mmol g^-1 h^-1,which is 213.6 times and 4.3 times higher than that of pristine Nb₂O₅ and2 D-C₃N₄,respectively.Moreover,the champion heterostructure possesses a high apparent quantum efficiency(AQE)of 45.08%atλ=405 nm and superior cycling stability.Furthermore,a possible photocatalytic mechanism of the energy band alignment at the hetero-interface is proposed based on the systematical characterizations accompanied by density functional theory(DFT)calculations.This work paves the way for the precise construction of a high-quality heterostructured photocatalyst with efficient charge separation to boost hydrogen production.     

Is it universal that the layered-spinel structure can improve electrochemical performance?

The introduction of spinel phase to form the layered-spinel structure(LSS)is an effective way to improve the electrochemical performance of Li-and Mn-rich layered oxides(LMR).But is this structure universal for all LMR systems?In this work,different Mn/Ni ratio systems with the LSS are discussed in detail.It is found that,high discharge capacity(200.8 mA h g^-1 at 1C rate;1C=250 mA h g^-1)as well as high capacity-retention(94%at 1C rate after 100 cycles)can be achieved by forming the LSS for low-Ni system(Mn/Ni=5.0).However,the capacity retention decreases severely in the high-Ni system(Mn/Ni=3.5,2.6).For example,when the ratio of Mn/Ni is 3.5,the capacity-retention of the layered-spinel sample was only 65.8%,compared to the 83%of the original LMR sample.The Ex-situ XRD,XPS,and HRTEM results demonstrate that the introduction of spinel phase in high-Ni system accelerates the transition and collapse of the crystal structure.This work provides guidance for optimizing the proportions of elements and the design of structures for the LMR.     

非富勒烯受体DA'D型稠环单元的结构修饰及电池性能研究

近年来,设计和合成高性能非富勒烯受体(NFAs)材料已经成为太阳能电池研究领域的前沿课题。基于DA'D型稠环结构的NFAs由于具有吸光系数高、能级和带隙可调、结构易于修饰、分子可高效合成、光电学性能优异等优点而受到了越来越广泛的关注。在短短7年的时间里,能量转换效率(PCE)从3%~4%提高到18%。2019年初邹应萍等报道了一个优秀的受体分子Y6,与PM6共混制备单结电池,获得了15.7%的能量转换效率。Y6类受体材料的中心给电子单元为DA'D型稠环结构,缺电子单元(A')通过氮原子与两个给电子单元(D)并联形成稠环结构,这有助于降低前线分子轨道能级并增强吸收,同时与氮相连的两个烷基链和位于噻吩并噻吩β位的两个侧链则有助于提高溶解度及调节结晶性。自Y6问世以来,人们对分子的结构剪裁进行了深入的研究,并报道了数十种新的结构。在这些新的受体中,DA'D部分的结构裁剪对提高器件效率和太阳能电池的性能起着至关重要的作用。本文对A'、D单元和侧链结构修饰的研究进展进行了综述。通过选择几组受体,对最近报道的分子进行分类,并将它们的光学、电化学、电学和光电性质与精确的结构修饰相关联,从而对结构-性能关系进行全面概述。     

基于抛光基材的热蒸镀铜箔生长高平整单层石墨烯薄膜

在石墨烯的化学气相沉积工艺中,铜箔是决定石墨烯薄膜质量的重要因素。传统铜箔由于制备工艺的限制,存在大量的缺陷,导致石墨烯薄膜的成核密度较高。本工作选用抛光铝板、抛光不锈钢板、微晶玻璃和SiO₂/Si作为基材,用热蒸镀法制备了不同粗糙度的铜箔,并详细讨论了以该系列铜箔生长高平整度石墨烯薄膜的条件及铜箔对石墨烯薄膜品质的影响。实验结果表明,铜箔以(111)取向为主,与基材分离后,表面具有纳米级平整度。在生长石墨烯后,从SiO₂/Si剥离的铜箔成核密度是4种基材中最小的。同时,从SiO₂/Si剥离的铜箔晶体结构变化最不明显,具有良好的结晶性,表面几乎不存在铜晶界缺陷。当压强为3 000 Pa,氢气和甲烷流速分别为300 mL/min和0.5 mL/min时,可以获得约1 mm横向尺寸的石墨烯单晶晶畴。     

水热法制备二氧化锡/钨酸铋复合光催化材料及其催化活性研究

本文用水热法制备了正交晶系的纳米球状结构的二氧化锡和正交晶系的由片状聚集成球状结构的钨酸铋,并且对二者进行了复合,制备出了二氧化锡/钨酸铋复合光催化材料。采用X射线衍射(XRD)、扫描电子显微镜(SEM)、比表面积测试仪(BET)、紫外可见分光光度计等技术对复合样品的结构、形貌、比表面积、孔容孔径和光学性质进行了表征。用碘钨灯模拟太阳光,分别以二氧化锡、钨酸铋和二氧化锡/钨酸铋复合材料为催化剂降解罗丹明B(RhB),研究所制备的二氧化锡/钨酸铋复合材料的光催化活性。光催化90 min时二氧化锡、钨酸铋和二氧化锡/钨酸铋对罗丹明B的降解率分别是9%、22%和30%。实验结果表明,在可见光下,二氧化锡/钨酸铋复合材料的光催化活性要高于单一的二氧化锡和钨酸铋。     

单元教学设计过程中的“教学问题链”设计——以上海科学技术出版社《物理·必修》(第三册)静电场单元为例

根据教育部颁布的《普通高中物理课程标准(2017年版)》,在上海市物理教育教学基地(上海高校“立德树人”人文社会科学重点研究基地)的大力支持下,由上海市教育委员会组织编写的上海高中物理非统编教材进行了正式使用前的试教试用活动,此教材是在上海高中物理“二期课改”教材的基础上全面改写而成的.单元教学设计已成为当前教学设计的焦点问题,以《物理·必修》(第三册)静电场单元为例,详细阐述了“教学问题链”的设计理念,希望与广大一线教师交流试教试用的心得与反思,推动新课改课堂转型.     

A Triphenylphosphonium Functionalized AIE Conjugated Macrocyclic Tetramal&mide for Mitochondrial-targeting Bioimaging

Developme nt of subcellular orga nelle-targeted bioimagi ng probes is of great imports nee in the field of early detection of diseases and exploring the behaviors of subcellular organelles.Herein,we present a triphenyIphosphonium functionalized conjugated macrocyclic tetramaleimide(TPP-CMT)as a mitochondrial-targeting bioimaging probe.The core of TPP-CMT is obtained by connecting two pyrenes and two benzenes through four maleimides.This unique structure endows TPP-CMT with exceptional far red/near-i nfirared aggregati on-induced emissi on(FR/NIR-AIE)characteristics.TPP-CMT is an excelle nt fluoresce nt emitter in most solve nts and eve n in solid states.The qua ntum yield of TPP-CMT was higher tha n 27% when dissolved in comm on middle-polarity orga nic solve nt and this value remained at 28.2% in its solid state.The in troducti on of four triphe ny Iphosph onium on maleimide positions endows TPP-CMT with mitochondrial-targeting ability.Thanks to the FR/NIR-AIE characteristics and the mitochondri-al-targeti ng ability,this well-desig ned fluoresce nt probe was successfully employed for mitochondrial targeti ng bioimaging of HeLa and HepG2 cells.     

嵌锁式CFRP方形蜂窝夹芯梁低速冲击响应及失效机理

采用嵌锁组装工艺制备了碳纤维/树脂基复合材料方形蜂窝夹芯梁，实验研究了低速冲击载荷下简支和固支夹芯梁的动态响应及失效机理，获得了不同冲击速度下夹芯梁的失效模式，分析了其损伤演化过程和失效机理，探讨了冲击速度、边界条件、面板质量分布以及槽口方向等因素对夹芯梁破坏模式及承载能力的影响。研究结果表明，芯材长肋板槽口方向对夹芯梁的失效模式有较大影响，槽口向上的芯材跨中部分产生了挤压变形，而槽口向下的芯材跨中部分槽口在拉伸作用下出现了沿槽口开裂失效，继而引起面板脱粘和肋板断裂；同等质量下，较厚的上面板设计可以提高夹芯梁的抗冲击能力，冲击速度越大，夹芯梁的峰值载荷和承载能力越高；固支边界使得夹芯梁的后失效行为呈现出明显的强化效应，在夹芯梁跨中部分发生初始失效后出现了后继的固支端芯材和面板断裂失效模式。