The morphology modulation of graphene to produce wrinkles and folds for effective electrochemical determination of Hg(II)

A highly efficient electrode material, three-dimensional reduced graphene oxide with varying wrinkles and folds (WRGO), applicable for electrochemical determination of Hg(II) was obtained by treating graphene oxide (GO) with KOH aqueous solution. After alkaline etching, the relatively flat graphene was altered and its self-aggregation was significantly alleviated, producing more wrinkles and folds, which provided more active adsorption sites for heavy metal ions. WRGO-5 modified electrode system herein offers a highest sensitivity of (31.83 μAμM⁻¹) and a lowest LOD of (16.28 nM). Moreover, the electrode sensor possesses good stability and reproducibility.     

Wearable Electrochemical Sensors Based on Nanomaterials for Healthcare Applications

Wearable electrochemical sensors have attracted great interest in health care applications because of their flexibility, biocompatibility, low cost and light weight. This review briefly focuses on the main concepts and methods that are related to the application of nanoparticles (NPs) in wearable electrochemical sensors. Moreover, attempts to bring together different perspectives and terms that are commonly used in NPs-based wearable electrochemical sensors along with the introduction and discussion of common manufacturing methods and recent achievements. In the end, future challenges and prospects are also discussed on the development of wearable electrochemical sensors based on nanoparticles.     

An Organodiselenide Comediator to Facilitate Sulfur Redox Kinetics in Lithium–Sulfur Batteries with Encapsulating Lithium Polysulfide Electrolyte

Lithium–sulfur (Li–S) batteries are regarded as promising high-energy-density energy storage devices. However, the cycling stability of Li–S batteries is restricted by the parasitic reactions between Li metal anodes and soluble lithium polysulfides (LiPSs). Encapsulating LiPS electrolyte (EPSE) can efficiently suppress the parasitic reactions but inevitably sacrifices the cathode sulfur redox kinetics. To address the above dilemma, a redox comediation strategy for EPSE is proposed to realize high-energy-density and long-cycling Li–S batteries. Concretely, dimethyl diselenide (DMDSe) is employed as an efficient redox comediator to facilitate the sulfur redox kinetics in Li–S batteries with EPSE. DMDSe enhances the liquid–liquid and liquid–solid conversion kinetics of LiPS in EPSE while maintains the ability to alleviate the anode parasitic reactions from LiPSs. Consequently, a Li–S pouch cell with a high energy density of 359 Wh kg⁻¹ at cell level and stable 37 cycles is realized. This work provides an effective redox comediation strategy for EPSE to simultaneously achieve high energy density and long cycling stability in Li–S batteries and inspires rational integration of multi-strategies for practical working batteries.     

Water-Driven Synthesis of Deep-Blue Perovskite Colloidal Quantum Wells for Electroluminescent Devices

Perovskite colloidal quantum wells (QWs) are promising to realize narrow deep-blue emission, but the poor optical performance and stability suppress their practical application. Here, we creatively propose a water-driven synthesis strategy to obtain size-homogenized and strongly confined deep-blue CsPbBr₃ QWs, corresponding to three monolayers, which emit at the deep-blue wavelength of 456 nm. The water controls the orientation and distribution of the ligands on the surface of the nanocrystals, thus inducing orientated growth through the Ostwald ripening process by phagocytizing unstable nanocrystals to form well-crystallized QWs. These QWs present remarkable stability and high photoluminescence quantum yield of 94 %. Furthermore, we have prepared light-emitting diodes based on the QWs via the all-solution fabrication strategy, achieving an external quantum efficiency of 1 % and luminance of 2946 cd m⁻², demonstrating state-of-the-art brightness for perovskite QW-based LEDs.     

Complete Peripheral Fluorination of the Small-Molecule Acceptor in Organic Solar Cells Yields Efficiency over 19 %

Due to the intrinsically flexible molecular skeletons and loose aggregations, organic semiconductors, like small molecular acceptors (SMAs) in organic solar cells (OSCs), greatly suffer from larger structural/packing disorders and weaker intermolecular interactions comparing to their inorganic counterparts, further leading to hindered exciton diffusion/dissociation and charge carrier migration in resulting OSCs. To overcome this challenge, complete peripheral fluorination was performed on basis of a two-dimensional (2D) conjugation extended molecular platform of CH-series SMAs, rendering an acceptor of CH8F with eight fluorine atoms surrounding the molecular backbone. Benefitting from the broad 2D backbone, more importantly, strengthened fluorine-induced secondary interactions, CH8F and its D18 blends afford much enhanced and more ordered molecular packings accompanying with enlarged dielectric constants, reduced exciton binding energies and more obvious fibrillary networks comparing to CH6F controls. Consequently, D18:CH8F-based OSCs reached an excellent efficiency of 18.80 %, much better than that of 17.91 % for CH6F-based ones. More excitingly, by employing D18-Cl that possesses a highly similar structure to D18 as a third component, the highest efficiency of 19.28 % for CH-series SMAs-based OSCs has been achieved so far. Our work demonstrates the dramatical structural multiformity of CH-series SMAs, meanwhile, their high potential for constructing record-breaking OSCs through peripheral fine-tuning.     

Site-Selective C−H Allylation of Alkanes: Facile Access to Allylic Quaternary sp3-Carbon Centers

The construction of allylic quaternary sp³-carbon centers has long been a formidable challenge in transition-metal-catalyzed alkyl-allyl coupling reactions due to the severe steric hindrance. Herein, we report an effective carbene strategy that employs well-defined vinyl-N-triftosylhydrazones as a versatile allylating reagent to enable direct assembly of these medicinally desirable structural elements from low-cost alkane feedstocks. The reaction exhibited excellent site selectivity for tertiary C−H bonds, broad scope (>60 examples and >20 : 1:0 r. r.) and good efficiency, even on a gram-scale, making it a convenient alternative to the well-known Trost–Tsuji allylation reaction for the formation of alkyl–allyl bonds. Combined experimental and computational studies were employed to unravel the mechanism and origin of site- and chemoselectivity of the reaction.     

Self-assembly of organic-inorganic hybrid materials constructed from eight-connected coordination polymer hosts with nanotube channels and polyoxometalate guests as templates

Two polyoxometalate-templated organic-inorganic hybrid porous frameworks, namely, [Cu2(H2O)2(bpp)2Cl][PM12O40].approximately 20H2O (for 1, M = W; for 2, M = Mo; bpp = 1,3-bis(4-pyridyl)propane), were self-assembly obtained and structurally determined by elemental analyses, inductively coupled plasma analyses, infrared spectroscopy, and single-crystal X-ray diffraction analyses. Single-crystal X-ray analysis of these crystals revealed that both of the structures are constructed from eight-connected three-dimensional coordination polymer hosts [Cu2(H2O)2(bpp)2Cl]n(3n+) and ball-shaped Keggin-type guests [PM12O40]n(3n-) as templates. The polymer hosts resulted from a bcc-type framework with nanotubes, and the nanotubes can be regarded as a tetra-stranded helix structure. Furthermore, compounds 1 and 2 exhibit photoluminescent properties at ambient temperature, and the compound 2 bulk-modified carbon paste electrode ( 2-CPE) displays good electrocatalytic activity toward the reduction of nitrite.     

新型碳材料在钙钛矿太阳电池中的应用研究进展

新型碳材料如石墨烯及其氧化物、碳纳米管、富勒烯及石墨炔等因其优异的热学、力学、电学、光学性能成为了钙钛矿太阳电池研究的又一亮点. 本文总结了新型碳材料在钙钛矿太阳电池对电极、电子传输材料及空穴传输材料中的研究进展, 新型碳材料的引入有效地提高了钙钛矿电池的性能, 为下一步新型碳材料的应用开发以及钙钛矿电池器件的研究提供了新的思路.     

一种基于激光辐照热效应的薄膜参数反演方法

本文研究并建立了一种基于激光辐照热效应的薄膜参数反演方法.首先给出激光辐照薄膜产生温升问题的热传导理论模型,并利用拉普拉斯变换得到了膜层和基底温度场的解析解;然后以膜层和基底的导热系数为反演参数,基于非线性共轭梯度算法给出反演基本原理及流程,并推导得到了反演过程中灵敏度系数的解析表达式;以aluminum,silver,copper和gold四种金属薄膜为例,通过与有限元法的计算结果对比验证了温度场解析解的正确性;最后结合四种金属薄膜进行了参数反演,通过考察分析不同随机噪声等条件下的参数反演结果,验证了本文方法在薄膜参数反演精度与反演效率等方面的有效性.反演结果显示:本文方法具有较高的反演精度和效率,在迭代截止误差为10~(-7)时只需用少于20次迭代就能收敛;在测量数据中加入的随机噪声越小,反演的迭代收敛次数就越少,即使是在迭代初值与反演结果相差较大时,用包含5%随机噪声的测量数据反演也能快速收敛.本文提出的薄膜参数反演方法不仅适用于反演导热系数,也可扩展用于反演膜层反射系数或吸收率等参数,具有一定的适用性.本文方法对于激光加工或激光损伤过程中的参数反演及优化具有一定的指导意义.     

反对角算子矩阵及其平方的(ω)性质的摄动

设H为复的无限维可分的Hilbert空间,B(H)为H上的有界线性算子的全体.若σ_a(T)\σ_(ea)(T)=π_(00)(T),则称T∈B(H)满足(ω)性质,其中σ_a(T)和σ_(ea)(T)分别表示算子T的逼近点谱和本质逼近点谱,π_(00)(T)={λ∈isoσ(T):0dimN(T-λI)∞}.T∈B(H)称为满足(ω)性质的摄动,若对任意的紧算子K,T+K满足(ω)性质.本文证明了反对角算子矩阵及其平方具有(ω)性质的摄动的等价性.