Progress of Phosphate-based Polyanion Cathodes for Aqueous Rechargeable Zinc Batteries

Aqueous rechargeable zinc batteries (ARZBs) are recently prevailing devices that utilize the abundant Zn resources and the merits of aqueous electrolytes to become a competitive alternative for large-scale energy storage. Benefiting from the unique inductive effect and flexible structure, the past five years have experienced a diversiform of phosphate-based polyanion materials that are used as cathodes in ARZBs. In this review, the most recent advances in the Zn²⁺ storage mechanisms and electrolyte optimization of the phosphate-based cathodes of ARZBs, which mainly focus on vanadium/iron-based phosphates and their derivatives are presented. Furthermore, in addition to significant progress on polyanion phosphate-based cathode materials, the design strategies both for electrode materials and compatible electrolytes are also elaborated to improve the energy density and extend the cycling life of aqueous Zn/polyanion batteries.     

Carbon Black-Supported Single-Atom Co?N?C as an Efficient Oxygen Reduction Electrocatalyst for H2O2 Production in Acidic Media and Microbial Fuel Cell in Neutral Media

Single metal atom isolated in nitrogen-doped carbon materials (M N C) are effective electrocatalysts for oxygen reduction reaction (ORR), which produces H₂O₂ or H₂O via 2-electron or 4-electron process. However, most of M N C catalysts can only present high selectivity for one product, and the selectivity is usually regulated by complicated structure design. Herein, a carbon black-supported Co N C catalyst (CB@Co N C) is synthesized. Tunable 2-electron/4-electron behavior is realized on CB@Co-N-C by utilizing its H₂O₂ yield dependence on electrolyte pH and catalyst loading. In acidic media with low catalyst loading, CB@Co N C presents excellent mass activity and high selectivity for H₂O₂ production. In flow cell with gas diffusion electrode, a H₂O₂ production rate of 5.04 mol h⁻¹ g⁻¹ is achieved by CB@Co N C on electrolyte circulation mode, and a long-term H₂O₂ production of 200 h is demonstrated on electrolyte non-circulation mode. Meanwhile, CB@Co N C exhibits a dominant 4-electron ORR pathway with high activity and durability in pH neutral media with high catalyst loading. The microbial fuel cell using CB@Co N C as the cathode catalyst shows a peak power density close to that of benchmark Pt/C catalyst.     

Ultraefficient Non-Doped Deep Blue Fluorescent OLED: Achieving a High EQE of 10.17% at 1000 cd m−2 with CIEy<0.08

The pursuit for efficient deep blue material is an ever-increasing issue in organic optoelectronics field. It is a long-standing challenge to achieve high external quantum efficiency (EQE) exceed 10% at brightness of 1000 cd m⁻² with a Commission International de L'Eclairage (CIE_y) <0.08 in non-doped organic light-emitting diodes (OLEDs). Herein, this study reports a deep blue luminogen, PPITPh, by bonding phenanthro[9,10-d]imidazole moiety with m-terphenyl group via benzene bridge. The non-doped OLED based on PPITPh exhibits an exceptionally high EQE of 11.83% with a CIE coordinate of (0.15, 0.07). The EQE still maintains 10.17% at the brightness of 1000 cd m⁻², and even at a brightness as high as 10000 cd m⁻², an EQE of 7.5% is still remained, representing the record-high result among non-doped deep-blue OLEDs at 1000 cd m⁻². The unprecedented device performance is attributed to the reversed intersystem crossing process through hot exciton mechanism. Besides, the maximum EQE of orange phosphorescent OLED with PPITPh as host is 32.02%, and remains 31.17% at the brightness of 1000 cd m⁻². Such minimal efficiency roll-off demonstrates that PPITPh is also an excellent phosphorescent host material. The result offers a new design strategy for the enrichment of high-efficiency deep blue luminogen.     

In Situ Topochemical Transformation of ZnIn2S4 for Efficient Photocatalytic Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran

Photocatalytic selective oxidation of 5-hydroxymethylfurfural (HMF) coupled H₂ production offers a promising approach to producing valuable chemicals. Herein, an efficient in situ topological transformation tactic is developed for producing porous O-doped ZnIn₂S₄ nanosheets for HMF oxidation cooperative with H₂ evolution. Aberration-corrected high-angle annular dark-field scanning TEM images show that the hierarchical porous O-ZIS-120 possesses abundant atomic scale edge steps and lattice defects, which is beneficial for electron accumulation and molecule adsorption. The optimal catalyst (O-ZIS-120) exhibits remarkable performance with 2,5-diformylfuran (DFF) yields of 1624 µmol h⁻¹ g⁻¹ and the selectivity of >97%, simultaneously with the H₂ evolution rate of 1522 µmol h⁻¹ g⁻¹. Mechanistic investigations through theoretical calculations show that O in the O-ZIS-120 lattice can reduce the oxidation energy barrier of hydroxyl groups of HMF. In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) results reveal that DFF^* (C₄H₂(CHO)₂O^*) intermediate has a weak interaction with O-ZIS-120 and desorb as the final product. This study elucidates the topotactic structural transitions of 2D materials simultaneously with electronic structure modulation for efficient photocatalytic DFF production.     

Optoelectronic Synapses and Photodetectors Based on Organic Semiconductor/Halide Perovskite Heterojunctions: Materials,Devices, and Applications

Both photodetectors (PDs) and optoelectronic synaptic devices (OSDs) are optoelectronic devices converting light signals into electrical responses. Optoelectronic devices based on organic semiconductors and halide perovskites have aroused tremendous research interest owing to their exceptional optical/electrical characteristics and low-cost processability. The heterojunction formed between organic semiconductors and halide perovskites can modify the exciton dissociation/recombination efficiency and modulate the charge-trapping effect. Consequently, organic semiconductor/halide perovskite heterojunctions can endow PDs and OSDs with high photo responsivity and the ability to simulate synaptic functions respectively, making them appropriate for the development of energy-efficient artificial visual systems with sensory and recognition functions. This article summarizes the recent advances in this research field. The physical/chemical properties and preparation methods of organic semiconductor/halide perovskite heterojunctions are briefly introduced. Then the development of PDs and OSDs based on organic semiconductor/halide perovskite heterojunctions, as well as their innovative applications, are systematically presented. Finally, some prospective challenges and probable strategies for the future development of optoelectronic devices based on organic semiconductor/halide perovskite heterojunctions are discussed.     

Boosting Piezo-Catalytic Activity of KNN-Based Materials with Phase Boundary and Defect Engineering

Although the piezo-catalysis is promising for the environmental remediation and biomedicine, the piezo-catalytic properties of various piezoelectric materials are limited by low carrier concentrations and mobility, and rapid electron-hole pair recombination, and reported regulating strategies are quite complex and difficult. Herein, a new and simple strategy, integrating phase boundary engineering and defect engineering, to boost the piezo-catalytic activity of potassium sodium niobate ((K, Na)NbO₃, KNN) based materials is innovatively proposed. Tur strategy is validated by exampling 0.96(K_0.48Na_0.52)Nb_0.955Sb_0.045O₃-0.04(Bi_xNa_4-3x)_0.5ZrO₃-0.3%Fe₂O₃ material having phase boundary engineering and conducted the defect engineering via the high-energy sand-grinding. A high reaction rate constant k of 92.49 × 10⁻³ min⁻¹ in the sand-grinding sample is obtained, which is 2.40 times than that of non-sand-grinding one and superior to those of other representative lead-free perovskite piezoelectric materials. Meanwhile, the sand-grinding sample has remarkable bactericidal properties against Escherichia coli and Staphylococcus aureus. Superior piezo-catalytic activities originate from the enhanced electron-hole pair separation and the increased carrier concentration. This study provides a novel method for improving the piezo-catalytic activities of lead-free piezoelectric materials and holds great promise for harnessing natural energy and disease treatment.     

Aperture-Adjustable and Repairable Metal-Based MOFs Catalysis Membrane for Water Purification

Precise adjustment of the pore size, damage repair, and efficient cleaning is all challenges for the wider application of inorganic membranes. This study reports a simple strategy of combining dry-wet spinning and electrosynthesis to fabricate stainless-steel metal–organic framework composite membranes characterized by customizable pore sizes, targeted reparability, and high catalytic activity for membrane cleaning. The membrane pore size can be precisely customized in the range of 14–212 nm at nanoscale, and damaged membranes can be repaired by targeted treatment in 120 s. In addition, advanced oxidation processes can be used to quickly clean the membrane and achieve 98% flux recovery. The synergistic actions of the membrane matrix and the selective layer increase the adsorption energy of active sites to oxidant, shorten the electron transfer cycle, and enhance the overall catalytic performance. This study can provide a new direction for the development of advanced membranes for water purification and high-efficiency membrane cleaning methods.     

一种临近空间高动态飞行器等离子鞘套自动判别方法

临近空间高动态飞行器在高速飞行过程中与大气强烈作用,形成十分复杂的高温等离子鞘套,改变了目标的散射回波特性,给目标探测带来不确定性,需要及时判别当前目标是否处于等离子鞘套状态。本文提出一种基于波形熵判别和变带宽确认的等离子鞘套自动判别方法,首先提取目标回波波形熵、包络长度等特征信息,利用模糊分类器进行基于波形熵的群目标判别,其次根据鞘套与目标和目标之间的距离与信号带宽的关系差异,通过检测不同带宽回波的包络长度变化,对鞘套和目标进行判别。仿真结果验证了本文所提方法的有效性。     

面向同步辐射光源图像的可并行智能压缩方法

在建的高能同步辐射光源预计会产生海量原始数据,其中硬X射线实验线站产生的图像数据占比最高且具有高分辨率和高帧率的特点,亟需有效的无损压缩方法缓解存储和传输压力,然而现有通用无损压缩方法对该类图像压缩效果不佳,基于深度学习的无损压缩方法又耗时较长。结合同步辐射光源图像的特点,提出一种在保证图像压缩比前提下的可并行智能无损图像压缩方法。通过参数自适应的可逆分区量化方法,大幅缩小图像经过时间差分后的像素值分布范围,能够节省20%以上的存储空间。将以CNN为基础架构的时空学习网络C-Zip作为概率预测器,同时以数据集为单位过拟合训练模型进一步优化图像压缩比。针对压缩过程中耗时较长的算术编码过程,利用概率距离量化代替算术编码,结合深度学习进行无损编码,增加编码过程的并行度。实验结果表明,该方法的图像压缩比相比于PNG、FLIF等传统图像无损压缩方法提升了0.23~0.58,对于同步辐射光源图像具有更好的压缩效果。     

An Artificial Autonomic Nervous System That Implements Heart and Pupil as Controlled by Artificial Sympathetic and Parasympathetic Nerves

The autonomic nervous system maintains homeostasis in organisms through complex neural pathways and responds adaptively to changes in the external and internal environment. The fabrication of an artificial autonomic nervous system is reported that replicates combined effects of sympathetic and parasympathetic nerves on cardiac activity and pupillary control, to mimic the regulation of autonomic nervous system to external changes. The artificial autonomic nerve-controlled pupil contraction and relaxation, modulating the rate of heartbeats for normal cardiac rhythm and arrhythmia as reflected by blink rates of a signal indicator. These functions are switched by using a parallel-channeled synaptic transistor with a special n-i-p heterostructure that has a 2D h-BN insulator in the middle to provide barrier against ion injection into the 2D MoS₂ bottom n-channel and enable short-term plasticity as induced by acetylcholine, and the electrochemical doping reaction occurred at the P3HT nanowire p-channels on top to enable relatively long-term plasticity as induced by noradrenaline. Low-energy consumption down to femtojoule and an ultrahigh paired-pulse facilitation index up to ≈455% are demonstrated. An artificial neural network based on device characteristics achieves a high recognition accuracy for electrocardiogram patterns. This study extends insights into artificial nerves-inspired biological signal processing and recognition.