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Small · 2025 ·Vol. 21 ·期 16 ·2501370 · IF 12.1

High-Entropy Electrolytes Toward Aqueous Ammonium-Ion Batteries with High Capacity and Long Lifetime

Juan Zou,Chenyang Wang,Bi Xu,Yuanhao Shen,Ziyue Zeng,Lei Fu,Mengqi Zeng

Aqueous ammonium-ion batteries (AAIBs) enjoy the merits of resource affordability, environmental sustainability, and rapid ion transport capabilities. However, achieving both high capacity and long lifetime, which are critical performance metrics for AAIBs, presents a significant challenge. This difficulty arises from the fact that enhancing capacity, such as constructing multiple active sites, often results in the degradation of the electrode structure. It is imperative to devise innovative strategies for enhancing performance of AAIBs. The novel high-entropy electrolytes (HEEs) exhibit a multi-component disordered structure that facilitates ion transport and hinders the dissolution of elements in electrode materials, showing great potential to enhance electrochemical performance. Herein, taking Prussian blue analogues (PBAs) as an illustration, high-performance AAIBs are devised by constructing HEEs. Benefiting from the synergistic effect of multiple cationic additives, ultra-stable electrode materials are obtained while maintaining their inherent high capacity. When using HEEs, it demonstrates remarkable performance with a specific capacity of 86.8 mAh g −1 and cycling stability of 1700 cycles at 0.2 A g −1 . Furthermore, the assembled full battery presents a stable lifespan, demonstrating the significance of HEEs for the practical application of AAIBs, thus laying out a blueprint for large-scale energy storage.

CAS / MDL: 10026-22-9 10031-43-3
研究领域: 材料科学 · 电化学
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Advanced Optical Materials · 2025 · IF 7.2

Dual-Emission Self-Protective Phosphorescent Carbon Dots with Ultra-Long Lifetime and Time-Dependent Afterglow Colors for Tri-Mode Encryption

Yueyue Wu,Zifan Li,Zhe Zhou,Zicheng Zhang,Duoyi Zhu,Xuemei Dong,Fei Xiu,Wei Huang,Juqing Liu

Developing matrix-free phosphorescent carbon dots (CDs) with tunable color emission and exceptionally long lifetimes is highly desirable for sophisticated information encryption. However, the majority of reported matrix-free CDs demonstrate only single-color emission and short lifetimes, restricting their practical applications. Herein, dual-emission self-protective room temperature phosphorescent CDs (DE-CDs) with ultra-long lifetimes and time-dependent afterglow colors are prepared. These DE-CDs are synthesized through a microwave heating process involving 1-butylamine and phosphoric acid aqueous solution. By adjusting excitation wavelength, they display green and yellow phosphorescence with ultra-long lifetimes of up to 1.25 and 1.74 s, respectively, representing the longest lifetime among matrix-free green and yellow CDs to date. The dual emission is attributed to the coexistence of a high-energy state within the carbon core and a low-energy state associated with C─N/C═N bonds on DE-CDs surface. The ultra-long lifetimes originate from the self-protective internal hydrogen bonds formed between P and N heteroatom-containing functional groups on the dot surface, which stabilize the emissive species. Intriguingly, under 365 nm irradiation, the afterglow color transitions from yellow to green due to differing triplet-state decay rates. Leveraging these time-dependent afterglow colors, a triple-code mode is achieved for advanced dynamic encryption.

CAS / MDL: 109-73-9
研究领域: 材料科学 · 光学 · 信息加密技术
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Low-Strain Reticular Sodium Manganese Oxide as an Ultrastable Cathode for Sodium-Ion Batteries

Wen-Jing Shi,Ding Zhang,Xiao-Meng Meng,Chen-Xun Bao,Shou-Dong Xu,Liang Chen,Xiao-Min Wang,Shi-Bin Liu,Yu-Cheng Wu

Sodium-ion batteries (SIBs) are recognized as attractive alternatives for grid-scale electrochemical energy storage applications. Transition metal oxide cathodes represent one of the most dynamic materials for industrialization among the various cathodes for SIBs. Here, a cation-doped cathode Na0.44Mn0.89Ti0.11O2 with a tunnel structure is introduced, which undergoes a lowered volume change of only 5.26% during the Na+ insertion/extraction process. Moreover, the average Na+ diffusion coefficients are enhanced by more than 3-fold upon the doping of the Ti cation. The obtained cathode delivers a practically usable capacity of 119 mAh g–1 at 0.1 C as well as an enhanced discharge capacity of 96 mAh g–1 at 5 C. Durability is demonstrated by the retained 71 mAh g–1 after 1000 cycles, corresponding to a capacity retention of 74%. This work demonstrates that the reticular Na0.44Mn0.89Ti0.11O2 is a promising ultrastable cathode material for the development of long-life sodium-ion batteries.

研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry C · 2020 ·Vol. 8 ·期 29 ·10031-10038 · IF 7.059

Energy-saving and long-life electrochromic materials of naphthalene diimide-cored pyridinium salts

Feng Li,Zhen-jie Huang,Qian-hua Zhou,Ming-yue Pan,Qian Tang,Cheng-bin Gong

Developing electrochromic materials with energy-saving (i.e., low driving voltage) and long-life (i.e., high switching stability) properties is highly desirable with respect to practical application. In this work, we report the synthesis of two N,N′-di(4-pyridyl)-1,4,5,8-naphthalene diimide derivatives (DPNDIs), (Me2DPNDI)·(2I) and (benzyl2DPNDI)·(2Br), and the characterization of their electrochemical and electrochromic properties. Both DPNDIs showed two quasi-reversible redox couples in the cyclic voltammograms with cathodic peak potentials of approximately −0.30 and −0.70 V vs. Ag/Ag+. The electrochromic devices based on ((Me2DPNDI)·(2I) and (benzyl2DPNDI)·(2Br)) gave a colored state of dark orange and orange, respectively, which are colored states that have rarely been reported, and both DPNDIs had a low onset bias of −0.7 V and good switching stabilities (the change in optical contrast after 7200 s of <4%). The introduction of pyridinium salts at the DPNDI core enhanced its solubility and switching stability. In combination with density functional theory (DFT) calculations, it was shown that the formation of pyridinium salts modified the electronic properties of 1,4,5,8-naphthalenetetracarboxylic dianhydride (NDA) and DPNDI, and both pyridinium salt and NDA units contributed to electrochemical reduction. The results demonstrate that (Me2DPNDI)·(2I) and (benzyl2DPNDI)·(2Br) are promising electrochromic materials and can be used in energy-saving buildings, smart windows, traffic signs, electronic paper, sunglasses, and anti-glare rearview mirrors.

研究领域: 材料科学 · 化学
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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 38 ·21695-21702 · IF 12.732

Multifunctional SnSe–C composite modified 3D scaffolds to regulate lithium nucleation and fast transport for dendrite-free lithium metal anodes

Xiaojie Shen,Guangyu Zhao,Xianbo Yu,Huihuang Huang,Ming Wang,Naiqing Zhang

Undesirable lithium dendrite growth limits the application of lithium metal anodes in high-energy storage batteries. Here, multifunctional SnSe–C composite modified 3D scaffolds are constructed to achieve dendrite-free lithium deposition. During the initial lithiation stage, the porous SnSe–C composite converts into a Li–Sn alloy and Li2Se by lithium reduction. The lithiophilic Li–Sn alloy exhibits a low nucleation barrier and realizes homogeneous lithium nucleation. The reductive product Li2Se with a high ionic conductivity facilitates lithium ion transport, which helps realizing the homogeneous lithium ion flux and reducing concentration polarization. Benefitting from the synergistic effect of the Li–Sn alloy and Li2Se, the Li/SnSe–C anode exhibits an ultralong lifespan over 1100 h with a low overpotential of 18 mV. In full-cell configurations with LiFePO4 cathodes, the Li/SnSe–C anode demonstrates enhanced rate capability and cycle stability with a high-capacity retention of 85% over 750 cycles. This work prepares multifunctional SnSe–C composite modified 3D scaffolds to regulate lithium nucleation and transport, which offers new insights and opportunities for developing dendrite-free lithium metal battery technology.

研究领域: 材料科学 · 电化学 · 储能技术
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Nanoscale · 2021 ·Vol. 13 ·期 16 ·7744-7750 · IF 7.79

A yolk–shell Fe3O4@void@carbon nanochain as shuttle effect suppressive and volume-change accommodating sulfur host for long-life lithium–sulfur batteries

Ting Zhou,Zihan Shen,Yong Wu,Tianli Han,Mengfei Zhu,Xue Qiao,Yajun Zhu,Huigang Zhang,Jinyun Liu

A lithium–sulfur (Li–S) battery is considered a promising next-generation secondary battery owing to its high theoretical capacity and energy density. However, the volume change and poor conductivity of sulfur, and the shuttle effect, restrict its practical applications. Herein, we develop a yolk–shell Fe3O4@S@C nanochain as the Li–S battery cathode in which sulfur is encapsulated between the Fe3O4 core and the carbon shell. After cycling 500 times at 0.2C, the Fe3O4@S@C nanochains exhibit a stable capacity of 625 mA h g−1 and a coulombic efficiency exceeding 99.8%. When measuring at temperatures of −5 and 45 °C, the capacities remain stable, and a well-reversible rate performance under repeated testing for three rounds is also achieved. Furthermore, density functional theory (DFT) calculations show large adsorption energies of Fe3O4 towards polysulfides, indicating the capability of suppressing the shuttle effect during long-term charge and discharge.

研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry C · 2020 ·Vol. 8 ·期 11 ·3678-3687 · IF 7.059

Photon upconversion afterglow materials toward visualized information coding/decoding

Xinxin Han,Enhai Song,Yayun Zhou,Tao Hu,Zhiguo Xia,Qinyuan Zhang

The development of a luminescent material with visualized afterglow plays a crucial role in information security. Herein, a long-lived phosphor, KCaF3:Yb3+,Mn2+, with a visualized photon upconversion (UC) afterglow is presented. The UC emission spectrum consists of a high color purity (∼99.33%) yellow emission band peaking at ∼570 nm, and the UC afterglow signal can be observed by the naked eye in both bright and dark fields even at a high temperature of 200 °C. Moreover, the demonstration background and pigments have little influence on the UC afterglow identification. The density functional theory (DFT) calculations and the up-/down-conversion luminescence characteristics suggest that the UC afterglow originates from the long-lived exchange coupled Yb3+–Mn2+ dimers formed in KCaF3:Yb3+,Mn2+, which is independent of the conventional “afterglow trap”. The random distribution characteristics of Mn2+, and the oxygen ion (O2−) introduced by Yb3+ non-equivalent doping are the key factors for forming the efficient UC emission center in this system. Using the photon UC afterglow phosphor in screen printing ink, a visualized information encoding/decoding prototype suitable for both human and machine fast identification is demonstrated.

研究领域: 材料科学 · 光学 · 信息安全
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CHEMISTRY-A EUROPEAN JOURNAL · 2020 ·Vol. 26 ·期 26 ·5818-5823 · IF 4.857

Graphene/Amorphous Carbon Restriction Structure for Stable and Long-Lifespan Antimony Anode in Potassium-Ion Batteries

Xu Yang,Rongyu Zhang,Shifeng Xu,Dan Xu,Jia Ma,Zhongyu Zhang,Shu Yang

Graphical Under cover : A graphene/amorphous carbon restriction structure is designed for an Sb anode, in which the anode is protected from pulverization and aggregation, thus leading to the excellent stability and long lifespan of Sb in K-ion batteries. Sb-based materials have attracted much attention owing to their ability to undergo a multi-electron alloy reaction with K + . However, there are still the serious problems of volume change and aggregation of particles, which lead to rapid capacity fading and a limited lifespan. In this work, a graphene/amorphous carbon restriction structure is proposed, in which the amorphous carbon layer on the surface of Sb nanoparticles can protect the particles from pulverization, and the graphene can buffer the volume change of the material. In addition, the conductive network formed by the dual carbon structure effectively improves the rate performance of the material. Thus, the material delivers a high capacity of 550 mA h g −1 at 100 mA g −1 , a rate capability of 370 mA h g −1 at 2000 mA g −1 , and a long lifespan of 350 cycles without significant capacity fading. The dual carbon strategy proposed offers a reference for the design of high-performance anode materials.

研究领域: 材料科学 · 能源存储技术
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ADVANCED MATERIALS · 2025 · IF 26.8

Construction of Acceptor-Multi-F State Electrolyte to Enable Unprecedented Long-Life and High-Capacity Fluoride-Ion Batteries

Decheng Li,Guyue Li,Yifan Yu,Chilin Li

Fluoride ion batteries (FIBs) have garnered significant attention due to their ultrahigh theoretical energy density, dendrite-free safety, and resource abundance. Although some anion acceptors have been proposed to address the insolubility of inorganic fluoride salts, the difficulty in dissociating fluoride ions from acceptors results in short lifespan and extremely low specific capacity of FIBs. Here, a fluoride ion battery is demonstrated with unprecedented long life and ultrahigh specific capacity through the design of an acceptor-multi-F state electrolyte. The high Lewis acidity of triphenylantimony chloride (TSbCl) as a novel anion acceptor in electrolyte facilitates the complete dissociation of CsF, and the resulting TSbCl-F complex can further interact with fluoride ions to form the acceptor-multi-F states. This strategy combines the high dissociation capability for fluoride salts with the minimal thermodynamic barriers for releasing fluoride ions at electrode-electrolyte interface. This electrolyte design endows FIBs with durable reversible fluorination/defluorination reaction (3700 cycles with high coulombic efficiency of 99.5% and small voltage polarization of 30 mV) and ultrahigh reversible capacity (580 mAh g −1 after 40 cycles at 100 mA g −1 ). The high-output voltage FIBs of CuF 2 //Li configuration (with discharge plateau of 2.9 V) and larger-sized pouch-type FIBs of CuF 2 //Sn+SnF 2 configuration (with reversible capacity of 530 mAh g −1 ) are demonstrated.

研究领域: 材料科学 · 电化学
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Advanced Optical Materials · 2024 · IF 8

Dynamic Long-Afterglow Materials with Ultralong Lifetime for Advanced Message Encryption

Zhaorun Tang,Jianwen Zeng,Yuewei Zheng,Zhihao Guan,Xinghai Liu

Ultralong afterglow materials has special optical properties and a broad application prospect in the field of information encryption. A single afterglow color largely limits the application of afterglow materials in the direction of advanced encryption, and materials with dynamic afterglow are more popular. However, most of the dynamic afterglow materials are doped with multiple chromophores, and these materials with a single chromophore are rarely reported and have low lifetimes. Herein, a series of dynamic afterglow materials with time-dependent phosphorescence is obtained by a simple one-step strategy, and the longest lifetime reached 1.39 s, the maximum PLQY reached 85.9%, and the naked-eye duration reached 20 s, which is the best level reported so far. The dynamic afterglow phenomenon is attributed to the multiple phosphorescence emission centers of the guest molecule with different decay rates, which results in a dynamic shift of the phosphorescence color. It is demonstrated through a series of characterizations that the covalent bonding interaction between the guest molecule and the host boric acid largely inhibits the nonradiative leaps of the guest molecule and provides it with a rigid matrix environment. Crucially, the dynamic afterglow material has been successfully applied in the field of displays and advanced information encryption.

研究领域: 材料科学 · 光学
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EcoMat · 2022 ·Vol. 4 ·期 3 ·e12173 · IF 12.213

Assembling metal-polyphenol coordination interfaces for longstanding zinc metal anodes

Yu Huyan,Jian-Gan Wang,Shan Tian,Lingbo Ren,Huanyan Liu,Bingqing Wei

Zn metals have gained the immense attention of researchers for their wide employment as the anode of high-performance aqueous batteries. Nonetheless, the Zn anodes suffer from uncontrollable dendrite growth and parasitic side reactions, which substantially shorten the battery lifespan. This study proposes an interfacial assembly of a metal-polyphenol coordination coating on Zn anodes to regulate Zn 2+ deposition behavior. Bismush-coordinated polyphenolic ligands (i.e., tannic acid, TA) create a functional interface that could promote Zn's uniform nucleation and plating/striping kinetics. Moreover, the artificial coating acts as a physical barrier to inhibit surface corrosion. As a consequence, the TA-Bi-modified Zn anodes display a small voltage hysteresis of ~38 mV at 1 mA cm −2 over 2600 h and an ultra-long lifespan for 3100 h (~4.3 months) even at a high-current density of 10 mA cm −2 . When assembled with a vanadium-based cathode, the full Zn-ion batteries achieve improved electrochemical performance.

研究领域: 材料科学 · 电化学 · 能源存储
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RSC Advances · 2022 ·Vol. 12 ·期 32 ·20481-20491 · IF 4.036

Preparation and photodynamic antibacterial/anticancer effects of ultralong-lifetime room-temperature phosphorescent N-doped carbon dots

Yanming Miao,Xinhao Zhang,Jinyao Li,Wenli Yang,Xiaomin Huang,Jinzhi Lv

Room-temperature phosphorescent (RTP) N-doped carbon-dots (CNDs) featuring eco-friendliness, low cost and high biocompatibility, are ideal photodynamic antibacterial and anticancer nanomaterials. However, the existing CNDs are limited by low singlet oxygen (1O2) quantum yield, which has become a bottleneck in the development of CNDs. One basic reason is the short T1-state exciton lifetime of CNDs. Herein, triethylenetetramine hexaacetic acid was used to synthesize CNDs via a one-step hydrothermal method. CNDs are characterized with low toxicity, high biocompatibility and ultralong-lifetime RTP (URTP). In addition to the URTP (average lifetime 414 ms) under solid conditions, CNDs even had URTP (average lifetime 320 ms) in a water environment. The ultralong T1 exciton lifetime largely extends the collision time between T1 state excitons and O2 and prolongs the energy transfer time, not only improving the quantum yield (0.63) of singlet oxygen (1O2) in solution, but also facilitating the photodynamic antibacterial and anticancer effects.

CAS / MDL: 869-52-3
研究领域: 材料科学 · 生物医学 · 纳米技术
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