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Science China-Materials · 2021 ·Vol. 64 ·期 6 ·1378-1385 · IF 8.273

Interplay between Li3YX6 (X = Cl or Br) solid electrolytes and the Li metal anode

Fu Yuanyuan,Ma Cheng

The interplay between solid electrolytes and electrodes is of vital importance to the performance of all-solid-state Li batteries. Recently, halide superionic conductors have emerged as a new family of high-performance solid electrolytes, but their compatibility with Li metal, i.e., the anode with the highest theoretical capacity, has not been systematically studied. Here, we investigate the interaction between Li metal and two representative halide solid electrolytes: Li 3 YCl 6 and Li 3 YBr 6 . Both materials are found to form interphases with Li, similar to most solid electrolytes. However, the interphases observed here contain electronic conducting components, which are detrimental to their compatibility with Li. By elucidating this phenomenon, the present study provides guiding principles for improving the Li compatibility of halide solid electrolytes.

研究领域: 材料科学 · 电化学 · 固态离子学 · 能源存储 · 电池技术
✓ 已验证 DOI 高影响因子
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JOURNAL OF SOLID STATE CHEMISTRY · 2021 · IF 3.498

Immobilization of nickel ions by the confinement of surface aluminate spinel at low temperature

Xia Hua,Zhihong Gao,Qianqian Wang,Wenming Hao,Xiaoliang Yan,Ruifeng Li

The accumulation of heavy metal on catalysts during petrochemical process produces deactivated catalysts that cannot be directly disposed in nature, due to the high toxicity. The elimination of the detrimental effect of heavy metal ions can be achieved by immobilizing these ions in the form of spinel structure, yet this requires high-temperature calcination . Herein, Ni 2+ ions are stabilized and confined within the surface NiAl 2 O 4 on Al 2 O 3 through hydrothermal process and subsequent low-temperature thermal treatment. The formation of nickel aluminum layered double hydroxide (NiAl-LDH) as intermediate favors the generation of surface aluminate spinel at the temperature as low as 450 ​°C. The formation of surface spinel is beneficial to restricting the mobility of Ni 2+ ions. The growth and immobilization mechanisms of the surface spinel structure were proposed, which contributes to alternative and promising route for the low-temperature approach of the retention of the heavy metal ions mobility.

研究领域: 环境催化 · 材料化学 · 工业化学 · 固体化学 · 污染控制
✓ 已验证 DOI 高影响因子
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FUEL PROCESSING TECHNOLOGY · 2019 · IF 4.507

Metal-organic framework containing Brønsted acidity and Lewis acidity for efficient conversion glucose to levulinic acid

Haonan Qu,Bingyi Liu,Guohua Gao,Yiming Ma,Yanmei Zhou,Hua Zhou,Li Li,Yonghong Li,Shengjian Liu

Levulinic acid (LA) is a versatile key building block in the conversion of carbohydrates and it is an important basic chemical with various potential uses. MIL-100(Fe) loading with insoluble lysine functionalized phosphotungstic acid (Lys-PM 2 ) as heterogeneous catalysts have been synthesized for the conversion of glucose to LA in water. The optimized yield of LA is obtained by using Lys-PM 2 to catalyze glucose conversion is comparable to the majority of effective catalysts. The highest yield of LA (57.9%) is obtained at 150 °C for 9 h with 100 mg glucose and 25 mg Lys-PM 2 , since the Brønsted acidity and Lewis acidity of Lys-PM 2 . And the catalyst is able to recycle at least four times. It demonstrates the potential of Lys-PM 2 for the conversion of biomass.

研究领域: 催化化学 · 绿色化学 · 生物质能源 · 有机转化 · 材料化学 · 可持续化学
✓ 已验证 DOI 高影响因子
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Small · 2019 ·Vol. 15 ·期 30 ·1902280 · IF 10.856

High Energy Capacitors Based on All Metal-Organic Frameworks Derivatives and Solar-Charging Station Application

Xijun Wei,Wanping Hu,Huarong Peng,Yuli Xiong,Peng Xiao,Yunhuai Zhang,Guozhong Cao

High energy and efficient solar charging stations using electrochemical capacitors (ECs) are a promising portable power source for the future. In this work, two kinds of metal-organic framework (MOF) derivatives, NiO/Co 3 O 4 microcubes and Fe 2 O 3 microleaves, are prepared via thermal treatment and assembled into electrochemical capacitors, which deliver a relatively high specific energy density of 46 Wh kg −1 at 690 W kg −1 . In addition, a solar-charging power system consisting of the electrochemical capacitors and monocrystalline silicon plates is fabricated and a motor fan or 25 LEDs for 5 and 30 min, respectively, is powered. This work not only adds two novel materials to the growing categories of MOF-derived advanced materials, but also successfully achieves an efficient solar-ECs system for the first time based on all MOF derivatives, which has a certain reference for developing efficient solar-charge systems.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 可再生能源
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Improved zinc-ion storage performance of the metal-free organic anode by the effect of binder

Yu Liu,Meng Huang,Fangyu Xiong,Jiexin Zhu,Qinyou An

Zinc-ion batteries (ZIBs) using zinc metal as anode materials suffer from Zn dendrite formation and hydrogen evolution during the stripping/plating process, which will lead to performance degradation and hinder practical application. Herein, the 1,4,5,8-naphthalene diimide (NI) is proposed as a promising dendrite-free organic anode material for ZIBs . Moreover, the effect of different binders on electrochemical performance of NI electrode is investigated. Compared NI electrode with polyvinylidene fluoride (PVDF) binder, the NI electrode with the polytetrafluoroethylene (PTFE) binder shows highly enhanced rate capability (122.2 mA h g – 1 at 5 A g – 1 ) and cycling performance (123.3 mA h g – 1 at 3 A g – 1 after 2200 cycles). The improvement cycling stability of NI is attributed to PTFE binder, which effectively maintains electrode structure and inhibits dissolution of organic molecules during the cycling process. In addition, the ion kinetics analyses reveal that the superior rate capability is provided by the capacitive charge storage. And the carbonyl group of NI is active center of electrochemistry, which is revealed by in-situ attenuated total reflection–Fourier transform infrared (ATR-FTIR) and ex-situ Raman. Besides, the aqueous Zn-ion full cell based on metal-free NI anode and Prussian blue analogues (PBAs) cathode exhibits excellent rate capability (113.9 mA h g – 1 at 10.0 A g – 1 ), high operation voltage of ~ 1.2 V (at 1.0 A g – 1 ) and energy density of 50.2 Wh kg total – 1 . This work may provide a new design inspiration to develop organic dendrite-free zinc anodes for high-performance aqueous ZIBs batteries.

研究领域: 电化学 · 能源材料 · 电池技术 · 功能材料 · 应用化学
✓ 已验证 DOI 高影响因子
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PHYSICA B-CONDENSED MATTER · 2022 · IF 2.988

Structural and magnetic properties of CaCo2-xAs2 (x = 0–0.3) in ThCr2Si2-type structure

Wei Zhang,Zhiwei Gu,Bingbing Zong,Yueju Fu,Kai Zhang,Yubao Li

Defects is of special importance in tuning the structure and physical properties of layered materials. Here the influence of transition metal Co vacancies on the structure and magnetism in collapsed tetragonal CaCo 2- x As 2 (0 ≤  x  ≤ 0.3) solid solutions are systematically investigated. The electrical properties show metallicity in all compounds. The crystal structure refinement exhibits that the lattice constant of the c axis and c / a ratio decreases as Co vacancies increase, revealing the formation of a more collapsed tetragonal structure in CaCo 2- x As 2 . Moreover, these introduced Co vacancies suppress the antiferromagnetic Néel temperature from 80 K down to 18 K until it disappears above 10 K in CaCo 1 · 7 As 2 . X-ray photoelectron spectroscopy reveals increased Co 3+ /Co 2+ value in CaCo 2- x As 2 with higher Co vacancies, which may result in the charge balance and the gradually suppressed T N . This study offers insights into tuning and understanding the magneto-structural characteristics in ThCr 2 Si 2 -type layered materials through transition metal vacancies.

研究领域: 凝聚态物理 · 材料科学 · 固体化学 · 磁学 · 晶体工程 · 缺陷工程
✓ 已验证 DOI 高影响因子
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Advanced Optical Materials · 2022 ·Vol. 10 ·期 15 ·2200605 · IF 10.05

Highly Reversible Moisture-Induced Bright Self-Trapped Exciton Emissions in a Copper-Based Organic–Inorganic Hybrid Metal Halide

Shaofan Fang,Bo Zhou,Huixia Li,Hanlin Hu,Haizhe Zhong,Henan Li,Yumeng Shi

Metal halide perovskites are promising optoelectronic materials due to their unique luminescent properties. However, their practical application is limited by their poor chemical stability, especially in humid environments. Moisture can cause phase changes or chemical decomposition, resulting in significant fluorescence quenching. In this study, a copper-based organic–inorganic hybrid metal halide (t-BA) 3 Cu 6 I 9 is synthesized (t-BA + is the tert-butyl-ammonium ion (C(CH 3 ) 3 NH 3 + )). This material exhibits water-induced luminescence, and its chemical stability in humid environments is being investigated. Tetragonal t-BA 3 Cu 6 I 9 is not luminescent, but it reacts quickly with water in the air. The resultant (t-BA) 2 Cu 2 I 4 ·H 2 O has a broad green emission peak at 520 nm, high photoluminescence quantum yield of 59.4%. Remarkably, (t-BA) 2 Cu 2 I 4 ·H 2 O is converted back to t-BA 3 Cu 6 I 9 at temperatures above 40 °C. This phase conversion is highly repeatable, and the luminescent intensity can be fully recovered after 50 transformation cycles. The mechanism of luminescence is investigated through temperature-dependent photoluminescence spectra and theoretical calculation, which suggests that (t-BA) 2 Cu 2 I 4 ·H 2 O has a more localized charge distribution and sufficient polyhedral distortion, resulting in a bright and efficient emission from self-trapped excitons. This is the first report of water-induced luminescence in copper-based metal halides, and it paves the way for stable luminescent materials that are responsive to humidity.

研究领域: 材料化学 · 光物理学 · 无机化学 · 功能材料 · 发光材料
✓ 已验证 DOI 高影响因子
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TETRAHEDRON · 2019 ·Vol. 75 ·期 31 ·4174-4179 · IF 2.379

An internal oxidant-directing strategy enabling transition metal-free C–S bond ligation

Yingying Zuo,Feng Xiong,Jing Zhao

Organic sulfur compounds have broad applications in biology, medicine and material sciences and intensive efforts have been devoted to developing mild and general C–S bond-forming methods. However, a mild, transition-metal-free, direct C–H bond functionalization method remains elusive. Here, we report the use of an internal oxidant-directing strategy to achieve this goal. The cascade reactions described here show excellent chemoselectivity and a wide substrate scope for both oxyamines and sulfenylation reagents. This study enlarges the synthesis toolbox for preparing structurally diverse sulfilimines under mild conditions.

研究领域: 有机化学 · 合成化学 · 药物化学 · 生物医学材料 · 分子生物学
✓ 已验证 DOI 高影响因子
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Journal of Chemistry · 2021 ·Vol. 2021 ·期 1 ·5685596 · IF 2.506

A New (3, 6)-Connected Heterometallic Coordination Polymer: Therapeutic and Protective Effect on Ischemic Cerebral Infarction

Jia Ma,Jianer Wang,Yuping He,Yiwei Huang,Yejun Chen

Solvothermal reaction of 4,4’,4’-nitrilotribenzoic acid (H 3 TCA) with Ca(NO 3 ) 2 ·4H 2 O and Cd(NO 3 ) 2 ·4H 2 O successfully afforded a heterometallic compound, that is, [Cd 2 Ca(TCA) 2 (DMA) 2 (H 2 O) 3 ] n ·2n(DMA) ( 1 , DMA = N,N’-dimethylacetamide). The structure of 1 was further characterized through EA, diffraction of single crystal X-ray, and thermogravimetric analysis (TGA) together with powder X-ray diffraction (PXRD). Moreover, complex 1 ’s luminescent performance in solid state was also discussed at environmental temperature. The applications on the ischemic cerebral infarction therapy were evaluated, and the specific mechanism was investigated at the same time. Firstly, the hypersensitivity C-reactive protein (hs-CRP) content in human brain microvascular endothelial cell (HBMEC) was measured with real-time reverse transcription-polymerase chain reaction (RT-PCR). Then, interleukin-18 and interleukin-1 β content released through the HBMEC was detected with enzyme-linked immunosorbent assay (ELISA).

研究领域: 生物无机化学 · 神经药理学 · 炎症生物学 · 转化医学 · 分子影像学
✓ 已验证 DOI 高影响因子
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PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION · 2018 ·Vol. 35 ·期 4 ·1700471 · IF 4.384

Gold-Cluster-Based Dual-Emission Nanocomposite Film as Ratiometric Fluorescent Sensing Paper for Specific Metal Ion

Shanliang Song,Chuanxi Wang,Yue Zhao,Tantan Hu,Xinxin Zhou,Tianxin Zhao,Minghui Yang,Quan Lin

A dual-emission ratiometric fluorescent sensing film for metal ion detection is designed. This dual-emission film is successfully prepared from chitosan, graphitic carbon nitride (g-C 3 N 4 ), and gold nanoclusters (Au NCs). Here, it is shown that the g-C 3 N 4 not only serves as the fluorescence emission source, but also enhances the mechanical and thermal stability of the film. Meanwhile, the Au NCs are adsorbed on the surface of chitosan film by the electrostatic interaction. The as-prepared dual-emission film can selectively detect Cu 2+ , leading to the quench of red fluorescence of Au NCs, whereas the blue fluorescence from g-C 3 N 4 persists. The ratio of the two fluorescence intensities depends on the Cu 2+ concentration and the fluorescence color changes from orange red to yellow, cyan, and finally to blue with increasing Cu 2+ concentration. Thus, the as-prepared dual-emission film can be worked as ratiometric sensing paper for Cu 2+ detection. Furthermore, the film shows high sensitivity and selectivity, with low limit of detection (LOD) (10 ppb). It is observed that this novel gold-cluster-based dual-emission ratiometric fluorescent sensing paper is an easy and convenient way for detecting metal ions. It is believed that this research work have created another avenue for the detection of metal ions in the environment.

研究领域: 分析化学 · 环境科学 · 材料科学 · 纳米技术 · 生物传感器 · 环境监测 · 分子探针
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Anion receptor and heavy metal-free redox mediator decorated separator for lithium-sulfur batteries

Xin Guan,Huijie Pei,Xiaoyu Chen,Chen Chang,Siyuan Shao,Yu-Mo Zhang,Xingping Zhou,Hui Nie,Xiaolin Xie

The adsorption-catalysis synergy for accelerated conversion of polysulfides is critical toward the electrochemical stability of lithium-sulfur battery (LSB). Herein, a non-metallic polymer network with anion receptor units, trifluoromethanesulfonyl (CF 3 SO 2 -) substituted aza-ether, was in-situ integrated on PE separator, working as an efficient host for anchoring lithium thiophosphates (LPS) as redox mediators and polysulfides through Lewis acid-base interaction. The anchored LPS on the modified PE separator displayed a robust chemical adsorption ability towards polysulfides through the formation of S S bond. Meanwhile, LPS decreased the energy barrier of Li 2 S nucleation and promoted redox reaction kinetics. The battery with LPS decorated separator revealed a long cycling lifespan with a per cycle decay of 0.056 % after 600 cycles, and a competitive initial capacity of 889.1 mAh/g when the of sulfur cathode increased to 3 mg cm −2 . This work developed a new design strategy to promote the utilization of lithium phosphorus sulfide compounds in LSB.

研究领域: 电化学 · 能源材料 · 纳米材料 · 界面化学 · 储能技术
✓ 已验证 DOI 高影响因子
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Small · 2024 ·Vol. 21 ·期 4 ·2410657 · IF 13

2D MOF Structure Tuning Atomic Ru Sites for Efficient and Robust Proton Exchange Membrane Water Electrolysis

Jia Wang,De Wang,Zelin Zhao,Ganggang Chang,Wei Guo,Jun Xu,Yinyu Xiang,Junrui Li,Junsheng Li

Developing cost-effective ruthenium (Ru)-based HER electrocatalysts as alternatives to commercial Pt/C is crucial for the advancement of proton exchange membrane water electrolysis (PEMWE). However, the strong hydrogen adsorption of Ru-based catalysts restricts its activity. Herein, a strategy is reported to tune the electronic structure and improve mass transfer by implanting Ru atoms onto the (002) facet of two-dimensional zeolitic imidazolate framework-67 (Ru@ L ZIF (002) ) to optimize the d -band center ( ε d ) of Ru and the hydrogen spillover behavior. Benefiting from the ultrathin nanosheet structure and optimized ε d of Ru, the over-strong H adsorption energy is weakened and the electron/mass transfer is facilitated. Ru@ L ZIF (002) exhibits an overpotential of 9.2 mV at 10 mA cm −2 and a long-lasting stability of 35 days at 100 mA cm −2 . The mass activity and price activity of Ru@ L ZIF (002) is 2.9 and 14.7 times higher than Pt/C, respectively. More impressively, Ru@ L ZIF (002) delivers a cell voltage of 2.01 V at a high current density of 4 A cm −2 in PEMWE. The excellent long-term durability of 1200 hours operating at 4 A cm −2 with an ultralow decay rate of 7.5 × 10 −3 mV h −1 has been achieved, making it promising as a cost-effective alternative to Pt/C catalyst for PEMWE applications.

研究领域: 电催化 · 材料科学 · 能源化学 · 纳米材料 · 电化学工程 · 可持续能源技术
✓ 已验证 DOI 高影响因子
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