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MOLECULES · 2024 ·Vol. 29 ·期 7 ·1432 · IF 4.2

Spherical Binderless 4A/5A Zeolite Assemblies: Synthesis, Characterization, and Adsorbent Applications

Tong Li,Shuangwei Wang,Jinqiang Gao,Ruiqiang Wang,Guifeng Gao,Guangming Ren,Shengnan Na,Mei Hong,Shihe Yang

Zeolite microspheres have been successfully applied in commercial-scale separators such as oxygen concentrators. However, further enhancement of their applications is hampered by the post-synthetic shaping process that formulates the zeolite powder into packing-sized spherical bodies with various binders leading to active site blockage and suboptimal performance. Herein, binderless zeolite microspheres with a tunable broad size range from 2 µm to 500 µm have been developed with high crystallinity, sphericity over 92%, monodispersity with a coefficient of variation (CV) less than 5%, and hierarchical pore architecture. Combining precursor impregnation and steam-assisted crystallization (SAC), mesoporous silica microspheres with a wide size range could be successfully transformed into zeolite. For preserved size and spherical morphology, a judicious selection of the synthesis conditions is crucial to ensure a pure phase, high crystallinity, and hierarchical architecture. For the sub-2-µm zeolite microsphere, low-temperature prolonged aging was important so as to suppress external zeolization that led to a large, single macroporous crystal. For the large 500 µm sphere, ultrasound pretreatment and vacuum impregnation were crucial and facilitated spatially uniform gel matrix dispersion and homogenous crystallization. The obtained zeolite 5A microspheres exhibited excellent air separation performance, while the 4A microspheres displayed ammonium removal capabilities. This work provides a general strategy to overcome the existing limitations in fabricating binder-free technical bodies of zeolites for various applications.

CAS / MDL: 7783-33-7
研究领域: 材料科学 · 化学工程
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 168 ·期 1 ·010536 · IF 4.316

Binder-Free and Flexible Carbon-Encapsulated Oxygen-Vacancy Cerium Dioxide Electrode for High-Performance Supercapacitor

Huan Kang,Liming Xu,Yue Cai,Yao He,Jingkun Xu,Weiqiang Zhou

Binder-free and flexible oxygen-vacancy CeO2@C core–shell nanocomposites directly anchored on carbon cloth (CC) are prepared via a simple two-step process, in which CeO2 nanoparticles are hydrothermally fabricated and mixed with polyvinylpyrrolidone (PVP) composites, subsequently, as-formed CeO2@PVP composites coated on CC are calcined at 700 °C. The morphologies, structures and electrochemical properties of as-obtained CeO2@C nanocomposites are studied by SEM, HRTEM, XRD, XPS and electrochemical techniques, respectively. The CeO2@C nanocomposites are composed of the CeO2 core with diameter of about 10 nm and the carbon shell with thickness of about 1.5 nm. The electrochemical results reveal that the CeO2@C nanocomposites show a wide electrochemical active window of −1.0 ∼ 0.8 V and a specific capacitance of 141.56 F g−1 at 1 A g−1 in 1.0 M Na2SO4 electrolyte. In addition, an asymmetric supercapacitor (ASC) assembled with CeO2@C and poly(3,4-ethylene dioxythiophene) (PEDOT) can work in the wide operational voltage region of 2.0 V and deliver the energy density of 11.12 Wh kg−1 at 2000 W kg−1. The present study indicates that the CeO2@C will have a greater advantage in terms of energy density for CeO2 and its carbon-based composites supercapacitor electrodes.

CAS / MDL: 9003-39-8
研究领域: 材料科学 · 电化学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2020 · IF 7.864

Binderless and Oxygen Vacancies Rich FeNi/Graphitized Mesoporous Carbon/Ni Foam for Electrocatalytic Reduction of Nitrate

Xiaotong Chen,Ting Zhang,Miao Kan,Dinggui Song,Jinping Jia,Yixin Zhao,Xufang Qian

Energy consumption and long-term stability of a cathode are two important aspects of great concern in electrocatalytic nitrate reduction. This work studied a binderless FeNi/graphitized mesoporous carbon directly formed on Ni Foam (FeNi/g-mesoC/NF, 7.3 wt % of Fe) and evaluated its electrocatalytic nitrate reduction performance. We proposed a unique structure model of FeNi/g-mesoC/NF cathode in which FeNi alloy nanoparticles were uniformly embedded in mesoporous carbon and graphitized carbon shells were coated on isolated alloy nanoparticles. Oxygen vacancies (OVs) in FeNi oxide passivating layer facilitate the conversion of NO3–-N anions on cathode. Toxic NO2–-N was almost undetected due to the synergetic effects of FeNi electrocatalysis, and the NO3–-N conversion was high in comparation with ever reported iron-based cathode. The NO3–-N conversion showed ultrahigh electrocatalytic stability during one-month-recycling test while the physiochemical properties showed negligible change for FeNi/g-mesoC/NF except the increase of OVs. The energy consumption to treat simulated underground water (50% of NO3–-N conversion) was low (0.7 kWh mol–1) for 50 mg L–1 NO3–-N. This binderless composite cathode shows great potential in electrocatalytic NO3–-N removal in underground water.

研究领域: 环境科学 · 材料科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2019 · IF 4.175

Binder-free flexible Li2ZnTi3O8@MWCNTs stereoscopic network as lightweight and superior rate performance anode for lithium-ion batteries

Chenying An,Caihui Li,Haoqing Tang,Tao Liu,Zhiyuan Tang

High performance flexible electrodes with ultrathin and ultralight characteristics are great potential as power supply for foldable and wearable electronic devices. One major problem is how to combine active material with conductive substrate firmly in the absence of polymeric binder. Here, sandwich structure of flexible electrode is successfully prepared which Li 2 ZnTi 3 O 8 @multi-walled carbon nanotubes (MWCNTs) composite as intermediate anode active ingredient and three-dimensional network MWCNTs as top and bottom conductive layers. The MWCNTs in active material and conductive layers cross-link each other to form a firm and stable three-dimensional network, which provides stereoscopic electron and ion transmission channels without metal copper substrate. This particular structure of electrode is effectively reduce the total weight and improve flexibility. Typically, the flexible Li 2 ZnTi 3 O 8 @MWCNTs electrode shows good cycling stability and achieved a high reversible capacity of 95.2 mAh g −1 after 1000 cycles at current density of 7000 mA g −1 with 89.0% capacity retention and 99% Coulombic efficiency. This study offers a new strategy for the development of high conductivity flexible electrode for wearable devices and deformable electronic devices.

研究领域: 材料科学 · 能源技术
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Small · 2022 ·Vol. 18 ·期 28 ·2202651 · IF 15.153

Interfacial Engineering of Binder-Free Janus Separator with Ultra-Thin Multifunctional Layer for Simultaneous Enhancement of Both Metallic Li Anode and Sulfur Cathode

Shuanglin Wu,Yingmei Yao,Xiaolin Nie,Zhifeng Yu,Yanting Yu,Fenglin Huang

Exploring a scalable strategy to fabricate a multifunctional separator is of great significance to overcome the challenges of lithium polysulfides (LiPSs) and dendritic growth in lithium-sulfur batteries (LSBs). Herein, a binder-free Janus separator is constructed by interfacial engineering. At the cathode interface, an ultra-thin covalent triazine piperazine film containing tailorable micropores and adsorption sites is decorated on polyacrylonitrile (PAN) membrane by in situ interfacial polymerization, building a triple barrier for LiPSs. The combination of steric hindrance and chemical adsorption reduces LiPS's migration by 81.85%. Meanwhile, at the anode interface, a fast-ionic conductor Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) is created on the surface of PAN nanofiber by magnetron sputtering to suppress dendrite growth. Even though there is no binder between the ceramic layer and the fibrous separator, sputtering creates an inter-embedded structure that ensures no depowering after cycling. Furthermore, the PAN-based separator displays a high temperature tolerance of 180 °C. Consequently, the cell delivers a high capacity of 1287.9 mAh g −1 at 0.5 C and stable cycling performance with an ultra-low capacity decay rate of 0.059% per cycle over 500 cycles. This work provides a scalable strategy for functionalizing separators to tackle the challenges in LSBs, which is binder-free, stripping-free, and essentially thickening-free.

CAS / MDL: 108-77-0
研究领域: 材料科学 · 能源存储技术
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CARBON · 2023 · IF 10.9

Selective laser carving-induced patterned electrodes for high-performance binder-free and substrate-free all-carbon-based micro-supercapacitors

Xinrui Ding,Xiaolin Xu,Zihan He,Yifu Liang,Xiaohua Wu,Zongtao Li

Activated carbon is one of the most widely used electrode materials for supercapacitors owing to its excellent porosity, large specific surface area and long cycle life. However, its utilization in electrode fabrication necessitates the incorporation of insulating binders to facilitate shaping due to its powdery nature. This may obstruct the pores and increase the internal resistance of the electrode, resulting in poor flexibility and electrochemical performance. To address this problem, an innovative and universal packaging strategy is proposed, in which composite films are prepared by double vacuum filtration, coated with gel electrolyte and then patterned by selective laser carving based on the principle of “Selective Optical Transmittance”, to achieve the fabrication of binder-free and substrate-free all-carbon-based micro-supercapacitors. The areal capacitance of obtained Activated Carbon/Super P-Reduced Graphene Oxide Micro-supercapacitors (AC/SP-rGO MSCs) without binder are three times higher than those with binder. The prepared AC/SP-rGO MSCs exhibit remarkable areal capacitance of 177.32 mF cm −2 , volumetric capacitance of 52.15 F cm −3 and high energy density of 4.44 mWh cm −3 . Meanwhile, they also exhibit excellent flexibility with no capacitance degradation after 5000 bending cycles. Specifically, the energy provided by four AC/SP-rGO MSCs connected in series can light up to 46 red LEDs or provide a thermo-hygrometer with a long endurance of over 45 min. This packaging method has proven to be an effective strategy for the fabrication of powdery materials into binder-free electrodes, presenting a unique idea for the fabrication of electrodes within the realm of flexible electronics.

研究领域: 材料科学 · 能源存储
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ENERGY & FUELS · 2020 · IF 3.421

Enhanced Performance of Adsorptive Removal of Thiophene from Model Fuel over Micro–Mesoporous Binderless ZSM-5 Prepared by In Situ Crystallization

Yonghou Xiao,Qiangqiang Xue,Kerun Zhu,Gaohong He

High-efficiency adsorbents are essential for ultradeep desulfurization through selective adsorption, which features low energy consumption without causing secondary pollution. Aluminum oxide is always added as a binder to form physically bound pellets, which weakens the adsorptive desulfurization performance. In this work, a novel micro–mesoporous binderless ZSM-5 (BL-ZSM-5) was successfully prepared through in situ crystallization, which could efficiently remove thiophene from model fuel. Desulfurization ability was investigated by static and fixed bed adsorption. The breakthrough adsorption capacity of thiophene on BL-ZSM-5 reaches 0.38 mg/g, which is twice as high as that of ZSM-5 with alumina binders (Al-ZSM-5). The improvement is attributed to the conversion of alumina into molecular sieves, which could increase the adsorption sites and provide appropriate mesoporous channels for thiophene transfer. The thermal stability of BL-ZSM-5 is superior to that of Al-ZSM-5. The adsorption performance of BL-ZSM-5 is maintained well after 6 cycles of regeneration. The results demonstrate that the attractive prospect of BL-ZSM-5 in highly efficient desulfurization of transport fuels through selective adsorption.

研究领域: 化学工程 · 环境科学
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Scientific Reports · 2015 ·Vol. 5 ·期 1 ·1-6 · IF 5.578

Flexible Membranes of MoS2/C Nanofibers by Electrospinning as Binder-Free Anodes for High-Performance Sodium-Ion Batteries

Xiong Xiaoqin,Luo Wei,Hu Xianluo,Chen Chaoji,Qie Long,Hou Dongfang,Huang Yunhui

A flexible membrane consisting of MoS 2 /carbon nanofibers has been fabricated by a simple electrospinning method. MoS 2 nanosheets are uniformly encapsulated in the inter-connected carbon nanofibers with diameters of ~150 nm. When evaluated as a binder-free electrode for sodium-ion batteries, the as-obtained electrode demonstrates high performances, including high reversible capacity of 381.7 mA h g −1 at 100 mA g −1 and superior rate capability (283.3, 246.5 and 186.3 mA h g −1 at 0.5, 1 and 2 A g −1 , respectively). Most importantly, the binder-free electrode made of MoS 2 and carbon nanofibers can still deliver a charge capacity of 283.9 mA h g −1 after 600 cycles at a current density of 100 m A g −1 , indicating a very promising anode for long-life SIBs.

CAS / MDL: 1317-33-5 25014-41-9
研究领域: 材料科学 · 能源存储 · 纳米技术
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PHYSICA STATUS SOLIDI A-APPLICATIONS AND MATERIALS SCIENCE · 2020 ·Vol. 217 ·期 8 ·1900806 · IF 1.759

K+ Intercalation of NH4HF2-Exfoliated Ti3C2 MXene as Binder-Free Electrodes with High Electrochemical Capacitance

Jingbo Li,Yu Liu,Fang Xu,Junping Hu,Nan Chen,Guoping Du,Changshuang Jiang

As a 2D material, Ti 3 C 2 (MXene) has been recently used as electrodes for electrochemical capacitors. Herein, a two-step procedure is used to obtain a highly opened layer structure for Ti 3 C 2 , which differs from the methods used in the literature for synthesizing exfoliated MXene. First, the mild NH 4 HF 2 etching agent is used to prepare the regular Ti 3 C 2 MXene. Second, KOH is added into the obtained solution for K + to intercalate the MXene. The K + intercalation is found to greatly increase the (002) crystal planar spacing of the Ti 3 C 2 from 10.8 to 12.4 Å. More importantly, this K + -intercalated MXene exhibits a highly opened layer structure, whereas the regular MXene only has a partially opened layer structure. Consequently, the former is expected to allow much more active sites exposed to liquid electrolyte, and also facilitates remarkably higher ion and electron transport efficiency. To investigate their electrochemical capacitance properties, the regular and K + -intercalated Ti 3 C 2 MXenes are used to fabricate binder-free electrodes on nickel foams by an electrophoretic deposition method. The K + -intercalated MXene-based electrode is found to have twice higher specific capacitance than the regular MXene. Furthermore, the K + -intercalated Ti 3 C 2 MXene-based electrode exhibits an excellent cyclic stability.

CAS / MDL: 1341-49-7
研究领域: 材料科学 · 电化学
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Journal of Materials Research and Technology-JMR&T · 2020 · IF 5.289

In-situ preparation and excellent performance of Co9S8/C/NF with binder-free as anodes for lithium-ion batteries

Chengli Yao,Jianglin Xu,Anjian Xie,Yuhua Shen

Nowadays, developing new anode material for lithium-ion batteries (LIBs) with distinguished electrochemical properties is still very significant and a huge challenge. Herein, a nanocomposite containing Co 9 S 8 /carbon (C)/nickel foam (NF) was synthesized. In the preparation process, ZIF-67 as the source of both Co 2+ and carbon was designedly grown in situ on the surface of NF with loose porous skeleton through the hydrothermal reaction. After sulfurization and pyrolysis of ZIF-67/NF, the porous flower-like Co 9 S 8 /C/NF composites formed. As a binder-free anode, Co 9 S 8 /C/NF exhibited excellent lithium storage performance, which showed a superior initial discharge capacity of 1926 mA h g −1 and reversible capacity of 1114 mA h g −1 after 200 cycles at 0.2 A g −1 . Even at 2 A g −1 current density, it could maintain a capacity of 578 mA h g −1 . The above outstanding electrochemical performances may be due to the following reasons. The loose flower-like structure assembled by lots of nanosheets, can provide a larger surface area for the transport and storage of Li + ions. With the cooperation of carbon matrix, the volume expansion of anodes can be effectively alleviated during charge and discharge process. At the same time, metal nickel foam as the current collector of the negative electrode also can increase the conductivity; promote the transport and diffusion of electrons. The loose skeleton enables the full contact of the active material with the electrolyte, which is beneficial to the transportation of Li + ions and electronics. This work provides an inspiration for designing and fabricating anode materials with distinguished-performance for LIBs.

研究领域: 材料科学 · 能源存储与转换
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JOURNAL OF ALLOYS AND COMPOUNDS · 2018 · IF 3.779

A N,S-codoped hierarchical carbon Foam@Porous carbon composite as freestanding cathode for high-performance lithium-sulfur batteries

He Yang,Xu Zhang,Junling Guo,Weili Zhu,Shupeng Zhao,Fang Wang,Qiuyu Fan,Hongyan Xiao,Fengxiang Zhang

Lithium sulfur (Li-S) battery is considered as one of promising energy-storage devices owing to its high energy density and low cost. However, it is still a great challenge to explore stable sulfur cathode with high sulfur loading and good cycling performance. Herein, we report a facile method to prepare N,S co-doped hierarchical pore structured carbon foam @porous carbon (CF@N-SPC) through a carbonation process from resin aerogel coated melamine foam with thiourea as the source for N and S codoping. The close combination of a carbon interconnected skeleton and the resin aerogel derived carbon forms the hierarchical pore structure that improves the electron and ion transport. The prepared CF@N-SPC can be used as a freestanding cathode without a conductive additive and a binder. Due to the synergistic effect of the hierarchical pore structure and N, S codoping, the sulfur loading in the carbon foam-based cathode can reach up to 10.6 mg cm −2 . Owing to these unique merits, the CF@N-SPC/S cathode exhibits high capacity and good cycling performance: it yields a discharge capacity of 1212 mA h g −1 at 0.1 C with 4.0 mg cm −2 sulfur loading; it also exhibits a good discharge capacity of 668 mA h g −1 at 0.5 C when the sulfur loading increases to 10.6 mg cm −2 , capacity retained by 72% in 200 cycles; it experiences a very small capacity decay rate of 0.05% per cycle in 700 cycles at 1 C. Our rational design and facile synthesis of the carbon foam-based freestanding cathode is promising and applicable for development of high performance Li-S batteries.

研究领域: 材料科学 · 能源存储技术
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Inorganic Chemistry Frontiers · 2023 ·Vol. 10 ·期 7 ·2125-2135 · IF 7

In situ growth of amorphous vanadium oxide nanospheres on carbon cloth as free-standing cathodes used in high performance aqueous zinc-ion batteries

Xuguang Han,Yan Zhang,Mengmeng Liu,Yifei Sun,Wenshan Gou,Zhao Xu,Chang Ming Li

Vanadium oxide with abundant interchangeable oxidation states and a variety of different crystal structures is considered to be the most promising Zn-ion host material for high-performance aqueous zinc-ion batteries (AZIBs). Nevertheless, certain constraints, including poor reversibility, low intrinsic conductivity, sluggish electrochemical kinetics, low density of exposed active sites, and low actual capacity of the material, limit their performance in AZIBs. In this work, we in situ grew 3D amorphous mixed-valence VOx microspheres on alkali-treated carbon cloth (VOx MSs@ACC) as cathodes for AZIBs. In comparison with a VOx MSs powder-constructed cathode, VOx MSs@ACC cathodes exhibit higher specific capacity (1.79 mA h cm−2 at 2.7 A m−2) and longer cycling performance over 2500 cycles mainly due to their faster ion transport rates, abundant ion storage sites and more effective easing of volume expansion. This work thus sheds light on the design of free-standing vanadium-based cathodes for AZIBs.

研究领域: 材料科学 · 能源存储
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