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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Performance enhancement of Hf-Ta-O nanofiber based energy storage materials using oxygen-vacancy and its application for supercapacitor

Yi Cao,Piao Ruan,YuFeng Xue,Yue Cao,Huang He,Wenfeng Qiu

Nowadays, materials that possess high activity and natural oxygen vacancy have garnered significant attention as potential electrode materials for supercapacitors . In this study, we successfully prepared the Hf 6 Ta 2 O 17 (HTO) nanofibres (NFs) with an orthorhombic superlattice structure using the electrospinning technique and sintering process. The characterization results indicate that the HTO NFs synthesized at 750 °C show good micro nanostructures and outstanding electrochemical properties . To enhance its energy storage performance, additional oxygen vacancies (OVs) were introduced through a carbothermal treatment under an Ar atmosphere. Although longer reduction reaction times can produce more OVs, the integration of grain boundaries and the growth of grain size caused by large annealing times may limit its electrochemical performance. Therefore, the HTO NFs treated for 1 h (HTO/C-1) exhibited the maximum C s of 925 F·g −1 at 1 A·g −1 with a larger voltage window of 2.1 V. Furthermore, a symmetric supercapacitor fabricated by two reduced HTO NFs electrodes and 1 M Na 2 SO 4 solution, recorded as r-HTO NFs//r-HTO NFs. The device demonstrated excellent energy density of 73.3 Wh·kg −1 (at power density of 1050 W·kg −1 ) and a long cycling life (81.8% retained after 5000 cycles). These results suggest that the optimized reduction process can provide appropriate oxygen vacancies in HTO NFs, thereby effectively enhancing its performance.

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CERAMICS INTERNATIONAL · 2019 · IF 3.45

Pressureless sintering of Al-free Ta-doped lithium garnets Li7-xLa3Zr2-xTaxO12 and the degradation mechanism in humid air

Tianhang Zhang,Timothy Daniel Christopher,Saifang Huang,Yan’gai Liu,Wei Gao,Tilo Sӧhnel,Peng Cao

In this work, pressureless sintering (PLS) method was used to prepare Li 7 La 3 Zr 2 O 12 based Al-free garnet electrolytes with the substitution of tantalum (Ta). A series of Ta-doped lithium garnets Li 7- x La 3 Zr 2- x Ta x O 12 (LLZTO, x  = 0, 0.25, 0.5, 0.75 and 1.0) were prepared, and the effect of Ta on the structure, densification and ionic conductivity was investigated. Both relative density and ionic conductivity of the LLZTO pellets are dependent on the content of Ta substitution, with the maximum values being reached at x  = 0.5. We also studied the stability and degradation mechanism of lithium garnets (Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 ) in humid air with relative humidity of above 70%. It is revealed that after exposure in the humid air for 4 weeks, a layer of LiOH∙H 2 O was observed on the grain boundaries, which lowered its ionic conductivity considerably. In comparison, the pellet stored in a desiccator had clear surface with negligible change in the ionic conductivity.

CAS / MDL: 1312-81-8 1314-23-4
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Advanced Science · 2023 ·Vol. 10 ·期 10 ·2206877 · IF 15.1

Multiprincipal Element M2FeC (M = Ti,V,Nb,Ta,Zr) MAX Phases with Synergistic Effect of Dielectric and Magnetic Loss

Lu Chen,Youbing Li,Biao Zhao,Shanshan Liu,Huibin Zhang,Ke Chen,Mian Li,Shiyu Du,Faxian Xiu,Renchao Che,Zhifang Chai,Qing Huang

Electromagnetic (EM) wave pollution is harmful to human health and environment, thus it is absolutely important to develop new electromagnetic wave absorbing materials. MAX phases have been attracted more attention as a potential candidate for electromagnetic wave absorbing materials due to their high conductivity and nanolaminated structure. Herein, two new magnetic MAX phases with multiprincipal elements ((Ti 1/3 Nb 1/3 Ta 1/3 ) 2 FeC and (Ti 0.2 V 0.2 Nb 0.2 Ta 0.2 Zr 0.2 ) 2 FeC) in which Fe atoms replace Al atoms in the A sites are successfully synthesized by an isomorphous replacement reaction of multiprincipal (Ti 1/3 Nb 1/3 Ta 1/3 ) 2 AlC and (Ti 0.2 V 0.2 Nb 0.2 Ta 0.2 Zr 0.2 ) 2 AlC MAX phases with Lewis acid salt (FeCl 2 ). (Ti 1/3 Nb 1/3 Ta 1/3 ) 2 FeC and (Ti 0.2 V 0.2 Nb 0.2 Ta 0.2 Zr 0.2 ) 2 FeC exhibit ferromagnetic behavior, and the Curie temperature ( T c ) are 302 and 235 K, respectively. The dual electromagnetic absorption mechanisms that include dielectric and magnetic loss, which is realized in these multiprincipal MAX phases. The minimum reflection loss (RL) of (Ti 1/3 Nb 1/3 Ta 1/3 ) 2 FeC is −44.4 dB at 6.56 GHz with 3 mm thickness, and the effective bandwidth is 2.48 GHz. Additionally, the electromagnetic wave absorption properties of the magnetic MAX phases indicate that magnetic loss also plays an important role besides dielectric loss. This work shows a promising composition-design strategy to develop MAX phases with good EM wave absorption performance via simultaneously regulating dielectric and magnetic loss together.

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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Covalent cross-linking mediated TA-APTES NPs to construct a high-efficiency GO composite membrane for dye/salt separation

Yingfa Liu,Zhongxiang Bai,Guo Lin,Lingling Wang,Xiaoqian Xu,Liang He,Xiaobo Liu

The excellent water transport and molecular sieving properties of graphene oxide (GO)-based membranes have shown application prospects in solving the freshwater crisis. However, it is challenging to further increase water permeability while ensuring separation efficiency, and the destruction of the membrane structure caused by the electrostatic repulsion between the graphene oxide nanosheets also hinders its practical application. In this study, a simple vacuum-assisted method is proposed to prepare a chemical cross-linking mediated composite graphene oxide nanofiltration membrane (GO-TA-APTES-x) by adding tannic acid (TA)-aminopropyltriethoxysilane (APTES) nanoparticles (TA-APTES NPs). Thanks to the expansion of GO membrane interlayer spacing by TA-APTES NPs, the permeability of the GO-TA-APTES-10 membrane is 15 times higher than that of the original GO membrane, and the rejection rate of Congo red remains at 99.9%. In addition, TA-APTES NPs improves the application stability of composite membrane in water environment by means of chemical crosslinking agent, which is expected to promote the transformation of GO nanofiltration membrane from the laboratory environment to industrial application.

CAS / MDL: 919-30-2 1401-55-4
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MATERIALS RESEARCH BULLETIN · 2022 · IF 5.6

Construction of a stable and superhydrophilic PHMG/TA/Fe(III) composite coating-modified membrane for for oil–water separation

Qianyu Wei,Qiuhu Lin,Zezhen Zhang,Lili Wu,Chaocan Zhang

Polyvinylidene fluoride (PVDF)/polyhexamethylene guanidine (PHMG)/tannic acid (TA) coatings have some degree of hydrophilicity but lack stability. To improve the hydrophilicity and stability of antimicrobial PVDF/PHMG/TA membranes, Fe(III) is introduced into the composite system. As a weakly acidic hydrophilic nanoion, Fe(III) can enhance the hydrophilicity and resistance to contamination of the membranes. Furthermore, the stability can be enhanced because a three-dimensional cross-linked coating structure is formed by the complexation of Fe(III), TA and PHMG. This work investigates the effects of different tannic acid concentrations and pH conditions on the hydrophilicity, anti-pollution and stability of the modified coatings. The surface morphology of the membranes was analyzed by field-emission scanning electron microscopy. Additionally, the hydrophilicity and the antipollution performance were evaluated based on the water contact angle, submerged oil contact angle, emulsion flux and flux recovery rate. The stability was evaluated by the changes in flux recovery rate and water contact angle before and after emulsion scouring and ultrasonic treatment. The results show that the modified membranes have favorable hydrophilicity and stability after the addition of Fe(III). The water contact angle can be reduced to 19°, the pure water flux can reach 13,850 L·m −2 ·h −1 , and the emulsion flux can reach 2650 L·m −2 ·h −1 . Moreover, 99.68% flux recovery was achieved after 7 days of deionized water flushing, and the water contact angle remained almost unchanged.

CAS / MDL: 75-11-6 1401-55-4
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

Supramolecule self-assembly synthesis of condensed C-TA/g-C3N4 composites for promoting charge transfer and photocatalytic H2 evolution

Fang He,Lan Luo,Zhenxing Wang,Shaoqin Peng,Yuexiang Li

Design of highly condensed g-C 3 N 4 is a prospective way to optimize the photoreactivity of g-C 3 N 4 as it possesses condensed structure with decreased interlayer spacing, which benefits both charge transfer and light harvesting. Herein, we report that novel condensed carbonized-tannic acid (C-TA)/g-C 3 N 4 composites have been acquired via a supramolecular self-assembly of TA and melamine into TA/melamine precursors followed by thermal condensation. The acquired condensed C-TA/g-C 3 N 4 composites present superior visible-light photocatalytic activity for H 2 evolution. The 1 wt% C-TA/g-C 3 N 4 composite shows 4.2 times enhancement of photocatalytic activity for H 2 evolution compared to pristine g-C 3 N 4 . The TA with distinct adhesion properties and functional groups of OH, which is firmly linked with melamine, can confine the melamine inside to promote the condensation to gain more condensed g-C 3 N 4 . The condensed C-TA/g-C 3 N 4 composites with decreased interlayer distance effectively promote charge transfer and photocatalytic H 2 evolution.

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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Pod-like TA-ZIF-8/TCOH composite filler for the preparation of mixed matrix membrane for efficient CO2 separation

Yuanyuan Wang,Suyue Zhong,Shumin Li,Yangyang Dai,Wenjun Su,Jian Li

Rapid industrialization poses a serious threat to the balance of ecosystems and environmental sustainability, and the application of membrane technology is an effective way to alleviate this situation. Two-dimensional (2D) MXene nanosheets are superior materials for constructing high-performance separation membranes, but their biggest drawback is that they are prone to agglomeration. After alkalizing them, the obtained alkaline MXene (TCOH) nanosheets have hydroxyl-rich surfaces, stabilized structure and great affinity for CO 2 . Based on this, a self-supported TA-ZIF-8/TCOH@Pebax mixed matrix membranes (MMMs) with block polymer Pebax-1657 as matrix and TA-ZIF-8/TCOH as composite filler were prepared in this work. ZIF-8 was modified with tannic acid (TA) to enrich the surface with hydroxyl groups, yielding TA-ZIF-8 that is both pro-CO 2 and well interfacially compatible. The using of TA-ZIF-8 not only improves the selectivity of the separation membrane, but also its mutually repulsive electrostatic force with TCOH can expand the layer spacing of TCOH nanosheets as much as possible, which leads to a rich gas transportation channel of the membrane. Experiments have shown that the prepared TA-ZIF-8/TCOH@Pebax MMM had outstanding separation performance beyond the 2019 Robinson upper bound when the content of TA-ZIF-8 was appropriate. Also, the TA-ZIF-8/TCOH@Pebax MMM showed superior thermal stability, durability and mechanical properties. In summary, the strategy of combining nanoparticles and nanosheets as composite fillers in this study provides an effective way to regulate the low permeance of MMMs. In the meantime, the application of TCOH provides a novel idea for further research on gas separation membranes.

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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

PPS/TA-PEI/β-FeOOH membranes with powerful photo-Fenton self-cleaning capability for efficient oil–water emulsion separation

Shiwei Tian,Yaqi Zhang,Qiankun Sha,Xingxiang Zhang,Tian Yang,Xuhuan Yan,Na Han

Polyphenylene sulfide (PPS) microporous membranes have garnered extensive research enthusiasm concerning their outstanding permeation performance and separation accuracy in treating oily wastewater. Nevertheless, the inherent hydrophobic chemical structure, along with the noticeable concentration polarization effect, predisposes them to severe membrane contamination during the separation process. Accordingly, it is desirable to design a PPS self-cleaning membrane with superior anti-fouling capability, fast transport, and remarkable flux recovery. This study marks the first combination of PPS membrane materials with the photo-Fenton process. In detail, the polyphenol (tannic acid, TA)-polycation (polyethyleneimine, PEI)-metal ion (Fe 3+ ) double cross-linking coatings were first assembled on the PPS substrate surface. Subsequently, β-FeOOH photocatalysts were synthesized through in-situ mineralization to further strengthen the hydrophilicity of the membranes. The obtained PPS/TA-PEI/β-FeOOH composite membrane achieved exceptional separation of diverse oil-in-water (O/W) emulsions. The PPS/TA-PEI/β-FeOOH membranes exhibited in-air superhydrophilic and under-water superoleophobicity, exhibiting under-water oil contact angles greater than 151° for diverse oil agents. The fabricated composite membranes displayed high permeability (a flux of the petroleum ether-in-water (P/W) emulsion reached 3400.5 L m −2 h −1 bar −1 driven by a pressure of 0.05 MPa) along with ideal oil rejection (98.6 %). Significantly, the PPS/TA-PEI/β-FeOOH membrane possessed powerful photo-Fenton self-cleaning capability, and its flux recoveries of the contaminated membrane exceeded 90.3 % for varied O/W emulsions after being cleaned by visible light for 10 min. We believe that our research presents a novel approach for the exploitation of PPS-based photo-Fenton self-cleaning membranes, which also exhibit great applicative potential in oily wastewater treatment.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Quantitative assessment of structure-performance relationship of loose nanofiltration membranes with TA-MoS2 interlayer for effective dye/salt separation

Tingyan Deng,Zhen Cao,Fan Ni,Li Zhao,Fei Shen,Jianmei Zou,Yanzong Zhang,Yating Chen,Jinsong He

The novel strategy of thin-film nanocomposite loose nanofiltration (LNF) membranes incorporating an interlayer of nanomaterials has raised growing interests for the high-performance membrane design. Although the effects of membrane structure on separation performance have been elucidated for a long time, however, the quantitative structure-performance relationship of interlayer-based LNF membranes has not been established. In this study, we established the structure-performance relationship of TA-MoS 2 interlayer based LNF membranes from a quantitative level for the first time. The correlation heat map analysis identified four key structural parameters (e.g. selective layer thickness, crosslinking degree, water contact angle, and zeta potential) for water permeability as well as dye rejection, and three key structural parameters (e.g. selective layer thickness, crosslinking degree, and zeta potential) for salts rejection, respectively. Furthermore, the multiple linear regression analysis revealed the rigorous mathematic modeling of key structural parameters-separation performance relationships with all R 2 values above 0.899, and determined the contributions of each key structural parameter to the separation performance in a quantitative level. Finally, the optimal TA-MoS 2 interlayer based LNF membrane exhibited a high water permeability of 80.2 LMH·bar −1 , effective separation of dye/salts (rejection rate: congo red (99.0%), methyl blue (95.1%), Na 2 SO 4 (1.5%) and NaCl (0.5%)), good stability and antifouling properties (i.e. water flux recovery rate (FRR) of 96% for humic acid). This study can pave the way of quantitatively design of interlayer-based LNF membrane with targeted performance.

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REACTIVE & FUNCTIONAL POLYMERS · 2025 · IF 5.1

The effect of coordination state on the activity of TA-Zr supramolecular networks for heavy metals removal from water

Shuxin Chen,Liting Wang,Wenxiang Ni,Hui Qiu

The self-assembly behavior of the MPNs-based adsorbent is substantially influenced by changes in solution pH. In this study, a highly negatively charged tannic acid‑zirconium (TA-Zr) macromolecular network has been successfully synthesized. As pH increases from 3 to 11, the coordination structure of TA with Zr(IV) changes from mono- to tri-complexation state, resulting in enhanced electronegativity and increased structural stability of tri-complex TA-Zr(9) due to its higher charge density. The TA dissolution experiments and zeta potential measurements confirm this conclusion. The tri-complex TA-Zr(11) underwent structural changes in its macromolecular network due to partial zirconium hydroxide formation under strongly alkaline conditions, as confirmed by X-ray photoelectron spectroscopy analysis, which in turn impacted its stability. Meanwhile, the adsorption capacity of TA-Zr materials for Pb(II) ion increases with the pH of the synthesis solution. XPS analysis suggested that the underlying adsorption mechanism involved ligand exchange between Pb(II) ion and phenolic hydroxyl groups on TA-Zr(9). After batch adsorption-regeneration cycles, TA-Zr(9) could be regenerated with an acidic solution while maintaining consistent Pb(II) ion removal efficiency. Furthermore, TA-Zr(9) effectively treated 12,150 bed volumes (BV) of synthetic water at pH 5.6, which is 18 times more than commercial D001. These results confirm that TA-Zr(9) shows great potential as an effective adsorbentfor Pb(II) removal in practical wastewater treatment, making it a promising candidate for water remediation.

CAS / MDL: 13520-92-8 1401-55-4
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ENERGY · 2021 · IF 7.147

Electrochemical CO2 reduction to CO using solid oxide electrolysis cells with high-performance Ta-doped bismuth strontium ferrite air electrode

Yifeng Zheng,Shun Wang,Zehua Pan,Bo Yin

Electrochemical CO 2 reduction to CO by using solid-oxide electrolysis cells (SOECs) is a promising option to produce useable fuels using renewable energy. However, traditional cobalt-based air electrodes exhibit high thermal-expansion coefficients and a tendency of Co segregation, compromising long-term stability. Here, Co-free Bi 0.5 Sr 0.5 FeO 3-δ perovskite was explored with Ta doping into the B-site as the air electrode (BSFTx). Doping Ta enabled a decrease in polarization resistance by 45% from 0.31 Ω cm 2 to 0.17 Ω cm 2 at 700 °C. The distribution function of relaxation times analysis suggested that the observed improvements can be ascribed to the enhanced mass-transfer processes, which include oxygen diffusion, association, and desorption. The performance of a cathode-supported Ni-YSZ (ytttria-stabilized zirconia)|YSZ|Gd-doped ceria|BSFTx cell was characterized by an electrolysis current of −0.81 A cm −2 under 1.5 V at 800 °C, which corresponds to a CO-production rate of 4.2 × 10 3  nmol s −1  cm −2 and an electrical efficiency of 98%. Excellent stability of the cell was also demonstrated by steady current density during the 32-h test executed under 1.2 V at 800 °C. The nearly 100% electrical efficiency and the satisfactory performance and stability of SOEC with Ta-doped BSF air electrode indicated its potential use in CO 2 reduction technique.

研究领域: 材料科学 · 能源化学 · 电化学工程
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MATERIALS RESEARCH BULLETIN · 2023 · IF 5.4

Enhanced energy storage performance in Na(Nb,Ta)O3-doped Ba(Ti,Ca)O3-based ceramics through bidirectional optimization strategy

Zhiwei Li,Zhengxiang Bian,Yurong Ren,Zhihui Chen,Jiujun Xu

(1-x)(0.9Ba 1.003 Ti 0.97 Ca 0.03 O 3 –0.1(Bi 0.51 Na 0.47 ) 0.94 Ba 0.06 TiO 3 )-xNa(Nb 0.85 Ta 0.15 )O 3 ( x  = 0.03–0.15) ceramics were designed and fabricated through a bidirectional optimization strategy using traditional solid reaction method. The results revealed that the introduction of Na(Nb 0.85 Ta 0.15 )O 3 increased the vacancy concentration at the A site , conducing to improved polarization and reduced grain size. The substitution at the B site disrupted the long-range ordered ferroelectric domains and generated polar nanodomains, leading to enhanced relaxation behavior. The optimum energy storage density of 3.57 J/cm 3 and efficiency of 87.5% were simultaneously achieved under the electric field of 220 kV/cm in the sample with x  = 0.09. Moreover, it also exhibits extremely high-power density (∼57 MW/cm 3 ), ultrafast discharge time (∼103 ns), high discharge density (1.35 J/cm 3 ), along with excellent temperature (30‒120 °C) and frequency stability (1‒100 Hz) under the equivalent electric field of 120 kV/cm. This novel design strategy provides theoretical guidance for the development of advanced electrical energy storage devices.

研究领域: 材料科学 · 能源存储
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