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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Oxidative desulfurization of model oil over Ta-Beta zeolite synthesized via structural reconstruction

Zhiguo Zhu,Haikuo Ma,Hao Xu,Bo Wang,Peng Wu,Hongying Lü

As to metallosilicate zeolites, ions with larger size such as Ta 5+ in the gels greatly retarded their crystallization during the hydrothermal synthesis, affording long-winded synthesis periods, up-limited framework-substituted metal contents, or even frustrated outcome. An efficient hydrothermal synthesis strategy for metallosilicate, in this case of Ta framework-substituted *BEA zeolite, via structural reconstruction was proposed to stride the gap. The Ta content in our developed Ta-Beta-Re-50 zeolite achieved up to 5.48 % (Si/Ta = 52), breaking through the limitation of Ta contents for conventional method (Si/Ta > 100). Additionally, this Ta-Beta-Re zeolite possessed nanosized crystals (20–40 nm) and short crystallization time (8 h), significantly improving space-time yields of practical zeolite production. Through spectroscopic study, it was confirmed that the existence of zeolite structural units intensively facilitated the formation of nucleation and crystal growth. This innovative Ta-Beta zeolite demonstrated high catalytic performances for oxidation desulfurization, far outperforming traditional fluoride-mediated Ta-Beta-F, which was ascribed to its excellent diffusion properties and incredible high isolated Ta contents. Additionally, the catalytic performance of Ta-Beta-Re could be regenerated after simple calcination and the deactivation may be caused by pore blocking of organics. This work provides a new method for rationally design and construction of metallosilicate materials with high activity for catalytic oxidation applications, which can bridge the conceptual and technical gap between periodic trends and zeolite material synthesis.

研究领域: 化学工程 · 材料科学 · 催化 · 环境科学
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CATALYSIS LETTERS · 2021 ·Vol. 152 ·期 8 ·2524-2532 · IF 3.186

Understanding Ta as an Efficient Promoter of MgO–SiO2 Catalyst for Conversion of the Ethanol–Acetaldehyde Mixture into 1,3-Butadiene

Jiang Haoxi,Jiang Angjiong,Gao Qiang,Yang Guochao,wang Lingtao

In this work, Ta was firstly reported as an efficient promoter of MgO–SiO 2 for the conversion of ethanol and acetaldehyde to 1,3-butadiene. The doping of Ta into MgO–SiO 2 forms Ta–O–Si bonds and generates more strong Lewis acid sites, which not only promote the aldol condensation reaction but also significantly facilitate the Meerwein–Ponndorf–Verley reduction, the total conversion around 80% which drops to 65% after 24 h. In addition, the catalyst showed desirable stability in 24 h long-term stability evaluation, the selectivity remained stable at 80%. Graphic Abstract

CAS / MDL: 75-07-0 7721-01-9
研究领域: 催化化学 · 材料科学
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ChemistrySelect · 2024 ·Vol. 9 ·期 28 ·e202304550 · IF 1.9

Lattice Distortion Induced Ta-doped BaTiO3 for Efficient Photocatalytic Water Splitting for Hydrogen Production

Zishuang Guo,Zeyi Wang,Haiwang Wang,Changxiang Xie,Xiao Xiang,Chengang Zhang,Jian Qi

Graphical A sol-gel assisted solid-phase method was employed to prepare BaTiO 3 doped with varying Ta 5+ doping amounts. The results showed that Ta 5+ doped into the BaTiO 3 lattice and caused lattice distortion when the heat treatment temperature reached 1052.7 °C. The 1.25 mol %Ta 5+ -doped BaTiO 3 exhibited the best activity of photocatalytic water splitting for hydrogen production, which was 2.4 times that of BaTiO 3 . BaTiO 3 , as a perovskite type material with excellent chemical stability and suitable conduction, has been widely studied in the field of photocatalysis. However, it can only absorb ultraviolet light because of its wide band gap. Herein, the lifetime of photogenerated electrons of BaTiO 3 doped with Ta 5+ can be enhanced. To study the band structure and photocatalytic performance of Ta-doped BaTiO 3 , sol-gel assisted solid-phase method was employed to prepare BaTiO 3 doped with varying Ta 5+ doping amounts, and the structure characteristic and formation mechanism of the Ta-doped BaTiO 3 were analyzed. The results showed that the heat treatment temperature reached 1052.7 °C, sufficient thermodynamic conditions were obtained for Ta 5+ to dope into the BaTiO 3 lattice, and lattice distortion occurred in BaTiO 3 . Meanwhile, the particle size after doping decreased with the increase of Ta 5+ doping amount. The 1.25 mol %Ta 5+ -doped BaTiO 3 had the lowest band gap (3.077 eV), and the photocatalytic water splitting had the best hydrogen evolution activity, which was 2.4 times that of BaTiO 3 . Furthermore, the conductance potential of 1.25 mol %Ta 5+ -doped BaTiO 3 was more negative than that of BaTiO 3 , which improved the thermodynamic advantage of the photocatalytic water splitting, and it had higher and more stable photoresponse and photogenerated carrier migration rate.

CAS / MDL: 513-77-9
研究领域: 材料科学 · 光催化 · 可再生能源
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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.

研究领域: 材料科学 · 光催化 · 能源化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Enhanced performance of mixed matrix PVDF/TA membranes in treating wastewater containing heavy metals and organics

Qian Wang,Xinglin Li,Shasha Guo,Hengyang Mao,Xiaoshan Meng,Taoli Huhe,Zhengzhong Zhou

Industrial wastewater is complex, containing a significant amount of heavy metals and organics, which needs complicated traditional treatment processes. Ultrafiltration (UF) membranes process can remove various organic pollutants, but exhibit no removal capacity for heavy metal. In this work, we directly blended tannic acid (TA) with polyvinylidene fluoride (PVDF) to fabricate membranes, based on the chelating ability. TA not only improves heavy metal adsorption properties to the membrane but also enhances its acid resistance. The PVDF/TA membrane maintained over 99 % remove rate to Fe 3+ in five adsorption–desorption tests and also exhibited effective rejection of bovine serum albumin after the cycling test. The PVDF/TA membrane achieved efficient treating processing of oil and Fe 3+ mixed solutions, with 100 % rejection for oil and over 99 % for Fe 3+ . In this study, the PVDF/TA membranes presented tremendous potential for application in complex wastewater treatment.

CAS / MDL: 9048-46-8
研究领域: 环境工程 · 材料科学 · 水处理
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2023 · IF 5.2

A novel UIO-66-NH2@TA adsorbent for effective solid-phase extraction of Pb (II) from environmental water and juices

Xiaoyan Duan,Kaiqiang Wang,Lei Wang,Limin Cao,Jianxin Sui,Hong Lin

In this study, a new metal-organic framework adsorbent (UIO-66-NH 2 @TA) which can efficiently and selectively capture lead ions was developed by functionalizing UIO-66-NH 2 with tannic acid (TA) by Michael addition reaction. The structural and morphological properties of the produced adsorbent, as well as its adsorption mechanism for Pb (II) were discussed. The maximum adsorption capacity of Pb (II) was 475.78 mg/g at pH 5.0, which was significantly higher than the adsorption capacity of many adsorbents reported in the literature. In addition, the adsorption isotherms and kinetics conformed to the Langmuir model and pseudo-second-order kinetic model , respectively. The results indicated that the adsorptive behavior of the adsorbent mainly depended on the active sites on the surface of the adsorbents. The UIO-66-NH 2 @TA showed favorable selectivity toward Pb (II) against the interference of coexisting metal ions . It was found that the excellent Pb (II) removal performance of UIO-66-NH 2 @TA was mainly attributed to the synergistic effect of physical adsorption and chemisorption . Moreover, the UIO-66-NH 2 @TA showed extraction efficiencies of 88.01%, 82.44%, 80.20% and 74.99% for Pb (II) with initial concentration of 100 mg/L in river water, sea water, peach juice drink, and grape juice, respectively. This work proved that the UIO-66-NH 2 @TA had a wide application prospect in the field of Pb (II) treatment.

CAS / MDL: 1401-55-4
研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Dual-mode conductive organohydrogel with TA-AgNPs synergy for multifunctional sensing

Ruyue Guo,Yan Bao,Junbin Zhou,Jie Chen,Xinjie Li,Chao Liu,Wenbo Zhang

The synergistic advantages of high conductive and histology-like properties of hydrogel make it promising candidate for flexible electronic devices. However, it still remains huge challenge to build conductive hydrogel with high sensing performance and versatility. Herein, a platform of multifunctional organohydrogel was tailored by dual-mode conduction and tannic acid‑silver system, which demonstrated excellent mechanical, conductive, antibacterial, freezing tolerance, moisture retention and sensing capabilities. Thanks to the multiple energy dissipation by the synergistic effect between different components during deformation, the average stress and strain of organohydrogel were 6.18 ± 0.313 MPa and 695.15 ± 25.956 %, respectively. At the same time, the combination of tannic acid and silver guaranteed the antibacterial property of organohydrogel, which was an advantage as flexible sensor for long-term human-machine interface contact without worrying about bacterial growth. Moreover, the organohydrogel exhibited freezing tolerance and moisture retention performances based on the ability of water/glycerin binary solvents to inhibit ice crystal growth and water evaporation, laying the foundation for its long-term stability in harsh environments. In addition, the construction of dual-mode conduction and the corresponding structural changes of organohydrogel during deformation resulted in excellent average conductivity of 19.70 ± 0.145 S m −1 and strain sensitivity of 17.10. It enabled organohydrogel to act as flexible sensor to realize coding language communication, real-time monitoring of wrist pulse and collecting pressure information in space. In summary, a multifunctional organohydrogel was developed, which provided feasible and promising strategy for the enhanced performance and modified function of conductive hydrogel.

研究领域: 材料科学 · 纳米技术 · 生物医学工程 · 柔性电子学 · 传感器
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Science China-Materials · 2023 ·Vol. 66 ·期 8 ·3213-3222 · IF 8.1

Non-equimolar (Hf,Zr,Ta,W)B2 high-entropy diborides enable superior oxidation resistance

Wen Zihao,Meng Hong,Jiang Shengda,Tang Zhongyu,Liu Yiwen,Chu Yanhui

Developing superior oxidation resistance of high-entropy diborides is critical for extending their potential applications in harsh environments. Herein, we developed non-equimolar (Hf,Zr,Ta,W)B 2 high-entropy diborides with superior oxidation resistance by adjusting W contents for the first time. The as-fabricated (Hf 0.28 Zr 0.28 Ta 0.28 W 0.15 )B 2 samples are predicted to possess superior oxidation resistance at 1473–1773 K through the oxidation depth quantitative analysis obtained by machine learning, which is attributed to the reason that the moderate WO 3 can effectively inhibit the volatilization of B 2 O 3 . Furthermore, a four-layered structure is found in the generated product layers at 1773 K, which is due to the preferential oxidation of Hf and Zr elements at low oxygen partial pressure and the different diffusion activation energies of oxide products. The preferential oxidation of Hf and Zr elements is further demonstrated by the computational phase stability diagrams, and oxygen adsorption energies and charge transfer between oxygen atoms and different metal adsorption sites via first-principles calculations. Such superior performance endows (Hf 0.28 Zr 0.28 Ta 0.28 W 0.15 )B 2 with potential applications as ultrahigh-temperature structural materials.

CAS / MDL: 7440-42-8
研究领域: 材料科学 · 高温材料 · 计算材料科学
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MICROCHEMICAL JOURNAL · 2025 · IF 5.1

Bimetallic synergistic regulation of CuFe@TA nanozyme targeted boosting multi-enzymes activities for sensitive colorimetric detection of glucose

Jianhui Xin,Mengxia Yan,Zhuqing Wang,Xin Luo,Xue Yu,Jiangyang Mo,Jingqiao Guo,Jine Wang

Nanozymes have been widely used in the field of biosensing owing to their high stability, low cost and adjustable catalytic activity. It is of great value to develop methods to construct nanozymes and to study their application. Here, a bimetallic synergistic enhancement CuFe@TA nanozyme was obtained by a simple and environmentally friendly one-pot aqueous phase method, in which Cu 2+ and Fe 3+ were bound to tannic acid (TA) by the strong coordination. In this process, the polyphenols in TA have reducing property that ensure the formation of hetero-valent metal pairs (Fe 3+ /Fe 2+ , Cu 2+ /Cu + ), thus enhancing the conversion of H 2 O 2 into more reactive radical species. Notably, the synthesized CuFe@TA nanozyme exhibited higher oxidase-like and peroxidase-like catalytic activities than a single metal ion due to the synergistic effect of the two transition metal components. Besides, based on the cascade catalysis of glucose oxidase (GOx) and CuFe@TA nanozyme, a sensitive colorimetric sensing platform for glucose assay was constructed with a good linear range of 3.03 ∼ 363.6  µM and a calculated limit of detection of 2.59  µM. This as-developed method was applied to detect glucose in real human serums and juice drink samples sensitively and accurately, consistent with measurement results made by commercial glucose meters. This work broadens the species of nanozymes, and provides a more sensitive glucose detection platform in medical diagnostics and the food industry.

研究领域: 生物传感 · 纳米医学 · 分析化学
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JOURNAL OF MEMBRANE SCIENCE · 2022 · IF 10.53

Robust PAAm-TA hydrogel coated PVDF membranes with excellent crude-oil antifouling ability for sustainable emulsion separation

Yuxie Jiang,Caiyun Xian,Xuanfei Xu,Weiwei Zheng,Tianxue Zhu,Weilong Cai,Jianying Huang,Yuekun Lai

Hydrogel coating was widely studied in the field of oil/water separation due to its underwater superoleophobic performance, which could avoid the blockage of the separation membrane by oil effectively, especially high viscosity crude oil. In this manuscript, a layer of ultra-thin Polyacrylamide-Tannic (PAAm-TA) hydrogel coating was coated on the surface of PVDF microfiltration membrane by a simple immersion process, which could endow it with superhydrophilic and underwater superoleophobic performance. Due to the outstanding superhydrophilic and ultrathin hydrogel coating, the obtained sample showed an ideal emulsion separation efficiency and flux, 99.47% and 1184.3 L/(m 2  h bar) for toluene-in-water emulsion. Additionally, the residual crude oil on the membrane surface can be easily and quickly removed by rinsing with water. Attributed to a variety of chemical and hydrogen bonding and negatively charged groups on the tannic acid molecules, the membranes possess good mechanical stability and electrostatic adsorption properties. The obtained PVDF/PAAm-TA membrane could maintain its special wettability in a wide range of chemical environments, enabling it great potential to be used in complex water treatment. In summary, this study will provide new insights into a new idea and method for the preparation of hydrogel coated porous materials for oil/water separation.

研究领域: 材料科学 · 环境工程 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Peroxymonosulfate activation by mineralized PVDF-TA@Co template based ZIF-67/8 electrospinning membranes for ofloxacin degradation under visible-light

Liusha Cen,Fan Yu,Chengcai Li,Guojin Liu,Wangyong Jin,Hailin Zhu,Yuhai Guo

Recently, heterogeneous catalysts prepared by two phase metals were commonly used to activate PMS degradation. However, the synergistic effects of Zn and other metals on the activation of PMS were infrequently studied. In this work, novel PVDF@TA-ZIF-67/8 nanofibers were prepared successfully by first mineralization and then in-situ growth. The prepared PTZ70 exhibited an evidently higher photocatalytic activity than PVDF, PTC, PTZ0, PTZ10 and PTZ100 to degradation OFX (96.5 %). The effects of the mass ratio of Co and Zn, PMS dosage, coexisting ions and organic solvents on the degradation of OFX were concretely investigated. The radical trapping experiment and mechanism analysis showed that the synergistic effect of Co and Zn played a key role in PMS activation, accelerating the generation of 1 O 2 and •O 2 – . Combining the discussion of influencing factors and LC-MS analysis, four OFX degradation pathways were illustrated. In particular, we observed that the degradation OFX of PTZ70 was only slightly reduced by 5.6 % after five cycling, indicating the reusability, good stability and high environmental suitability of PTZ70 performance . This study offers a novel path for the design of catalytic membranes with controllable heterogeneous metal doping.

研究领域: 环境科学 · 材料科学
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International Journal of Minerals Metallurgy and Materials · 2024 ·Vol. 31 ·期 9 ·2102-2109 · IF 5.6

Investigation and optimization of high-valent Ta-doped SrFeO3−δ as air electrode for intermediate-temperature solid oxide fuel cells

Jiang Shanshan,Qiu Hao,Xu Shaohua,Xu Xiaomin,Jiang Jingjing,Xiao Beibei,Julião Paulo Sérgio Barros,Su Chao,Chen Daifen,Zhou Wei

To explore highly active and thermomechanical stable air electrodes for intermediate-temperature solid oxide fuel cells (IT-SOFCs), 10mol% Ta 5+ doped in the B site of strontium ferrite perovskite oxide (SrTa 0.1 Fe 0.9 O 3− δ , STF) is investigated and optimized. The effects of Ta 5+ doping on structure, transition metal reduction, oxygen nonstoichiometry, thermal expansion, and electrical performance are evaluated systematically. Via 10mol% Ta 5+ doping, the thermal expansion coefficient (TEC) decreased from 34.1 × 10 −6 (SrFeO 3− δ ) to 14.6 × 10 −6 K −1 (STF), which is near the TEC of electrolyte (13.3 × 10 −6 K −1 for Sm 0.2 Ce 0.8 O 1.9 , SDC), indicates excellent thermomechanical compatibility. At 550–750°C, STF shows superior oxygen vacancy concentrations (0.262 to 0.331), which is critical in the oxygen-reduction reaction (ORR). Oxygen temperature-programmed desorption (O 2 -TPD) indicated the thermal reduction onset temperature of iron ion is around 420°C, which matched well with the inflection points on the thermos-gravimetric analysis and electrical conductivity curves. At 600°C, the STF electrode shows area-specific resistance (ASR) of 0.152 Ω·cm 2 and peak power density (PPD) of 749 mW·cm −2 . ORR activity of STF was further improved by introducing 30wt% Sm 0.2 Ce 0.8 O 1.9 (SDC) powder, STF + SDC composite cathode achieving outstanding ASR value of 0.115 Ω·cm 2 at 600°C, even comparable with benchmark cobalt-containing cathode, Ba 0.5 Sr 0.5 Co 0.8 Fe 0.2 O 3− δ (BSCF). Distribution of relaxation time (DRT) analysis revealed that the oxygen surface exchange and bulk diffusion were improved by forming a composite cathode. At 650°C, STF + SDC composite cathode achieving an outstanding PPD of 1117 mW·cm −2 . The excellent results suggest that STF and STF + SDC are promising air electrodes for IT-SOFCs.

研究领域: 材料科学 · 能源化学 · 电化学 · 无机非金属材料 · 热力学与动力学分析
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