SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Yun Long,Jian Sun,Changnian Mo,Xiangyao She,Pengxin Zeng,Hongqiang Xia,Jubing Zhang,Zijian Zhou,Xinming Nie,Chuanwen Zhao
Calcium looping (CaL) belongs to a promising high-temperature CO 2 capture technology because of adopting cheap and extensive source CaO-based sorbents . However, CaO-based sorbents are prone to occur the issues of sintering and elutriation in the fluidized-bed reactors. To further enhance the practicability, the Zr-supported, CaO-based sorbent pellets were produced using the graphite-moulding method. Different synthesis modes (i.e., sol-gel, hydration-mixing, and wet-mixing) were compared for preparing CaO-based composite slurry before pelletization. Sol-gel is the promising synthesis mode to prepare Zr-supported, CaO-based pellets with outstanding CO 2 capture performance due to achieving a more uniform distribution of inert CaZrO 3 spacer. Moreover, the Zr-based stabilizer content within sorbent pellets produced by the combined method of sol-gel and graphite-moulding was further studied. The higher content of Zr-based stabilizer promotes the enhancement of cyclic stability and mechanical strength of Zr-supported, CaO-based pellets. After 17 cycles, the sorbent pellets containing 20 wt% of Zr-based stabilizer display a high CaO carbonation conversion of 74.1 %. Moreover, CaO-based pellets with 20 wt% of Zr-based stabilizer possess a higher compression strength of 4.84 ± 1.08 MPa, which is as high as 1.8 times that of the pellets with 5 wt% of Zr-based stabilizer.
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PubMed
高影响因子
PLoS One
·
2022
·Vol. 17
·期 8
·e0271075
·
IF 3.752
Bicun Jiang,Fuqiang Liu,Yang Pan,Yan Tan,Chendong Shuang,Aimin Li
Tetracycline (TC) is widely-used antibiotic pollutant with high toxicity, refractory, persistence and bacteriostasis, and its removal from water needs to be enhanced. In this work, a novel Graphite-UiO-66(Zr)/Ti electrode was successfully prepared and evaluated for electrochemical oxidation degradation of TC. The electrochemical performance tests indicate the Graphite-UiO-66(Zr)/Ti electrode had higher electrochemical oxidation activity, which achieved higher TC removal efficiency (98.1% ± 1.5%) than Ti plate (65.2% ± 3.5%), Graphite-MIL-53(Al)/Ti electrode (79.5% ± 2.9%) and Graphite-MIL-100(Fe)/Ti electrode (89.0% ± 2.6%). The influence of operating condition was also systematically studied, and the optimized condition was pH 5.0, 20 mA/cm 2 current density and 0.1 M electrolyte (Na 2 SO 4 ). Through the liquid chromatography mass spectrometry (LC-MS), the TC degradation pathway by Graphite-UiO-66(Zr)/Ti electrode oxidation was proposed. Under the •OH free radical oxidative decomposition effect, the double bond, phenolic group and amine group of TC were attacked. TC was transformed into intermediate product ① (m/z = 447), then was further degraded to intermediates ② (m/z = 401) and ③ (m/z = 417). The latter was fragmented into small fractions ④ (m/z = 194), ⑤but-2-enedioic acid (m/z = 116) and ⑥oxalic acid (m/z = 90, the proposed intermediate). In addition, TC removal remained at 89.6% ± 2.7% in the sixth cycle of operation, which confirmed the efficient reusability and stability for antibiotics removal from water.
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高影响因子
Small Structures
·
2022
·Vol. 4
·期 1
·2200161
·
IF 11.343
Lu Chen,Youbing Li,Ke Chen,Xiaojing Bai,Mian Li,Shiyu Du,Zhifang Chai,Qing Huang
Entropy stabilization is an effective method to design and explore MAX phases with outstanding properties via tuning constituent elements and crystal structures, which have received considerable critical attention. Currently, some medium-/high-entropy (ME/HE) MAX phases, whose A layers are composed of Al, S, and magnetic elements, are reported, while few discussions about ME/HE-MAX phases with other A elements (e.g., Sn) are conducted. Herein, fully dense ME/HE-MAX phase bulks ((TiVNb) 2 SnC, (TiVNbZr) 2 SnC, and (TiVNbZrHf) 2 SnC) are designed and synthesized because of the chemical diversity of MAX phases. The results of Rietveld refinement of X-ray diffraction, scanning electron microscopy, and high-resolution scanning transmission electron microscopy-affiliated energy-dispersive spectrometer analysis comprehensively verify the crystal structure of ME/HE-MAX phases. Both the electrical conductivity and the charge carrier mobility are significantly lower than the reported correlation ternary MAX phases, due to the electron scattering and structural defects in ME/HE-MAX phase crystal structures. Similarly, the electron contribution of thermal conductivity is gradually declining; on the contrary, the phonon plays an increasingly dominant role as temperature increases. Owing to the richness in composition of MAX phases, herein, a composition design route for discovering new MAX phases and tuning their properties is indicated.
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高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Yue Zhou,Zijian Zhou,Lei Liu,Xiangyao She,Ruichang Xu,Jian Sun,Minghou Xu
Calcium looping is a potential thermochemical energy storage technology applied in a high-temperature working window. However, CaCO3/CaO materials are prone to encounter severe sintering, exhibiting poor thermal energy storage/release stability. To improve the thermochemical energy storage stability, different amounts (5, 15, and 30 wt %) of a Zr-based stabilizer were incorporated into CaCO3/CaO materials. Moreover, the graphite-casting method was adopted to prepare the Zr-stabilized, CaO-based composite pellets aiming to improve the practicability. The incorporation of the Zr-based stabilizer can effectively resist the sintering of CaO-based composite powders during a high-temperature precalcination process. It is mainly attributed to the large amounts of generated, nanosized CaZrO3 grains possessing desirable antisintering ability evenly distributed within the composites. Particularly, the Zr-stabilized, CaO-based composite pellets containing 30 wt % of CaZrO3 possess a relatively high compression strength of 2.28 ± 0.87 MPa and a desirable thermal storage density of 1.15 GJ/t after 20 cycles. Additionally, the graphite-casted, Zr-stabilized, CaO-based composite pellets have potential to be applied in a large-scale thermochemical energy storage system because the graphite-casting method is easy to be scaled-up.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Lei Chen,Huan Wang,Xiaohong Cao,Yue Feng,Zhibing Zhang,Youqun Wang,Yunhai Liu
A simple hydrothermal method was adopted to synthesize different inorganic-organic hybrid materials (Zr -x ), including zirconium ethylenediamine tetramethylene phosphine (Zr-EDTMP), 2-phosphobutane-1,2,4-zirconium tricarboxylate (Zr-PBTC), odium creatine phosphate zirconium phosphate (Zr-CP), and creatinol zirconium phosphate (Zr–COP). Various characterizations were utilized to explore the physical and chemical properties of materials. The applications of Zr -x in removing U(Ⅵ) were studied comprehensively. The effects of solution's pH value, contact time, initial concentration of U(Ⅵ), and temperature on adsorption were examined. Besides, the desorption, reusability, as well as adsorptive selectivity were investigated. The present study revealed that the U(Ⅵ) adsorption on Zr-EDTMP was in accordance with Sips isothermal model with the greatest adsorption capacity (317.4 mg/g) and the superior adsorptive selectivity for U(Ⅵ). Zr-EDTMP is a potentially high-efficient adsorbent for extracting U(Ⅵ) from radioactive wastewater .
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
·
2020
·Vol. 97
·期 1
·1-4
·
IF 2.008
Chen Wenming,Wang Haibo,Guo Xuan,Zhong Jinyi
Self-detoxifying materials for capturing and destructing chemical warfare agents (CWAs) have attracted intense attention in efficient personal protection and safe handling of contaminated materials. In this study, we reported an approach for synthesis of flexible Zr(OH) 4 -carbon fiber composite by sol–gel method. Activated carbon fibers serving as substrate carrier and adsorption conveyor could effectively make Zr(OH) 4 evenly distributed on the surface, which has excellent sorption properties and wide-ranging reactivity toward CWAs. The results demonstrated that the Zr(OH) 4 -carbon fiber composite could quickly remove (within 10 s) and 6-h degradation efficiency to 10-mg/mL sulfur mustard (HD) and O-ethyl S-(2-diisopropylamino)-ethyl methylphosphonothioate (VX) could reach 92.2 and 99.99%. In addition, it was found that Zr(OH) 4 -carbon fiber composite remained intact after adsorption, which could recollect resources and avoid Zr(OH) 4 leakage into waters. Therefore, the designed Zr(OH) 4 -carbon fiber composite will be a good potential application in precision equipment or skin decontamination equipment.
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高影响因子
Inorganic Chemistry Frontiers
·
2020
·Vol. 7
·期 12
·2343-2351
·
IF 5.958
Ran Wang,Guoan Lin,Xiaoxiang Xu
La/Zr co-doped SrTaO2N has been investigated as visible-light-active photocatalysts for water reduction. Unlike previous aliovalent doping that leads to a decrease in light absorption, La/Zr co-doping largely preserves the visible light absorption of SrTaO2N. More importantly, the La/Zr co-doping not only helps to improve surface hydrophilicity and reduce particle sizes but also effectively inhibits defect formation (e.g. Ta4+) in SrTaO2N. These modifications are responsible for significant enhancements in photocatalytic H2 production. AQE as high as 0.84% was achieved at 420 ± 20 nm for Sr0.4La0.6Ta0.4Zr0.6O2N (x = 0.6), which also showed good durability and stability. Further analysis suggests that La/Zr co-doping negatively shifts the conduction band edge positions of SrTaO2N and contributes to better charge separation conditions.
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JOURNAL OF MOLECULAR LIQUIDS
·
2019
·
IF 4.561
Zhen Huang,Minghu Zhao,Shixing Wang,Linqing Dai,Libo Zhang,Chen Wang
A trithiocyanuric-Zr based MOFs adsorbent (ZT-MOFs) was synthesized by using trithiocyanuric acid as a linker and zirconium chloride as a metal matrix and used to recover Au(III). ZT-MOFs was characterized by FT-IR, BET, Raman and FE-SEM. ZT-MOFs are porous material and have good stability in the range of pH 1–9. ZT-MOFs showed a higher adsorption capacity for Au(III) (333.34 mg/g) at 480 min and pH = 7. The experimental data fitted to Freundlich and pseudo second-order models, indicating a heterogeneous multi-layer chemadsorption is the dominated step. ZT-MOFs separated selectively Au(III) from laboratory wastewater containing various interfering ions. The removal rate of Au(III) decreased only from 94.5% to 87.5% after 4 adsorption and desorption cycles. This shows that ZT-MOFs have good repeatability. FT-IR, XPS and Zeta potential data shows that the adsorption mechanism of Au(III) on ZT-MOFs is coordination. Therefore, ZT-MOFs have great potential in extracting Au(III) from wastewater.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2019
·Vol. 98
·期 3
·767-774
·
IF 1.61
Yuchao Li,Yun Tian,Yanxia Zheng,Tingting Ge,Zhongjun Fu,Tiantian Jiao,Ming Wang,Haofei Huang,Cuncun Zuo
A series of Zr-doped CeO 2 nanorods supported by Au nanoparticle catalysts with different morphologies were prepared for methyl methacrylate (MMA) synthesis via direct oxidation esterification of methacrolein (MAL) with methanol. Catalytic activities under mild conditions (0.3 MPa; 80°C) were evaluated in the kettle reactor. Different characterization methods, such as XRD, Raman, N 2 adsorption, ICP, TEM, SEM, XPS, and H 2 -TPR techniques, were applied to study the relationship between catalytic activity and structural characteristics, especially the form of Zr doped into the lattice of CeO 2 and the promotion mechanism of selective oxidation. The influence of Au supported on Ce 0.6 Zr 0.4 O 2 nanorods (Au/CZ-R) was also discussed. The results exhibited that the highest catalytic activity for the oxidative esterification with a MAL conversion of 99% and a MMA selectivity of 74% was achieved. The MMA synthesis performance correlated well with the surface oxygen vacancies, in particular for the active oxygen species around the Au particles.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 48
·期 3
·1181-1198
·
IF 3.134
Zhang Zhongze,Liu Zonghui,Gu Zhiyuan,Wen Zhe,Xue Bing
The catalytic transfer hydrogenation (CTH) reaction of ethyl levulinate (EL) with alcohol to γ-valerolactone (GVL) has been investigated over a series of Zr-based catalysts, including ZrO 2 , ZrP, Zrβ, ZrP/Hβ and ZrO 2 /HZSM-5. It is found that the simplest ZrO 2 was the most efficient for GVL production, giving an EL conversion as high as 97% and GVL selectivity of 91% after 7 h at 170 °C using 2-propanol as the hydrogen donor and solvent. The effects of reaction temperature, time and solvent on catalytic performance were investigated. Moreover, the kinetic behavior of CTH reaction of EL was also studied over ZrO 2 catalyst. The as-prepared ZrO 2 gives an Ea value of 32.9 kJ/mol, which is much lower than other catalysts in the literatures. Furthermore, those catalysts have been, respectively, characterized by XRD, IR, BET and NH 3 -TPD techniques to reveal the physical properties and structures of these materials. Correlating the catalyst performance with its physical and chemical properties uncovers that the higher pore diameter, lower total acidity and higher Lewis acid sites of catalyst surface would be the key to the catalyst performance. Graphical abstract
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Fengyue Shi,Siyu Huang,Jianwen Wang,Jun Li,Yang Yang,Guangdong Zhao,Dongyu Zhao
Hollow-structured ceramic fibers with multiple components are ideal as lightweight insulation materials. In this study, tetraethyl orthosilicate , boric acid, and zirconia octahydrate were used as raw materials for fabricating SiZrBOC hollow ceramic fibers through coaxial electrospinning. These ceramic fibers exhibit a low thermal conductivity and an excellent temperature resistance. The electrospun SiZrBOC hollow ceramic fibers display a clean and compact morphology with internal folds. Fourier-transform infrared spectroscopy and thermogravimetric analysis (TGA) were used to assess the transformation process and thermal behavior of the hollow ceramic fibers. The results suggest that the incorporation of B promotes the formation of Si–O–B bonds within the system, leading to a maximum yield of 75.49 wt% for the production of the SiZrBOC hollow ceramic fibers. The phase composition and microstructure of the SiZrBOC hollow ceramic fibers were analyzed via X-ray diffraction (XRD) measurements. The pyrolysis at 1000 °C resulted in the appearance of diffraction peaks corresponding to SiO 2 and SiC in the XRD patterns of the SiZrBOC hollow ceramic fibers. Laser thermal conductivity measurements reveal that the SiZrBOC hollow ceramic fibers exhibit a thermal conductivity of only 0.06 W‧m −1 K −1 at 25 °C and 0.124 W‧m −1 K −1 at 500 °C, indicating a significantly superior thermal insulation performance compared with conventional solid SiZrBOC ceramic fibers.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Zhangyi Huang,Zhengwei Zhu,Mingyu Su,Yang Shi,Mao Deng,Ruichong Chen,Zhijun Wang,Zhi Zhou,Jianqi Qi,Haomin Wang
This study investigated the high-temperature oxidation behaviors of TMC ceramics. The results indicate that the high-temperature oxidation curves of the four TMC ceramics follow a parabolic law, suggesting a diffusion-controlled process. The activation energies for the oxidation of TaC, NbC, TiC, and ZrC ceramics are 105.4, 124.3, 169.3, and 78.7 kJ/mol, respectively, with oxidation rate constants at 1000 °C of 16.84, 40.45, 0.18, and 14.43 mg 2 /cm 4 ·h for each ceramic, respectively. The temperatures at which the ceramics disintegrate into fragments in high-temperature air are 800, 800, >1000, and 600 °C, respectively. The anti-oxidation performance of the four TMC ceramics ranks as follows: TiC > TaC > NbC > ZrC. In comparison to the reported high-entropy carbide ceramics, the TiC ceramic in this study demonstrates superior anti-oxidation performance due to dense TiO 2 layer formation, characterized by significantly low oxidation rates and excellent structural stability.
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