CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Daoyan Feng,Yu Liu,Chen Zhao,Han Su,Xia Kong,Yu Zhong,Junzhang Wang,Zhou Xu,Xiuli Wang,Xingzhong Guo,Jonghee Lee,Jiangping Tu
Achieving a stable interface between sulfide solid-state electrolytes (SSEs) and high-voltage Ni-rich oxide cathodes is crucial for enhancing the electrochemical performance of all-solid-state batteries (ASSBs). However, addressing the interface challenges through surface coating modifications remains a significant hurdle. In this work, a straightforward modification approach is proposed to achieve a highly stable interface by surface dual doping of Zr and F in LiNi 0.83 Co 0.12 Mn 0.05 O 2 (NCM83) cathodes via acid washing followed by annealing. First-principle calculations demonstrate the thermodynamic stability of Zr-F doped NCM83, effectively inhibiting the formation of unfavorable interfaces with decomposition products. The modified NCM83-1% ZrF cathode exhibits exceptional long-cycle stability, retaining 85.1% of its capacity after 1000 cycles at 0.5C rate. This simple and scalable modification strategy offers a new perspective for the design of high-performance sulfide-based ASSBs.
研究领域:
材料科学
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电化学
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固态电池
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能源存储
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界面工程
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JOURNAL OF POROUS MATERIALS
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2023
·Vol. 30
·期 6
·2129-2137
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IF 2.6
Tao Ruyu,Liu Hao,Xiang Pan,Lin Yichao,Zhou Junjie,Zhou Chen,Zhao Yayun,Tian Ziqi,Zhang Qiuju
Nanoscale Zr-based metal-organic framework (MIP-202) particles were successfully prepared via a seeds-assisted hydrothermal secondary synthesis. The uniformly-shaped MIP-202 particles exhibit excellent performance on selective CO 2 adsorption from CO 2 /CH 4 and CO 2 /N 2 mixtures. At 298 K and 1 bar, the uptake ratios of CO 2 /CH 4 and CO 2 /N 2 of MIP-202 particles are as high as 32.6 and 65.2, respectively. The IAST (ideal adsorbed solution theory)-predicted selectivities of CO 2 /N 2 (50/50, v/v) and CO 2 /CH 4 (50/50, v/v) reach to 4.5 × 10 10 and 102.2, respectively. The breakthrough experiments further demonstrate that the CO 2 /CH 4 and CO 2 /N 2 mixtures can be efficiently separated through an adsorption column packed with MIP-202 particles. In addition, the as-prepared MIP-202 particles had a low iso-enthalpy of adsorption of CO 2 of 32.95 kJ/mol, which is favorable for the regeneration of the adsorbent. Herein the as-prepared MIP-202 is a potential material for efficient separation of CO 2 from CH 4 or N 2 through an energy- and cost-saving CO 2 capture process.
研究领域:
材料科学
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环境化学
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能源工程
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纳米技术
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MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Meimei Guo,Fang Li,Qiwen Ran,Gan Zhu,Yunhang Liu,Jiale Han,Guifang Wang,Hongyuan Zhao
A novel methyl parathion (MP) electrochemical sensor was fabricated from the multifunctional composite of Zr-based metal–organic framework (UiO-66) and Ketjen black-carbon nanotubes (KB-CNTs), which achieved the sensitive detection of MP in food samples. For the UiO-66/KB-CNTs composite, Zr-based UiO-66 with Zr-OH groups possessed good affinity for phosphate groups on methyl parathion molecules, which enhanced the selective recognition and enrichment capability towards MP, and KB-CNTs possessed three-dimensional interconnected carbon conductive network with synergistic point-line carbon conductive contact, which showed excellent electrical conductivity. Moreover, KB with pearl chain-like structure and more conductive contact points realized the full contact between KB-CNTs and UiO-66 with Zr-OH groups. The fabricated UiO-66/KB-CNTs/GCE sensor showed good MP detection performance with low limit of detection of 1.53 nM in linear MP concentration range of 0.005–12 µM. Moreover, the fabricated sensor showed good repeatability, reproducibility, and selectivity. A good practical feasibility can be achieved at the UiO-66/KB-CNTs/GCE sensor for the detection of MP in grape juice and apple juice samples (Recovery rate: 96.14–102.93, relative standard deviation: 2.17%-4.95%).
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Chi Ma,Chenyu Qi,Dingbo Wei,Zhenzhen Jiang,Yafei Guo,Nelson Belzile,Tianlong Deng
The efficient and renewable recovery of cesium and strontium by absorption from a new type of geothermal water liquid mineral resource is highly desirable but still challenging. In this work, a new Zr-doped layered potassium thiostannate adsorbent (KZrTS) was first synthesized and used for Cs+ and Sr2+ green and efficient adsorption. It was found that KZrTS had very fast adsorption kinetics toward both Cs+ and Sr2+ with an equilibrium reached within 1 min, and the theoretical maximum adsorption capacities for Cs+ and Sr2+ were 402.84 and 84.88 mg/g, respectively. Moreover, to solve the loss problem of the engineering application of the powdered adsorbent KZrTS, KZrTS was uniformly coated with polysulfone by wet spinning technology to form micrometer-level filament-like absorbents (Fiber-KZrTS), whose adsorption equilibrium rates and capacities toward Cs+ and Sr2+ are almost the same as that of powder. Furthermore, Fiber-KZrTS showed excellent reusability, and the adsorption performance remained virtually unchanged after 20 cycles. Therefore, Fiber-KZrTS has potential application for green and efficient cesium and strontium recovery from geothermal water.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2022
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IF 10.319
Linjing Liu,Bin Yang,Rui Lv,Qiangwei Kou,Shuai Yang,Hang Xie,Yuan Sun,Yunfei Chang,Shan-Tao Zhang,Fei Li
Piezoceramics with high and fatigue-resisted piezoelectric properties are strongly desired for actuator applications. In this work, textured Pb(Mg 1/3 Nb 2/3 )O 3 -Pb(Zr, Ti)O 3 ceramics with Lotgering factor F 001 ∼98% were fabricated by templated grain growth technique. Strong [001] c -grain orientation ( f ∼90% and r ∼0.22) of the textured ceramics effectively produced about 230% enhanced piezoelectric coefficient d 33 * (i.e., S max / E max ) and substantially improved unipolar electrical fatigue resistance. Unipolar polarization P max and d 33 * of the textured ceramics were nearly maintained up to 10 6 unipolar cycles, while 19% and 14% degradations were respectively observed from randomly oriented counterparts. Especially, normalized d 33 * of the textured ceramics shows better unipolar fatigue resistance than those of piezoceramics reported previously. Much lower bipolar strain asymmetry γ s (∼4%) was observed from the textured samples fatigued after 10 6 unipolar cycles as compared to γ s ∼23% for randomly oriented counterparts. While charged defect accumulation model described the serious fatigue deteriorations in randomly oriented ceramics, the current work revealed that substantially enhanced unipolar fatigue resistance of the textured ceramics is mainly associated with the inherent fatigue anisotropy, weakened local bias fields owing to both enhanced domain mobility and lower defect density near grain boundaries/interfaces, and increased intrinsic contribution due to more tetragonal content. These superior characteristics suggest the great potential of textured ceramics for high-performance and robust actuator applications.
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PROGRESS IN ORGANIC COATINGS
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2023
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IF 6.6
Min Cao,Guoqing Xiao,Chunlin Chen,Chunyan Chen,Zhengwei Yang,Fei Zhong,Shuyi Shang,Mingtan Wang,Rui Zou
In this study, in an attempt to get an excellent flame retardant , herein, a new nanofiller (CNP@UiO-66@TEOS) with polyethyleneimine (PEI) as a crosslinker, Zr-based metal-organic framework (UiO-66) and tetraethoxysilane (TEOS) modified graphitic carbon nitride (CN) was synthesized. Different characterization tests confirmed the successful preparation of CNP@UiO-66@TEOS. Then, CNP@UiO-66@TEOS was doped into intumescent fire retardant (IFR) coating by solution blending method and the coating (CNP@UiO-66@TEOS/EP) was gained after curing. As expected, the CNP@UiO-66@TEOS significantly improved the fire performance of the IFR coating. The coating (CNP@UiO-66@TEOS/EP) with the addition of 2 wt% CNP@UiO-66@TEOS reduced the backside temperature by 102.9 °C over that of pure EP, proving enhanced flame retardancy. Meanwhile, CNP@UiO-66@TEOS/EP achieved the highest expansion height (21.5 mm) in the furnace experiment, contributing to a lower heat transfer ratio. In addition, the thermogravimetric analysis revealed an increase in residual char content to 31.84 wt%, which helped to resist external heat penetration. Cone calorimeter testing (CCT) showed that the peak heat release rate (PHRR), total heat release rate (THR), peak smoke production rate (PSPR), total smoke production (TSP), peak CO production rate (PCOPR), and peak CO 2 production rate (PCO 2 PR) of CNP@UiO-66@TEOS/EP were reduced by 29 %, 19 %, 35 %, 37 %, 36 %, and 19 %, respectively, compared to pure EP, demonstrating the improved flame retardancy and smoke suppression properties. The results indicated that CN formed a thermal barrier at a high temperature and UiO-66 generated zirconium oxide (ZrO 2 ) to catalyze the formation of residual char, thus producing a barrier effect. The TEOS on the UiO-66 surface further decomposed to form a silicon network to enhance the char layer strength of the composite. The synergistic outcome of CN, UiO-66, and TEOS offers potential avenues for the development of efficient IFR coating.
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ACS Catalysis
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2023
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IF 12.9
Xugang Yang,Zaihao Yuan,Minghao Zhou,Feng Chen,Bo-Qing Xu,Hui Shi
Lewis acidic heterogeneous catalysts are known to be active for transfer hydrogenation of carbonyl compounds, which occur naturally or can be derived from renewable feedstocks. While previous studies have explored a myriad of Zr-based catalytic systems toward the Meerwein–Pondorf–Verley (MPV) reductions, few have determined intrinsic, site-specific rates under strict kinetic control across a sufficiently wide range of process conditions, causing misconceptions about the true potentials of these catalysts for the targeted transformations. Here, we present a quantitative assessment on the intrinsic activities of four types of Zr catalysts that are purportedly promising candidates for the MPV reductions; the selected catalysts contain active Zr sites within diversified local coordination and secondary solvating environments. A comprehensive kinetic study of ethyl levulinate (EL) MPV reduction in 2-butanol, combined with in situ quantitative titration of the active sites by selective poisoning with alkylphosphonic acid titrants of Lewis acid sites during the reaction, reveals dramatic differences in the relative fraction of active sites (13–78% of total Zr) and turnover rates (>300-fold) among the studied catalysts. Mechanistically, the hydride shift invariably remains as the sole rate-limiting step, regardless of the catalyst; the free energy barriers in both first-order and zero-order kinetic regimes and kinetic isotope effects, however, differ significantly among the catalysts. Through mechanism-based rate equations and transition-state-theory treatments, we further delineate that the wide variations in enthalpic and entropic components not only suggest disparate transition state structures and energetics but also reflect varying adsorption thermodynamics that are influenced by both reactant coordination at and solvent restructuring near the active sites.
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ChemCatChem
·
2023
·Vol. 15
·期 16
·e202300475
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IF 4.5
Haoxi Jiang,Bingyu Wang,Lingtao Wang,Guochao Yang
Graphical Dissolution-recrystallization strategy benefits both the porosity and Lewis acidity in Zr- β zeolite, which promotes catalytic conversion of ethanol-acetaldehyde. Zr based metallosilicalites, especially Zr- ß , is promising catalyst for the conversion of ethanol to 1,3-butadiene, which is considered to be a sustainable alternative to petroleum steam cracking. However it is suffering from deactivation derived from coking and unsatisfied catalytic activity derived from deficient Lewis acidity. For these issues, a dissolution-recrystallization process through tetraethyl ammonium hydroxide treatment (TEAOH) for enhancing porosity and Lewis acidity of Zr- ß zeolite was developed in this study. A balance of dissolution and recrystallization existed in this process, which was produced by OH − etching and templating of TEA + ions, creating additional mesoporosity. Zirconium active sites maintained tetrahedral coordination, while the Lewis acidity was enhanced by creating higher proportion open sites in framework. The recrystallized Zr- ß exhibited higher catalytic activity and stability in the conversion of ethanol-acetaldehyde to butadiene due to the compromise of microporosity and mesoporosity, as well as the appropriate enhancement of Lewis acidity.
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PROGRESS IN ORGANIC COATINGS
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2022
·
IF 6.206
Dehong Fan,Xiaobang Liu,Kai Qi,Zhenyu Chen,Yubing Qiu,Bokai Liao,Xingpeng Guo
A smart-sensing coating is developed by adding a dual-emission fluorescent zirconium metal-organic framework/rhodamine B composite (Zr-MOF@RhB) into the commercial epoxy resin coating, which can autonomously detect and distinguish the damage of surface coating and the corrosion of substrate aluminum . The orange-yellow fluorescence can be observed to identify the area of mild coating damage without metal corrosion, resulting from the cumulative release of Zr-MOF@RhB with the emission wavelength of 583 nm. In case of the occurrence of aluminum corrosion, the fluorescence color turns from orange-yellow to green, in which the emission behavior of Zr-MOF@RhB at 490 nm is greatly enhanced with the presence of Al 3+ ions. The smart-sensing ability can availably and robustly operate in the conditions of long term, wide ranges of pH and temperature, and diverse interfering substances. This simple and powerful warning system relying on fluorescent MOFs would not only extend the practical applications of MOFs but also be a promising candidate for smart coating strategies.
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ACS Applied Energy Materials
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2022
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IF 6.959
Jian Sun,Shengbin Bai,KeKe Li,Yue Zhou,Yuning Chen,Lei Liu,Zijian Zhou
CaCO3/CaO materials possess the advantages of low cost, high energy storage density, and working temperature, which offer these materials the potential to be used in thermochemical energy storage systems for concentrated solar power plants. However, CaCO3/CaO materials possess poor antisintering and optical absorption abilities, largely limiting their practicability for direct solar utilization. In this study, binary ion doping of Fe/Mn and Zr-based stabilizer incorporation were simultaneously conducted to improve the cyclic thermal energy storage/release performance of CaCO3/CaO materials. The spectral absorbance of synthetic CaO-based composites (ranging from 77.8% to 84.0%) doped with binary ions of Fe/Mn is greatly increased in comparison to that of pure CaO (∼12.2%) due to the generation of black Ca2Fe2O5 and Ca4Mn3O10. The cyclic thermal energy storage/release performances of synthetic CaO-based composites were comparatively investigated under two thermal energy storage modes (CSP-N2 and CSP-CO2). The Zr-doped, CaO-based composites exhibit a cycling stability superior to those of Zr-free CaO-based composites due to the generated inert CaZrO3 with desirable antisintering ability, and the superiority is more prominent under CSP-CO2 mode. After 50 cycles, the CaO-based composite with a molar ratio of Ca:Zr = 100:6.7 exhibits a remarkably stable energy release density of 1.02 MJ/kg under CSP-CO2 mode, retaining 88.9% of its initial energy release density.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Xueting Liu,Chunhui Hu,Jingjing Wu,Peng Cui,Fengyu Wei
In this study, a series of metal–organic frameworks (MOFs) NH 2 -UiO-66- x HAc catalysts were synthesized by solvothermal method using acetic acid (HAc) as a modulator, and were applied to the cycloaddition of CO 2 and epichlorohydrin (EPIC) under ambient pressure. Influences of the modulation by HAc on morphologies and structures of the MOFs are demonstrated via PXRD, FESEM, FTIR, N 2 adsorption–desorption, XPS and 1 H NMR characterizations. The results show that the MOFs containing mesoporous pores can be prepared by adjusting the concentration of HAc. By optimizing the amount of HAc added, the specific surface area of NH 2 -UiO-66-8HAc is as high as 879.17 m 2 ·g −1 , which is 28.3% higher than that of the original MOFs. And the evaluation of catalytic performance showed that HAc modulation enhanced the activity of NH 2 -UiO-66- x HAc under mild conditions. The exposure of Lewis acid sites, increased specific surface area and porosity via the modulation of HAc defective ligand can be supposed the key factors to determine the enhanced catalytic activities. In addition, considering the influence of gas concentration on the reaction, the concept of TOP (Turnover of Pressure, defined as the mass of conversions of a unit mass catalyst under unit pressure and unit time) was first proposed in this article.
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CERAMICS INTERNATIONAL
·
2021
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IF 4.527
Hongrong Mei,Liangbin Zhang,Chunchun Li,Zhenggang Rao,Longlong Shu
Two garnet-structured Ca 3 MgBGe 3 O 12 (B = Zr, Sn) ceramics with tetravalent cations at B-site were prepared by conventional solid state reaction. The crystal structure, microstructure evolution, and microwave dielectric performance were investigated using X-ray powder diffraction, Rietveld refinement , scanning electron microscopy, Raman spectroscopy , and infrared spectroscopy techniques . Dense Ca 3 MgZrGe 3 O 12 and Ca 3 MgSnGe 3 O 12 ceramics were obtained at sintering temperatures of 1420 and 1400 °C, respectively. The dielectric constant, unloaded quality factor, and temperature coefficient of resonance frequency of Ca 3 MgZrGe 3 O 12 were 10.80 ± 0.2; 79,600 ± 1000 GHz ( f = 12.61 GHz); and −66.8 ± 1 ppm/°C, respectively, and the corresponding values for Ca 3 MgSnGe 3 O 12 were 9.68 ± 0.2; 83,400 ± 1000 GHz ( f = 14.19 GHz); and −57.9 ± 1 ppm/°C, respectively. The dielectric performances of the two ceramics were compared by analyzing the ionic polarizability, packing fraction, and bond valence. The intrinsic dielectric properties were predicted by fitting the infrared reflectivity spectra.
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