SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Qin Wang,Xue Bai,Shiyu Sun,Yan Li,Mingzhe Tan,Yanfeng Wang,Na Wang,Ting Wang,Lina Zhou,Zijian Zhou,Xin Huang,Hongxun Hao
The fluorine chemical industry's rapid growth demands efficient strategies for treating and utilizing the costly and inefficient byproduct, fluoride-containing hydrochloric acid, posing a significant challenge. In this study, a cost-effective method was developed for preparing an acid-resistant and efficient defluorination material. Carbon nitride (C 3 N 4 ) was chosen for its exceptional acid resistance and was modified via template-free doping with different zirconium source. Characterization results through XRD, FTIR, BET, XPS, SEM, and TEM confirm the successful synthesis of CN-Zr using zirconium chloride (ZrCl 4 ) with a specific surface area of 87.77 m 2 /g. Furthermore, the adsorption results indicate outstanding fluoride adsorption performance of CN-Zr in hydrochloric acid, with a maximum adsorption capacity of 145.34 mg/g and minimal zirconium leaching. Moreover, the adsorption mechanism was systematically studied using Zeta potential, FTIR and XPS characterization. The findings indicate that Zr was integrated with C 3 N 4 uniformly by forming a deep eutectic system (DES), utilizing exposed terminal amino groups for effective hydrogen bonding with HF which predominates as the primary fluorine existence in hydrochloric acid. Meanwhile, the enhanced ion exchange, complexation of Zr-F and strong electrostatic attraction all contribute to improving adsorption. Finally, the assessment of recyclability performance and operation cost demonstrate that the material can maintain 80% of its initial adsorption capacity after five cycles. The cost analysis results indicate that the adsorption cost is only 0.3157 CNY/g, making it considerable competitive in the industry.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Xiaoxiao Zheng,Xiaoping Chen,Xiaoqing Li,Jide Zhu,Jipeng Chen,Fengcai Lin,Lijuan Shen,Yanlian Xu,Lilong Jiang
The development of stable and effective catalysts to convert toxic H2S into high value-added sulfur is essential for production safety and environmental protection. However, the inherent defects of traditional iron- and zirconium-based catalysts, such as poor activity, high oxygen consumption, and low sulfur selectivity, limit their further developments and applications. Herein, the Fe–Zr bimetallic organic framework FeUIO-66(x) with different cubic morphologies was synthesized via a facile solvothermal method. The results indicate that the introduction of Fe not only increases the specific surface area and weak L-sites of the catalyst without changing its crystal structure, which provides enough reaction space and more active sites for the adsorption and activation of H2S, but also reduces the activation energy of the reaction, significantly promoting the selective oxidation of H2S. As a result, the as-obtained FeUIO-66(1) catalyst exhibits the highest desulfurization activity and superior durability and water resistance stability, and its H2S conversion and sulfur selectivity within 50 h are 100 and 88%, respectively. More importantly, the structure of the catalyst after the desulfurization reaction is consistent with that of the fresh counterpart. The study offers new insights into the development of effective and stable bimetallic catalysts to eliminate H2S and recycle sulfur.
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PubMed
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Hua Yan,Yu-hong Luo,Ying Lei,Qing-lin Pan,Jun-chao Zheng
N ickle (Ni)-rich layered oxides as promising candidate of high-capacity cathode materials have aroused extensive concern primarily regarding their higher specific capacity. However, the major hurdle of Ni-rich cathodes (Ni content ≥0.7) is their poor cycling stability, which often suffers from the release of oxygen, structural degradation and increased impedance during cycling, especially at high voltage or high temperature. Herein, we demonstrated a feasible solid phase method for easy industrialization based on the Al 3+ /Zr 4+ co-doping in LiNi 0.72 Co 0.05 Mn 0.23 O 2 (A X Z Y -NCM) single-crystal cathode. The optimized A 0.5 Z 0.5 -NCM single-crystal material exhibited greatly enhanced structural and thermal stability. XRD refinement results indicated that both Al 3+ and Zr 4+ were mainly located in transition metal (TM) sites, strengthening the layered structure through strong M-O bonds and inhibiting cation mixing. In-situ XRD revealed that the synergistic rivet effect of Al/Zr co-doping alleviates anisotropic lattice stress-strain during charge/discharge process. Accordingly, the A 0.5 Z 0.5 -NCM cathode can output a high initial capacity of 177.3 mAh g −1 at 1 C, and captured a more desirable capacity retention of 85.10 % than that of U-NCM (74.33 %) at 1 C over 200 cycles. Even at a high voltage of 4.5 V, its capacity retention can still reach 82.37 %, significantly surpassing the unmodified U-NCM (31.0 %). The above results demonstrated that well-designed dual doping is highly effective for strengthen structure stability and cycling performance of Ni-rich cathodes.
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Journal of the Australian Ceramic Society
·
2024
·
IF 1.8
Lin Jia,Wang Shuai,Yang Yihang,Huang Guimei,Wang Jinhuo
In this study, Zr-modified Si-O-C precursor ceramics were prepared using three-dimensional (3D) printing. Ceramic sintering was completed by printing four precursors containing different zirconium acetylacetone contents. Comparative analysis was conducted on the ceramic yield, size shrinkage, mechanical properties, and microstructure. The results showed that the ceramic yield and size shrinkage of the four samples were increased with the increasing zirconium acetylacetone contents. The sample containing 30 wt% zirconium acetylacetone exhibited good compressive performance, with a compressive strength of 50.2 ± 0.6 MPa. Cracks were observed on the surface of samples containing 40 wt% zirconium acetylacetone, while those containing 10, 20, and 30 wt% zirconium acetylacetone were relatively intact. Therefore, a stable Si-Zr-O-C precursor ceramic with good mechanical properties, which can be used for 3D printing, was obtained.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Yu-Xuan Zheng,Xuwen Wu,Wei-Guang Yang,Bai-Xue Li,Kejing Gao,Jingsheng Zhou,Yunfang Liu,Dongzhi Yang
Radioactive nuclides and highly toxic organophosphates are typical deadly threats. Materials with the function of radioactive substances adsorption and organophosphates degradation provide double protection. Herein, dual-functional polyamide (PA)/polyethyleneimine (PEI)@Zr-MOF fiber composite membranes, fabricated by in-situ solvothermal growth of Zr-MOF on PA/PEI electrospun fiber membranes, are designed for protection against two typical model compounds of iodine and dimethyl 4-nitrophenyl phosphate (DMNP). Benefiting from the unique core-sheath structure composed of inner nitrogen-rich fibers and outer porous Zr-MOF, the composite membranes rapidly enrich iodine through abundant active sites of the outer sheath and form complexes with the amine of inner PEI, exhibiting a highly competitive adsorption capacity of 609 mg g −1 . Moreover, it can adsorb and degrade DMNP with the synergy of PEI component and Zr-MOF, achieving an 80 % removal of DMNP within 7 min without any additional co-catalyst. This work provides a feasible strategy to fabricate dual-functional materials that protect against radioactive and organophosphorus contaminants.
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PubMed
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Kai Han,Chen Zhou,Jianlong Wang,Nana Zhao,Jinfeng Yuan,Zhicheng Pan,Mingwang Pan
Robust, self-healing waterborne coatings have become the preferred choice in the field of flexible electronic devices owing to their outstanding compliance, restorability, and environmental friendliness. Nevertheless, most of the existing self-healing waterborne polymers exhibit viscoelasticity, irreversible fatigue damage, and the challenge of reconciling self-healing functions with mechanical properties, all stemming from inherent molecular structure contradictions between flexibility and rigidity. Here, we propose a novel strategy that utilizes a nanofiller with dynamic reversible bonds to overcome the self-healing limitations that theoretically demand flexible chain, for achieving both mechanical robustness and self-healing ability in the waterborne polyurethane (WPU) hybrid coating system. We modified tetrapropyl zirconate (TPOZ) with 3-aminopropyltriethoxysilane (APTES) to enhance compatibility between the matrix and inorganic particles, while the formation of dynamic reversible bonds through both condensation hydrolysis endows the self-healing abilities. The WPU hybrid coating was designed by covalently incorporating amino-modified TPOZ (A-ZrO 2 ) into a glycinamide-functionalized WPU network, conferring excellent fracture energy (50.3 kJ/m 2 ), elastic recovery, along with antistatic capability to the coating. Furthermore, the hybrid coating maintains a robust mechanical performance alongside 92.58 % of healing efficiency, exhibiting a potential for flexible electronics application. The hybridization strategy via incorporation of the nanofillers with hard but reversible covalent bond resolves the inherent robustness-healing trade-off, providing exciting thoughts to expand WPU applications.
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APPLIED SURFACE SCIENCE
·
2025
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IF 6.9
WooYeon Moon,Dong Gyu Park,Younghu Son,Minyoung Yoon,Kyung Min Choi
The removal of bromide ions (Br − ) from water is critical, as these ions can generate bromate and brominated disinfection by-products that are toxic, carcinogenic, and corrosive. Previous research has not focused on the removal of Br − from water with a heavy presence of chloride ions (Cl − ). To address this research gap, we proposed a defective Zr-based metal–organic framework (MOF) to selectively remove trace Br − in environments with high concentrations of Cl − . We demonstrated that the open acidic sites on the secondary building units in a defective Zr-based MOF-808 (MOF-808-Cl) selectively removed the trace Br − in the presence of high concentration of Cl − using varying degrees of electrostatic interactions induced by their own polarizability. The Br − removal was performed with the mixed mechanism of ion-exchange and −adsorption, with contributions of approximately 70% and 30%, respectively. The Br − was successfully removed when the concentration of Cl − was 100 times higher than that of Br − . Our findings demonstrate the potential of MOF-808-Cl for industrial applications requiring trace ion removal and can provide insights for future research on selective ion removal in a competitive environment.
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APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Tinghao Han,Zhongdi Liu,Lincai Peng,Weipeng Song,Huai Liu,Wenlong Jia,Rui Zhang
The efficient production of γ-valerolactone (GVL) with high yield directly from xylose is of particular interest but remains a great challenge due to the long reaction path. We herein developed a facile catalytic system to directly convert xylose to GVL with a record-high yield of 54.3 %, employing β-zeolite supported Zr-based catalyst in 1,4-dioxane/isopropanol co-solvent. Using Zr(NO 3 ) 4 ·5 H 2 O as the Zr sources resulting in well-retained β-zeolite structure, larger surface area and pore volume and better dispersion of Zr species, as well as balanced acidic sites where higher amount of Brønsted acid sites promoted the ring-opening of furfural alcohol for this cascade reaction. Notably, the introduction of 1,4-dioxane facilitated the in situ formation of furfural (i.e. yield-determining step) by diluting the competitive adsorption behavior between isopropanol and xylose, allowing more xylose molecules to access the active center, thus promoting the sequential production of GVL with unexpectedly high yield. The present work provides a efficient and straightforward preparation of GVL from xylose, paving the pathway towards higher atom economy.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2025
·Vol. 36
·期 24
·1-13
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IF 2.8
Rafiq Muhammad Nasir,Dai Zhonghua,Zheng Yuanyuan,Li Xujun,Liu Chenxi,Zhao Xin,Cong Yu,Gu Shuitao
The performance of lead-based ceramics in energy storage applications is often hindered by their low energy density and inadequate phase transition properties. The (Pb, La) (Zr, Sn, Ti)O 3 (PLZST) antiferroelectric ceramics have attracted much attention as energy storage materials. In this work, ceramics Pb 1−1.5 x La x (Zr 0.93 Sn 0.05 Ti 0.02 )O 3 at ( x = 0.015, 0.025, 0.035, and 0.045) were prepared using a solid-state method, and their dielectric and energy storage characteristics were studied. It was observed that integrating lanthanum significantly improved the perovskite structure, reducing grain size and boosting the polarization intensity. In this present study, a recoverable energy storage density ( W rec ) of 6.24 J/cm 3 was achieved under an electric field of 270 kV/cm. Moreover, these ceramics demonstrated an impressive discharge energy density ( W dis ), with 90% of the energy released within 1.29 μs. The outcomes show that PLZST is a highly effective material for advanced energy storage, pulse power applications, and paving the way for technological advancements.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lihua Liu,Miao Zhang,Luqing Zhang,Yizhen Song,Lin Sun,Pengtao Ma
Photoresponsive functional materials, especially photochromic materials, have recently emerged as critical players in advancing cutting-edge optical applications. Herein, a Dawson-type Zr-substituted phosphotungstate, [NH 2 (CH 3 ) 2 ] 6 H 3 [( α 1 -P 2 W 17 O 61 )Zr(HCIT)]·9H 2 O ( 1 ; H 4 CIT = citric acid), was synthesized from a hexavacant precursor [H 2 P 2 W 12 O 48 ] 12− via a conventional solution method. A notable feature of compound 1 is that the substitution site of the polyanion [( α 1 -P 2 W 17 O 61 )Zr(HCIT)] 9− is positioned at the equator of the Dawson structure. This sharply contrasts with the previously reported polar substitution sites. Compound 1 was systematically characterized by IR, PXRD, XPS, UV, 31 P NMR and TGA. This compound possesses conspicuous photochromism with the half-life (t 1/2 ) achieved 0.140 min. The in vitro cytotoxicity assessment of compound 1 revealed minimal toxic effects on the normal cell lines NIH-3 T3 (mouse embryonic fibroblasts) and AML-12 (mouse normal hepatocytes). Even at a high concentration of 80 μg/mL, cell viability remained greater than 90 %. Additionally, a photochromic composite film GEL/TEG/ 1 was prepared by incorporating 1 into a triethylene glycol (TEG) and gelatin (GEL) matrix. The GEL/TEG/ 1 composite film exhibited a pronounced color change within 30 s of UV irradiation (λ = 365 nm) and reached saturation in 6 min. Photochromic films demonstrate rapid, light-induced patterning capabilities that enable facile image formation without conventional printing processes. The photopatterned images on the film demonstrated reversible behavior, with complete erasure occurring within 3 h under ambient conditions. The GEL/TEG/ 1 film demonstrated excellent cycling stability, maintaining reproducible coloration–decoloration behavior over at least 10 consecutive cycles without significant performance degradation. The GEL/TEG/ 1 film demonstrates potential for applications in ink-free patterning and advanced anti-counterfeiting technologies, leveraging its reversible photochromic properties.
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JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Yu-Teng Zhang,Jing- Yu Sun,Jian Li,De-Sheng Wei,Wan-Yi Lan,Nan Lv,Shuang-Bao Li
This study reports one-pot microwave-assisted solvothermal synthesis of Ti-Zr bimetallic organic cages (TiZrT-BTC-α, where α denotes the actual Ti molar percentage and T represents the tetrahedral cage structure). The reaction employed zirconocene dichloride (Cp 2 ZrCl 2 , Cp = η 5 -C 5 H 5 ), titanocene dichloride (Cp 2 TiCl 2 ) and 1,3,5-benzenetricarboxylic acid (H 3 BTC) as solid precursors to form a V 4 F 4 (V = vertex and F = face) coordination tetrahedron. The presence of the characteristic Ti-O vibration band at 420 cm -1 in the FT-IR spectrum, along with the characteristic Ti 4+ band signal at 458.6 eV in the XPS spectrum, collectively demonstrates the successful incorporation of titanium into the molecular cage structure. Notably, the introduction of titanium endowed the material with visible light absorption capability and modulates its electronic structure, reducing the band gap value from 3.73 eV (ZrT-BTC) to 2.48 eV (TiZrT-BTC-7.9). The photocatalytic activities of TiZrT-BTC-α were evaluated using tetracycline hydrochloride (TC) as a target pollutant under visible light illumination. Among the series, TiZrT-BTC-7.9 demonstrated excellent photocatalytic activity, achieving 92.17% degradation efficiency for TC (20 mg/L) within 3 hours. Electron spin resonance (ESR) spectroscopy combined with radical trapping experiments identified superoxide radicals (·O 2 - ) served as the dominant reactive species. This work paves the way for developing cage-based photocatalysts with tunable optoelectronic properties.
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Chem
·
2024
·
IF 19.1
Xiaoze Wang,Xia Wang,Jianxin Song,Hongliang Bao,Mengjia Yuan,Yanlong Wang,Lingxin Kong,Wei Liu
Developing materials capable of converting high-energy photons into visible (vis) or ultraviolet (UV) light serves as an effective approach for achieving X-ray detection and imaging. In this work, highly luminescent metal-organic gel (MOG), YTU-G-1, was obtained by self-assembling the aggregation-induced emission luminogen (AIEgen)-functionalized ligand and Zr oxo-hydroxy clusters via a mild solvothermal method. The dense and rigid MOG skeleton offers the opportunity to maximize the AIE effect, achieving near-unity quantum efficiency of 95.5%. Under X-ray irradiation, YTU-G-1 exhibits bright luminescence and can detect low-dose radiation down to 44 nGy s −1 . The robust Zr–O bond imparts the material with excellent chemical and physical resistance, making it an ideal candidate for fabricating large-area flexible membranes. Consequently, the spatial imaging resolution of the flexible scintillating membrane reaches 20 lp mm −1 . This work offers a general strategy for fabricating scintillators based on MOGs and facilitates the construction of flexible X-ray imaging membranes.
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