Catalysts
·
2026
·Vol. 16
·期 4
·312
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IF 4.5
Xuelai Zhao,Wuyu Wang,Zhenjing Jiang,Xinghua Zhang,Xiuzheng Zhuang,Qi Zhang,Longlong Ma
The homogeneous nature of L-proline organocatalysts restricts their application in aldol condensation due to poor recyclability and stability. Herein, L-proline was heterogenized by ionic intercalation into Mg–Al layered double hydroxides (LDHs), yielding a series of proline-intercalated catalysts with tunable layer structures. Co-precipitation and memory-effect reconstruction strategies were employed to regulate interlayer spacing and proline loading. The resulting catalysts exhibited efficient performance in the aldol condensation of furfural with ketones under mild conditions. The reconstructed catalyst re-Mg4Al1P achieved a furfural conversion of 88.67% and a total product yield of 85.54% at room temperature, with product selectivity exceeding 95%. Structural characterizations confirmed that proline was stabilized within the LDH interlayers via R–COO—Mg electrostatic interaction while preserving the secondary amine active site. Mechanistic analysis indicated that the reaction proceeded through enamine- or enol-mediated pathways depending on water content, while the layered LDH framework imposed geometric confinement that suppressed side reactions. Catalyst deactivation in aqueous systems was mainly attributed to proline leaching rather than structural collapse.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2026
·
IF 6.7
Wenjing Zhang,Yun Wang,Hao Xu,Hui Zhang,Xiaoxia Lv,Xiaobo Pan
The development of high-performance aqueous zinc-ion batteries (AZIBs) is hindered by the intrinsic limitations of manganese-based cathodes, such as poor electronic conductivity and structural instability. Herein, we report a rational Mg²⁺/Al³⁺ co-doping strategy to engineer the properties of α-MnO₂. The optimized Mg₁Al₁@MnO₂ cathode exhibits a remarkable Zn²⁺ storage performance, delivering a high reversible capacity of 354 mAh g⁻¹ at 0.1 A g⁻¹ , exceptional rate capability, and outstanding cycling stability with 74.7% capacity retention after 1000 cycles at 2 A g⁻¹ . Comprehensive characterization reveals that the larger Mg²⁺ ions act as pillars to expand the (2 ×2) tunnels, while the similarly-sized Al³⁺ ions substitute for Mn⁴⁺ to reinforce the host framework. This synergistic modification induces a charge compensation effect, generating abundant oxygen vacancies and optimizing the Mn³⁺/Mn⁴⁺ ratio, which collectively enhance the intrinsic conductivity and ion diffusion kinetics. Furthermore, a highly reversible H⁺/Zn²⁺ co-(de)intercalation mechanism is confirmed. This work provides a generalizable design principle for developing durable cathode materials for advanced energy storage systems.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Zilin Meng,Ziwei Ju,Jiaxuan Fan,Yujiao Wang,Xingyi Wu,Runhua Lu,Wenfeng Zhou,Haixiang Gao
A low-cost and environmentally friendly polydopamine modified layered double hydroxides (PDA/LDH) was prepared, and a novel fluorescent “turn-off” sensor was established for rapid detection of thiram. The material was characterized using the transmission electron microscope (TEM), Fourier transform-infrared (FT-IR), X-ray diffraction (XRD), X-ray photo-electronic spectroscopy (XPS) and other methods. The electrostatic interaction, hydrogen bonding and S-π interaction between PDA/LDH and thiram were mostly attributed to the sensing of thiram. Through the internal filter effect (IFE), the fluorescence of the PDA/LDH could be effectively quenched by thiram. The limit of detection (LOD) was determined to be 25 μg L −1 under optimal conditions, while the concentration of thiram in the range of 50–50000 μg L −1 exhibited a satisfactory relationship with the change in fluorescence intensity. Furthermore, the prepared probes were successfully applied on apple and pear samples, in which the recovery rate could reach 92.06–104.90 %. The synthesis of PDA/LDH was quite simple, and the detection of thiram could be accomplished right away when the sensor and thiram were combined. All the above results demonstrated the high potential of the established method in practical applications.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Rehan Khan,Wei-Min Liu,Ihtisham Ul Haq,Hong-Gang Zhen,Heng Mao,Zhi-Ping Zhao
Pyridine is generally found in the effluents from the synthesis of paints, rubber chemicals, vitamins, and pesticides. This study focused on improving the pervaporation (PV) performance of polyether block-amide (PEBA-2533) membranes cast on polyvinylidene fluoride (PVDF) substrate, by incorporating the MIL-53 (Al) particles to prepare mixed matrix membranes (MMMs) for pyridine separation from the aqueous solution. MIL-53 (Al) has a larger aperture size (8.5 Å) than the molecular size of the pyridine (6.0 Å), which could allow pyridine molecules to efficiently pass through its channels. The coadjacent MIL-53 particles created relatively continuous permeation pathways for the penetrants in the MMMs, which substantially enhanced the separation performance. Impressively, the resultant MMMs displayed superior pyridine separation performance at complex conditions. At 65 °C and 0.5 wt% pyridine aqueous solution, the separation factor and pyridine flux of PEBA/PVDF membrane were 17.3 and 143.5 g m −2 h −1 , which were improved using MIL-53@PEBA/PVDF MMMs to 48.1 and 226.9 g m −2 h −1 , respectively. Owing to the enhanced pyridine affinity, hydrophobic property, and thermal robustness, the resultant MMMs overcame the inherent trade-off between selectivity and permeability, and also displayed the promising long-term stability. These findings may provide valuable insights for developing novel MMMs with superior separation performance.
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Materials Research Express
·
2022
·Vol. 9
·期 6
·065505
·
IF 2.025
Qinghong You,Xiulian Yin,Jun Wang,Chunhua Dai
A recyclable heterogeneous KF/Ca-Mg-Al-O catalyst was prepared by co-precipitation and calcination processes. The characteristics of the catalyst were investigated using FTIR, XRD, TG-DTG and SEM. Response surface methodology was utilized to obtain the best most extreme biodiesel production yield. The ideal biodiesel production conditions were: the amount of catalyst was 3 wt%; the reaction temperature was 65 °C; the alcohol oil molar ratio 9.8:1, the reaction time was 3.5 h. Under these amended conditions, the average biodiesel yield was 95.19%, which is well in close concurrence with the worth anticipated by the model. The repeatability of catalysts was studied. After using the catalyst seven times, the catalytic efficiency was only reduced by 2.7%. These results indicate that the catalyst has good catalytic efficiency and is recyclable.
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FUEL
·
2022
·
IF 8.035
Miao Zuo,Xinyu Wang,Wenlong Jia,Yanzhong Zhu,Xianhai Zeng,Lu Lin
As one of the essential building blocks for bio-chemicals and bio-fuels, the 5-Hydroxymethylfurfural (HMF) production is still challenging in a green and cheap way. This work developed a bio-derived aqueous-natural deep eutectic solvent (A-NADES) to synthesize HMF using α-Al 2 O 3 or Al(OH) 3 as robust catalysts, obtaining high yields of 67.1% and 63.6% HMF from glucose under mild reaction reactions, respectively. Different kinds of starches and starchy food waste also exhibited high conversion efficiency in the A-NADES system. The mechanistic study indicated that the in-situ formed Al (III) site of α-Al 2 O 3 during the reaction was critical for converting glucose-based carbohydrates. A-NADES could be effectively reused six times with a more convenient direct reuse method without significant activity loss. This study suggested a novel A-NADES reaction media in the synergistic reaction with robust aluminum-based catalysts for HMF synthesis, and proposed a novel process of food waste utilization in green solvents.
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CHEMOSPHERE
·
2022
·
IF 8.943
Chao Ren,Hongtao Wang,Junfeng Ji,Wei Li
Calcination is an effective way to improve the F − adsorption capacity of layered double hydroxide (LDH) materials, however, a molecular scale understanding of the enhanced defluoridation capability of calcined LDHs (CLDH) is lacking. This study investigated the mechanisms of F − adsorption by CLDH using 19 F solid-state NMR, X-ray photoelectron spectroscopy (XPS), and high-resolution TEM . Under calcination process, LDH underwent three periods: surface dehydration below 200 °C, structural dehydroxylation at 200–400 °C, and release of interlayer carbonate groups above 400 °C. Additionally, XPS and XRD characterization showed that CLDH could not recover to the original structural symmetry even after rehydration and reconstitution. The F − affinity was greatly enhanced for the calcined LDH, especially at high pH. At pH 10, the adsorption capacity could reach 22.0 mg F − /g for CLDH (500 °C calcined), about 6 times larger than that of LDH. The XRD analyses revealed that the F-adsorbed CLDH had a poorer crystalline degree as the calcination temperature increased, consistent with the TEM observation of abundant defects and Mg/Al oxides on the CLDH sheets. 19 F solid-state NMR spectra of the CLDH after F − adsorption showed that the formation of surface Al–F is the predominant F − adsorption mode at pH 7, whereas the Mg–F local coordination mode is the pronounced F − adsorption mechanism under alkaline conditions (pH 10). The present study provided a comprehensive understanding of CLDH in F − adsorption and suggested that calcination is a promising treatment for promoting the efficacy of polluted anion scavenging.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhiyu Wei,Xiaoqin Li,Shuang Han,Cihang Yan,Mingchao Sun,Yong Liu,Lu Fan
To expand the working pH range of NO 3 – -N reduction from aqueous solution, a two-step method including the Al/Cu bimetal and sulfamic acid reduction was developed. In this process, Al/Cu bimetallic materials were prepared by chemical deposition method and characterized by EDS, SEM, XRD and XPS. The NO 3 – -N reduction batch experiment showed that 100% of NO 3 – -N was reduced and converted to N 2 at pH of 7, Al/Cu dosage of 30 g/L and EDTA-2Na concentration of 6 mmol/L. When the pH value was adjusted to 3, 5 and 9, NO 3 – -N reduction efficiencies ca. 80–97% were also obtained in the first step, and 100% N 2 selectivity was further obtained with the second reduction step at pH of 3, 7 and 9. The kinetics study indicated that the Al/Cu reduction process was in accordance with the pseudo-second order kinetics model.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Huan Yao,Ruifeng Zhang,Yu Wen,Yue Liu,Gang Yu,Zhi-Hui Xie
Metal-organic framework [MOF, i.e., NH 2 -MIL-53(Al)] modified TiO 2 (NMT) composite photoanodes were successfully prepared by hydrothermal synthesis and were used for the photoelectrochemical cathodic protection (PECCP) of nickel-plated magnesium alloy (Mg/Ni). Results showed that the synthesis temperature significantly impacted the morphology and PECCP performance of the NMT photoanodes. The NMT@150 photoanode prepared at a reaction temperature of 150 °C exhibited the best PECCP performance and produced a current density of 1980 μA cm −2 under visible light irradiation, which was 19.8 times higher than that of a single TiO 2 photoanode. The composite photoanode could polarize the open circuit potential of the coupled Mg/Ni electrode to -876 mV and remain relatively stable within 35 h. XPS and EPR tests showed that a Z -scheme heterojunction was formed between the NH 2 -MIL-53(Al) and TiO 2 nanotubes, allowing the photogenerated electrons to accumulate mainly on the conduction band of NH 2 -MIL-53(Al). The heterojunction greatly promoted the separation and transfer of photogenerated electron-hole in the NMT composite photoanode, significantly enhancing the PECCP performance for Mg/Ni.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jian Zhang,Jia-Fang Xie,Jia-Cheng E. Yang,Ding Li,Lu-Bin Zhong,Yu-Ming Zheng
CoFe 2 O 4 /BHC-LDH3 catalyst was constructed by decoration of Co/Al layered double hydroxides (Co/Al-LDH) on bamboo hydrochar (BHC) loaded with magnetic CoFe 2 O 4 to activate peroxymonosulfate (PMS) for ciprofloxacin (CIP) degradation. Taking advantage of structural modulation and synergistic effects between the multi-components, CoFe 2 O 4 /BHC-LDH3 demonstrated high efficient PMS activation and ultra-fast CIP removal (91.50 % within 10 min), compared with BHC (6.26 %), CoFe 2 O 4 (26.32 %), and Co/Al-LDH (40.10 %). Both free radical (SO 4 – ) and non-radical ( 1 O 2 ) were crucial during the degradation process, and a substantial decrease in aquatic toxicity of the intermediates was observed. Additionally, the stability of CoFe 2 O 4 /BHC-LDH3 in actual water environment was tested using a fixed-bed reactor, illustrating the CoFe 2 O 4 /BHC-LDH3 has good stability and anti-interference ability in long-term operation. Possible degradation pathways of CIP in the CoFe 2 O 4 /BHC-LDH3 + PMS system were proposed based on liquid chromatography-mass spectrometer analysis and density functional theory calculation. This work provides new strategies for hydrochar-supported catalyst synthesis for organic pollutants decomposition.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yu-Hua Wu,Yu-Long Ma,Yong-Gang Sun,Wen-Xin Ji,Feng Lin,Yi-Peng Yang,Li-Juan Ma,Chun-Hong Zhu,Yi-Jie Xu,Qing Miao
The development of synthetic methods to obtain high value-added mesoporous Al-MCM-41 from a low-cost silicon-aluminum source with low toxicity is an active research topic in solid waste resource utilization. In particular, the controlled synthesis of MCM-41 with a two-level pore distribution is a challenging task. In this work, the synthesis of unimodal and bimodal mesoporous Al-MCM-41s was achieved using acids with different degrees of ionization from coal gasification fine residue (CGFR) as bulk solid waste generated by the coal gasification process. We determined that the degree of acid ionization affected the self-assembly of inorganic/organic species as well as condensation processes , resulting in some changes of the hexagonal mesoscopic structure. The unimodal mesoporous Al-MCM-41 with acetic acid HAc and bimodal mesoporous Al-MCM-41s with an inorganic acid environment (HCl, HNO 3 or H 2 SO 4 ) could be effectively prepared in a controllable manner by the silicon and aluminum source obtained at alkali dissolution time 6 h and crystallization conditions at pH 10.5 and 383 K in 72 h. Moreover, the synthesis of Al-MCM-41-HAc with different SiO 2 /Al 2 O 3 molar ratios (18–89) could also be realized by different alkali dissolution times. And alkali dissolution time (2–24 h) and the crystallization conditions (pH 4.5–11.5, temperatures 373–393 K, and time 48–96 h) also affected the formation of unimodal and bimodal mesoporous Al-MCM-41-HAc. In addition, the maximum adsorption amount onto bimodal mesoporous Al-MCM-41-H 2 SO 4 (476.19 mg g −1 at 308 K) was larger than that onto unimodal mesoporous Al-MCM-41-HAc (243.90 mg g −1 at 303 K). The mesoporous Al-MCM-41s showed good stability.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yi Zhai,Xubin Zhang,Fumin Wang,Guojun Lv,Tao Jiang,Yuzhou Wu,Mengyue Li,Mengyao Li,Qing Zhang,Yongkui Liu
Development of economic strategy to synthesize hollow zeolite with widely tunable Si/Al ratios providing variable acidity is of great significance in industry. Here, a one-step and low-cost strategy without mesoporogen was successfully developed to synthesize single-crystal hollow ZSM-5 containing mesopores/macropores, with variable Si/Al ratios of about 14–∞ and 114–∞ at critical TPA+/SiO2 ratios of 0.05–0.1 and 0.05, respectively. This is the first time the usage of a large amount of TPAOH was avoided while breaking the traditional limitation of Si/Al ratio (25–50). The component of synthesis system and crystallization temperature acting as the vital roles in hollow structure has been confirmed by a series of characterization. Moreover, according to the investigation of the evolution process, a novel racing crystallization mechanism based on the competition relationship between surface crystallization and the internal dissolution rate was proposed for the first time. The racing crystallization mechanism and internal nonprotective aluminum become the crucial factors for synthesis. The prepared hollow ZSM-5 zeolites exhibit superior catalytic performance in the different acidity-catalyzed condensation involving large molecules between benzaldehyde and n-butyl alcohol as well as 2-hydroxyacetophenone, which is mainly attributed to the property acidity, more accessible active Al sites on the surface, and shorter diffusion path. By calculating, the effectiveness factor (η) of hollow zeolite is close to 1, further confirming its better mass transfer ability. The strategy has also been successfully extended to the synthesis of high-amount Fe-doped, Ga-doped, and B-doped hollow silicate-1.
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