MOLECULES
·
2026
·Vol. 31
·期 15
·2726
·
IF 5.1
Huidong Tang,Pengcheng Jiang,Xin Xiong,Xinyi Wen,Jingdan Yan,Simeng Wu,Zhi Wu,Yanqiao Xu,Qing Hu
Blue-excitable lead-free metal halide microcrystals (MCs) with high efficiency and narrow emission are highly desired for next-generation wide-gamut displays. Herein, an ultrafast self-assembly strategy is developed to prepare hybrid manganese bromide MCs with tunable alkyl-chain lengths. With increasing alkyl-chain length, the emission intensity of the obtained MCs first improves significantly and then deteriorates, accompanied by a gradual narrowing of the full width at half maximum (FWHM) from 46.37 to 41.97 nm. The optimized [(C2H5)4N]2MnBr4MCs exhibit strong narrow-band green emission at 518 nm with a FWHM of 43.30 nm and a high photoluminescence quantum yield of 98.70% under 455 nm excitation. This superior emission performance is ascribed to cooperative weak interactions, an appropriate Mn-Mn distance, and highly localized electronic transitions within isolated [MnBr4]2−tetrahedra. Moreover, the [(C2H5)4N]2MnBr4MCs show moderate thermal stability, retaining 52.03% of their initial emission intensity at 413 K. By integrating [(C2H5)4N]2MnBr4with K2SiF6: Mn4+red phosphors on a blue chip, a white light-emitting diode with a high luminous efficacy of 134.60 lm/W and a wide gamut of 112.6% NTSC is achieved, demonstrating the great promise of ultrafast-assembled hybrid manganese bromides for efficient and wide gamut display backlighting.
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高影响因子
ACS Catalysis
·
2026
·
IF 13.6
Mengqi Ding,Xinhong Zhao,Yanru Li,Xuefeng Long,Hongwei Li,Dong Ji,Guixian Li
Iron-containing zeolites have shown great potential in catalyzing phenol hydroxylation with H2O2 to produce dihydroxybenzenes (catechol and hydroquinone). However, their industrial application has been hindered by low selectivity and the complexity of active-site identification. This study addresses these challenges by synthesizing a series of Fe-ZSM-5 catalysts with iron contents up to 4 wt % via an ionic liquid-assisted interzeolite transformation route. Through systematic regulation of transformation temperature and calcination atmosphere, combined with an acid treatment step, a catalytically inert benchmark sample (T180-Air) was strategically prepared and compared with three active variants (T200-Air, T180-N2, T200-N2) to achieve the isolation and identification of active sites. Employing a “differential comparison strategy”, combined with DR UV–vis, Raman, Mössbauer, XANES/EXAFS, EPR, H2-TPR, in situ FT-IR characterizations, and DFT calculations, we systematically excluded the possibility of binuclear iron species, small FexOy clusters, and distorted tetrahedral iron as primary active sites. The evidence consistently points to extra-framework octahedrally coordinated mononuclear iron as the key active species, which effectively activates both phenol and H2O2 to generate reactive intermediates. Moreover, the high-selectivity formation of dihydroxybenzenes is driven by a synergistic interaction between these mononuclear octahedral iron sites and neighboring strong acid centers. The optimal catalyst (T200-Air) achieved a phenol conversion of 46.7% and a dihydroxybenzene selectivity of 95.6% under dark conditions, with its dihydroxybenzene selectivity surpassing that of state-of-the-art Fe-based catalysts at comparable phenol conversion levels. This work elucidates the critical importance of the synergistic design between the active iron species and the local acidic microenvironment, providing clear experimental evidence and structure-performance guidelines for the rational design of high-performance iron-zeolite catalysts for selective phenol hydroxylation reactions.
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ChemistrySelect
·
2026
·Vol. 11
·期 13
·e05885
·
IF 2.3
Yongzhi Pu,Wenbo He,Yanting Zhang,Ning Li,Zelong Li,Jiayin Wang,Yunlong Ding,Xiaofeng Li
A novel organosiloxane (KHPA) was synthesized using 3-glycidyloxypropyltrimethoxysilane (GPTMS) and propylamine as raw materials. The effects of KHPA addition on the physicochemical properties of hierarchical ZSM-5 zeolite were investigated. The synthesized zeolite samples were systematically characterized by x-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), low-temperature N 2 adsorption-desorption, x-ray fluorescence (XRF), thermogravimetric (TG) analysis, and ammonia temperature-programmed desorption (NH 3 -TPD). The results indicated that the addition of KHPA into the synthesis system hindered the growth of zeolite crystals, leading to the formation of abundant inter-crystalline mesopores. When the KHPA addition amount was 6 g, the synthesized sample exhibited the highest external surface area (303.5 m 2 /g) and mesopore volume (0.38 cm 3 /g), and the SEM and TEM images revealed intergranular mesopores formed by the stacking of nanoparticles. Furthermore, the Z-KHPA-6 sample exhibited optimal catalytic performance in the trimethylbenzene isomerization reaction, demonstrating a 1,2,4-trimethylbenzene mass conversion of 36.26%, 1,3,5-trimethylbenzene mass yield of 22.61%, and 1,3,5-trimethylbenzene selectivity of 62.36%. Graphical Using GPTMS and propylamine as raw materials, a novel organosiloxane KHPA was synthesized as a mesoporous template. A hierarchically porous ZSM-5 zeolite was successfully prepared via the hydrothermal method. The introduction of KHPA into the synthesis system impeded the crystal growth of the zeolite, resulting in abundant intercrystalline mesopores. This unique pore structure effectively enhanced the isomerization of 1,2,4-trimethylbenzene, significantly improving catalytic efficiency and reaction selectivity.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Shiwei Luo,Die Gao,Hui Ma,Zhenyu Guo,Huimin Cao,Jingliang Xu,Shen Zhang
Most high-value-added sugars and rare sugars are isomers and epimers of natural carbohydrates. Chemical isomerization or epimerization reactions are typically unselective, leading to complex distributions of products, and are not easy to separate. In this study, an alkaline hydrothermal pretreatment and recrystallization process were used to modulate the zeolite crystal structure and Mo active sites on zeolite (Mo/alk@ZSM) for high-value-added sugar production. New Mo species on zeolite were generated after the recrystallization process. The new species precisely regulate glucose isomerization and epimerization routes by changing interactions between active sites and different carbons on glucose. DFT results indicate that Mo–O–Al sites facilitate epimerization through carbon migration (10.48 kJ/mol), whereas Mo–S sites promote isomerization by electronically polarizing sulfur, which lowers the barrier for hydrogen transfer (23.57 kJ/mol). The catalyst with 85 °C alkaline hydrothermal pretreatments (Mo/alk@ZSM-85) predominantly drives glucose isomerization toward fructose, affording a fructose yield of 32.28 with 74.80% selectivity. Mo/alk@ZSM-65 favors the epimerization pathway, delivering a mannose yield of 30.12% with a selectivity of 95.53%. The etching-recrystallization strategy offers a robust platform for selective conversion of glucose to mannose or fructose, providing a promising approach for high-efficiency biomass valorization.
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高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Linlong Zhang,Jingqing Tian,Ruiqiang Liu,Bing Ma,Chen Zhao
Developing synthetic strategies for high-quality metal-zeolite composites is critical for achieving advanced catalytic performances. One major challenge lies in addressing the rate mismatch between rapid metal deposition and slow zeolite crystallization, which leads to the segregation of large metal particles. Herein, we propose a universal strategy via quaternary ammonium alkali–metallic acid (QAMA) pairs for fabricating highly dispersed metal@zeolite materials with nearly 100% metal (Ru, Ir, Pd, Pt, and Zn) utilization. Using tetrapropylammonium hydroxide (TPAOH) as both a structural-directing agent and basic medium, the interaction of TPA+ with acidic metal precursors forms the “QAMA” pairs, which inhibit the precipitation of metal precursors and guide their dispersion into the 10-membered ring channels of MFI topology. Furthermore, the appropriate Si–OH groups on the silicalite-1 (S-1) seeds surface anchor the “QAMA” pairs and thus assist in the subnanometer PtZn particle dispersion. A series of PtZn@S-1 catalysts exhibited outstanding catalytic activity (14.1 molC2H4·gPt–1·h–1 at 24 h–1 weight hourly space velocity (WHSV)) and stability (Kd = 0.0004 h–1) in ethane dehydrogenation (EDH), particularly at relatively low temperature (550 °C) with pure ethane feed.
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Catalysts
·
2026
·Vol. 16
·期 3
·
IF 4.5
Yao He,Jie Zhang,Renhua Huang,Nanxin Li,Yunwu Zheng
CO2-assisted catalytic pyrolysis presents a viable and promising approach to addressing plastic waste pollution and mitigating climate change. However, the effects of the metal–catalyst combination mode and the spatial distance between metal–acid sites on catalytic performance remain unclear. In this study, the reaction behaviors of the configurations, Fe3O4and ZSM-5 in tandem catalysis (Fe3O4&HZ), their physical mixture (Fe3O4-HZ), and Fe-loaded ZSM-5 (Fe/HZ), were compared in polypropylene pyrolysis under a CO2atmosphere. The aromatic contents followed this order: Fe/HZ > Fe3O4-HZ > Fe3O4&HZ > ZSM-5 > Fe3O4. Specifically, Fe/HZ with the highest degree of metal–zeolite proximity achieved an aromatic content of 66.1%, significantly higher than the 34.2% obtained with Fe3O4&HZ, demonstrating that closer metal–acid proximity promoted aromatic formation. Moreover, Fe/HZ significantly reduced coke deposition. Based on characterization results from XRD, SEM, TEM, XPS, and NH3-TPD, the enhanced spatial proximity between metal and acid sites strengthened the functional synergy between iron-based redox sites and zeolitic Brønsted acid sites. This synergy facilitated the reverse water–gas shift reaction of CO2, which consumed hydrogen generated during aromatization and shifted the reaction equilibrium toward enhanced aromatic production. These findings would offer theoretical and strategic insights into the optimization of CO2-assisted catalytic pyrolysis systems for the sustainable upcycling of plastic waste.
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高影响因子
Catalysts
·
2023
·Vol. 13
·期 3
·464
·
IF 3.9
Xia Zhang,Zhengkai Cao
Sub-nanosized PtAu particles within three-dimensional carbon materials were obtained via a mercaptosilane-assisted preparation method. This strategy can effectively control the size of PtAu particles while avoiding the use of an additional carbon precursor. The as-synthesized three-dimensional carbon (3D carbon) material possesses excellent properties compared to other carbon materials. PtAu particles on three-dimensional carbon (PtAu/3D carbon) exhibited superior activities for methanol oxidation and hydrogen evolution reactions compared to Pt/3D carbon and a commercial Pt/Carbon (Pt/C) catalyst. Specifically, the methanol peak current density on PtAu/3D carbon was almost 2.3 times higher than that of Pt/3D carbon and 1.9 times higher than that of commercial Pt/C. The Tafel slopes of PtAu/3D carbon, Pt/3D carbon, and the commercial Pt/C were approximately 112, 124, and 106 mV dec−1, respectively, demonstrating that electrochemical desorption is the rate-limiting step in the hydrogen evolution reaction of the as-synthesized catalysts.Keywords:noble metals;alloy nanocrystals;methanol oxidation;hydrogen evolution;electrocatalytic
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Tingjun Fu,Lihan Jia,Guoqiang Hou,Zhong Li
Dealuminization over aluminium-containing ZSM-5 could create silanol nests and improve catalytic activity for alkylation of toluene with methanol. However, obviously damaged microporous structure seriously accelerated catalyst deactivation. Here, we demonstrate highly stable alkylation on ZSM-5 by deboronation treatment over boron-containing ZSM-5. 11 B MAS NMR, 1 H MAS NMR and OH-IR suggested that silanol nests with hydrogen bonds were created at the expenses of the removal of skeleton-B atoms. The formed silanol nests promote the adsorption of toluene, inhibit the methanol self-reaction and corresponding the deep alkylation process. Therefore, alkylation efficiency and toluene conversion could reach 70.8% and 33.5%, respectively. Importantly, the microporous structure of deboronized ZSM-5 was well maintained during deboronation, which determined a greatly improved catalytic stability compared with that of traditional dealuminized ZSM-5. Moreover, the deboronized ZSM-5 still presented relatively good catalytic stability under a higher methanol feedstock although the coke deposition was accelerated.
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yifan Wu,Guangbing Liang,Xinna Zhao,Hui Wang,Zhenping Qu
It is feasible and profitable to figure out multidiscipline environmental issues synergistically. Coal fly ash based adsorbent materials are widely used in the emission control of volatile organic compounds. A solvent-free method which was more environmental-friendly for ZSM-5 zeolites synthesis from coal fly ash was proposed to eliminate toluene. The results indicated that ZSM-5 zeolites were successfully synthesized from the precursor gel of coal fly ash with 30–60 wt% moisture contents. The SiO 2 /Al 2 O 3 mole ratio of gel was up to 99 after the pretreatment of alkali roasting and acid precipitation. During the synthesis process, the appropriate Na 2 CO 3 -to-SiO 2 ratio was 0.3, and the mesoporous formation would be facilitated along with the moisture content of gel. On the tendency of adsorption testing, the microporous structure was prone to the toluene adsorption, and the desorption was dependent on the mesoporous structure. The maximum adsorption capacity of 75.1 mg·g −1 was observed on S-40 sample, and the minimum desorption activation energy of 39.97 kJ·mol −1 was found on S-60 sample. The humid condition can reduce the toluene adsorption performance, and the maximum adsorption capacity was down to 63.7 mg·g −1 . Additionally, the synthetic ZSM-5 zeolites still have some superiority in economics and ecology when compared with commercial zeolites. The novel synthesis method, preparing controllable ZSM-5 zeolites from coal fly ash with the advantages of low cost and environmental friendliness, exhibited the tremendous application potential in environmental field.
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高影响因子
Nature Nanotechnology
·
2023
·Vol. 18
·期 7
·772-779
·
IF 38.3
Du Junjie,Zeng Lin,Yan Tao,Wang Chuanhao,Wang Menglin,Luo Lei,Wu Wenlong,Peng Zijun,Li Hongliang,Zeng Jie
Plastic pollution is a planetary threat that has been exacerbated by the COVID-19 pandemic due to the surge in medical waste, personal protective equipment and takeaway packaging. A socially sustainable and economically viable method for plastic recycling should not use consumable materials such as co-reactants or solvents. Here we report that Ru nanoparticles on zeolitic HZSM-5 catalyse the solvent- and hydrogen-free upcycling of high-density polyethylene into a separable distribution of linear (C 1 to C 6 ) and cyclic (C 7 to C 15 ) hydrocarbons. The valuable monocyclic hydrocarbons accounted for 60.3 mol% of the total yield. Based on mechanistic studies, the dehydrogenation of polymer chains to form C=C bonds occurs on both Ru sites and acid sites in HZSM-5, whereas carbenium ions are generated on the acid sites via the protonation of the C=C bonds. Accordingly, optimizing the Ru and acid sites promoted the cyclization process, which requires the simultaneous existence of a C=C bond and a carbenium ion on a molecular chain at an appropriate distance, providing high activity and cyclic hydrocarbon selectivity.
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PubMed
高影响因子
Catalysts
·
2023
·Vol. 13
·期 7
·1080
·
IF 3.9
Shiyuan Lin,Ruosong He,Wenhang Wang,Yang Wang,Yongqiang Gu,Qiang Liu,Mingbo Wu
The abundant C1 source CO2can be utilized to produce value-added chemicals through hydrogenation technology. A bifunctional catalyst consisting of reducible metal oxide Cr2O3and acidic zeolite ZSM-5 was designed for the direct conversion of CO2+ H2into valuable aromatics, especially para-xylene (PX), via the methanol-mediated pathway. The twin structure of ZSM-5 (ZSM-5T), with sinusoidal channels that are predominantly exposed to the external surface, enhances the possibility of the transformation of methanol into PX due to the favorable diffusion dynamic of PX in the sinusoidal channels. Via the bifunctional catalyst Cr2O3&ZSM-5T, a PX selectivity of 28.7% and PX space-time yield (STY) of 2.5 gCH2h−1kgcat−1are achieved at a CO2conversion rate of 16.5%. Furthermore, we rationally modify the ZSM-5Tzeolite via Cu species doping and amorphous SiO2shell coating (Cu-ZSM-5T@SiO2). After combining with the Cr2O3catalytic component, the CO2conversion (18.4%) and PX selectivity (33.8%) are increased to some extent, which systematically increases the STY of PX to 3.0 gCH2h−1kgcat−1. The physicochemical property of the acidic zeolite and the corresponding structure-function relationship in enhancing the PX productivity are discovered. Our work provides a novel catalyst design idea to boost PX synthesis performance from CO2hydrogenation.Keywords:CO2hydrogenation;bifunctional catalysts;para-xylene;H-ZSM-5 zeolites
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CHEMOSPHERE
·
2023
·
IF 8.8
Jida Gao,Qianji Lin,Tingzhi Yang,Yong chao Bao,Juan Liu
Coal gangue is a kind of solid waste produced in the process of coal mining and washing. Its silicon aluminum silicon aluminum oxide content is high, respectively, which are suitable for resource utilization as raw materials for Si–Al molecular sieving. In this paper, a novel, simple, low-cost, and environmentally friendly process was carried out to prepare ZSM-5 zeolite by solvent free method after calcination, acid leaching, and alkali melting. The obtained samples were characterized by Energy Dispersive Spectrometer (EDS), Inductively Coupled Plasma (ICP), Thermo-gravimetry Analysis (TG), X-ray Photoelectron Spectroscopy (XPS), Fourier Transform Infrared Spectrometer (FTIR) X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM) and N 2 adsorption isotherm. The characteristics of the raw materials and the adsorption mechanism of the prepared samples were characterized. Through a series of pretreatment such as calcined acid leaching and alkali melting of the raw materials, the silicon-aluminum ratio of the sample reaches 1.749, and the maximum specific surface area of the sample can reach 252.59 m 2 /g. The obtained samples were used to adsorb heavy metal ions and methylene blue solution, and the removal rate of lead ions and methylene blue solution was more than 95%. The theoretical maximum adsorption capacity of Pb ion, methylene blue solution and copper ion can reach 232.56 mg/g and 118.34 mg/g. The adsorption process is mainly chemical adsorption. The product could be suitable for removing both heavy metal ions and cationic dyes from the wastewater and had broad application prospects.
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高影响因子
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