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CHEMISTRY OF MATERIALS · 2025 · IF 7

Synthesis of ZSM-5 Zeolite Nanosheets Using Fluorine-Free Additives

Jiaxing Zhang,Ajuan Zhou,Fang Hao,Kexin Yang,Yiren Yu,Yucai Qin,Xiongfu Zhang,Limin Ren,Anfeng Zhang,Guanghui Zhang,Chunshan Song,Xinwen Guo

The green synthesis of b-axis-oriented ZSM-5 nanosheets (NSs) is essential for facilitating their industrial production. Here, a set of cost-effective and eco-friendly additives is introduced for the tailored synthesis of thin ZSM-5 NSs with a b-axis thickness of 40 nm with the assistance of small seeds. Through a comprehensive exploration of synthesis methods and electron microscopy analysis, this work elucidates the pivotal roles of seeds and additives in controlling the crystal size and steering anisotropic growth kinetics during the crystallization process. The shortened straight channels of the thin ZSM-5 NSs along the b-axis significantly enhance the rapid transport of molecules within the micropores, thus manifesting a distinct catalytic advantage in the alkylation of benzene with methanol and methanol-to-propylene (MTP) conversion. Notably, the utilization of fluorine-free additives in the synthesis of thin ZSM-5 NSs marks an important step forward in zeolite materials, bridging the gap between laboratory experimentation and industrial scale-up.

研究领域: 材料科学 · 化学工程 · 环境科学
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AICHE JOURNAL · 2024 · IF 3.5

Channel–molecule attraction mediated molecule transport in confined nanochannels of COF membranes for nanofiltration

Ruilong Li,Yongjian Yang,Jingjing Chen,Chongchong Chen,Wenpeng Li,Xiaoli Wu,Jingtao Wang

Porous membranes, a type of material widely used in nanofiltration, are confronted with the limitation that the influence of channel–molecule interactions on transport behaviors has yet been investigated in detail. Herein, covalent organic framework membranes with adjustable pore sizes (⁓ 2.5 nm and ⁓ 1.2 nm) and chemical groups (−F, −OH, and −CO−) were prepared by interfacial polymerization. We demonstrate that strong channel–molecule attraction induces the formation of stable solvent layers along nanochannel walls, which protect central molecules from the attraction of chemical groups. Significantly, stable solvent layers permit fast transport of ethanol (245.6 L m −2 h −1 bar −1 ) with reactive black (RB) rejection of 96%. Likely, for membranes with weak channel–molecule attraction, no solvent layers are formed and molecules also transport smoothly. Interestingly, membranes that exhibit moderate channel–molecule attraction exert metastable solvent layers, thus displaying high transport resistance. This hindrance effect on molecule transport becomes more pronounced in smaller nanochannels.

研究领域: 材料科学 · 化学工程 · 分离技术
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JOURNAL OF MEMBRANE SCIENCE · 2018 · IF 6.578

Highly water-selective membranes based on hollow covalent organic frameworks with fast transport pathways

Hao Yang,Xiaopo Cheng,Xuanxuan Cheng,Fusheng Pan,Hong Wu,Guanhua Liu,Yimeng Song,Xingzhong Cao,Zhongyi Jiang

Covalent organic frameworks (COFs) are attractive candidates for membrane separation owing to their well-ordered channels and facilely tailored functionalities. However, the development of COF-based membranes remains in its infancy. To establish novel hierarchical structures in COFs, in this study, a facile template-directed approach is exploited for constructing hollow COF nanospheres . An imine-linked COF TpBD, derived from 1,3,5-triformylphloroglucinol (Tp) and benzidine (BD), was selected as the building block due to its rich hydrophilic groups and high stability. The synthesized hollow TpBD (H-TpBD) nanospheres were introduced into sodium alginate (SA) matrices to fabricate water-selective hybrid membranes. The H-TpBD nanospheres confer the membranes rapid diffusion pathways and abundant interacting sites for water molecules, thus fast water-selective permeation through the membranes was achieved. The hybrid membranes exhibit the optimal performance with permeation flux of 2170 g m −2 h −1 and separation factor of 2099 when used for dehydrating 90 wt% ethanol aqueous solution at 76 °C. The effects of hollow structures of H-TpBD on membrane performance were investigated and the molecular transport mechanisms through the membranes were elucidated. Besides, the favorable compatibility between SA and H-TpBD endows the hybrid membranes with long-term stability.

研究领域: 材料科学 · 膜分离技术 · 纳米技术
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Investigating molecule transport behaviors in two-dimensional nanochannels with adjusted interlayer spacing

Xiaoli Wu,Xingya Huang,Yongzheng Wang,Jingjing Chen,Ye Wan,Jianhua Liu,Wenpeng Li,Jingtao Wang

Two-dimensional (2D) lamellar membranes are favored over other membrane materials. However, the molecule transport behaviors in confined 2D nanochannels remain ambiguous, specifically the role of interlayer spacing which determines the confined effect. Herein, vertically-aligned nanochannel membranes with adjusted interlayer spacing (0.6 nm, 2.1 nm, and 3.9 nm) were fabricated by vermiculite lamellar membranes. These robust and long-range 2D nanochannels maintain stable molecule configuration state throughout the transport process, providing ideal platforms for investigating molecule transport behaviors. We demonstrate that molecules with weak molecule-molecule interactions (mainly nonpolar molecules) continuously collide with each other in the nanochannels. The extremely confined nanochannels (0.6 nm) restrict the random molecule collision and permit the oriented flow along transport direction, thus offering the highest transport efficiency. In contrast, molecules in wider nanochannels (3.9 nm) collide randomly, impairing the velocity of molecules or even compelling some of them to move to the adverse flow direction. This consumes cohesive energy and leads to lower permeance. The transport rate of benzene reaches over 130 L m -2 h -1 bar -1 nm -1 for 0.6 nm-nanochannel membrane, which is 8 times higher than that of 3.9 nm-nanochannel membrane. Compared to nonpolar molecules, the strong molecule-molecule and molecule-channel interactions for polar molecules would weaken this collision effect, thus the difference of transport rate is relatively small with nanochannel size.

研究领域: 材料科学 · 化学工程
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CARBOHYDRATE POLYMERS · 2024 · IF 10.7

Base on photothermal interfacial molecular transfer for efficient biodiesel catalysis via enzyme@cyclodextrin metal-organic frameworks loaded MXene

Qi Ao,Lin Jiang,Ying Song,Xinglai Tong,Tuohao Jiang,Xiaoxiao Lv,Jun Tang

Efficient, green and stable catalysis has always been the core concept of enzyme catalysis in industrial processes for manufacturing. Therefore, we construct a new strategy with photothermal interfacial molecular transfer for green and efficient biodiesel catalysis. We encapsulate Candida albicans lipase B (CalB) in a γ-cyclodextrin metal-organic framework (γ-CD-MOF) loading with Ti 3 C 2 T X by in situ growth and electrostatic assembly. The γ-CD-MOF not only protects the fragile enzyme, but also enhances the catalytic performance through the synergistic effects of porous adsorption (MOF pore structure) and interfacial enrichment (cyclodextrins host-guest assembly structure) for accelerating substrate transfer (642.6 %). The CalB@γ-CD-MOF/MXene-i activity can be regulated up to 274.6 % by exposure to near-infrared (NIR). Importantly, CalB@γ-CD-MOF/MXene-i achieves 93.3 % biodiesel conversion under NIR and maintained 86.9 % activity after 6 cycles. Meanwhile, the MXene after the CalB@γ-CD-MOF/MXene catalytic cycle can be almost completely recovered. We verify the mechanism of high catalytic activity of γ-CD-MOF and rationalize the mechanism of CD molecular channel by DFT. Therefore, this highly selective enzyme catalytic platform offers new possibilities for green and efficient preparation of bioenergy .

研究领域: 生物化学 · 能源科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Construction of water molecular transport channel by ortho-hydroxyazo-linked framework material for enhanced nanofiltration performance and anti-bacterial properties

Xueling Wang,Weiwei Bai,Man Wang,Jing Wang,Chuyang Y. Tang,Yatao Zhang

Membrane technology has been being widely employed in wastewater treatment in recent years. Developing high-permeability and high-selectivity separation membrane is a key to expand their applications. In practice, biofouling often has a negative effect on membrane performance and membrane life span. Therefore, it is urgently needed to develop novel high-performance separation membrane with fast water molecular transport channel and excellent anti-bacterial properties. Owing to the abundant water molecular transport provided by ortho -hydroxyazo-linked porous organic polymer ( o -POP) with polar functional groups and high hydrophilicity, and the excellent anti-bacteria and abundant oxygen-containing functional groups of graphene oxide (GO) material, high stable o -POP/GO composite membrane with abundant transport channel was constructed on a nylon substrate via simple in situ method in this work. The synergistic effect of o -POP and GO effectively improved the ability of water transport and anti-bacteria performance of the composite membrane. The o -POP/GO composite membrane not only possessed high water permeability of 151.3 L m –2 h −1 bar −1 and excellent dye rejection (Evans blue (EB): 96.3 %, Methyl blue (MB): 98.0 %, Congo red (CR): 99.0 %, Eriochrome black T (EBT): 97.3 %, Methyl orange (MO): 71.5 %), but also exhibited positive anti-bacterial effect for Escherichia coli.

研究领域: 材料科学 · 环境工程 · 生物学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-14 · IF 14.7

Coacervate-pore complexes for selective molecular transport and dynamic reconfiguration

Wang Hao,Zhuang Hui,Tang Wenjing,Zhu Jun,Zhu Wei,Jiang Lingxiang

Despite surging interests on liquid-state coacervates and condensates, confinement within solid-state pores for selective permeation remains an unexplored area. Drawing inspiration from nuclear pore complexes (NPCs), we design and construct coacervate-pore complexes (CPCs) with regulatable permeability. We demonstrate universal CPC formation across 19 coacervate systems and 5 pore types, where capillarity drives the spontaneous imbibition of coacervate droplets into dispersed or interconnected pores. CPCs regulate through-pore transport by forming a fluidic network that modulates guest molecule permeability based on guest-coacervate affinity, mimicking NPC selectivity. While solid constructs of NPC mimicries are limited by spatial fixation of polymer chains, CPCs of a liquid nature feature dynamic healing and rapid phase transitioning for permeability recovery and regulation, respectively. Looking forward, we expect the current work to establish a basis for developing liquid-based NPC analogs using a large pool of synthetic coacervates and biomolecular condensates.

研究领域: 材料科学 · 生物物理学 · 化学工程 · 分子生物学
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