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ACS Applied Materials & Interfaces · 2018 · IF 8.097

Nacre-Templated Synthesis of Highly Dispersible Carbon Nanomeshes for Layered Membranes with High-Flux Filtration and Sensing Properties

Meng Kong,Mingjie Li,Ruoxu Shang,Jingyu Wu,Peisong Yan,Dongmei Xu,Chaoxu Li

Marine shells not only represent a rapidly accumulating type of fishery wastes but also offer a unique sort of hybrid nanomaterials produced greenly and massively in nature. The elaborate “brick and mortar” structures of nacre enabled the synthesis of carbon nanomeshes with <1 nm thickness, hierarchical porosity, and high specific surface area through pyrolysis, in which two-dimensional (2D) organic layers served as the carbonaceous precursor and aragonite platelets as the hard template. Mineral bridges within 2D organic layers templated the formation of mesh pores of 20–70 nm. In contrast to other hydrophobic carbon nanomaterials, these carbon nanomeshes showed super dispersibility in diverse solvents and thus processability for membranes through filtration, patterning, spray-coating, and ink-writing. The carbon membranes with layered structures were capable of serving not only for high-flux filtration and continuous flow absorption but also for electrochemical and strain sensing with high sensitivity. Thus, utilization of marine shells, on one hand, relieves the environmental concern of shellfish waste, on the other hand, offers a facile, green, low-cost, and massive approach to synthesize unique carbon nanomeshes alternative to graphene nanomeshes and applicable in environmental adsorption, filtration, wearable sensors, and flexible microelectronics.

研究领域: 材料科学 · 环境科学 · 纳米技术
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DESALINATION · 2024 · IF 8.3

Building ordered graphene membranes by intermediate layer assisted stacking method for promoted desalination

Leyao Liu,Yunchen Wu,Luzheng Peng,Yan Lv,Qianqian Lan,Tianxi Liu

Laminar separation membranes stacked by graphene and its derivatives hold the merit of controlled mass transfer behaviors. However, precise ion separation is challenged by the disordered assembly of nanosheets on macroporous substrates with complicated surface properties. Herein, we prepare ultrathin ordered graphene membranes by an intermediate layer assisted stacking method. Nanoporous covalent organic framework (COF) nanosheets are first vacuum-filtered on macroporous substrates, followed by deposition and thermal reduction of graphene oxide nanosheets to deliver ultrathin reduced graphene oxide (rGO) layers. The COF-decorated substrates provide a hydrophilic surface with reduced pores and roughness, facilitating the formation of ultrathin rGO layers with ordered stacking patterns and reduced microporous defects. Consequently, the obtained rGO/COF composite membranes can reject ∼90% of Na 2 SO 4 , ∼50% of NaCl, and >98% of various organic dyes, which are higher than pure rGO membranes. Meanwhile, the rGO/COF composite membranes can maintain good stability in solutions with different pH values and salt concentrations, and can be long-term operated for at least 10 days. This work is expected to deepen the understanding of the structure of laminar membranes and provides new perspectives to design ordered laminar membranes.

研究领域: 材料科学 · 环境工程
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CHEMICAL ENGINEERING SCIENCE · 2021 · IF 4.311

Boosting ion exclusion of two dimensional TMD lamellar membranes via in-plane engineering strategy

Qiang Huang,Xinxin Li,Pengpeng Zhang,Shichao Zhang,Yahua Liu,Peng Cui,Jin Ran

Transition metal dichalcogenide (TMD) derived stratiform membranes exhibit sub-nanometer scale interlayer distances and exceptional anti-swelling property in water environments but they are frustrated in ion rejections. Herein, the in-plane regulating concept to improve ion exclusion of TMD laminates was proposed. We demonstrate this concept using flexible and hydrophilic polyvinyl alcohol (PVA) polymers as the intercalators to implant TMDs. The resulting TMD/PVA membranes show obviously decreasing ion permeation. Taking the TaS 2 /PVA membrane as an example, its monovalent, divalent and trivalent ion transport rates reduce by 87, 131 and 168 times respectively compared with the pristine TaS 2 membrane. Additionally, the ion permeation behaviors of TMD/PVA membranes reveal long-term and cyclic stability. For the practical desalination process under the forward osmosis mode, the TaS 2 /PVA membrane shows an extraordinarily high water flux of 3.9 L m −2 h −1 together with a promising NaCl rejection of 98.7%, which is superior to the existing two dimensional membranes.

CAS / MDL: 111-30-8 7440-25-7
研究领域: 材料科学 · 环境工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

2D lamellar membrane with MXene hetero-intercalated small sized graphene oxide for harsh environmental wastewater treatment

Xinyu Ma,Aiqi Wang,Jinlei Miao,Tingting Fan

Efficient wastewater treatment under harsh conditions remains a great challenge, while traditional filtration membranes are inefficient to meet the demands due to its poor chemical resistance as well as the “trade-off” effect between high permeability and selectivity. Herein, a chemical-resistant 2D lamellar membrane simultaneously with high flux and rejection for harsh environmental wastewater treatment was proposed, via assembled small sized graphene oxide nanosheets (NGO) layer-by-layer on polyphenylene sulfide (PPS) while hetero-intercalated with MXene. As the performance of 2D laminated membranes is determined by the length/tortuosity of transport channels and interlayer spacing between the flakes, NGO nanosheets were sonicated into small sizes (<500 nm) and intercalated with MXene to engineer shorter/less tortuous transport pathways while tuning the interlayer spacing for fast and selective separation. The membranes exhibit remarkably high-water permeability (up to 136.68 L·m −2 ·h −1 ·bar −1 ) while simultaneously with excellent retention (>99.99 %) for various dyes (molecular weight 288.77–1017.65) at the NGO/MXene ratio of 1/7, which is much higher than most reported membranes. Meanwhile, the Ti-O-C covalent bonding between NGO and MXene nanosheets also enables stable ultrafast water transmission and anti-swelling stability. The PPS-NGO/MXene membranes could still exhibit excellent separation performance even under various harsh environments (strong acids, bases, high pressures, high temperatures, bacteria, organic solvents), which holds great promise for sustainable wastewater treatment under harsh conditions.

研究领域: 材料科学 · 环境工程
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Scientific Reports · 2025 ·Vol. 15 ·期 1 ·1-14 · IF 3.9

MXene-supported Ni–Co bimetallic MOF 2D lamellar membrane for enhanced electrochemical oxygen reactions and Li–O2 battery

Liu Liming,Lian Hongxia,Deng Heming,Zhang Weixin

Challenges associated with the cathode material of Lithium–oxygen (Li–O 2 ) battery, particularly the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction, as well as the accumulation of discharge product Li 2 O 2 , have hindered its further advancement. Here, an in-situ synthesis strategy was adopted to load a bimetallic Ni–Co metal–organic framework (Ni/Co-MOF) onto MXene (Ti 3 C 2 ) layers. Subsequently, a free-standing and flexible Ni/Co-MOF@Ti 3 C 2 hybrid membrane is prepared via a layer-by-layer self-assembly method, specifically designed for efficient ORR and as a cathode for Li–O 2 batteries. The Ni/Co-MOF@Ti 3 C 2 hybrid membrane integrates the high conductivity, unique two-dimensional layered structure, and excellent mechanical properties of Ti 3 C 2 with the bimetallic active sites of Ni/Co-MOF, exhibiting remarkable ORR catalytic activity in an O 2 -saturated 1 M LiTFSI electrolyte. The structural characteristics of the hybrid membrane provide smoother expansion pathways for Li + and O 2 , effectively promoting the deposition and decomposition of Li 2 O 2 . This not only enhances the electrochemical performance of the Li–O 2 battery but also overcomes the inherent limitations of traditional slurry-based cathode preparation methods. Experimental results demonstrate that Li–O 2 batteries utilizing the Ni/Co-MOF@Ti 3 C 2 hybrid membrane as the cathode achieve an ultra-high capacity of 36,125 mAh/g at a current density of 1000 mA/g, while exhibiting excellent cycle stability (271 cycles with a limited capacity of 1000 mAh/g at 1000 mA/g) and outstanding rate performance. The hybrid membrane’s capacity and cycle performance can be further optimized by controlling its thickness. These promising results offer novel insights into the innovative design of air cathodes for metal–air batteries, and the proposed method provides a new route for the manufacture of high-performance battery cathodes.

研究领域: 材料科学 · 电化学 · 能源存储与转换
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Engineering fast water-selective pathways in graphene oxide membranes by porous vermiculite for efficient alcohol dehydration

Zhiming Zhang,Hong Wu,Li Cao,Meidi Wang,Hongjian Wang,Fusheng Pan,Zhongyi Jiang

Graphene oxide (GO) lamellar membranes with well-aligned architecture hold promising potential for molecular separations. However, the tortuous transport pathways and weak interlamellar interactions between stacked GO nanosheets cause low flux and poor stability, which are major drawbacks for their practical applications. Herein, we report a strategy to engineer fast and robust water-selective pathways within GO-based lamellar membranes by porous vermiculite (PVMT), a naturally layered magnesium aluminosilicate . PVMT nanosheets conferred abundant in-plane pores, which decreased the tortuosity and shortened the mass transport distance inside lamellar membranes. Meanwhile, PVMT nanosheets enhanced the hydrophilicity and fixed the interlayer distance, contributing to robust water-selective transport. The physicochemical properties of membranes, such as thickness and hydrophilicity, were manipulated by the loading amount of PVMT nanosheets. The resulting lamellar membranes exhibited excellent n -butanol dehydration performance with a permeation flux of 9554 g m −2  h −1 and a separation factor of 2678, which increased by up to 91% and 328% compared to pristine GO/PTFE membranes. Moreover, membranes remain stable for 192 h operation. Our study may stimulate further research on precise construction of mass-transfer pathways within lamellar membranes.

研究领域: 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Contribution of nano-network structure and charge manipulation of 2D laminar membrane to selectivity and fouling control in wastewater treatment

Yuan Li,Jixiang Dai,Yuyang Yao,Yan Guo,Yilin Lu,Menglu Zhang,Jiangnan Shen,Lijun Wu

The assembly of two-dimensional (2D) nanomaterials into laminar membranes with sub-nanometer interlayer spacing provides a platform for fouling control in wastewater treatment with membrane technology. However, the strong stacking of nanomaterials limits membrane applications, and although studies have been conducted to modulate the interlayer structure, the enlarged interlayer channels weaken salt ions rejection and foulants removal. Therefore, this study proposed strategies for designing steric network nanostructures and altering the electrical properties at the sub-nanometer scale to improve the interlayer channels of MXene nanosheets and enhance membrane application properties. The functionalized composite membranes exhibit excellent stability due to hydrogen and covalent bonding effects that enhance the binding energy between the nanomaterials. The formation of three-dimensional (3D) nano-interwoven structures significantly enhanced the rejection of salt ions, and the optimized M/PC membrane retained 79.9% of CaCl 2 compared to only 5.3% of the pristine membrane, and without attenuating the water flux due to the deposition of nanomaterials. The improvement of the positive electrical characteristics, competitive adsorption and polar force-driven enabled the effective separation of organic matter and salt ions in the leachate and synthetic solution, the selectivity value of HA/NaCl reached to 40.6. Theoretical calculations showed that polar acid-base ( ΔG AB ) dominated the resistance of membrane fouling and that M/PC membrane significantly repel foulants. This work highlights the importance of MXene sub-nanofluidic channels improvement and interfacial charge modulation for permeability, selectivity and elucidates the mechanisms of fouling control using functionalized membranes.

研究领域: 环境科学 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2022 · IF 10.53

Secondary-assembled defect-free MOF membrane via triple-needle electrostatic atomization for highly stable and selective organics permeation

Jingjing Chen,Xiaoli Wu,Chongchong Chen,Yihao Chen,Wenpeng Li,Jingtao Wang

Two-dimensional lamellar membranes featuring well-defined nanochannels hold great promise for efficient organics separation. However, the extensively existed non-selective microdefects within laminate architecture would impair separation efficiency and structure stability of membranes. Herein, defect-free metal-organic framework (MOF) lamellar membrane is facilely constructed by triple-needle electrostatic atomization technology. Specifically, one needle atomizes small-sized Cu-TCPP MOF nanosheets (TCPP = meso-tetra(4-carboxyphenyl)porphyrin) to build lamellar skeleton, and the other two needles meantime atomize Cu 2+ and TCPP to secondary-assemble crystals among nanosheets. In this manner, these non-selective microdefects are subtly sutured by the regenerated crystals with identical chemical components, resulting in a defect-free MOF lamellar membrane with enhanced structural stability. Importantly, this novel secondary-assembly method highly enhances the separation efficiency and meanwhile keeps high organics permeation for MOF membrane, with rejection of 93.8% for Rose Bengal (1.2 nm) and acetone permeance of 86.9 L m −2 h −1 bar −1 . In addition, the multipoint connection between nanosheets and crystals ensures excellent surface shearing and compaction resistance for MOF membrane, permitting high and steady operation performance for over 100 h. This secondary-assembly methodology by one-step process to construct defect-free and steady lamellar membrane provides a new avenue for the development of efficient separation membranes .

研究领域: 材料科学 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Construction of a 2D lamellar membrane for a combination of photocatalytic hydrogen evolution and photothermal water evaporation

Weiming Zhou,Hongqiang Huang,Yiting Wu,Jun Wang,Yusuke Yamauchi,Jeonghun Kim,Sameh M. Osman,Xingtao Xu,Liwei Wang,Chong Wang,Zhanhui Yuan

Solar energy can help solve the energy and water shortage crisis. Developing a single material that can exhibit both photocatalytic hydrogen evolution (PHE) and photothermal water evaporation (PWE) represents a new concept to simultaneously realize green energy and fresh water supply. In this study, a series of 2D lamellar membranes (2DLMs) based on a conventional semiconductor BiOCl nanosheet was designed as an ensemble, and its combined application for PHE and PWE was explored, in which cellulose nanofibers (CNFs), carbon nanotubes (CNTs), and a self-assembly of CNF@CNT were also used. The PHE and PWE efficiencies are closely related to the conversion of solar energy and the state of the water molecules. Owing to the high light-to-thermal conversion, enhanced water transfer, and the low evaporation enthalpy of confined water, a composite made of BiOCl and CNF@CNT 2DLM (BOC-CNF@CNT) could rapidly reach a surface temperature of 46.6 °C, with its PWE rate reaching up to 2.05 kg·m −2 ·h −1 . Moreover, owing to the high photogenerated carrier transport, strong photothermal effect, and the action of confined water, the PHE rate of BOC-CNF@CNT is 1.99-fold that of the composite made of BiOCl and CNF 2DLM (BOC-CNF) and 1.42-fold that of the composite made of BiOCl and CNT 2DLM (BOC-CNT). This work provides a new and effective strategy for a comprehensive utilization of solar energy to simultaneously produce clean hydrogen and fresh water.

CAS / MDL: 308068-56-6
研究领域: 材料科学 · 能源科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Structural design of Janus lamellar membrane based on bismuth oxychloride for comprehensive solar energy utilization

Weiming Zhou,Hongqiang Huang,Chong Wang,Liwei Wang,Xiangfeng Lin,Yusuke Asakura,Yusuke Yamauchi,Sameh M. Osman,Zhanhui Yuan

Photocatalysis and photothermal water evaporation (PWE), as two technologies that utilize solar energy, have received special attention in the context of carbon neutrality. It is undoubtedly attractive if a structure can effectively combine the two technologies. However, it remains a huge challenge to simplify structural design while improving energy efficiency and mass transfer. Herein, a Janus lamellar membrane (JLM) with an asymmetric bi-layered structure was constructed using facile vacuum filtration. Specifically, the top layer consists of BiOCl nanosheets (BNs) and cellulose nanofibers@carbon nanotubes (CNF@CNT), forming a functional layer that facilitates solar energy utilization. Within the top and bottom layers, CNF@CNT and CNFs are respectively embedded into the interlayer space formed by stacked BNs, offering abundant nanochannels for continuous and rapid water supply. Moreover, as the weight ratio of the BN-CNF@CNT and BN-CNF precursors is optimized to 1:1 with the BN-CNF@CNT layer facing light source, the photocatalytic hydrogen evolution (PHE) rate of JLM reaches up to 39.81 μmol·g −1 ·h −1 , corresponding to approximately 3.12 and 1.57 times that of the BN-CNF and BN-CNF@CNT lamellar membranes, respectively. Importantly, the PHE rate remains consistent within ten cyclic stability experiments. Furthermore, the PWE rate of JLM achieves 1.98 kg·m −2 ·h −1 under 1.0 solar irradiation (100 mW·cm −2 ). A vital advantage of the JLM is its ability to float on the liquid surface, enabling concurrent photocatalytic decontamination and PWE processes. The research on designing JLM with an asymmetric structure for both photocatalysis and PWE provides a practical approach to the comprehensive utilization of solar energy.

研究领域: 材料科学 · 能源技术 · 环境科学
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JOURNAL OF MEMBRANE SCIENCE · 2022 · IF 10.53

Exquisite manipulation of two-dimensional laminar graphene oxide (GO) membranes via layer-by-layer self-assembly method with cationic dyes as cross-linkers

Yi-Hang Gu,Xi Yan,Yan Chen,Xiao-Jing Guo,Wan-Zhong Lang

Herein, we propose one novel strategy by layer-by-layer (LBL) self-assembly method to prepare two-dimensional (2D) laminar membranes assembled between sulfonated graphene oxide (S-GO) nanosheets and various cationic dyes on the polyethyleneimine (PEI) -modified Nylon-6 (PA6) substrate. The membrane performances are manipulated exquisitely by the charge of substrate, the assembled dye type, dye size, self-assembly layer number etc. The water permeance positively correlates with the height of assembled cationic dyes. The amido bonds or sulfamide bonds and π–π conjugation endow the resulted membrane with strong performance stability. Furthermore, by precisely selecting the size and charge the assembled dye, the prepared LBL GO membranes can efficiently separate mixed dyes in aqueous solution via charge repulsion or/and size sieving mechanism. For example, the separation selectivity of 39.2 for the mixed Rhodamine B/Ethyl Violet (RB/EV) dyes can be achieved with the LBL MV-0.25-2-2 membrane (it was assembled by 2 mmol L −1 Methyl violet solution for two S-GO layers with the Nylon-6 substrate modified with 0.25 wt % PEI aqueous solution). Simultaneously, the introduced cationic dyes endow these membranes with extra antibacterial capacity to both E. coli and S. aureus .

研究领域: 材料科学 · 环境工程 · 化学工程
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2025 · IF 7.8

Construction of MXene-based laminar membranes with aminated Fe3O4 via electrostatic self-assembly for selective dye/salt separation

Yufen Kong,Hongdan Wu,Zhihui Zhou,Xianyuan Fan,Ming Li

To address the long-standing trade-off between flux and selectivity, as well as the structural instability of conventional nanofiltration (NF) membranes, this study proposes a novel intercalation strategy for constructing two-dimensional laminar NF membranes based on MXene for efficient dye/salt separation. Spherical Fe 3 O 4 nanoparticles were functionalized with amino groups using 3-aminopropyltriethoxysilane (APTES) to impart positive surface charges, and subsequently assembled onto hydrophilic MXene (Ti 3 C 2 T x ) nanosheets via electrostatic self-assembly, forming a structurally stable MXene/NH 2 -Fe 3 O 4 composite membrane. The surface functionalization of Fe 3 O 4 plays a critical role in regulating the interlayer structure of MXene, thereby enhancing membrane stability and selective transport performance. At a mass ratio of MXene to NH 2 -Fe 3 O 4 of 1:6, the membrane exhibited a pure water flux of 136.6 L/(m 2 ·h) and rejection rates of up to 99.9 % for Congo Red (CR) and Evans Blue (EB). In contrast, the rejection rates for NaCl, MgSO 4 , and Na 2 SO 4 were 7.0 %, 15.4 %, and 26.4 %, respectively. In mixed dye/salt systems, the membrane exhibited excellent selectivity, with separation factors of 839 for CR/NaCl, 704 for CR/MgSO 4 , and 566 for CR/Na 2 SO 4 , attributed to synergistic contributions of size exclusion, electrostatic repulsion, and the Donnan exclusion effect. Furthermore, the composite membrane demonstrated outstanding dye removal efficiency, acceptable salt rejection, and robust structural integrity under prolonged operation, wide pH variations, and challenging conditions involving organic foulants and surfactants, offering a practical strategy for developing advanced NF membranes for complex wastewater treatment.

CAS / MDL: 1317-61-9 919-30-2
研究领域: 材料科学 · 膜分离技术 · 环境工程 · 纳米材料 · 化学工程 · 水处理
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