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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Polydopamine-assisted minute fabrication of vertically aligned ZIF-L membranes for CO2/N2 separations

Keming Zhang,Sihui Li,Xiaohe Tian,Rui Zhang,Xiaoting Feng,Qingnan Wang,Yanting Tang,Chenlu Liu,Hongxia Gao,Shaofei Wang

Metal-organic framework (MOF) membranes demonstrate significant potential for industrial gas separations, yet fabricating vertically aligned two-dimensional (2D) MOF membranes on polymer substrates remains a considerable challenge due to the weak adhesion and difficulty in achieving precise alignment. This study presents a one-step method for the rapid synthesis of vertically aligned ZIF-L membranes, using a polydopamine (PDA)-assisted approach. This method enables the rapid formation of homogenous, thin but defect-free membranes on polymer substrates within 5 min, drastically reducing the preparation time by over 200 times. The vertically aligned ZIF-L membranes, characterized by the interlayer galleries facing the gas mixtures, exhibit an excellent CO 2 permeance exceeding 1200 GPU and a CO 2 /N 2 selectivity of 14.5. The versatility of this approach allows for its application on various flat-sheet or even hollow fiber supports. Our findings highlight the potential of PDA-assisted synthesis for efficient, scalable preparation of high-performance MOF membranes for industrial gas separations.

研究领域: 化学工程 · 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Enhancing CH4/N2 separation performance within aluminum-based Metal-Organic Frameworks: Influence of the pore structure and linker polarity

Zhenghui Huang,Peng Hu,Jia Liu,Fang Shen,Youquan Zhang,Kungang Chai,Yunpan Ying,Chengjun Kang,Zhaoqiang Zhang,Hongbing Ji

Efficient CH 4 /N 2 separation is necessitated for obtaining purified methane from natural gas. Aluminum-based metal–organic frameworks (Al-MOFs) have potential for industrial separation applications due to their structure-tunable, low-cost, and scalable features. Intrigued by the impressive selectivity of a recently reported Al-MOF (Al-CDC) toward CH 4 over N 2 , we herein further study the potential of Al-MOFs as adsorbent for CH 4 /N 2 separation, mainly considering the effects of pore geometry and linker polarity. Utilization of two bent ligands and two linear ligands with different polarity afforded two one-dimensional square-shaped Al-MOFs i.e., CAU-10-H, MIL-160, and two rhombic-shaped counterparts i.e., Al-Fumarate (Al-Fum), MIL-53(Al)), respectively. Afterward, pure CH 4 and N 2 adsorption experiments were conducted at 273–313 K for assessing the CH 4 /N 2 separation performance. The results indicated that all the Al-MOFs exhibited superior affinity toward CH 4 over N 2 , and the CH 4 uptake followed the sequence of Al-Fum > CAU-10-H > MIL-53(Al) > MIL-160. Exhilaratingly, Al-Fum exhibited unprecedented CH 4 /N 2 selectivity (17.2) and high CH 4 uptake at 273 K and 1.0 bar. The mechanism underlying the disparity of Al-MOFs affinity toward CH 4 was deciphered via theoretical simulation, suggesting that the synergetic effects of accessibility of strong affinity sites (μ 2 -OH) on AlO 6 chains and polar pore surface induced by varying linkers highly promoted the CH 4 uptake. Furthermore, the results of cyclic adsorption–desorption experiments and binary breakthrough tests validated the feasibility of Al-Fum for practical application.

研究领域: 材料科学 · 化学工程 · 气体分离
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2025 · IF 5.4

Synergistic enhancement of surface deposition and moisturizing performance of trehalose and N2-(2,3-dihydroxypropyl)arginine hydrochloride through hydrogen bonding interactions

Bingqing Wang,Haofeng Sun,Jun Gao,Liying Kang,Haixiao Wan,Ying Wu,Hui Ma,Ziling Teng,Xian Xu,Lin Geng,Xiaozhi Wang,Li Ye,Yan Huang,Dongcui Li,Naisheng Jiang

Effective moisturizing agents are crucial for improving the performance of rinse-off cosmetic formulations. Herein, we explored the synergistic effects of trehalose and N 2 -(2,3-dihydroxypropyl)arginine hydrochloride (DPAH), a glycerol derivative of L-arginine, on enhancing surface deposition and moisturizing performance. Using various surface-sensitive characterization techniques, we observed significant enhancements in the surface deposition of the trehalose/DPAH mixture compared to trehalose alone or glycerol-based controls. Molecular dynamics simulations further revealed strong intermolecular hydrogen bonds between trehalose and DPAH, contributing to the observed synergistic effects. A moisture-retention study using a model anionic surfactant-based system demonstrated that the trehalose/DPAH mixture achieves higher skin hydration levels and reduced transepidermal water loss compared to trehalose and DPAH alone. These findings offer new insights into the molecular interactions that enhance the surface deposition and moisturizing efficacy of trehalose, presenting promising opportunities for developing advanced cosmetic formulations with optimized moisture-retaining properties.

研究领域: 化妆品科学 · 分子生物学 · 表面化学
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ARABIAN JOURNAL FOR SCIENCE AND ENGINEERING · 2023 ·Vol. 48 ·期 12 ·16471-16482 · IF 2.9

Poly(4-Methyl-1-Pentene) (PMP) with Nano Fumed Silica as Filler for CO2/N2 Gas Separation

Zainuddin Muhd Izzudin Fikry,Ahmad Abdul Latif,Subramaniam Reasmyraj R.

Carbon dioxide (CO 2 ) separation with membrane technology has become the focus of researchers over the past decades due to its lower energy consumption and cheaper alternative. Mixed matrix membrane (MMM) of poly(4-methyl-1-pentene) (PMP) with nano fumed silica particles was studied to determine the feasibility of using MMM to separate CO 2 from nitrogen (N 2 ) gas. The critical concentration of PMP (7 wt%) was utilized to form the membrane in this study in order to ensure the polymer chain entanglement occurs to form a dense structure. Agglomeration of particle can be observed on the surface with scanning electron microscopy (SEM) imaging with 10 and 15 wt% of nano fumed silica loading in PMP matrix. This observation is further confirmed with energy-dispersive X-ray (EDX) mapping across the cross-sectional area which shows clustered nano fumed silica particle with loading of 10 and 15 wt%. With 7.5 wt% filler loading and at 1 bar, the MMM seems to give the best gas permeance performance with CO 2 permeance of 4.62 GPU (100.54 Barrer) and N 2 permeance of 0.20 GPU (4.31 Barrer) which makes the highest ideal selectivity to be about 23, which was the highest ideal selectivity achieved in this study. Meanwhile, when the pressure was increased from 1 to 7 bar, the CO 2 permeability increased almost linearly followed by a steady decline in CO 2 /N 2 ideal selectivity.

研究领域: 膜技术 · 气体分离 · 高分子科学 · 纳米复合材料 · 环境工程
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LANGMUIR · 2025 · IF 3.9

Photo-Fenton Degradation of Tetracycline Boosted by Charge Redistribution in g-C3N4 with Fe–N2 Configuration and O/P Dual Doping

Xiao Zhang,Menglin Zhang,Zhiren Guo,Xiang Li,Ting Liu,Jinying Li,Dongxiang Zhang,Xiyan Xu

The persistent contamination of aquatic environments by tetracycline (TC) necessitates advanced remediation strategies. Herein, a ternary Fe–O–P-co-modified graphitic carbon nitride (FOPCNx) was synthesized via structural integration of Fe–N2 configurations with O/P dual doping for efficient TC degradation in a solar-driven photo-Fenton system. This study pioneers the synergistic coupling of Fe–N2 coordination and heteroatomic O/P substitution to optimize charge dynamics. Comprehensive characterization confirmed the formation of Fe–N2 active sites and aromatic structures incorporated with the aromatic group, which collectively enhanced visible-light absorption, suppressed electron–hole recombination, and facilitated charge carrier redistribution. The optimized FOPCN2 demonstrated exceptional photoelectric efficiency (3.7-fold higher photocurrent density than pristine g-C3N4) and achieved 98.9% TC removal within 40 min of irradiation with a kinetic constant of 0.113 min–1, outperforming conventional systems. Mechanistic studies revealed dual enhancement pathways: Fe–N2 sites promoted electron transfer and Fe(III)/Fe(II) cycling, while the O/P dual doping enabled electron delocalization for improved charge mobility. The system exhibited remarkable pH adaptability (3–7), robust resistance to inorganic anions, and universal degradation capability for mixed organic pollutants. Three TC degradation pathways were identified through intermediate analysis, with radical trapping and EPR verification confirming the dominant roles of •OH, e–, and O2•–. This work provides critical insights into structure–activity relationships for carbon nitride modification, establishing a paradigm for designing multifunctional photocatalysts for antibiotic-contaminated wastewater remediation.

研究领域: 环境科学 · 材料科学 · 光催化 · 水处理 · 纳米技术
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Tuning the Pore Environment of MOFs toward Efficient CH4/N2 Separation under Humid Conditions

Tong Li,Xiaoxia Jia,Hui Chen,Zeyu Chang,Libo Li,Yong Wang,Jinping Li

Adsorption separation technology using adsorbents is promising as an alternative to the energy-demanding cryogenic distillation of natural gas (CH4/N2) separation. Although a few adsorbents, such as metal–organic frameworks (MOFs), with high performance for CH4/N2 separation, have been reported, it is still challenging to target the desired adsorbents for the actual CH4/N2 separation under humid conditions because the adsorption capacity and selectivity of the adsorbents might be mainly dampened by water vapor. Except for the high CH4 uptake and CH4/N2 selectivity, the adsorption material should simultaneously have excellent stability against moisture and relatively low-water absorption affinity. Here, we tuned the ligands and metal sites of reticular MOFs, Zn-benzene-1,4-dicarboxylic acid–1,4-diazabicyclo[2.2.2]octane (Zn-BDC–DABCO) (DMOF), affording a series of isostructural MOFs (DMOF-N, DMOF-A1, DMOF-A2, and DMOF-A3). Because of the finely engineered pore size and introduced aromatic rings in the functional DMOF, gas sorption results reveal that the materials show improved performance with a benchmark CH4 uptake of 37 cm3/g and a high CH4/N2 adsorption selectivity of 7.2 for DMOF-A2 at 298 K and 1.0 bar. Moisture stability experiments show that DMOF-A2 is a robust MOF with low water vapor capacity even at ∼40% relative humidity (RH) because of the presence of more hydrophobic aromatic rings. Breakthrough experiments verify the excellent CH4/N2 separation performances of DMOF-A2 under high humidity.

研究领域: 材料科学 · 化学工程 · 环境科学
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Promoting effect of Ti addition on three-dimensionally ordered macroporous Mn-Ce catalysts for NH3-SCR reaction: Enhanced N2 selectivity and remarkable water resistance

Xiaofeng Wang,Zhe Zhao,Yang Xu,Qingbo Li

A series of 3DOM-Mn x Ce y Ti z catalysts with three-dimensionally ordered macroporous (3DOM) structure were synthesized by a soft template method. The high SCR activity of the 3DOM-Mn 3 Ce 1 catalyst at low temperature was owing to the excellent redox ability and rich Lewis and Brønsted acid sites of the catalysts, which were beneficial to improve the catalytic activity. However, the strong oxidizability of MnO x resulted in the nonselective oxidation of NH 3 and generation of N 2 O, decreasing the N 2 selectivity. After addition of Ti, the redox capacity of the 3DOM-Mn 3 Ce 1 Ti 1 catalyst decreased, and the NH 3 were strongly adsorbed on the acid sites, which enhanced the N 2 selectivity with a broadened temperature window of 240–440 °C and a high GHSV of 120000 h −1 . Furthermore, both the 3DOM-Mn 3 Ce 1 and 3DOM-Mn 3 Ce 1 Ti 1 catalysts showed remarkable tolerance of H 2 O. Finally, through in situ DRIFT analysis, the Langmuir-Hinshelwood (L-H) mechanism was confirmed as the dominant reaction pathway over the 3DOM-Mn 3 Ce 1 Ti 1 catalyst.

研究领域: 环境科学 · 催化化学
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ACS Catalysis · 2023 · IF 12.9

Unraveling the Lattice O Assisted Internal Selective Catalytic Reduction Mechanism on High N2 Selectivity of CuOx/PtCu Catalysts in NH3-SCO

Yanfei Liu,Zhang Liu,Chengxiong Wang,Jie Xu,Jianping Ai,Xiao Liu,Aimin Zhang,Yunkun Zhao,Chun Du,Bin Shan

Supported Pt catalysts suffer from low reaction selectivity (<65% at 100% conversion) in the selective catalytic oxidation of ammonia (NH3-SCO) because of their intrinsic over-oxidation tendencies. Herein, a strategy based on facilitating byproduct NOx reduction to N2 is demonstrated at CuOx/PtCu catalysts, aiming to tackle the low selectivity challenge. This PtCu alloy sample with a CuOx-rich surface displays an N2 selectivity of 95%, while its turnover frequencies are the highest among reported supported Pt-based catalysts. The enhanced reaction activities and N2 selectivities are primarily attributed to the Pt-Cuδ+ dual-site synergies at the CuOx/PtCu interface, in which dual sites exhibit distinct NH3 adsorption, activation, and dehydrogenation behaviors. The Olat assisted internal selective catalytic reduction mechanism at CuOx/PtCu with N2O22– as the central intermediates is proposed. Density functional theory calculation and temperature-programmed surface reaction measurements show that the N–O bond in N2O22– tends to break simultaneously with the assistance of Ov in CuOx followed by the easy transition from N2O22– to N2, which serve as the origin of the high selectivity.

研究领域: 催化化学 · 环境科学 · 材料科学
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JOURNAL OF MEMBRANE SCIENCE · 2020 · IF 7.183

Fabrication of highly CO2/N2 selective polycrystalline UiO-66 membrane with two-dimensional transition metal dichalcogenides as zirconium source via tertiary solvothermal growth

Rong Rong,Yanwei Sun,Taotao Ji,Yi Liu

Zirconium-based MOF (Zr-MOF) membranes have attracted widespread attention due to their highly tailorable pore aperture and adsorption behavior achieved by functional group decoration and ligand/cluster-missing defect regulation as well as extraordinary chemical/thermal stability. Nevertheless, it has remained a great challenge to further improve the separation performance of Zr-MOF membranes due to very limited available zirconium sources and heating modes. In this study, we prepared polycrystalline UiO-66 membranes exhibiting unprecedented CO 2 /N 2 selectivity (31.3). The use of layered ZrS 2 , a representative of transition-metal dichalcogenides (TMDCs), as zirconium source during tertiary solvothermal growth was found to be indispensable for improving the separation performance of UiO-66 membranes. As far as we know, the CO 2 /N 2 selectivity reported in this study was the highest among all pristine polycrystalline MOF membranes measured under ambient conditions. More importantly, our study highlighted the importance of concurrent metal source and fabrication process innovation in performance enhancement of polycrystalline MOF membranes.

研究领域: 材料科学 · 化学工程 · 膜技术
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POLYMER SCIENCE SERIES A · 2018 ·Vol. 60 ·期 5 ·612-617 · IF 0.729

Formation and CO2/N2 Switchable Ability of a Novel Copolymer Poly(N,N-Diethylaminoethyl Methacrylate-co-Sodium Vinylsulfonate)

Wang Jinjing,Wang Huifeng,Li Yan,Tian Li,Chen Shanmin,Liu Qiang,Guo Zhen

A novel copolymer surfactant has been prepared via a free radical copolymerization of CO 2 -switchable monomer N , N -diethylaminoethyl methacrylate and the hydrophilic monomer sodium vinyl-sulfonate and characterized. The results of conductivity, dynamic light scattering and cryogenic transmission electron microscopy study showed the change of the microstructure of copolymer in water by adding or removing of CO 2 . The copolymer aqueous solution was found to exhibit reversible switchability by the bubbling of CO 2 /N 2 .

研究领域: 高分子化学 · 材料科学
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Materials Today Communications · 2022 · IF 3.662

Synthesis of dual-functionalized APTES-Bentonite/PVDF mixed-matrix membranes for the efficient separation of CO2/CH4 and CO2/N2

Shaocan Dong,Weiqiu Huang,Xufei Li,Xinya Wang,Baoyou Yan,Zhen Zhang,Jing Zhong

In response to global climate change, most countries have set carbon reduction targets. Mixed matrix membranes (MMMs), which combine the characteristics of inorganic nanofillers and organic matrices, have received wide attentions because of their good permeability and selective performance for the separation of CO 2 from industrial waste gases. However, the poor dispersion, compatibility and interfacial defects often lead to poor gas separation performance. In this paper, according to the dissolution-diffusion and Lewis acid-base theories, inorganic filler of amino-functionalized Bentonite (APTES-Bentonite) with -NH 2 was firstly synthesized to improve the affinity of CO 2 . Then, the dual-functionalized MMMs of APTES-Bentonite/PVDF (A-B/P MMMs) was prepared and adopted for the separation of CO 2 /CH 4 and CO 2 /N 2 , showing the increase of 87.76% and 75.31% compared to the pristine PVDF membrane, respectively. These excellent performances were attributed to the synergistic effect of APTES-Bentonite with -NH 2 groups and PVDF with -F groups, which provide a dual-functional transport pathway for CO 2 molecules due to the interactions of host-guest. Overall, the customized A-B/P MMMs offer superior CO 2 separation performance, which provides some valuable references for large-scale CO 2 capture studies.

研究领域: 材料科学 · 环境工程 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

High-pressure separation performance of Ni(TMBDC)(DABCO)0.5 featured low-polarity channel for CH4/N2 mixture

Xun Wang,Zewei Liu,Jian Yan,Daofei Lv,Xin Chen,Feng Xu,Xin Zhou,Zhong Li

Developing adsorbents with exceptional CH 4 /N 2 selectivity under high pressure is a crucial commercial requirement and a significant technical challenge for the industrial high-pressure swing adsorption (HPSA) in CH 4 /N 2 separation. Only a few adsorbents were reported to address this issue. In this work, we aimed to explore two microporous MOFs with low-polarity channels for high-pressure CH 4 /N 2 separation. The Ni(BDC)(DABCO) 0.5 and its isostructural analog Ni(TMBDC)(DABCO) 0.5 were synthesized, characterized, and examined for high-pressure CH 4 /N 2 adsorption property. Due to the lower polarity channel originating from tetramethyl groups, Ni(TMBDC)(DABCO) 0.5 exhibited an exceptional methane capacity of 4.23 mmol/g and an IAST selectivity of 5.1 for the CH 4 /N 2 binary mixture at a pressure of 10 bar, surpassing the majority of previously reported materials. The GCMC simulation revealed that the low-polarity pore surfaces in both materials exhibited a higher affinity for CH 4 molecules compared to N 2 molecules, under both ambient and high pressures. The breakthrough experiments showed that Ni(TMBDC)(DABCO) 0.5 exhibited excellent dynamic separation towards CH 4 /N 2 under both 1 bar and 5 bar, indicating great potential as an emerging candidate for the recovery of CH 4 from coal-mine methane in industrial PSA processes.

研究领域: 材料科学 · 化学工程 · 吸附技术
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