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Aqueous hydrotrope-based green extraction of alkaloids: insights into mechanism and experimentation with Coptis chinensis 水相萃取法提取黄连生物碱的机理及实验研究
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-07 DOI: 10.1016/j.seppur.2026.137195
Nhan Trong Le , The-Huan Tran , Vy Khanh Thi Nguyen, Tuong Cat Chau Mai, Hoai Thi Nguyen
The search for environmentally benign solvents has become a central task in natural product research, as conventional organic solvents remain problematic for both safety and sustainability. Hydrotropes (HTs) are emerging as an attractive alternative because they can significantly increase the aqueous solubility of poorly soluble compounds. This study explored the use of aqueous HT solutions for alkaloid recovery, exemplified by the case of Coptis chinensis. Initial screening highlighted sodium salicylate (SS) as a particularly effective solvent, affording higher yields of coptisine, palmatine, berberine, and total alkaloids than conventional or other green solvents. Through response surface methodology, the optimum conditions were identified (46.4% SS, liquid–solid ratio 26.7 mL/g, 21.8 min, 60 °C), under which the yields of coptisine, palmatine, berberine, and total alkaloids reached 1.85%, 1.39%, 8.97%, and 15.57%, respectively. Mechanistic analyses, combining electrostatic potential mapping, interaction region indicator plots, and molecular dynamics simulations, revealed that the strong performance of SS stems from cooperative anion–Cδ+ electrostatic interactions together with dispersion forces and weak hydrogen bonding. The extraction followed a second-order kinetic model (Ea = 26.14 kJ/mol), suggesting contributions from both dissolution and diffusion. Importantly, alkaloids were efficiently recovered with macroporous resins (best with HPD-400), and both SS and the resins could be reused for at least five cycles with negligible efficiency loss. Sustainability was further quantitatively assessed using the AGREEprep metric. Taken together, these findings establish aqueous SS as a practical, reusable, and environmentally responsible solvent system for sustainable alkaloid extraction, with mechanistic validation demonstrated for berberine.
寻找对环境无害的溶剂已经成为天然产物研究的中心任务,因为传统的有机溶剂在安全性和可持续性方面仍然存在问题。水变性物(HTs)正成为一种有吸引力的替代品,因为它们可以显著提高难溶性化合物的水溶性。本研究以黄连(Coptis chinensis)为例,探讨了高温水溶液在生物碱回收中的应用。最初的筛选突出了水杨酸钠(SS)作为特别有效的溶剂,提供比传统溶剂或其他绿色溶剂更高的黄柏碱、棕榈碱、小檗碱和总生物碱的产量。通过响应面法确定了最佳工艺条件(SS 46.4%,液料比26.7 mL/g, 21.8 min, 60℃),黄柏碱、棕榈碱、小檗碱和总生物碱的得率分别为1.85%、1.39%、8.97%和15.57%。通过静电势作图、相互作用区域指示图和分子动力学模拟等方法,揭示了SS的强性能源于阴离子- cδ +静电相互作用、色散力和弱氢键的协同作用。萃取符合二级动力学模型(Ea = 26.14 kJ/mol),表明溶出和扩散都有贡献。重要的是,生物碱可以用大孔树脂(最好是用HPD-400)有效地回收,并且SS和树脂都可以重复使用至少5次,效率损失可以忽略不计。使用AGREEprep指标进一步定量评估可持续性。综上所述,这些发现确立了水溶SS作为一种实用的、可重复使用的、对环境负责的可持续提取生物碱的溶剂体系,并证实了对小檗碱的机理验证。
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引用次数: 0
Fabrication and properties of air filter materials with fluffy multi-scale micro/nano bimodal fibers via multi-nozzle solution blow spinning 多喷嘴溶液纺制蓬松多尺度微纳双峰纤维空气过滤材料及其性能
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-08 DOI: 10.1016/j.seppur.2026.137183
Pengqi Shi , Gaohui Fan , Wanli Yue , Yanru Bai , Xu Zhao , Hao Guo , Qiaomei Zhang , Bowei Liu , Guorui Zhang , Jingyi Sun , Xuling Jin , Baokang Yu , Rongwu Wang , Jianxin He
To address the challenge of balancing high efficiency, low resistance, and long-term stability in fibrous filter materials, this study proposes an innovative parallel-integrated spinning strategy. By combining solution blow spinning and electrostatic solution blow spinning units in situ, a three-dimensional fluffy micro/nano-bimodal fiber composite filter material was successfully prepared in a single step. This method achieves the synchronous formation and uniform interweaving of a microfiber skeleton and a nanofiber filtration network, while allowing precise optimization of the material's pore size distribution and pore structure through adjustment of the spinning unit ratio. The results show that the prepared filter material exhibits a distinct bimodal fiber distribution, high porosity (>92%), and strong hydrophobicity endowed by its micro-nano multi-scale rough structure. Among them, the filter prepared with a spinning unit ratio of 1 (WNfm1/1) demonstrates the optimal initial comprehensive filtration performance (99.648 ± 0.36% efficiency, quality factor of 0.03646 ± 0.0002 Pa−1). In contrast, the filter prepared with a spinning unit ratio of 2 (WNfm2/1), benefiting from its more open pore structure, exhibits higher dust-holding capacity (29.54 g/m2), longer service life (34 days), and excellent stability in long-term tests, revealing the balance between initial efficiency and long-term, low-resistance operation. Combined with microstructural evolution observations and numerical simulations, the research elucidates the synergistic mechanism of micro- and nanofibers in depth filtration. The material also possesses good mechanical resilience and thermal stability. This work provides a novel preparation strategy and theoretical foundation for the development of high-performance and sustainable air filter materials.
为了解决纤维过滤材料在高效、低阻力和长期稳定性之间的平衡问题,本研究提出了一种创新的平行集成纺丝策略。通过原位溶液吹丝和静电溶液吹丝装置相结合,一步成功制备了三维蓬松微纳双峰复合过滤材料。该方法实现了微纤维骨架和纳米纤维过滤网络的同步形成和均匀交织,同时通过调整纺丝单元比,实现了材料孔径分布和孔结构的精确优化。结果表明:制备的过滤材料具有明显的双峰纤维分布,高孔隙率(>92%),微纳多尺度粗糙结构赋予其强疏水性。其中,纺丝单元比为1 (WNfm1/1)时制备的过滤器初始综合过滤性能最佳(效率为99.648±0.36%,品质因子为0.03646±0.0002 Pa−1)。相比之下,纺丝单元比为2 (WNfm2/1)时制备的过滤器,由于其更开放的孔隙结构,具有更高的粉尘容量(29.54 g/m2),更长的使用寿命(34天),并且在长期试验中具有优异的稳定性,体现了初始效率和长期低阻力运行之间的平衡。结合微观结构演变观察和数值模拟,阐明了微纳米纤维在深度过滤中的协同作用机制。该材料还具有良好的机械回弹性和热稳定性。本研究为开发高性能、可持续的空气过滤材料提供了新的制备策略和理论基础。
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引用次数: 0
Interchain hydrogen bonding in one-dimensional benzimidazolone-based covalent organic frameworks: charge modulation for improved gold recovery efficiency 一维苯并咪唑酮基共价有机骨架中的链间氢键:电荷调制提高金回收率
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-03 DOI: 10.1016/j.seppur.2026.137144
Zhen-Wen Zhang , Cheng-Peng Niu , Sai-Jin Xiao , Hao-Xuan He , Qiang Shi , Zhi-Hao Xue , Bin Lin , Ru-Ping Liang , Li Zhang , Jian-Ding Qiu
One-dimensional covalent organic frameworks (1D COFs), as linear crystalline porous polymers, are highly promising materials for gold recovery due to their exceptional atomic utilization efficiency and fully exposed active sites. However, their development for gold adsorption is constrained by the lack of gold-specific organic building blocks and limited electronic regulation strategies. Herein, we introduce benzoimidazolone units into 1D COFs and design interchain hydrogen bond through molecular engineering to rationally modulate their charge distribution. The constructed 1D COF, featuring improved crystallinity/stability, enriched recognition sites, and enhanced protonation capability, demonstrates superior performance in gold recovery with rapid kinetics, excellent selectivity and a high adsorption capacity of 2900.56 mg g−1. Theoretical calculations reveal the multiple and synergistic interactions between benzimidazolone and AuCl4, and elucidate the effect of hydrogen bonding on electron redistribution/transfer towards benzimidazolone, thereby promoting its protonation and significantly enhancing the adsorption and reduction capabilities for gold. This work highlights the significance of hydrogen bonding on charge modulation and develops a benzimidazolone-based 1D COFs for efficient gold recycling from electronic waste.
一维共价有机框架(1D COFs)作为一种线性晶体多孔聚合物,由于其优异的原子利用效率和充分暴露的活性位点,是一种非常有前途的金回收材料。然而,由于缺乏金特异性有机构件和有限的电子调节策略,它们在金吸附方面的发展受到限制。本文将苯并咪唑酮单元引入一维COFs中,通过分子工程设计链间氢键,合理调节其电荷分布。所构建的1D COF具有结晶度/稳定性提高、识别位点丰富、质子化能力增强等特点,具有快速的动力学、优异的选择性和2900.56 mg g−1的高吸附量,具有优异的金回收性能。理论计算揭示了苯并咪唑酮与AuCl4−之间的多重协同相互作用,并阐明了氢键对电子向苯并咪唑酮的再分配/转移的影响,从而促进了苯并咪唑酮的质子化,显著提高了对金的吸附和还原能力。这项工作强调了氢键在电荷调制中的重要性,并开发了一种基于苯并咪唑酮的1D COFs,用于从电子废物中高效回收金。
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引用次数: 0
Upcycled PET carbon dots build an S-scheme Fe2O3 heterojunction photocatalyst for visible-light degradation of tetracycline 升级后的PET碳点构建了S-scheme Fe2O3异质结光催化剂,用于四环素的可见光降解
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-01 DOI: 10.1016/j.seppur.2026.137122
Pandi Kalimuthu , Gopi Kalaiyarasan , Jinho Jung , Diwakar Tiwari
Polyethylene terephthalate-derived carbon dots (PET-CDs) were interfaced with iron oxide (Fe2O3) to develop a visible-light PET-CDs/Fe2O3 photocatalyst for tetracycline (TC) removal. Waste PET bottles were upcycled via a peroxide-free route, enabling oxidant-free operation. The photocatalyst forms a defect-rich, mesoporous carbon-dot network with uniformly dispersed Fe2O3 nanoparticles, enhancing adsorption and interfacial charge transport. This study demonstrates efficient TC removal at a relatively high initial concentration (C₀ = 100 mg L−1) under visible-light (λ > 420 nm) without added oxidants. The optimized PET-CDs/Fe2O3 (0.4) reaches 98.2% TC removal. Kinetics follow a pseudo-first-order model, and blank tests confirm negligible photolysis and dark adsorption. The TOC and LC-MS results show rapid degradation followed by slower oxidation. Mineralization is substantial, with TOC decreasing from 100 to 34 mg L−1 at 4 h and reaching 89.6% removal at 10 h. The PET-CDs/Fe2O3 photocatalyst operates across pH 3–11. Phosphate reduces activity by competitive site blocking. At least 80% efficiency is retained over repeated cycles. Convergent evidence supports an S-scheme pathway rather than a type-II junction. DRS-Tauc analysis and band alignment indicate favorable energetic offsets and interfacial band bending. Steady-state PL shows selective quenching of PET-CDs emission with enhanced red Fe2O3 or interfacial emission. Transient photocurrent and EIS Nyquist plots reveal enhanced charge separation and reduced charge-transfer resistance. Scavenger tests and ESR identify h+ and •O2 as dominant species, with •OH secondary. LC-MS tracking shows early functional-group loss products at m/z 417 and 402, followed by lower-mass fragments (m/z 301–231 and 189–72), confirming stepwise oxidation toward mineralization.
将聚对苯二甲酸乙二醇酯衍生的碳点(PET-CDs)与Fe2O3相结合,制备了四环素(TC)脱除可见光PET-CDs/Fe2O3光催化剂。废弃PET瓶通过无过氧化物路线升级回收,实现无氧化剂操作。该光催化剂与均匀分散的Fe2O3纳米颗粒形成了富含缺陷的介孔碳点网络,增强了吸附和界面电荷传输。本研究表明,在可见光(λ >; 420 nm)下,在相对高的初始浓度(C 0 = 100 mg L−1)下,不添加氧化剂,可以有效地去除TC。优化后的PET-CDs/Fe2O3(0.4)的TC去除率达到98.2%。动力学遵循伪一级模型,空白试验证实可忽略光解和暗吸附。TOC和LC-MS结果显示,降解速度快,氧化速度慢。矿化效果显著,在4 h时TOC从100降低到34 mg L−1,在10 h时达到89.6%的去除率。PET-CDs/Fe2O3光催化剂在pH值 3-11范围内工作。磷酸盐通过竞争性位点阻断降低活性。在重复循环中至少保持80%的效率。趋同的证据支持s方案途径,而不是ii型连接。drs - tac分析和带对准表明有利的能量偏移和界面带弯曲。稳态PL显示出PET-CDs发射的选择性猝灭,红色Fe2O3或界面发射增强。瞬态光电流和EIS奈奎斯特图显示电荷分离增强和电荷转移电阻降低。清道夫试验和ESR鉴定h+和•O2−为优势种,•OH为次要种。LC-MS追踪显示,在m/z 417和402处有较早的官能团损失产物,其次是较低质量的碎片(m/z 301-231和189-72),证实了逐步氧化到成矿的过程。
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引用次数: 0
Organic acid tailors anhydrous magnesium carbonate: DFT-guided dehydration mechanism and morphology engineering 有机酸裁剪无水碳酸镁:dft引导脱水机理及形态工程
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-10 DOI: 10.1016/j.seppur.2026.137211
Yahui Feng , Jiajun Xu , Jie Xu , Li Gao , Bingxin Liu , Chao Zhang , Shiai Xu , Yunhua Lu
Mineral carbonation into Anhydrous Magnesium Carbonate (AMC) is a promising pathway for permanent CO₂ storage, yet the strong hydration of Mg2+ hinders its precipitation under mild conditions. To overcome this limitation, organic acids (l-ascorbic acid (LA), citric acid (CA), malic acid (MA), and tartaric acid (TA)) are employed as dual-functional agents: carbon sources and hydration disruptors. Through combined density functional theory (DFT) calculations and experimental validation, it is revealed that organic acids weaken the hydration shell of [Mg(H₂O)₆]2+ by forming stable coordination bonds with Mg2+, significantly reducing the dehydration energy barrier (e.g., ΔG₆-₅ decreased from 180.53 kJ/mol in H₂O to 76.71 kJ/mol for LA). Systematic hydrothermal synthesis demonstrates that LA enables high-purity AMC formation at 450 K, the widest temperature window among the tested acids. At the same time, TA requires ≥525 K. Crucially, each acid directs distinct AMC morphologies, hydrangea-like (LA), cubic (CA), layered (MA), and block-like (TA), attributed to site-specific adsorption on crystal surfaces. This work provides a molecular-level blueprint for overcoming the dehydration barrier in AMC synthesis and advances strategies for accelerating sustainable CO₂ mineralization.
矿物碳酸化成无水碳酸镁(AMC)是一种很有前途的永久CO₂储存途径,但Mg2+的强水化阻碍了其在温和条件下的沉淀。为了克服这一限制,有机酸(l-抗坏血酸(LA)、柠檬酸(CA)、苹果酸(MA)和酒石酸(TA))被用作双重功能剂:碳源和水合干扰物。通过组合密度泛函理论(DFT)计算和实验验证,揭示了有机酸通过与Mg2+形成稳定的配位键来削弱[Mg(H₂O)₆]2+的水化壳,显著降低脱水能垒(例如ΔG‡₆-₅从H₂O中的180.53 kJ/mol降低到LA中的76.71 kJ/mol)。系统水热合成表明,LA可以在450 K形成高纯度的AMC,这是所测试酸中最宽的温度窗口。同时,TA要求≥525k。至关重要的是,每种酸都能指导不同的AMC形态,如绣球状(LA)、立方状(CA)、层状(MA)和块状(TA),这归因于晶体表面上的位点特异性吸附。这项工作为克服AMC合成中的脱水障碍提供了分子水平的蓝图,并提出了加速可持续CO 2矿化的策略。
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引用次数: 0
Construction of hydrophilic PDMS/PEI gutter layer to fabricate ultrathin Pebax membrane for CO2 capture 构建亲水PDMS/PEI沟层制备超薄Pebax CO2捕集膜
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-05 DOI: 10.1016/j.seppur.2026.137170
Danjiao Shi, Kai Cheng, Meng Guo, Rong Xu, Tiandan Lu, Dongliang Jin, Shengshen Gu, Yang Pan, Jing Zhong
Polydimethylsiloxane (PDMS) is extensively utilized as a gutter layer in thin-film composite membranes (TFC) owing to its exceptional gas permeability and mechanical robustness. However, the hydrophilic modification of PDMS is necessary to ensure the uniform coating of selective layer materials containing polar groups on the hydrophobic PDMS gutter layer surface. Conventional hydrophilic treatment such as plasma treatment or UV irradiation produces transient Si-OH groups but require controlled atmosphere or chemical grafting to maintain sustained hydrophilicity. To address these challenges, the inverted interfacial polymerization (IP) process (aqueous phase upper/organic phase down) was designed to construct the PDMS-polyethyleneimine (PEI) interpenetration network (IPN), so as called IP-IPN strategy. The anchored PEI segments endowed PDMS surface with superior hydrophilicity as the water contact angle decreased from 110o to 67o and the hydrophilicity was retained over 7 days. The introduction of glycerol as the thickener contributed significantly to tuning the PEI-TMC crosslinking process and improved the gas permeance effectively. The hydrophilic-modified PDMS membrane retained 87.9% of its original CO2 permeance (9100 GPU). The permeance decline rate was much smaller than plasma treatment and UV irradiation which usually generate dense SiOx layer. When integrated with an ultrathin Pebax selective layer (∼30 nm), the composite membrane exhibited exceptional CO2/N2 separation performance (CO2 permeance: 2300 GPU; CO2/N2 selectivity: 31.5). This work offered a feasible pathway to achieve hydrophilic-modification of PDMS gutter layer, showing great potential in developing highly permeable membrane for efficient CO2 capture.
聚二甲基硅氧烷(PDMS)由于其优异的透气性和机械坚固性,被广泛用作薄膜复合膜(TFC)的沟槽层。然而,为了保证含有极性基团的选择性层材料均匀地涂覆在疏水性PDMS沟槽层表面,必须对PDMS进行亲水性改性。传统的亲水性处理,如等离子体处理或紫外线照射产生瞬态硅- oh基团,但需要控制气氛或化学接枝来维持持续的亲水性。为了解决这些问题,设计了倒置界面聚合(IP)工艺(水相上/有机相下)来构建pdms -聚乙烯亚胺(PEI)互渗透网络(IPN),即IP-IPN策略。当接触角从110°降低到670°时,锚定的PEI片段赋予PDMS表面优越的亲水性,亲水性可保持7天以上。甘油作为增稠剂的引入对PEI-TMC交联过程的调整有显著的作用,并有效地改善了气体的渗透性。亲水性改性的PDMS膜保留了其原始CO2透过率的87.9% (9100 GPU)。与等离子体处理和紫外线辐照相比,其渗透率下降幅度要小得多,而等离子体处理和紫外线辐照通常会产生致密的SiOx层。当与超薄Pebax选择层(~ 30 nm)集成时,复合膜表现出优异的CO2/N2分离性能(CO2透过率:2300 GPU; CO2/N2选择性:31.5)。本研究为实现PDMS沟层亲水性改性提供了一条可行的途径,在开发高效捕集CO2的高透膜方面具有很大的潜力。
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引用次数: 0
The improvement of selective removal of nitrate using reactive cationic surfactant modified activated carbon in capacitive deionization 活性阳离子表面活性剂改性活性炭在电容去离子中对硝酸盐选择性去除的改进
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-08 DOI: 10.1016/j.seppur.2026.137188
Yubo Zhao , Yingyun Li , Xiaofei Liu , Silu Huo , Jinfeng Fang , Rupeng Liu , Cuizhen Sun , Linxu Xu , Xue Shen , Shuying Geng , Jin Wang , Kexun Li
Nitrate (NO₃) pollution in aquatic environments is a global problem of increasing concern. Capacitive deionization (CDI) exhibits remarkable potential for NO₃ removal due to its advantages of cost-effectiveness and environmental benignity. However, traditional activated carbon (AC) suffers from low electrosorption capacity and poor NO₃ selectivity in the presence of coexisting anions (e.g., Cl). To address this challenge, this study proposes a new surface functionalization strategy using the reactive cationic surfactant. 3-chloro-2-hydroxypropyltrimethylammonium chloride (CHPTAC) was used as the representative to modify AC via covalent grafting, yielding RCS-functionalized AC (RCS-AC). Multiple material characterizations confirmed the successful incorporation of CHPTAC-derived groups onto the surface of AC, which not only reversed the inherent negative surface potential of AC but also notably improved its surface hydrophilicity. CDI experiments demonstrated that the covalent modification endowed RCS-AC with superior electrosorption performance compared to pristine AC while maintaining exceptional cyclic stability. In the single-component experiments, RCS-AC achieved a maximum NO₃ adsorption capacity of 20.58 mg/g at 1.8 V according to Langmuir isotherm model. A high NO3/Cl selectivity coefficient of 5.75 was also obtained for RCS-AC at 0.8 V and retained at 2.47 upon voltage elevation to 1.8 V in the brine-component experiments, in contrast to the non-selective behavior of pristine AC. Density functional theory (DFT) calculations revealed that the enhanced adsorption and selective recognition of RCS-AC for NO₃ was related to the multi-dimensional specific interactions between CHPTAC-derived groups and NO₃, including strengthened electrostatic attraction, directional hydrogen bonding, and partial covalent interaction. This work offers a simple yet stable approach to enhance NO₃ selectivity via RCS modification and provide experimental evidence for adaptability of RCS-AC in competitive ion environments.
水生环境中的硝酸盐(NO₃-)污染是一个日益受到关注的全球性问题。电容式去离子(CDI)由于其成本效益和环境友好的优点,在去除NO₃−方面表现出显著的潜力。然而,传统的活性炭(AC)在共存阴离子(例如Cl−)的存在下存在低电吸附能力和较差的NO₃-选择性。为了解决这一挑战,本研究提出了一种新的表面功能化策略,即使用活性阳离子表面活性剂。以3-氯-2-羟丙基三甲基氯化铵(CHPTAC)为代表,通过共价接枝改性AC,得到了rcs功能化AC (RCS-AC)。多种材料表征证实了chptac衍生基团在AC表面的成功结合,这不仅扭转了AC固有的负表面电位,而且显著提高了AC的表面亲水性。CDI实验表明,共价改性使RCS-AC具有比原始AC更好的电吸附性能,同时保持了优异的循环稳定性。在单组分实验中,根据Langmuir等温模型,RCS-AC在1.8 V下的最大NO₃-吸附量为20.58 mg/g。与原始AC的非选择性行为相比,RCS-AC在0.8 V时获得了5.75的NO3−/Cl−选择性系数,并且在盐水组分实验中保持在2.47的选择性系数。密度泛函数理论(DFT)计算表明,RCS-AC对NO₃−的增强吸附和选择性识别与chptac衍生基团与NO₃−之间的多维特异性相互作用有关。包括加强静电吸引、定向氢键和部分共价相互作用。这项工作提供了一种简单而稳定的方法来通过RCS修饰来增强NO₃-选择性,并为RCS- ac在竞争离子环境中的适应性提供了实验证据。
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引用次数: 0
Programmable hourglass nanochannels in thermally rearranged copolyimides for advanced gas separation 可编程沙漏纳米通道在热重排共聚物先进气体分离
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-04 DOI: 10.1016/j.seppur.2026.137141
Haodi Wang , Yu Zhang , Hesheng Li , Shuangjiang Luo , Xin Wei
A central challenge in developing thermally rearranged (TR) polymer membranes lies in navigating the complex interplay between polymer structure and performance, where achieving a synergistic combination of high gas permeability, selectivity, and mechanical strength through precursor design is non-trivial. To overcome this limitation, we designed a series of copolyimide precursors from 4,4′-(hexafluoroisopropylidene)diphthalic anhydride (6FDA), a bulky diamine (TFDB), and ortho-functionalized diamines with varied bridging units (p-HAB, BAS, 6FAP). We demonstrate that the synergistic combination of rigid, bulky segments and ortho-functional groups guides the formation of a unique “hourglass-shaped” multi-modal pore architecture upon thermal rearrangement, as directly evidenced by positron annihilation lifetime spectroscopy (PALS). This tailored nanostructure serves as molecular highways, concurrently enhancing gas transport pathways and molecular sieving capability. The resulting TR membrane (CoHPI-6FAP-450) thus achieves an exceptional combination of a CO2 permeability of ∼8000 Barrer and a CO2/CH4 selectivity of 22, surpassing the 2008 Robeson upper bound, while retaining a robust mechanical strength (>60 MPa). This work provides a definitive precursor design strategy for engineering multi-modal pore architectures, paving the way for high-performance TR membranes that reconcile the critical balance between separation performance and mechanical integrity.
开发热重排(TR)聚合物膜的核心挑战在于如何处理聚合物结构与性能之间复杂的相互作用,通过前驱体设计实现高透气性、选择性和机械强度的协同组合是非常重要的。为了克服这一限制,我们设计了一系列由4,4 ' -(六氟异丙基)二苯酐(6FDA),大体积二胺(TFDB)和具有不同桥接单元(p-HAB, BAS, 6FAP)的正官能化二胺组成的共聚亚胺前体。我们证明了刚性,大块段和正交官能团的协同组合在热重排时引导形成独特的“沙漏形”多模态孔隙结构,正电子湮灭寿命谱(PALS)直接证明了这一点。这种定制的纳米结构作为分子高速公路,同时增强了气体输送途径和分子筛分能力。因此,所得到的TR膜(CoHPI-6FAP-450)实现了CO2渗透率约8000 Barrer和CO2/CH4选择性22的卓越组合,超过了2008年Robeson上限,同时保持了强大的机械强度(60 MPa)。这项工作为工程多模态孔隙结构提供了明确的前体设计策略,为实现高性能TR膜在分离性能和机械完整性之间的关键平衡铺平了道路。
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引用次数: 0
Enriching trace protein peptides from extract liquid with foaming deep eutectic solvent (FDES)-loaded effervescent discs 用含泡沫深共溶溶剂(FDES)的泡腾盘富集萃取液中的微量蛋白肽
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-07 DOI: 10.1016/j.seppur.2026.137181
Xinlu Li , Yong Cao , Jie Tang , Yihan Zhao , Subhan Mahmood , Shun Yao
Snake shedding skin (snake molt) exhibits good potential for nutritional and functional applications, yet current methods for sustainable and efficient extraction of protein peptides from such an animal raw material are relatively limited. Herein, we reported novel foaming deep eutectic solvents (FDES) loaded effervescent discs for enriching target protein peptides in hydrolyzed extract of snake molt. Two kinds of natural sweeteners were used in the FDESs, which played an important role on foam stabilization and endowed FDESs with higher biocompatibility. After comprehensive characterizations, the discs exhibited good properties and expected forming performance. Under the ideal conditions, the effervescent discs enriched 91.40% protein peptides within 4 min, which was much higher than the alcohol precipitation method (40.12% within 3 d) and the aqueous two-phase system (80.67% within 1 h). Green assessment and scale-up experiments were also carried out for possible actual applications. Finally, the enriched product was analyzed by comprehensive physicochemical characterizations confirmed structural integrity and performance. The developed method offers a rapid, sustainable approach for obtaining peptides from natural products.
蛇蜕皮具有良好的营养和功能应用潜力,但目前从这种动物原料中可持续和有效地提取蛋白质肽的方法相对有限。在此,我们报道了一种新型的泡沫深共晶溶剂(FDES)装载泡沫盘,用于富集蛇蜕皮水解提取物中的目标蛋白肽。在FDESs中加入了两种天然甜味剂,这两种甜味剂在泡沫稳定方面发挥了重要作用,使FDESs具有较高的生物相容性。经过综合表征,该圆盘具有良好的性能和预期的成形性能。在理想条件下,泡腾盘在4 min内富集了91.40%的蛋白肽,远高于醇沉法(3 d内富集40.12%)和水两相体系(1 h内富集80.67%)。对可能的实际应用进行了绿色评估和规模试验。最后对富集产物进行了综合理化表征,确定了富集产物的结构完整性和性能。所开发的方法为从天然产物中获得多肽提供了一种快速、可持续的方法。
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引用次数: 0
Nanoporous fibrous 3D solar evaporator for efficient freshwater generation and salt recovery 用于高效淡水生成和盐回收的纳米多孔纤维三维太阳能蒸发器
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-04 DOI: 10.1016/j.seppur.2026.137162
Mojtaba Ebrahimian Mashhadi, Md. Mehadi Hassan, Ningxin Chen, Ruijie Yang, Qingye Lu
Solar-driven interfacial evaporators (SDIEs) have advanced sustainable desalination by enabling freshwater production and salt harvesting from brines. Here, electrospun cellulose acetate (CA) films with aligned nanoporous fibers are rolled into a 3D cylinder and partially coated with a carbon black/poly(vinyl alcohol) (CB/PVA) photothermal layer to create an environmentally-friendly SDIE for concurrent desalination and salt recovery. The evaporator achieves a high evaporation rate of 4.44 kg m−2 h−1 under 1 sun, corresponding to a photothermal conversion efficiency of 107.3% based on equivalent evaporation enthalpy. This performance is ascribed to reduced vaporization enthalpy from material-water interactions and nanoporous structures, along with cold evaporation-induced environmental energy harvesting. Under 1 sun, the SDIE stably treats brines of 3.5–20 wt% salinity with edge-preferential salt crystallization due to its fibrous microporous architecture. This feature allows gravity-assisted salt collection and durable function in 10 wt% NaCl for 10 days, maintaining average steam generation and salt harvesting rates of 4.71 kg m−2 h−1 and 3.21 kg m−2 day−1, respectively. Condensed waters from 3.5 wt% NaCl and simulated seawater exhibit high purity with significantly lower conductivities. The outdoor experiment also reveals the stable performance of the SDIE under actual conditions. Computational fluid dynamics (CFD) simulation further validates edge-preferential salt aggregation. This innovative device offers a promising route for simultaneous freshwater and salt collection from brines.
太阳能驱动的界面蒸发器(SDIEs)通过实现淡水生产和从盐水中收集盐,推动了可持续的海水淡化。在这里,电纺醋酸纤维素(CA)薄膜与排列整齐的纳米多孔纤维被卷成一个3D圆柱体,并部分涂上炭黑/聚乙烯醇(CB/PVA)光热层,以创建一个环保的SDIE,用于同时脱盐和盐回收。蒸发器在1个太阳下的蒸发速率高达4.44 kg m−2 h−1,根据等效蒸发焓计算,光热转换效率为107.3%。这种性能归因于材料-水相互作用和纳米孔结构的蒸发焓降低,以及冷蒸发引起的环境能量收集。在1个太阳下,由于其纤维微孔结构,SDIE稳定地处理盐度为3.5 - 20%的盐水,并具有边缘优先的盐结晶。该功能允许重力辅助盐收集和在10 wt% NaCl中持续10天,保持平均蒸汽产生和盐收集率分别为4.71 kg m−2 h−1和3.21 kg m−2 day−1。3.5 wt% NaCl和模拟海水的凝结水纯度高,电导率明显降低。室外实验也显示了SDIE在实际条件下的稳定性能。计算流体动力学(CFD)模拟进一步验证了边缘优先的盐聚集。这种创新的设备为同时从盐水中收集淡水和盐提供了一条有前途的途径。
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引用次数: 0
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Separation and Purification Technology
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