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3D/4D Printing. 三维/四维印刷。
Pub Date : 2025-12-19 eCollection Date: 2026-01-22 DOI: 10.1021/cbe.5c00152
Tao Xie
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引用次数: 0
In Situ Incorporation of Macromolecules in Zr-MOF Membranes for Separation of Organic Azeotropic Mixtures. 大分子在Zr-MOF膜中的原位掺入用于有机共沸混合物的分离。
Pub Date : 2025-12-16 eCollection Date: 2026-01-22 DOI: 10.1021/cbe.5c00112
Lianhao Li, Binyu Mo, Renjie Miao, Wenqi Ji, Haonan Yang, Guozhen Liu, Gongping Liu, Wanqin Jin

Metal-organic framework (MOF) membranes with adjustable angstrom-scale channels and versatile topological structures are promising for molecular separation. However, it remains a challenge to construct MOF membranes with precisely tuned pore sizes and tailored molecular affinity for achieving high-efficiency liquid molecular separation, particularly for organic azeotropic mixtures. Herein, we proposed an in situ macromolecule incorporation strategy to fabricate a Zr-MOF membrane with a tunable pore microenvironment for pervaporation separation of butanol-water and ethanol-ethyl acetate azeotropic mixtures. The membranes were prepared by an in situ interfacial growth process. The amino macromolecules (poly-(ether imide), PEI) were dispersed into a metal cluster solution, followed by coordination with ligands on the substrate surface for membrane synthesis, wherein the macromolecule was in situ incorporated within MOF pore apertures. The incorporated macromolecule narrowed the membrane pore size and provided molecularly accelerated transport sites, thus facilitating the fast and selective transport of water or ethanol molecules. When incorporating PEI (M W = 10,000 g·mol-1) at a content of 1 wt %, the resulting MOF membrane displayed excellent separation performances with a total flux of 2.22 kg·m-2·h-1 and a separation factor of 140 for the ethanol-ethyl acetate system, and a total flux of 8.52 kg·m-2·h-1 and a separation factor of 1620 for the butanol-water system, outperforming the performance of state-of-the-art membranes. The proposed macromolecule-incorporated angstrom-sized channels demonstrate considerable potential for broad application in other fields, e.g., single-atom catalysis, sensing, and energy conversion.

具有可调埃级通道和多用途拓扑结构的金属有机骨架(MOF)膜在分子分离中具有广阔的应用前景。然而,构建具有精确调节孔径和定制分子亲和力的MOF膜以实现高效的液体分子分离仍然是一个挑战,特别是对于有机共沸混合物。在此,我们提出了一种原位大分子掺入策略来制备具有可调孔微环境的Zr-MOF膜,用于丁醇-水和乙醇-乙酸乙酯共沸混合物的渗透蒸发分离。采用原位界面生长法制备了膜。将氨基大分子(聚醚亚胺,PEI)分散到金属簇溶液中,然后与底物表面的配体配位进行膜合成,其中大分子在MOF孔径内原位结合。掺入的大分子使膜孔径变窄,提供了分子加速转运位点,从而促进了水或乙醇分子的快速和选择性转运。当加入浓度为1 wt %的PEI (M W = 10,000 g·mol-1)时,所制得的MOF膜表现出优异的分离性能,乙醇-乙酸乙酯体系的总通量为2.22 kg·M -2·h-1,分离因子为140,丁醇-水体系的总通量为8.52 kg·M -2·h-1,分离因子为1620,优于现有膜的性能。所提出的大分子结合的埃级通道在其他领域具有广泛的应用潜力,例如单原子催化、传感和能量转换。
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引用次数: 0
Molecularly Imprinted Membranes for Selective Biomarker Recognition: Recent Advances and Emerging Strategies. 分子印迹膜选择性生物标志物识别:最新进展和新兴策略。
Pub Date : 2025-11-18 eCollection Date: 2025-12-25 DOI: 10.1021/cbe.5c00056
Qingmei Song, Kelly Van Van, Xinhao Li, Ziman Chen, Yongqin Lv

Molecularly imprinted membranes (MIMs) epitomize the convergence of membrane science with molecular imprinted technology. Endowed with intrinsic molecular recognition and memory functionalities, MIMs have the potential to evolve into pivotal tools for the selective separation, identification, and purification of biomolecules. This review summarizes the forefront advancements in the selective recognition and separation of macromolecular biomarkers through MIMs, such as proteins, peptides, and nucleotides. A comprehensive overview of diverse imprinting polymerization methodologies employed in crafting MIMs tailored for specific biomacromolecule targets is presented. Additionally, the evolving research landscape concerning MIMs as a potent platform for the targeted capture of biomacromolecule-associated biomarkers is critically appraised and is discussed.

分子印迹膜是膜科学与分子印迹技术的结合。mim具有固有的分子识别和记忆功能,有可能发展成为生物分子选择性分离、鉴定和纯化的关键工具。本文综述了通过mim选择性识别和分离大分子生物标志物(如蛋白质、肽和核苷酸)的最新进展。全面概述了不同的印迹聚合方法在制作为特定的生物大分子目标量身定制的MIMs被提出。此外,关于mim作为靶向捕获生物大分子相关生物标志物的有力平台的不断发展的研究前景进行了严格的评估和讨论。
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引用次数: 0
Coarse-Grained Modeling and Simulation of Multistranded RNA Nanostars. 多链RNA纳米星的粗粒度建模与模拟。
Pub Date : 2025-11-03 eCollection Date: 2026-01-22 DOI: 10.1021/cbe.5c00093
Pradnya R Kadam, Justine Lim, Mahdi Dizani, Jaimie Marie Stewart

Biomolecular condensates are dynamic, membraneless compartments that emerge through phase separation of specific proteins and nucleic acids, regulating key biochemical processes within cells. Inspired by these natural systems, we recently developed a modular platform for engineering synthetic ribonucleic acid (RNA) condensates using a multistranded branched RNA motif, termed a nanostar. Here, we employ coarse-grained modeling and molecular dynamics (MD) simulations using the oxRNA2 platform to quantify conformational dynamics of 3-, 4-, and 5-arm nanostars. We define flexibility as the standard deviation of interarm angle distributions and geometry as the mean interarm angle. Across valencies at 37 °C and 0.15 M monovalent salts (NaCl), increasing the arm number reduces the mean angle as expected from geometry, while the dispersion of interarm angles remains comparable, indicating similar flexibility. Salt increases the mean angle in 4- and 5-arm nanostars and increases the temperature dependence of interarm angles. In contrast, the 3-arm nanostar is largely unaffected by salt and temperature over the studied ranges. Lastly, at 1.0 M salt and 37 °C, DNA nanostars adopt larger mean angles compared to RNA nanostars across all valencies, suggesting that backbone chemistry shifts preferred geometry more than it broadens fluctuations. These results illuminate how valency, salt, and temperature differentially control geometry versus flexibility, informing the design of synthetic RNA nanostars and thus condensates with predictable material responses.

生物分子凝聚体是动态的、无膜的隔室,通过特定蛋白质和核酸的相分离出现,调节细胞内的关键生化过程。受这些自然系统的启发,我们最近开发了一个模块化平台,用于工程合成核糖核酸(RNA)凝聚物,使用多链分支RNA基序,称为纳米星。在这里,我们采用粗粒度建模和分子动力学(MD)模拟,使用oxRNA2平台来量化3、4和5臂纳米星的构象动力学。我们将柔性定义为臂间角分布的标准差,几何定义为臂间角的平均。在37°C和0.15 M的一价盐(NaCl)中,增加臂数可以降低几何角度的平均值,而臂间角的分散保持相当,表明类似的灵活性。盐增加了4臂和5臂纳米星的平均角,增加了臂间角的温度依赖性。相比之下,3臂纳米星在研究范围内基本上不受盐和温度的影响。最后,在1.0 M盐和37°C下,与RNA纳米星相比,DNA纳米星在所有价态上采用更大的平均角度,这表明主链化学改变了首选的几何形状,而不是扩大了波动。这些结果阐明了价、盐和温度的差异如何控制几何形状与灵活性,为合成RNA纳米星的设计提供了信息,从而使凝聚物具有可预测的材料响应。
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引用次数: 0
600 Wh kg-1 Lithium Batteries Unlocked by Polymer Electrolytes. 聚合物电解质解锁600wh kg-1锂电池。
Pub Date : 2025-10-26 eCollection Date: 2025-12-25 DOI: 10.1021/cbe.5c00127
Ruhong Li, Xiulin Fan
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引用次数: 0
Supervised-Learning-Driven Interrogation of Organ-on-a-Chip Quality from Microscopy Images. 显微镜图像中器官芯片质量的监督学习驱动询问。
Pub Date : 2025-10-24 eCollection Date: 2025-12-25 DOI: 10.1021/cbe.5c00087
Rose Mary George, Kenry

We leverage supervised learning to realize high-throughput and objective interrogation of organ-on-a-chip quality from microscopy images. More than 600 images of two lung-related cell types in good and bad quality lung-on-a-chip models are assessed. We demonstrate that trained classifiers can predict different cell types and lung-on-a-chip quality with AUC and accuracy of above 95% and 83%, respectively. Coupled with a dimensionality reduction approach, the predictive capacity of certain classifiers can be enhanced, while the computational cost of resource-intensive algorithms can be significantly reduced. This study is anticipated to further encourage the implementation of machine learning for automating organ-on-a-chip development.

我们利用监督学习来实现对显微镜图像中器官芯片质量的高通量和客观的询问。对两种肺相关细胞类型的600多张图像进行了评估,这些图像的质量有好有坏。我们证明,经过训练的分类器可以预测不同的细胞类型和肺片质量,AUC和准确率分别超过95%和83%。结合降维方法,可以增强某些分类器的预测能力,同时可以显著降低资源密集型算法的计算成本。这项研究预计将进一步鼓励机器学习在自动化器官芯片开发中的应用。
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引用次数: 0
Scalable Room-Temperature Synthesis of the Ultramicroporous Metal-Organic Framework for Separation of the C2H6/ C2H4 Mixture. 用于分离C2H6/ C2H4混合物的超微孔金属-有机骨架的可扩展室温合成
Pub Date : 2025-10-09 eCollection Date: 2025-11-27 DOI: 10.1021/cbe.5c00063
Yu Zhang, Ting Wang, Xia Li, Hongxia Ren, Peng Zhao, Shubo Geng, Zhenjie Zhang

Ethylene (C2H4) is a vital industrial chemical with a growing market, similarly produced through the steam cracking of hydrocarbons, such as ethane (C2H6). However, separating C2H4 from a C2H6 and C2H4 mixture remains challenging due to their similar molecular sizes and boiling points, necessitating highly energy-intensive processes such as cryogenic distillation. This study introduces two ultramicroporous metal-organic frameworks (MOFs), NKMOF-17-Co and NKMOF-17-Cu, synthesized rapidly under ambient conditions as efficient materials for C2H6/C2H4 separation via physical adsorption. Gas adsorption experiments reveal that NKMOF-17-Co and -Cu exhibit a preference for adsorbing C2H6 over C2H4. Determined by these single crystal structures of loading gases into NKMOF-17-Co and -Cu, stronger hydrogen bonding and C-H···π interactions between C2H6 and MOFs were confirmed clearly. Verified by breakthrough tests of a C2H6 and C2H4 mixture for NKMOF-17-Co and -Cu, C2H4 was obtained in high purity (>99.96%). NKMOF-17-Co and -Cu were regenerated with low energy requirements and showed stable performance under repeated cycling tests. These findings suggest that NKMOF-17-Co and -Cu hold great promise for energy-efficient separation processes in the industrial separation of C2H6 and C2H4.

乙烯(C2H4)是一种重要的工业化学品,市场日益增长,同样是通过蒸汽裂解碳氢化合物(如乙烷(C2H6))生产的。然而,从C2H6和C2H4混合物中分离C2H4仍然具有挑战性,因为它们的分子大小和沸点相似,需要高能量密集型的过程,如低温蒸馏。本文介绍了两种超微孔金属有机骨架(mof), NKMOF-17-Co和NKMOF-17-Cu,作为物理吸附分离C2H6/C2H4的高效材料。气体吸附实验表明,NKMOF-17-Co和-Cu对C2H6的吸附优于C2H4。通过NKMOF-17-Co和-Cu加载气体的单晶结构,可以清楚地证实C2H6与mof之间存在更强的氢键和C-H··π相互作用。对NKMOF-17-Co和-Cu的C2H6和C2H4混合物进行了突破试验,得到了高纯度的C2H4(>99.96%)。NKMOF-17-Co和-Cu的再生能量要求低,在反复循环试验中表现出稳定的性能。这些发现表明NKMOF-17-Co和-Cu在C2H6和C2H4的工业分离中具有很大的节能前景。
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引用次数: 0
Visual Assessment of Methane Hydrate Dissociation Using a Multi-Rocking Cell: Roles of Surfactants, KHIs, and AAs in Water-Rich Systems. 多摇池对甲烷水合物解离的视觉评价:表面活性剂、KHIs和AAs在富水系统中的作用。
Pub Date : 2025-10-07 eCollection Date: 2026-01-22 DOI: 10.1021/cbe.5c00067
Sanehiro Muromachi, Michihiro Muraoka, Satoshi Takeya, Yoshihiro Konno, Kiyofumi Suzuki, Norio Tenma

This study uses a new multi-rocking cell system for visual, parallel assessment of methane hydrate (MH) dissociation. The method allows for systematic comparison of various fluidizerscomposed of thermodynamic hydrate inhibitors like urea and additives including surfactants, kinetic hydrate inhibitors, and antiagglomerantsunder controlled, water-rich conditions. Our findings show that surfactants, such as SDS, SO, and DDBSA, accelerate dissociation but cause MH migration and persistent foaming. In contrast, DTMAC and saponin effectively promote dissociation while suppressing foam and MH migration. Combination fluidizers (e.g., SDS + PVP, SDS + Tween 80) further fine-tuned the performance, demonstrating additive-specific effects such as foam suppression or accelerated dissociation. This work provides insights for designing effective fluidizers for hydrate management in subsea production environments.

本研究使用了一种新的多摇池系统,用于甲烷水合物(MH)解离的视觉并行评估。该方法允许在受控的富水条件下,系统地比较由尿素等热力学水合物抑制剂和添加剂(包括表面活性剂、动力学水合物抑制剂和抗团聚剂)组成的各种流化器。我们的研究结果表明,表面活性剂,如SDS, SO和DDBSA,加速解离,但导致MH迁移和持续发泡。相比之下,DTMAC和皂苷能有效地促进解离,抑制泡沫和MH迁移。组合流态器(例如,SDS + PVP, SDS + Tween 80)进一步微调了性能,展示了添加剂的特定效果,如泡沫抑制或加速解离。这项工作为在海底生产环境中设计有效的水合物管理流化器提供了见解。
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引用次数: 0
Photothermally Enhanced Electrocatalytic Water Splitting for Hydrogen Production. 光热强化电催化水裂解制氢研究。
Pub Date : 2025-10-03 eCollection Date: 2026-01-22 DOI: 10.1021/cbe.5c00075
Zeyu He, Junchao Huang, Dong Wei, Huibing He, Boran Wang, Jing Xu

Hydrogen energy is a promising solution to global energy and environmental challenges. Water electrolysis is a green technology for hydrogen production, but its efficiency is limited by the electrocatalytic performance of the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER). Elevating the temperature of the electrolysis system is effective in accelerating the electrocatalytic efficiency. However, conventional heating methods often increase the system complexity and energy consumption. The photothermal effect, where a substance generates heat upon light absorption, enables localized heating, improves energy utilization, and offers a promising strategy to enhance electrolyzer performance. Here, recent advances in photothermally enhanced electrocatalytic water splitting for hydrogen production are comprehensively reviewed. We elucidate the mechanisms of electrocatalytic water splitting and photothermal effects, with particular emphasis on the multiscale mechanisms of photoenhanced electrocatalysis that integrate nanoscale localized heating, hot-carrier generation, interfacial restructuring, and system-level modulation to collectively accelerate the HER and OER. We have systematically introduced recent advances in the design of photothermally enhanced electrocatalysts, specifically in the HER, OER, and various anode alternative reactions. This review also introduces representative designs of photothermally enhanced electrolyzers. By conducting a comparative economic analysis of various electrolyzers, this review demonstrates the significant economic benefits of photothermally enhanced water electrolysis for hydrogen production. We also provide a perspective on the future research direction of photothermally enhanced electrocatalytic hydrogen production. This review will inspire future endeavors toward realizing highly efficient, energy-saving, and cost-effective hydrogen production systems.

氢能是解决全球能源和环境挑战的一个有前途的解决方案。水电解是一种绿色制氢技术,但其效率受到析氢反应(HER)和析氧反应(OER)电催化性能的限制。提高电解系统温度对提高电催化效率是有效的。然而,传统的加热方式往往增加了系统的复杂性和能源消耗。光热效应,即物质在吸收光后产生热量,可以局部加热,提高能量利用率,并为提高电解槽性能提供了一个有前途的策略。本文综述了光热强化电催化水裂解制氢技术的最新进展。我们阐明了电催化水分解和光热效应的机制,特别强调了光增强电催化的多尺度机制,包括纳米尺度局部加热、热载流子生成、界面重组和系统级调制,以共同加速HER和OER。我们系统地介绍了光热增强电催化剂设计的最新进展,特别是在HER, OER和各种阳极替代反应中。本文还介绍了具有代表性的光热强化电解槽设计。通过对各种电解槽的经济比较分析,本文论证了光热强化电解制氢的显著经济效益。展望了光热强化电催化制氢的未来研究方向。这一综述将激励未来的努力,以实现高效,节能和成本效益的制氢系统。
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引用次数: 0
Metabolic Engineering of Saccharomyces cerevisiae for the Efficient Production of Human Milk Oligosaccharide, Lacto‑N‑neotetraose (LNnT). 高效生产人乳低聚糖乳酸- N -新四糖(LNnT)的酿酒酵母代谢工程
Pub Date : 2025-09-26 eCollection Date: 2026-01-22 DOI: 10.1021/cbe.5c00070
Nitesh Kumar Mund, Jialun Gao, Bo Sun, Muqiang Wang, Lirong Yang, Jianping Wu, Hao Fang, Haoran Yu

Lacto-N-neotetraose (LNnT) is one of the important ingredients of human milk oligosaccharides, with various promising health effects for infants. In this study, the biosynthetic pathway of LNnT was constituted in GRAS (generally recognized as safe) host Saccharomyces cerevisiae by coexpressing β1,3-N-acetylglucosaminyltransferase (LgtA), β1,4-galactosyltransferase (LgtB), lactose permease (Lac12), and UDP galactose 4-epimerase (Gal10). The engineered yeast strain designated LN1, coexpressing all these enzymes, achieved an LNnT production level of 1.54 g/L. To further enhance LNnT yield, the flux through the pathway was improved by employing both protein fusion and modular assembly strategies. The assembly of LgtA and LgtB using short peptide tags resulted in a significant increase in LNnT titers, reaching 2.42 g/L. Finally, the LNnT titer reached 6.25 g/L under fed-batch fermentation conditions in a 500 mL flask, representing the highest reported production level of LNnT in S. cerevisiae to date.

乳酸-n -新四糖(LNnT)是人乳低聚糖的重要成分之一,对婴儿具有多种有益的保健作用。本研究通过在GRAS(公认安全的)宿主酿酒酵母中共表达β1,3- n -乙酰氨基葡萄糖转移酶(LgtA)、β1,4-半乳糖转移酶(LgtB)、乳糖渗透酶(Lac12)和UDP半乳糖4- epimase (Gal10),构建了LNnT的生物合成途径。共表达所有这些酶的工程酵母菌株LN1的LNnT产量达到1.54 g/L。为了进一步提高LNnT的产率,通过采用蛋白质融合和模块化组装策略来提高途径的通量。利用短肽标签组装LgtA和LgtB导致LNnT滴度显著增加,达到2.42 g/L。最后,在500 mL烧瓶中分批补料发酵条件下,LNnT滴度达到6.25 g/L,这是迄今为止报道的酿酒酵母中LNnT的最高生产水平。
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引用次数: 0
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