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Toughening poly(lactic acid) with novel polyolefin-graft-poly(lactic acid) copolymers maintaining high transparency and stiffness 用新型聚烯烃-接枝-聚(乳酸)共聚物增韧聚(乳酸),保持高透明度和硬度
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-29 DOI: 10.1016/j.giant.2024.100274
Hao Cai , Yu Cheng , Zhenli Zhang , Li Pan , Kunyu Zhang , Yuesheng Li

The combination of well-balanced mechanical performance, high transparency and appealing eco-friendly attributes endows poly(lactic acid) (PLA) with significantly potential for wide-ranging applications in high-value packaging sectors. However, effectively toughening PLA without compromising its transparency and stiffness remains a formidable challenge. In this study, we synthesized a series of graft copolymers by incorporating hydroxyl-functionalized linear low density polyethylene (LLDPEOH) and copolymers of cycloolefin (COCOH) as the main chain and PLA as the side chain, which were subsequently employed as novel toughening agents for commercial PLA. The achievement of high-performance PLA blends with a balanced combination of toughness, strength, and transparency can be realized through meticulous tuning of the structure and mass fraction of the blended graft copolymers. The maximum elongation at break for the PLA blends increased by about 50 times that of neat PLA, reaching up to 300 %. Furthermore, these materials retained their high strength (54 MPa) and excellent transparency (light transmittance up to 90 %). The excellent properties of PLA blends could be ascribed to the well-designed chain structure of the graft copolymer which leaded to and excellent compatibility with the PLA matrix and unique phase morphology. This work is significant in guiding the design and synthesis of graft copolymers as toughening agents for PLA, thereby expanding its application range in areas where high transparency and toughness are required.

聚乳酸(PLA)兼具均衡的机械性能、高透明度和吸引人的环保特性,在高价值包装领域具有广泛的应用潜力。然而,如何在不影响聚乳酸透明度和刚度的前提下有效增韧聚乳酸仍是一项艰巨的挑战。在本研究中,我们以羟基官能化线性低密度聚乙烯(LLDPEOH)和环烯烃(COCOH)共聚物为主链,聚乳酸为侧链,合成了一系列接枝共聚物,随后将其用作商用聚乳酸的新型增韧剂。通过精心调整混合接枝共聚物的结构和质量分数,可以获得兼顾韧性、强度和透明度的高性能聚乳酸混合物。聚乳酸共混物的最大断裂伸长率是纯聚乳酸的 50 倍,最高可达 300%。此外,这些材料还保持了高强度(54 兆帕)和出色的透明度(透光率高达 90%)。聚乳酸共混物的优异性能可归因于接枝共聚物精心设计的链结构,它与聚乳酸基体具有良好的兼容性和独特的相形态。这项研究成果对设计和合成作为聚乳酸增韧剂的接枝共聚物具有重要指导意义,从而扩大了聚乳酸在要求高透明度和高韧性领域的应用范围。
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引用次数: 0
Hydrogel Nanocomposite Based Slow-Release Urea Fertilizer: Formulation, Structure, and Release Behavior 基于水凝胶纳米复合材料的缓释尿素肥料:配方、结构和释放行为
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-27 DOI: 10.1016/j.giant.2024.100270
Kezhu Lu , Ragab Abouzeid , Qinglin Wu , Qibing Chen , Shiliang Liu

To enhance the nitrogen utilization efficiency of fertilizers, we developed a novel slow-release fertilizer hydrogel through free radical polymerization, incorporating lignin-containing cellulose nanofiber (LCNF), clinoptilolite (CL), urea, and acrylic acid (AA)-co-acrylamide (AAm) polymer. Various analytical techniques were utilized to examine the structure, swelling, and release behaviors of the fabricated hydrogels with varying LCNF concentrations. The results indicated that the addition of 10% LCNF led to a decrease in water absorption from 72.44 g g−1 to 24.04 g g−1. However, re-swelling was significantly enhanced, with a reduction in re-swelling capacity loss from 32.91% to 23.52%. Concurrently, water retention capacity notably increased from 18.03% to 39.20%. The hydrogel containing 10% LCNF exhibited a slower urea release over 30 days. The kinetic studies revealed that the swelling and urea release behaviors align well with the second-order kinetics model and the Peppas-Sahlin model, respectively. In summary, the developed LCNF/CL/(AA-co-AAm)/urea hydrogel nanocomposites present a novel strategy for the future production and utilization of slow-release fertilizers in agricultural and horticultural fields.

为了提高肥料的氮利用效率,我们通过自由基聚合技术,将含木质素的纤维素纳米纤维(LCNF)、clinoptilolite(CL)、尿素和丙烯酸(AA)-共丙烯酰胺(AAm)聚合物结合在一起,开发了一种新型缓释肥料水凝胶。利用各种分析技术检测了不同浓度 LCNF 制成的水凝胶的结构、溶胀和释放行为。结果表明,添加 10% LCNF 后,吸水率从 72.44 g g-1 降至 24.04 g g-1。不过,再膨胀能力明显增强,再膨胀能力损失从 32.91% 降至 23.52%。同时,保水能力从 18.03% 显著提高到 39.20%。含有 10% LCNF 的水凝胶在 30 天内的尿素释放速度较慢。动力学研究表明,溶胀和尿素释放行为分别符合二阶动力学模型和 Peppas-Sahlin 模型。总之,所开发的 LCNF/CL/(AA-co-AAm)/尿素水凝胶纳米复合材料为未来在农业和园艺领域生产和使用缓释肥料提供了一种新策略。
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引用次数: 0
A Discotic Mesogenic near-infrared absorbing dye and its application in photo-responsive liquid crystal elastomers 一种 Discotic Mesogenic 近红外吸收染料及其在光响应液晶弹性体中的应用
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-26 DOI: 10.1016/j.giant.2024.100271
Shimin Shao , Miao Bao , Ruohan Chen , Zhenghao Zhang , Haifeng Lu , Meng Wang , Hong Yang

Near-infrared (NIR) light-responsive liquid crystal elastomers (LCEs) doped with organic small-molecule photothermal agents have garnered scientific attention. However, the challenge remains in designing and synthesizing mesogenic photothermal dyes with absorption wavelengths greater than 800 nm. In this research, we design a novel discotic mesogenic NIR absorbing dye, namely the nickel bis(dithiolene) complex YHD868, and prepare NIR-responsive LCE/YHD868 composite films. The discotic mesogenic molecule YHD868 possesses a columnar hexagonal mesophase and exhibits intense NIR absorption at 868 nm, with a photothermal conversion efficiency of about 27 % and a molar extinction coefficient of approximately 30000 M−1·cm−1. Due to the strong NIR absorption of YHD868, combined with its excellent photothermal stability, the LCE/YHD868 composite films exhibit remarkable photoresponse and mechanical properties. Even at a low doping concentration of 0.2 wt%, the composite film can achieve a tensile strength of 9.8 MPa and an elongation at break of 165 %. Under 880 nm NIR irradiation (3.3 W·cm−2), the film can complete reversible photo-induced shrinking deformation in just 2 s, with a shrinkage ratio of about 64 %. This work offers a new approach for the development of photo-responsive smart soft materials.

掺杂有机小分子光热剂的近红外(NIR)光响应液晶弹性体(LCE)已引起科学界的关注。然而,设计和合成吸收波长大于 800 纳米的介导型光热染料仍是一项挑战。在这项研究中,我们设计了一种新型盘状介原近红外吸收染料,即双二硫代二亚硝基镍络合物 YHD868,并制备了近红外响应型 LCE/YHD868 复合薄膜。盘状介原分子 YHD868 具有柱状六方介相,在 868 纳米波长处表现出强烈的近红外吸收,光热转换效率约为 27%,摩尔消光系数约为 30000 M-1-cm-1。由于 YHD868 具有很强的近红外吸收能力,再加上其出色的光热稳定性,LCE/YHD868 复合薄膜表现出卓越的光响应和机械性能。即使在 0.2 wt% 的低掺杂浓度下,复合薄膜也能达到 9.8 MPa 的拉伸强度和 165 % 的断裂伸长率。在 880 纳米近红外辐照(3.3 W-cm-2)下,薄膜可在短短 2 秒内完成可逆的光诱导收缩变形,收缩率约为 64%。这项研究为开发光响应智能软材料提供了一种新方法。
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引用次数: 0
Multifunctional ultraflexible neural probe for wireless optogenetics and electrophysiology 用于无线光遗传学和电生理学的多功能超灵活神经探针
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-26 DOI: 10.1016/j.giant.2024.100272
Suhao Wang , Lixuan Li , Shun Zhang , Qianqian Jiang , Pengxian Li , Chengjun Wang , Rui Xiao , Xiao-Ming Li , Jizhou Song

Electrophysiology and optogenetics are pivotal in neuroscience for probing and modulating neural activities, playing a vital role in unraveling the complexities of brain functionality. Despite their importance, the efficacy of existing devices is hampered by insufficient functional integration, pronounced foreign body reactions, and physical constraints that impede natural animal behaviors. Here, we develop a multifunctional, ultraflexible neural probe designed for simultaneous electrophysiological monitoring and optical neural modulation, along with mechanical properties that are conducive to flexibility and compliance. By integrating a wireless neural signal acquisition and stimulation circuit, we achieved wireless recording of brain signals in mice and wireless optogenetic control over their locomotor behavior. The multifunctional ultraflexible probe presented in this study holds substantial promise for closed-loop brain-machine interfaces and deepening our understanding of neural circuit functions. This innovative approach addresses the aforementioned limitations by a comprehensive solution for in vivo neural interrogation and manipulation, marking a significant advancement in the tools available for neuroscience research.

电生理学和光遗传学是神经科学中探测和调节神经活动的关键,在揭示大脑功能的复杂性方面发挥着至关重要的作用。尽管它们非常重要,但现有装置的功效却因功能整合不足、异物反应明显以及阻碍动物自然行为的物理限制而受到影响。在这里,我们开发了一种多功能、超柔性神经探针,可同时进行电生理监测和光学神经调制,并具有有利于灵活性和顺应性的机械特性。通过集成无线神经信号采集和刺激电路,我们实现了对小鼠大脑信号的无线记录和对其运动行为的无线光遗传控制。本研究中展示的多功能超柔性探针在闭环脑机接口和加深我们对神经回路功能的理解方面大有可为。这种创新方法解决了上述局限性,为体内神经检查和操作提供了全面的解决方案,标志着神经科学研究工具的重大进步。
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引用次数: 0
Ecological packaging: Creating sustainable solutions with all-natural biodegradable cellulose materials 生态包装:利用全天然可生物降解纤维素材料创造可持续解决方案
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-25 DOI: 10.1016/j.giant.2024.100269
Yijia Deng , Shaofeng Wu , Tianxue Zhu , Yukui Gou , Yan Cheng , Xiao Li , Jianying Huang , Yuekun Lai

Plastics, accumulating globally as microplastics in living organisms, significantly contribute to environmental issues. Current materials like polylactic acid and commercial paper face limitations due to inadequate heat and water resistance, resulting in various practical inconveniences. This study reports a high-strength, water-resistant, recyclable, and naturally degradable pure cellulose food packaging material, which is crafted from bacterial cellulose (BC) and ethyl cellulose (EC) by a straightforward filtration and scratch coating process. The use of the EC ethanol solution eliminates the need for additional binders. Remarkably, the EC-BC pure cellulose material exhibits excellent mechanical properties (tensile strength of 195.3 ± 23.2 MPa), a stability in liquid environments (136.9 ± 24.2 MPa mechanical strength after 30 minutes of immersion in water), recyclability, natural degradability, cost-effectiveness, and non-toxicity. These attributes position binder-free hybrid designs, based on cellulose structures, as a promising solution to address environmental challenges arising from the extensive use of single-use plastics.

塑料在全球范围内以微塑料的形式在生物体内积聚,极大地加剧了环境问题。聚乳酸和商业用纸等现有材料因耐热性和耐水性不足而受到限制,造成了各种实际不便。本研究报告介绍了一种高强度、防水、可回收、可自然降解的纯纤维素食品包装材料,它是由细菌纤维素(BC)和乙基纤维素(EC)通过直接过滤和刮涂工艺制成的。使用乙基纤维素乙醇溶液无需额外的粘合剂。值得注意的是,EC-BC 纯纤维素材料具有出色的机械性能(拉伸强度为 195.3 ± 23.2 兆帕)、在液体环境中的稳定性(在水中浸泡 30 分钟后的机械强度为 136.9 ± 24.2 兆帕)、可回收性、自然降解性、成本效益和无毒性。这些特性使基于纤维素结构的无粘合剂混合设计成为一种很有前途的解决方案,可用于解决一次性塑料的广泛使用所带来的环境挑战。
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引用次数: 0
Organocatalytic ring-opening polymerization of lactide by bis(thiourea) H-bonding donating cocatalysts with binaphthyl-amine framework 双(硫脲)H 键捐献催化剂与双萘胺框架对内酰胺的有机催化开环聚合反应
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-19 DOI: 10.1016/j.giant.2024.100268
Xiangzhong Qian , Mingqian Wang , Zhiqiang Ding , Xiaohui Liu , Bin Wang

Development of H-bonding organo-catalysts with high catalytic activity and high degree of control is significantly important for the metal-free polyesters that are potentially suitable for biomedical usage. The concomitant use of base and commercially available thiourea generally suffered from prolonged reaction time and resulted in incomplete monomer conversion in some cases. Introducing one or more (thio)urea H-bonding donating arms to the parent thiourea has been proved to be an effective method for substantially increasing the activity of thiourea H-bonding donors. Consequently, we synthesized bis-thioureas derived from binaphthyl-amine bearing different substituents and investigated their catalytic performance in ROPs of lactide in this work. The density functional theory (DFT) calculations suggested that the “activated-thiourea” mode is more preferred for the bis(thiourea) containing binaphthyl-amine framework. The bis(thiourea)/base binary systems could effectively promote the LA polymerization using benzyl alcohol as initiator. The polymerization rates and the degree of control over the polymerization are highly dependent on the structures of the bis(thiourea) and base. Bis(thiourea)/1,5,7-triazabicyclo[4.4.0]dec‑5-ene pairs exhibited highest catalytic activity compared to other bis(thiourea)/base pairs, and the turnover frequency is high up to 1980 h–1 at 75 °C. In addition, the bulky hindrance and axial chirality of the binaphthyl-amine framework could enable stereoselective ROP of rac-LA to produce isotactic-rich and crystalline PLAs at relatively low temperature (0 °C). Mechanistic studies indicated that both enantiomorphic site control (ESC) and chain end control (CEC) concurrently occurred in the rac-LA polymerization catalyzed by bis(thiourea)/base binary systems. This work will inspire future design of H-bonding donors with high catalytic performance.

开发具有高催化活性和高度可控性的 H 键有机催化剂对于可能适用于生物医学用途的无金属聚酯来说非常重要。同时使用碱和市售硫脲通常会延长反应时间,并在某些情况下导致单体转化不完全。事实证明,在母硫脲中引入一个或多个(硫)脲氢键供体臂是大幅提高硫脲氢键供体活性的有效方法。因此,我们合成了由带有不同取代基的二萘胺衍生的双硫脲,并在这项工作中研究了它们在内酰胺 ROPs 中的催化性能。密度泛函理论(DFT)计算表明,含有二萘胺框架的双(硫脲)更倾向于 "活化-硫脲 "模式。双(硫脲)/碱基二元体系能有效促进以苯甲醇为引发剂的 LA 聚合。聚合速率和对聚合的控制程度在很大程度上取决于双(硫脲)和碱的结构。与其他双(硫脲)/碱对相比,双(硫脲)/1,5,7-三氮杂双环[4.4.0]癸-5-烯对表现出最高的催化活性,而且在 75 ℃ 时的周转频率高达 1980 h-1。此外,双萘胺框架的笨重阻碍和轴向手性可以实现 rac-LA 的立体选择性 ROP,从而在相对较低的温度(0 °C)下生成富含同素异形体的结晶聚乳酸。机理研究表明,在双(硫脲)/碱二元体系催化的 rac-LA 聚合过程中,对映体位点控制(ESC)和链端控制(CEC)同时发生。这项工作将为今后设计具有高催化性能的 H 键供体提供启发。
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引用次数: 0
Compatibilized polylactide/poly(pentamethylene furanoate) blends for fully bioderived packaging films with enhanced fracture toughness and UV- and O2-barrier properties 复合聚乳酸/聚(呋喃五亚甲基酸酯)共混物用于全生物源包装膜,具有更高的断裂韧性以及紫外线和氧气阻隔性能
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-16 DOI: 10.1016/j.giant.2024.100267
Giulia Fredi , Davide Perin , Carlotta Zardo , Marco Rapisarda , Paola Rizzarelli , Michelina Soccio , Nadia Lotti , Andrea Dorigato

Polylactide (PLA) is a promising biopolymer from renewable resources but its brittleness and poor gas barrier properties limit flexible packaging applications. Therefore, in this work PLA was blended with a biobased rubbery poly(pentamethylene furanoate) (PPeF), acting as a toughening agent, and a commercial epoxy-functionalized compatibilizer (i.e., Joncryl® ADR-4468) was added to improve the interfacial interaction. The effect of PPeF loading (1–30 wt %) on phase morphology, mechanical properties, oxygen permeability, and degradability in compost was characterized. All blends displayed a sea-island morphology with refined PPeF domains upon compatibilization. Incorporating PPeF induced major tensile ductility enhancements from 5 % strain at break for neat PLA up to 200 % for the blend with 30 wt % PPeF, accompanied by progressive stiffness and strength declines. Through the application of the essential work of fracture (EWF) approach on the prepared films, the specific essential work of fracture (we) was seen climbing from 6.2 to 40.0 kJ/m2 with rising PPeF content, confirming its effectiveness as a toughness enhancer. PPeF contributed to increase the UV- and gas barrier properties of PLA. For example, the oxygen permeability dropped by 37 % for the blend with 30 wt % PPeF. Moreover, compost burial tests also revealed 26 % weight loss of PPeF after 60 days, proving its biodegradability. Hence, finely dispersed PPeF domains induced synergistic property improvements, making PLA/PPeF blends a promising sustainable option for flexible and biodegradable packaging.

聚乳酸(PLA)是一种从可再生资源中提取的前景广阔的生物聚合物,但其脆性和气体阻隔性较差,限制了其在软包装领域的应用。因此,本研究将聚乳酸与生物基橡胶聚(呋喃五亚甲基酸酯)(PPeF)共混,作为增韧剂,并添加商用环氧官能化相容剂(即 Joncryl® ADR-4468)以改善界面相互作用。研究表征了 PPeF 含量(1-30 wt %)对相形态、机械性能、透氧性和堆肥降解性的影响。所有混合物在相容后都呈现出具有细化 PPeF 结构域的海岛形态。加入 PPeF 可显著提高拉伸延展性,纯聚乳酸的拉伸延展性从断裂应变的 5% 提高到含有 30 wt % PPeF 的混合物的 200%,同时刚度和强度逐渐下降。通过在制备的薄膜上应用断裂基本功(EWF)方法,随着 PPeF 含量的增加,特定断裂基本功(we)从 6.2 kJ/m2 攀升到 40.0 kJ/m2,这证实了 PPeF 作为韧性增强剂的有效性。PPeF 还有助于提高聚乳酸的紫外线和气体阻隔性能。例如,PPeF 含量为 30 wt % 的混合物的氧气渗透率下降了 37%。此外,堆肥掩埋试验还显示,60 天后 PPeF 的重量减少了 26%,证明了其生物降解性。因此,细微分散的 PPeF 域可诱导协同性能改善,使聚乳酸/PPeF 混合物成为柔性可生物降解包装的一种有前途的可持续选择。
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引用次数: 0
Construction of highly active photocatalytic interfaces through light field modulation and photo-deposition of Pd sites 通过光场调制和钯位点光沉积构建高活性光催化界面
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-10 DOI: 10.1016/j.giant.2024.100266
Zheng Wang , Min Liao , Li Ling , Meng Zhang

Anchoring noble metal sites through photo-reduction is an effective way to modulate charge distribution on photocatalytic interfaces, thereby enhancing photocatalytic performance. The irradiation field on the exposed surfaces of photocatalysts has an important influence on the morphology and distribution of noble metal sites. However, non-uniform light field derived from the scattering effects of particle-form photocatalysts hinders the well-distributed photo-deposition of noble metal sites. To address this challenge, we proposed a photo-deposition method utilizing the optical fiber coated with photocatalysts. TiO2 nanorod (NR) array was coated on the optical fiber to achieve a well-distributed irradiation filed across the NR array. This resulted in a concentration of the irradiation field primarily within the NR array, maintaining uniformly distributed light intensities throughout. Palladium (Pd) sites dominated by nanoclusters were well distributed on TiO2 NR array utilizing a photo-reduction method. These Pd sites functioned as electron acceptors, facilitating the effective separation and transfer of photo-generated carriers. Consequently, an highly active photocatalytic reaction interface was constructed, demonstrating the accumulation of a substantial concentration of holes and their efficient conversion into hydroxyl radicals (·OH). Notably, hydroxyl radicals with a concentration of 62.6 μM could be generated within 14.4 min. The construction of this efficient photocatalytic interface offers an optimal platform for accelerating photocatalytic reactions and enhancing photocatalytic efficiency.

通过光还原锚定贵金属位点是调节光催化界面电荷分布从而提高光催化性能的有效方法。光催化剂暴露表面上的辐照场对贵金属位点的形态和分布有重要影响。然而,颗粒状光催化剂的散射效应所产生的不均匀光场阻碍了贵金属位点的均匀光沉积。为了解决这一难题,我们提出了一种利用涂有光催化剂的光纤进行光沉积的方法。在光纤上涂覆 TiO2 纳米棒(NR)阵列,以实现 NR 阵列上均匀分布的辐照。这使得辐照场主要集中在 NR 阵列内,从而保持了整个阵列均匀分布的光强度。利用光还原方法,以纳米团簇为主的钯(Pd)位点被很好地分布在 TiO2 NR 阵列上。这些钯位发挥了电子受体的作用,促进了光生载流子的有效分离和转移。因此,构建了一个高度活跃的光催化反应界面,展示了大量空穴的聚集及其向羟基自由基(-OH)的高效转化。值得注意的是,在 14.4 分钟内就能生成浓度为 62.6 μM 的羟基自由基。这种高效光催化界面的构建为加速光催化反应和提高光催化效率提供了一个最佳平台。
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引用次数: 0
Kinetics model of crystal nucleation and growth in supercooled water for designing ice-templating soft matter scaffold 超冷水中晶体成核与生长动力学模型,用于设计冰模板软物质支架
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-10 DOI: 10.1016/j.giant.2024.100265
Peizhao Li , Haibao Lu , Wenge Chen , Wei Min Huang , Yong-Qing Fu

Ice-templating technology has recently attracted extensive attention to achieve programed structure-property relationships in porous soft matter scaffolds. However, there is a huge gap existed between theoretical understanding and practical applications of nucleation kinetics and growth of ice crystals in supercooled water. This paper establishes a nucleation kinetics model of crystal growth in supercooled water, for designing ice-templating soft matter scaffolds with programmable structure-property relationship. A phase transition model was firstly formulated to characterize liquid-liquid phase transition of supercooled water, based on a two-state model and free-volume theory. Effects of diffusion coefficient and density of the supercooled water on ice nucleation kinetics and crystal growth were investigated, based on the classic nucleation theory. Analytical results showed excellent agreement with experimental data, with correlation indices of R2=90.7 % for diffusion coefficients and R2=94.0 % for densities, respectively. The model predicted a nucleation rate of 31.7 m−3∙s−1 at 200 K and peak nucleation rate and crystal growth rates appearing at 183 K and 227 K. Constitutive relationships among mechanical behaviors, ice nucleus radius, nucleation ratio, and crystallization growth rate, were developed for the ice-templating scaffolds, based on the affine model theory and verified with finite element analysis results (R2= 99.9 %) and experimental results (R2 = 95.8 %). Finally, the prediction results using the proposed model were further verified using the experimental data reported in the literature. This study provides a new methodology to describe the nucleation kinetics and growth of ice crystals in supercooled water and programmable structure-property relationships in ice-templating soft matter scaffolds.

近来,为在多孔软物质支架中实现程序化的结构-性能关系,制冰技术引起了广泛关注。然而,对过冷水中冰晶成核动力学和生长的理论理解与实际应用之间存在巨大差距。本文建立了过冷水中晶体生长的成核动力学模型,用于设计具有可编程结构-性能关系的冰模板软物质支架。首先,基于双态模型和自由体积理论,建立了一个相变模型来表征过冷水中的液-液相变。基于经典的成核理论,研究了过冷水的扩散系数和密度对冰成核动力学和晶体生长的影响。分析结果与实验数据非常吻合,扩散系数的相关指数 R2=90.7 %,密度的相关指数 R2=94.0 %。该模型预测了 200 K 时 31.7 m-3∙s-1 的成核率,以及 183 K 和 227 K 时出现的峰值成核率和晶体增长率。基于仿射模型理论,建立了冰模板机械行为、冰核半径、成核率和结晶增长率之间的构成关系,并与有限元分析结果(R2= 99.9 %)和实验结果(R2= 95.8 %)进行了验证。最后,利用文献中报道的实验数据进一步验证了使用所提模型得出的预测结果。这项研究提供了一种新的方法来描述过冷水中冰晶的成核动力学和生长过程,以及冰模板软物质支架中可编程的结构-性能关系。
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引用次数: 0
Mesoscopic dynamic Monte Carlo simulations of fluctuating fluid membrane shaping in biological processes: a review 生物过程中波动流体膜塑形的介观动态蒙特卡罗模拟:综述
IF 7 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-04-09 DOI: 10.1016/j.giant.2024.100263
Long Li, Xu Huang, Jizeng Wang

Plasma membranes not only serve as physical barriers to separate the cell or organelle from extracellular or intracellular environments, but also play important roles in many cellular processes, e.g., cell adhesion, cell migration, endocytosis as well as membrane budding, whose correct executions rely on locally highly curved membrane shaping. Mechanically, these membranes are soft fluid interfaces exhibiting extremely dynamic remodeling processes in response to mechanobiological stimulus from their surrounding complex intra/extra-membranous circumstances containing thermal fluctuations, protein binding, protein-protein interaction on the membrane surface forming protein superstructures and active cytoskeletal networks. Correlating these dynamic membrane shaping involving characteristic membrane mechanical properties with cellular functions is essential to improving fundamental understandings in cell physiology and cell biomechanics. The challenge here is to explicitly describe the dynamics of membrane remodeling under the complex biological situations. Interestingly, the developed mesoscopic Monte Carlo (MC) method has the capacity to concurrently capture the elasticity and fluidity of fluid membranes well on large time and length scales, as well as to successfully reproduce fluctuating membrane morphology as observed in experiments. In this review, we focus on this mesoscopic MC method used to depict the thermodynamics of fluctuating fluid membranes and further explore how diverse biophysical factors drive large membrane curvature generation. We also discuss the current efforts of the roles of membrane morphology on the regulation of biological processes on the basis of this mesoscopic MC method, provide the insights into the known biomechanical mechanisms of effect of membrane shape on cellular functions, and point out the potential opportunities where this mesoscopic dynamic MC method can be modified to investigate more intricate biological processes, such as membrane fusion and adhesion.

质膜不仅是将细胞或细胞器与细胞外或细胞内环境隔开的物理屏障,而且在许多细胞过程(如细胞粘附、细胞迁移、内吞以及膜出芽)中发挥着重要作用。从力学角度看,这些膜是柔软的流体界面,在周围复杂的膜内/膜外环境(包括热波动、蛋白质结合、膜表面形成蛋白质超结构的蛋白质-蛋白质相互作用以及活跃的细胞骨架网络)的机械生物学刺激下,表现出极其动态的重塑过程。将这些涉及膜机械特性的动态膜塑形与细胞功能相关联,对于提高细胞生理学和细胞生物力学的基本认识至关重要。这里的挑战在于如何明确描述复杂生物情况下的膜重塑动态。有趣的是,所开发的介观蒙特卡洛(MC)方法有能力在大时间和长度尺度上同时很好地捕捉流体膜的弹性和流动性,并成功地再现实验中观察到的波动膜形态。在这篇综述中,我们将重点介绍这种用于描述波动流体膜热力学的介观 MC 方法,并进一步探讨各种生物物理因素如何驱动大膜曲率的产生。我们还讨论了目前在这种介观 MC 方法基础上研究膜形态对生物过程调控作用的工作,深入探讨了膜形状对细胞功能影响的已知生物力学机制,并指出了这种介观动态 MC 方法可用于研究更复杂的生物过程(如膜融合和粘附)的潜在机会。
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