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Tailored Synthesis of Hierarchical All-Silica MEL Zeolites for Efficient Removal of Versatile VOCs 分级全硅MEL沸石的合成及其高效去除多种挥发性有机化合物的研究
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-11 DOI: 10.1021/acsami.5c17480
Qiang Yu, Zikai Xu, Wei Fan, Junjie Li, Xiangxue Zhu, Xiujie Li
The efficient removal of volatile organic compounds (VOCs) with different molecular sizes remains a great challenge in the field of zeolite-based adsorption technology. The conventional composite zeolite systems (e.g., MFI/FAU) suffer from nonuniform crystalline distribution. Herein, a novel synthesis strategy for all-silica MEL zeolites was developed featuring 10-membered ring (10-MR) micropores, extra-large micropores (0.8∼2.0 nm), and small mesopores (2.0∼5.0 nm). The hierarchical pore structure conferred exceptional adsorption capabilities for VOCs across diverse molecular dimensions. The volume and accessibility of extra-large micropores and small mesopores could be tuned by controlling the tetrabutylammonium hydroxide (TBAOH) content in the synthesis gel and crystallization temperature, while prolonged crystallization enhanced framework hydrophobicity due to the decrease of silanol group density. Notably, the optimal sample exhibited a superior m-xylene adsorption capacity of 85.2 mg/g. Meanwhile, high adsorption capacities of acetone, ethyl acetate, and toluene were also obtained, which can be attributed to its high 10-MR micropore volume of 0.178 cm3/g. Importantly, its m-xylene adsorption capacity remained unchanged across multiple regeneration cycles, demonstrating perfect recyclability and structural stability. Low desorption peak temperatures (<115 °C) for all adsorbates were acquired that facilitated regeneration under mild conditions. By integrating hierarchical pore engineering and surface chemistry control within a single zeolite framework, this work overcomes the limitations of traditional composite systems, offering a versatile and efficient system for industrial VOC abatement.
高效去除不同分子大小的挥发性有机物(VOCs)一直是沸石基吸附技术领域的一大挑战。传统的复合沸石体系(如MFI/FAU)存在晶体分布不均匀的问题。本文开发了一种新的全硅MEL沸石合成策略,该策略具有10元环(10-MR)微孔,超大微孔(0.8 ~ 2.0 nm)和小介孔(2.0 ~ 5.0 nm)。层次化的孔隙结构赋予了对不同分子尺度的挥发性有机化合物的特殊吸附能力。通过控制合成凝胶中四丁基氢氧化铵(TBAOH)的含量和结晶温度,可以调节超大微孔和小介孔的体积和可达性,而延长结晶时间会降低硅醇基密度,从而增强骨架的疏水性。最优样品对间二甲苯的吸附量为85.2 mg/g。同时对丙酮、乙酸乙酯和甲苯也有较高的吸附能力,这可归因于其高10-MR微孔体积为0.178 cm3/g。重要的是,其对间二甲苯的吸附能力在多次再生循环中保持不变,表现出良好的可回收性和结构稳定性。所有吸附物的低解吸峰温度(<115°C)有利于在温和条件下再生。通过在单一沸石框架内集成分层孔隙工程和表面化学控制,这项工作克服了传统复合系统的局限性,为工业VOC减排提供了一个多功能和高效的系统。
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引用次数: 0
Tailoring Pendant Group Chemistry and Thiol–Ene Network Structure of Thin-Film Composite Membranes to Optimize CO2 Gas Separation 调整垂坠基化学和巯基网络结构的薄膜复合膜优化CO2气体分离
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-11 DOI: 10.1021/acsami.5c18327
Yu-Shen Liu, Yu-Hsiang Kuo, Vijay M. Shah, Paul J. A. Kenis, Alexa S. Kuenstler
Carbon dioxide (CO2) capture is critical to mitigating the anthropogenic emissions that contribute to global warming. Polymer membranes can be applied in energy efficient gas separation methods, where chemical and structural features can be tuned to co-optimize selectivity and permeability. In this work, we developed a modular thiol–ene network platform to independently tune cross-link density and functionality to explicitly understand the impact of network architecture and polymer chain functionality on separation performance. By varying the pendant functional groups in the networks, we investigated how molecular substitutions affect the selectivity of CO2/N2 and CO2/O2 selectivity. These membranes were subsequently applied as a selective layer in a thin-film composite membrane system. In pure gas testing, the network with pendant aromatic rings elevated the CO2/N2 selectivity from ≈10 to 34 and CO2/O2 selectivity from ≈5 to 17 compared to bare polydimethylsiloxane (PDMS) membranes, with a CO2 permeability of 1426 barrer. Furthermore, the topologically regular and predictable cross-linking density features in this modular network system allowed us to unravel their effect on CO2 selectivity and permeability. We demonstrate that these functionalized thiol–ene network-based membranes can be used in a pseudomultistage gas separation configuration to concentrate CO2 from gas mixtures of industrially relevant composition.
二氧化碳(CO2)捕获对于减缓导致全球变暖的人为排放至关重要。聚合物膜可以应用于节能气体分离方法,其中化学和结构特征可以调整,以共同优化选择性和渗透性。在这项工作中,我们开发了一个模块化的巯基烯网络平台来独立调整交联密度和功能,以明确了解网络结构和聚合物链功能对分离性能的影响。通过改变网络中悬垂的官能团,我们研究了分子取代对CO2/N2和CO2/O2选择性的影响。这些膜随后被用作薄膜复合膜系统中的选择性层。在纯气体测试中,与裸聚二甲基硅氧烷(PDMS)膜相比,带有悬垂芳香环的网络将CO2/N2选择性从≈10提高到34,将CO2/O2选择性从≈5提高到17,CO2渗透率为1426。此外,这种模块化网络系统的拓扑规则和可预测的交联密度特征使我们能够揭示它们对二氧化碳选择性和渗透率的影响。我们证明了这些功能化的基于巯基网络的膜可以用于伪多级气体分离配置,从工业相关成分的气体混合物中浓缩二氧化碳。
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引用次数: 0
Employing Competitive Adsorption and Hollow Nanofiber Strategies toward High-Efficiency Hydrogen Evolution with Ru–Sn/SnO2 Heterojunction Catalysts 采用竞争吸附和中空纳米纤维策略制备Ru-Sn /SnO2异质结高效析氢催化剂
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-11 DOI: 10.1021/acsami.5c18381
Huan Liu, Duanduan Yin, Ke Li, Yiran Dong, Dan Li, Feng Li, Ying Yang, Xiangjie Bo, Xiangting Dong
Electrochemical water splitting is regarded as an efficient method for hydrogen production. Ru is theoretically deemed as an effective electrocatalyst for hydrogen evolution reactions (HERs) in alkaline media owing to its fast hydrolysis kinetics. Nevertheless, its strong OH adsorption affinity can lead to active site blockage, often resulting in a suboptimal performance in practical HER applications. In addition, electrocatalytic reactions predominantly take place at surface-active sites. In the case of conventional solid catalysts, the core active material remains largely inaccessible due to mass transfer limitations, significantly reducing the overall utilization of active sites. To address these challenges, the work introduces a competitive adsorption strategy and a hollow structure strategy for constructing Ru–Sn/SnO2 hollow carbon nanofiber electrocatalysts (Ru–Sn/SnO2 HCNFs). The introduction of Sn/SnO2 helps to modulate the intense interaction between Ru and OH; OH adsorption on SnO2 is more favorable than Ru, thereby successfully mitigating poisoning on Ru. This process also promotes OH transfer and Ru active site regeneration. Additionally, the specific surface area of Ru–Sn/SnO2–HCNFs (606.9 m2g–1) is higher than that of the solid fiber of Ru–Sn/SnO2–CNFs (22.7 m2g–1), highlighting the beneficial role of hollow fibers in enhancing the exposure of active sites. Consequently, Ru–Sn/SnO2–HCNFs exhibit an outstanding HER performance, achieving remarkably low overpotentials of only 6.8 mV in 1 M KOH and 23.3 mV in 0.5 M H2SO4 at 10 mA cm–2, respectively. This research offers a novel approach on rational design for high-efficiency HER electrocatalysts.
电化学水分解是一种高效的制氢方法。Ru具有快速的水解动力学,理论上被认为是碱性介质中析氢反应的有效电催化剂。然而,其强大的OH -吸附亲和力可能导致活性位点堵塞,通常导致在实际HER应用中的性能不理想。此外,电催化反应主要发生在表面活性位点。在传统固体催化剂的情况下,由于传质限制,核心活性物质在很大程度上仍然是不可接近的,这大大降低了活性位点的总体利用率。为了解决这些挑战,本研究介绍了一种竞争性吸附策略和一种空心结构策略,用于构建Ru-Sn /SnO2中空碳纳米纤维电催化剂(Ru-Sn /SnO2 HCNFs)。Sn/SnO2的引入有助于调节Ru与OH -之间强烈的相互作用;OH -在SnO2上的吸附比Ru更有利,从而成功地减轻了Ru上的中毒。该过程还促进了OH -转移和Ru活性位点的再生。此外,Ru-Sn / SnO2-HCNFs的比表面积(606.9 m2g-1)高于Ru-Sn / SnO2-CNFs的固体纤维(22.7 m2g-1),突出了中空纤维在增强活性位点暴露方面的有益作用。因此,Ru-Sn / SnO2-HCNFs表现出出色的HER性能,在1 M KOH和10 mA cm-2下,在0.5 M H2SO4中分别获得了6.8 mV和23.3 mV的过电位。本研究为高效HER电催化剂的合理设计提供了一条新途径。
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引用次数: 0
Inhalable Food-Grade MOFs Loaded Gas Messenger for Acute Lung Injury Treatment by Pulmonary Delivery. 可吸入食品级mof负载气体信使通过肺输送治疗急性肺损伤。
IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-11 DOI: 10.1021/acsami.5c20962
Zu-E Hu, Fu-Zhong Zhang, Minfeng Zeng, Ye-Tao Zhang, Jing Li, Yu-Ting Che, Jun-Feng Feng, Bang-Jing Li, Sheng Zhang

Acute lung injury (ALI) is a serious clinical disease the severe stage of which develops into acute respiratory distress syndrome (ARDS), with a high mortality rate of 35 to 40%. Despite decades of research and development of drugs such as corticosteroids and β-2 adrenergic agonists, treatment efficacy has been limited due to an insufficient drug concentration reaching the lungs. Here, a food-grade γ-cyclodextrin-based metal-organic framework (γCD-MOF) modified with cholesterol (CHS) is developed to load sulfur dioxide (SO2) as a dry powder inhaler (DPI) platform (CHS-CD-MOF@SO2) for ALI treatment. CHS-CD-MOF@SO2 has suitable storage stability and excellent aerodynamic characteristics, with a fine particle fraction (FPF) of 40%, a geometric standard deviation (GSD) value of 1.61, and a mass median aerodynamic diameter (MMAD) of 4.8 μm, which can effectively target the lungs. By employing rhodamine B (RhB) as a fluorescence indicator, in vivo fluorescence imaging confirms the superior lung-targeting capability of CHS-CD-MOFs. CHS-CD-MOF@SO2 can release 92.3 ± 4.4% of SO2 in PBS solution within 5 min. What's more, the permeability of simulated lung fluid within 30 min is as high as 85%, which has the potential for rapid treatment of ALI. In an ALI mouse model, CHS-CD-MOF@SO2 reduces the expression of pro-inflammatory factors tumor necrosis factor-alpha (TNF-α), interleukin-1 beta (IL-1β), and IL-6 by regulating the P38 and nuclear factor kappa B (NF-κB) pathways. It also significantly improves the lung tissue dry/wet ratio and reduces neutrophil infiltration. Importantly, this treatment achieves therapeutic outcomes in key efficacy parameters that was comparable to or better than those of dexamethasone (DXMS), a frontline drug for ALI, underscoring its significant therapeutic potential. This study presents a novel strategy for treating ALI using a DPI-based gas messenger platform. This study provides a novel therapeutic strategy to treat ALI using DPI-loaded gas messengers.

急性肺损伤(Acute lung injury, ALI)是一种严重的临床疾病,严重阶段发展为急性呼吸窘迫综合征(Acute respiratory distress syndrome, ARDS),死亡率高达35% ~ 40%。尽管皮质类固醇和β-2肾上腺素能激动剂等药物经过了数十年的研究和开发,但由于到达肺部的药物浓度不足,治疗效果受到限制。本文开发了一种以胆固醇(CHS)修饰的食品级γ-环糊精为基础的金属有机骨架(γCD-MOF),用于装载二氧化硫(SO2),作为用于ALI治疗的干粉吸入器(DPI)平台(CHS-CD-MOF@SO2)。CHS-CD-MOF@SO2具有良好的贮存稳定性和优良的气动特性,其细颗粒分数(FPF)为40%,几何标准偏差(GSD)为1.61,质量中位气动直径(MMAD)为4.8 μm,可有效靶向肺部。利用罗丹明B (rhodamine B, RhB)作为荧光指示剂,体内荧光成像证实了CHS-CD-MOFs优越的肺靶向能力。CHS-CD-MOF@SO2可在5 min内释放92.3±4.4%的SO2。模拟肺液在30min内通透性高达85%,具有快速治疗ALI的潜力。在ALI小鼠模型中,CHS-CD-MOF@SO2通过调节P38和核因子κB (NF-κB)通路降低促炎因子肿瘤坏死因子-α (TNF-α)、白细胞介素-1β (IL-1β)和IL-6的表达。显著提高肺组织干/湿比,减少中性粒细胞浸润。重要的是,这种治疗方法在关键疗效参数上取得的治疗结果与急性脑损伤的一线药物地塞米松(DXMS)相当或更好,强调了其显著的治疗潜力。本研究提出了一种使用基于dpi的气体信使平台治疗ALI的新策略。这项研究提供了一种新的治疗策略来治疗ALI使用dpi负载气体信使。
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引用次数: 0
Artificial Light-Harvesting System with Three-Step Cascade Energy Transfer Process for Full-Color Luminescence Modulation 全彩色光调制的三步级联能量传递人工光收集系统
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-11 DOI: 10.1021/acsami.5c20984
Hui-Cong Ge, Shengsheng Yu, Jian Zhu, Xiao-Tong Zhan, Shi-Qian Jia, Ling-Bao Xing, Long Yi Jin
The artificial light-harvesting system (LHS) based on the cascade fluorescence resonance energy transfer (FRET) mechanism has ability to widely regulate the luminescent performance, however, it still faces significant challenges to achieve full-color luminescent regulation covering the entire visible spectrum in a single LHS system. In this study, we designed and constructed an artificial LHS with a three-step cascade energy transfer mechanism, achieving effective emission of white light and multicolor fluorescence within the visible light range. A cationic 6-bromobenzo[de]isochromene-1,3-dione derivative (BNI) was prepared, which was able to generate a supramolecular complex with sulfobutylether-β-cyclodextrin (SBE-β-CD) via electrostatic interactions. Given that this complex has excellent dark blue fluorescence performance, it was selected as the energy donor and sequentially participated in FRET process with commercial dyes Fluorescein (Flu), Rhodamine B (RhB) and Sulforhodamine 101 (SR101), thereby constructing an artificial LHS with three-step sequential energy transfer. By precisely regulating the ratios of acceptor molecules, multicolor fluorescence emissions ranging from blue to red bands and white light emission were achieved. Ultimately, the synthesized supramolecular LHS was effectively utilized in the development of multicolor fluorescent light-emitting devices and demonstrated its potential application in information storage.
基于级联荧光共振能量转移(FRET)机制的人工光收集系统(LHS)具有广泛调节发光性能的能力,但要在单个LHS系统中实现覆盖整个可见光谱的全彩色发光调节仍面临重大挑战。在本研究中,我们设计并构建了一个具有三级级联能量传递机制的人工LHS,实现了可见光范围内白光和多色荧光的有效发射。制备了一种阳离子6-溴苯并[de]异铬烯-1,3-二酮衍生物(BNI),该衍生物能与磺基丁醚-β-环糊精(SBE-β-CD)通过静电相互作用生成超分子配合物。考虑到该配合物具有优异的深蓝色荧光性能,选择其作为能量供体,与荧光素(Flu)、罗丹明B (RhB)和硫代丹明101 (SR101)等商业染料依次进行FRET工艺,构建具有三步顺序能量转移的人工LHS。通过精确调节受体分子的比例,实现了从蓝到红波段的多色荧光发射和白光发射。最终,合成的超分子LHS被有效地应用于多色荧光发光器件的开发中,并在信息存储方面展示了其潜在的应用前景。
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引用次数: 0
“Continuously Touching ROS into NO” by Hemodialysis Membranes for Preventing Hemodialysis-Associated Thrombocytopenia 血液透析膜“连续接触ROS成NO”预防血液透析相关性血小板减少症
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-11 DOI: 10.1021/acsami.5c21229
Jian Ren, Lin Xu, Xianda Liu, Dongmei Tong, Shujing Wang, Shuxiang Zhang, Ran Wei, Weifeng Zhao, Changsheng Zhao
Hemodialysis membranes would easily accelerate excessive oxidative stress, leading to platelet adhesion and aggregation, which cause exacerbation of hemodialysis-associated thrombocytopenia. Notably, nitric oxide (NO) gas exerts an inhibitory effect on platelet activation by targeting key signaling molecules. Hence, we propose a strategy to inhibit platelet activation and adhesion by turning “harmful reactive oxygen species (ROS)” into “beneficial NO”, thereby preventing hemodialysis-associated thrombocytopenia. In this study, polydopamine-l-arginine (PDA-LA) molecules are coated onto the membrane surface to mainly enhance the mitigation of oxidative stress, while oxidized hyaluronic acid-l-arginine (OHA-LA) molecules are stably cross-linked into the membrane to ensure the sustained NO release for inhibition of platelet adhesion. As a result, the reactive oxygen and nitrogen species (RONS) scavenging capacities are improved to follow: H2O2 (50%), 2,2-diphenyl-1-picrylhydrazyl (DPPH, 85.60%), 2,2′-azinobis(3-ethylbenzothiazoline-6-sulfonate) radical (ABTS•+, 82.81%), and O2•– (0.125 U/mg). Surprisingly, the concentration of continuously released NO is still approximately 0.590 μM after six cycles (0.557 μM in the first cycle). Importantly, the platelet adhesion experiment demonstrates a sustained inhibition of platelet adhesion, diminished by a factor of 100 per square centimeter (100/cm2). In a simulated sieving experiment, the BSA rejection ratio (97.52%) and urea sieving ratio (98.38%) both meet the basic requirements for hemodialysis membranes. Thus, the obtained PES/PVA/OA@PA membrane is a promising candidate for preventing hemodialysis-associated thrombocytopenia.
血液透析膜容易加速过度氧化应激,导致血小板粘附聚集,加重血液透析相关性血小板减少症。值得注意的是,一氧化氮(NO)气体通过靶向关键信号分子对血小板活化起抑制作用。因此,我们提出了一种通过将“有害活性氧(ROS)”转化为“有益NO”来抑制血小板活化和粘附的策略,从而预防血液透析相关的血小板减少症。在本研究中,聚多巴胺-l-精氨酸(PDA-LA)分子包被在膜表面主要增强氧化应激的缓解作用,氧化透明质酸-l-精氨酸(OHA-LA)分子稳定交联进入膜内,保证NO持续释放,抑制血小板粘附。对H2O2(50%)、2,2-二苯基-1-吡啶酰肼(DPPH•,85.60%)、2,2 ' -氮化氮(3-乙基苯并噻唑-6-磺酸盐)自由基(ABTS•+,82.81%)和O2•- (0.125 U/mg)的清除能力均有提高。令人惊讶的是,6个循环后,连续释放的NO浓度仍然在0.590 μM左右(第一个循环为0.557 μM)。重要的是,血小板粘附实验证明了血小板粘附的持续抑制,每平方厘米(100/cm2)减少了100倍。在模拟筛分实验中,BSA截留率(97.52%)和尿素筛分率(98.38%)均满足血液透析膜的基本要求。因此,获得的PES/PVA/OA@PA膜是预防血液透析相关性血小板减少症的有希望的候选膜。
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引用次数: 0
Dual-Temperature Composite Phase Change Material Adapted for Wide-Temperature-Range Applications in Battery Thermal Management 适用于电池热管理宽温度范围应用的双温复合相变材料
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-10 DOI: 10.1021/acsami.5c17887
Shuheng Hu, Liangke Mao, Peng Qin, Zimu Xu, Lijian Ding, Helong Li, Ya Wei, Xiaoli Wang, Zhangyin Li, Zhaozhong Huang
To address the challenge of efficient thermal management for lithium-ion batteries across a wide temperature range, we developed a novel dual-temperature composite phase change material (CPCM). The CPCM, constructed with an expanded graphite matrix incorporating paraffin (∼45 °C) and potassium alum (∼90 °C), achieves two distinct phase change platforms and a high total latent heat of 211.4 J/g. Its thermal conductivity was significantly enhanced to 2.53 W/(m·K). In practical battery tests, the CPCM demonstrated superior performance: it reduced the maximum temperature by ∼10 °C across 0.2 to 1C discharge rates and maintained excellent temperature uniformity (ΔT < 2.2 °C). Crucially, under thermal runaway conditions, it lowered the peak temperature of adjacent cells by ∼134 °C, effectively delaying hazardous heat propagation. This work provides a material solution that synergistically combines efficient cooling at normal operating temperatures with robust thermal barrier functionality under extreme conditions.
为了解决锂离子电池在宽温度范围内高效热管理的挑战,我们开发了一种新型的双温复合相变材料(CPCM)。CPCM由含有石蜡(~ 45°C)和钾明矾(~ 90°C)的膨胀石墨基体构建,实现了两个不同的相变平台和211.4 J/g的高总潜热。其导热系数显著提高至2.53 W/(m·K)。在实际电池测试中,CPCM表现出卓越的性能:在0.2至1C的放电速率下,它将最高温度降低了约10°C,并保持了出色的温度均匀性(ΔT < 2.2°C)。关键是,在热失控条件下,它将相邻细胞的峰值温度降低了~ 134°C,有效地延缓了危险的热传播。这项工作提供了一种材料解决方案,将正常工作温度下的高效冷却与极端条件下的强大热障功能协同结合起来。
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引用次数: 0
Mitigating Ion Migration with Alternating Voltage for Stable Perovskite Image Sensors. 稳定钙钛矿图像传感器的交流电压抑制离子迁移。
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-10 DOI: 10.1021/acsami.5c18552
Sergey Tsarev,Yuliia Kominko,Kyuik Cho,Lorenzo J A Ferraresi,Gebhard Matt,Kostiantyn Sakhatskyi,Volodymyr Svintozelskyi,Daria Proniakova,Taekwang Jang,Maksym Kovalenko,Sergii Yakunin
Perovskite photodetectors have emerged as a potential replacement for silicon photodiodes in modern cameras due to their high sensitivity to visible light and ability to be easily integrated into existing electronics. However, the use of perovskite photodetectors in conventional CMOS image sensors requires the application of reverse bias, which can lead to unstable detector performance due to ion migration effects. In this article, we propose a new approach that involves the application of forward voltage pulses to attenuate ion migration while still enabling the capture of photocurrent under reverse bias. Our results show that using this technique after each cycle of signal integration allows for stable operation of perovskite photodetectors for over 180 h, while applying a constant reverse bias leads to degradation within just 10 min. Additionally, we demonstrate stable imaging using alternating voltage and 8 × 8 crossbar arrays of perovskite photodetectors.
钙钛矿光电探测器由于其对可见光的高灵敏度和易于集成到现有电子设备中的能力,已成为现代相机中硅光电二极管的潜在替代品。然而,在传统的CMOS图像传感器中使用钙钛矿光电探测器需要应用反向偏置,这可能导致离子迁移效应导致探测器性能不稳定。在本文中,我们提出了一种新的方法,该方法涉及应用正向电压脉冲来衰减离子迁移,同时仍然能够捕获反向偏压下的光电流。我们的研究结果表明,在每个信号集成周期后使用这种技术可以使钙钛矿光电探测器稳定运行超过180小时,而施加恒定的反向偏置会在10分钟内导致退化。此外,我们证明了使用交流电压和8 × 8钙钛矿光电探测器的横条阵列的稳定成像。
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引用次数: 0
Protein-Based Nanostructures: Column-free Biosynthesis of Bundlemer Peptides with Programmable, Orthogonally Reactive Handles for Nanomaterial Construction. 基于蛋白质的纳米结构:束状肽的无柱生物合成与可编程,正交反应处理纳米材料的建设。
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-10 DOI: 10.1021/acsami.5c17204
Caitlin D'Ambrosio,Nadim Massad,Amanda L McCahill,William Rears,Pierre Rouviere,Jeffery G Saven,Darrin J Pochan,Christopher J Kloxin,April M Kloxin,Wilfred Chen
Nature's protein sequences dictate structure and function across scales, from the nanometer-scale of viral capsids to micrometer- to millimeter-scale architectures of extracellular matrices and tissues. This multiscale precision underlies diverse functions, including molecular recognition, mechanical support, and dynamic responsiveness. Mimicking this complexity synthetically remains challenging. To address this, we engineered biosynthetic coiled-coil 'bundlemer' peptides as modular building blocks that can be conjugated and assembled into complex, higher-ordered materials. Using recombinant expression, we produced peptides and peptide fusion constructs that are otherwise difficult to achieve via solid-phase peptide synthesis. An N-terminal fusion protein with a pH-cleavable intein-inclusion body facilitated simple, scarless purification directly from insoluble fractions. We further incorporated SpyTag (-VPTIVMVDAYKRYK-) and sortase-recognition motifs (GGG-, -LPETGG) into the bundlemers, enabling precise, programmable assembly using genetically encoded and enzymatic ligation strategies. Using sortase-mediated ligation, we polymerized a single bundlemer into fibrillar structures, which were confirmed via TEM, SEC-MALS, SDS-PAGE, and native gels. Additionally, we constructed multicomponent architectures with a layered bundlemer and EGFP on an E2 nanocage using orthogonal linking chemistries, specifically SpyCatcher-SpyTag ligation and sortase-mediated ligation, and the associated increase in particle size and molecular weight was confirmed via TEM, DLS, and SDS-PAGE. This platform establishes a versatile framework for designing complex, protein-based nanostructures with defined architecture and function, offering possibilities in biomaterials engineering, targeted drug delivery, and synthetic biology.
从纳米级的病毒衣壳到微米级到毫米级的细胞外基质和组织结构,大自然的蛋白质序列决定了不同尺度的结构和功能。这种多尺度精度是多种功能的基础,包括分子识别、机械支持和动态响应。综合模仿这种复杂性仍然具有挑战性。为了解决这个问题,我们设计了生物合成的螺旋状“捆扎物”肽,作为模块化的构建块,可以共轭并组装成复杂的、高阶的材料。通过重组表达,我们产生了难以通过固相肽合成实现的肽和肽融合结构。n端融合蛋白具有ph可切割的包涵体,可以直接从不溶性组分中简单、无疤痕地纯化。我们进一步将SpyTag (- vptivmvdaykryk -)和排序酶识别基序(GGG-, - lpetgg)整合到捆绑器中,利用基因编码和酶联策略实现精确的可编程组装。利用排序酶介导的连接,我们将单个束聚物聚合成纤维状结构,通过TEM, SEC-MALS, SDS-PAGE和天然凝胶证实了这一点。此外,我们利用正交连接化学,在E2纳米笼上构建了多组分结构,特别是spycatch - spytag连接和排序酶介导的连接,并通过TEM, DLS和SDS-PAGE证实了颗粒大小和分子量的相关增加。该平台建立了一个多功能框架,用于设计具有定义结构和功能的复杂蛋白质纳米结构,为生物材料工程、靶向药物输送和合成生物学提供了可能性。
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引用次数: 0
Enhanced Elastic Multifunctional Dual-Network Hydrogel Microspheres for the Treatment of Intervertebral Disc Degeneration through Inflammation Modulation and Apoptosis Inhibition 增强弹性多功能双网水凝胶微球通过炎症调节和细胞凋亡抑制治疗椎间盘退变
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-12-10 DOI: 10.1021/acsami.5c17783
Fei Ma, Chuan Guo, Yuheng Liu, Daqiang Zheng, Walter Munesu Chirume, Dengbo Yao, Weiqiang Lan, Zhen Zhao, Chen Fan, Yu Wang, Qingquan Kong
Modulating the local inflammatory environment and restoring nucleus pulposus cell (NPC) function are essential strategies for mitigating IVDD. In this study, a microgel-based delivery system for microRNA therapeutics, termed POCM@MCCP (PMCCP), was developed. The system employs dual-network hydrogel microspheres composed of chitosan, citric acid, and poly(vinyl alcohol) (CCP), further functionalized with metal-phenolic networks (MPNs) formed from strontium ions (Sr2+) and epigallocatechin gallate (EGCG). This microgel enables dynamic, stimulus-responsive loading of phenylboronic acid-modified oxidized hyaluronic acid (PBA-oHA)-coated miR-155/chito-oligosaccharide (COS) complexes (POCM) through boronate ester linkages. The mechanical elasticity and stability of the CCP microspheres support the consistent and prolonged release of miR-155 even under mechanical compression. Incorporation of MPNs further endows the system with the ability to modulate and suppress the inflammatory microenvironment. In oxidative microenvironments, the boronate bonds cleave, triggering the release of POCM and its subsequent CD44 receptor-mediated internalization by NPCs. Subsequently, miR-155 and COS are released within the acidic intracellular space, modulating the Bcl-2/Bax/Caspase-3 signaling cascade and scavenging intracellular ROS, respectively. Both in vitro and in vivo IVDD models demonstrated that this multifunctional platform effectively suppresses inflammation and restores NPC function, highlighting its potential as a promising therapeutic strategy for IVDD.
调节局部炎症环境和恢复髓核细胞(NPC)功能是缓解IVDD的基本策略。在这项研究中,开发了一种基于微凝胶的microRNA治疗递送系统,称为POCM@MCCP (PMCCP)。该系统采用由壳聚糖、柠檬酸和聚乙烯醇(CCP)组成的双网络水凝胶微球,并通过由锶离子(Sr2+)和表没食子儿茶素没食子酸酯(EGCG)形成的金属酚网络(mpn)进一步功能化。这种微凝胶通过硼酸酯键实现苯硼酸修饰的氧化透明质酸(PBA-oHA)包被的miR-155/壳寡糖(COS)复合物(POCM)的动态、刺激响应加载。CCP微球的机械弹性和稳定性支持miR-155即使在机械压缩下也能持续和延长释放。mpn的结合进一步赋予系统调节和抑制炎症微环境的能力。在氧化微环境中,硼酸键断裂,触发POCM的释放和随后CD44受体介导的npc内化。随后,miR-155和COS在酸性细胞内空间释放,分别调节Bcl-2/Bax/Caspase-3信号级联和清除细胞内ROS。体外和体内IVDD模型都表明,这种多功能平台有效抑制炎症并恢复NPC功能,突出了其作为IVDD治疗策略的潜力。
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ACS Applied Materials & Interfaces
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