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A flexible composite electrode for effective real-time glucose monitoring via high-precision layer-by-layer inkjet printing 一种柔性复合电极,可通过高精度逐层喷墨打印进行有效的实时葡萄糖监测
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-25 DOI: 10.1016/j.jcis.2026.139977
Ziyue Ju , Ruichan Lv , Ji Zhang , Delong Shi , Yitong Chen , Anees A. Ansari
Conventional techniques such as screen printing and hand-brushing, though scalable, often compromise on patterning resolution and material waste. In contrast, advanced inkjet printing offers a promising route for high-resolution and efficient manufacturing. In this study, a flexible electrode based on Ni-MOF material used high-precision scalable inkjet printing was developed for glucose sensing in human body fluids for wearable devices. Initially, Ni-MOF material with a high specific surface area and porous structure was synthesized via a hydrothermal method, and its potential for electrochemical detection was investigated. Experimental results demonstrated that the material exhibited high sensitivity and a broad detection range for glucose. Importantly, graphite and carbon nanotubes were incorporated to construct a Ni-MOF composite material with the composition ratio optimized to enhance conductivity and mechanical stability, for further application in flexible electrodes. Typically, a cost-effective, high-efficiency, and scalable fabrication process was achieved through high-precision inkjet printing technology, which enables 1200 dpi resolution while supporting ultra-large-scale printing up to 1200 × 1200 mm. Simutaneously, simulation-based optimization was conducted to determine the most effective electrode shape. As a result, the detection range of the inkjet-printed flexible electrode was extended to 0.005–2.63 mM, with an improved sensitivity of 12.2 μA·μM−1·cm−2. Moreover, excellent mechanical stability and long-term durability were achieved, enabling precise differentiation of glucose fluctuations in low-concentration simulated sweat. Finally, a microfluidic channel to provide environment for the reaction was designed, thereby establishing a fundamental foundation for applying the flexible electrode in wearable devices.
传统的技术,如丝网印刷和手刷,虽然可扩展,但往往在图案分辨率和材料浪费方面妥协。相比之下,先进的喷墨打印为高分辨率和高效制造提供了一条有前途的途径。本研究开发了一种基于Ni-MOF材料的柔性电极,用于高精度可扩展喷墨打印,用于可穿戴设备中人体体液中的葡萄糖传感。首先,通过水热法合成了具有高比表面积和多孔结构的Ni-MOF材料,并对其电化学检测潜力进行了研究。实验结果表明,该材料对葡萄糖具有较高的灵敏度和较宽的检测范围。重要的是,将石墨和碳纳米管结合在一起构建了Ni-MOF复合材料,其成分配比优化以提高电导率和机械稳定性,从而进一步应用于柔性电极。通常,通过高精度喷墨打印技术实现了成本效益,高效率和可扩展的制造工艺,可实现1200 dpi分辨率,同时支持高达1200 × 1200 mm的超大尺寸打印。同时,进行了基于仿真的优化,以确定最有效的电极形状。结果表明,喷墨打印柔性电极的检测范围扩大到0.005 ~ 2.63 mM,灵敏度提高到12.2 μA·μM−1·cm−2。此外,它还具有优异的机械稳定性和长期耐用性,能够精确区分低浓度模拟汗液中的葡萄糖波动。最后设计了微流控通道为反应提供环境,为柔性电极在可穿戴设备中的应用奠定了基础。
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引用次数: 0
A trapdoor chabazite zeolite for elevated-temperature adsorption separation of ethylene and ethane 一种用于高温吸附分离乙烯和乙烷的活板门型钙辉石沸石
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-25 DOI: 10.1016/j.jcis.2026.139978
Yaohan Fu , Yuan Cao , Yaqi Wu , Rui Sun , Yang Zhang , Chenyang Yang , Beibei Gao , Qiuju Zhang , Liang Chen
Elevated-temperature gas separation offers significant advantages, such as energy savings and the ability to directly integrate with hot process streams. Despite this, research on the critical adsorptive separation of ethylene/ethane (C2H4/C2H6) has predominantly been confined to room or near-ambient temperatures. Herein, we report the application of K+-exchanged chabazite (KCHA) zeolite for efficient elevated-temperature C2H4/C2H6 separation via a trapdoor mechanism. KCHA exhibits a high C2H4 uptake of 1.6 mmol/g at 1 bar and 423 K and demonstrates a remarkable selectivity of 14 for C2H4/C2H6 (50:50) mixtures. Computational studies reveal that the gas-cation interaction governs the thermal oscillation of the “door-keeping” cation. Dynamic breakthrough experiments further confirm the excellent elevated-temperature C2H4/C2H6 separation performance and its robust cyclic stability. This successful elevated-temperature separation not only demonstrates the potential of trapdoor-enabled zeolites but also provides guidance for the design and application of elevated-temperature C2H4/C2H6 separations.
高温气体分离具有显著的优势,如节能和直接集成热工艺流的能力。尽管如此,对乙烯/乙烷(C2H4/C2H6)临界吸附分离的研究主要局限于室温或近环境温度。本文报道了KCHA沸石在高温下通过活板门机制高效分离C2H4/C2H6的应用。在1 bar和423 K条件下,KCHA对C2H4的吸收率高达1.6 mmol/g,对C2H4/C2H6(50:50)混合物的选择性为14。计算研究表明,气-阳离子相互作用支配着“看门”阳离子的热振荡。动态突破实验进一步证实了C2H4/C2H6优异的高温分离性能及其鲁棒循环稳定性。这一成功的高温分离不仅证明了活板门沸石的潜力,也为高温C2H4/C2H6分离的设计和应用提供了指导。
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引用次数: 0
Upgrading sustainability: Ammonium sulfate recovery from low-concentration nitrate groundwater by ion exchange, electrolysis and gas-permeable membrane contactor hybrid system 提升可持续性:通过离子交换、电解和透气膜接触器混合系统从低浓度硝酸盐地下水中回收硫酸铵
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-25 DOI: 10.1016/j.jcis.2026.139980
Chaosheng Zhu , Xiaobin Guo , Yonghong Zhang , Mengdi Lu , Yifan Li , Bo Jiang , Yijie Liu
In this study, an anion exchange, electrolytic reactor and membrane contactor coupled system (AE-ER-MC) was developed for high-performance recovering (NH4)2SO4 from the low-concentration NO3 contaminated groundwater, where the basic anion exchange resin selectively removed NO3 from the groundwater, the NO3 exhausted resin was regenerated by the NaCl catholyte, and ammonia was produced from the NO3 reduction at the Fe2O3-Ov cathode and recovered by membrane stripping process. The AE-ER-MC system achieved at 98% NO3 removal efficiency and 81% ammonia recovery efficiency at a current density of 20 mA cm−2 with the energy consumption of 19.78 kWh kg−1(NH4)2SO4, which was only 1 % of that of the ER-MC system. The AE-ER-MC system showed stable treatment performance in consecutive cycles with the ammonia recovery efficiency at near 80%. The direct electron transfer reaction was mainly responsible for the NO3 reduction at Fe2O3-Ov at cathode. The DFT calculation results shows that NO3 more favorably adsorbed at Fe2O3-Ov and could undergo spontaneous bond breaking of NO bond with the formation of NO2, bypassing the conversion of NO3 to *NO3H step in typical NO3 reduction process. In present combined system, the hardness ions were hardly present in the catholyte since the repulsion effect of basic anion exchange resin. And the developed system did not suffer from the cathode passivation, potential risk of membrane fouling, secondary pollution from high-salt regenerant. Generally, the AE-ER-MC system offers a meaningful paradigm for the design of energy-efficient and resource-recovery technique toward low-concentration NO3 water treatment.
本研究采用阴离子交换-电解反应器-膜接触器耦合系统(AE-ER-MC)从低浓度NO3 -污染的地下水中高效回收(NH4)2SO4,其中碱性阴离子交换树脂选择性去除地下水中的NO3 -, NO3 -排放的树脂被NaCl阴极液再生,Fe2O3-Ov阴极上的NO3 -还原产生氨,并通过膜剥离工艺回收。在电流密度为20 mA cm−2时,AE-ER-MC系统的NO3−去除率为98%,氨回收率为81%,能耗为19.78 kWh kg−1(NH4)2SO4,仅为ER-MC系统的1%。AE-ER-MC系统在连续循环中表现出稳定的处理性能,氨回收率接近80%。在Fe2O3-Ov阴极上,直接电子转移反应是NO3−还原的主要原因。DFT计算结果表明,NO3−在Fe2O3-Ov上的吸附更有利,NO2−的形成使NO键自发断键,绕过了典型NO3−还原过程中由NO3−转化为*NO3H的步骤。在本组合体系中,由于碱性阴离子交换树脂的排斥作用,硬离子在阴极液中几乎不存在。该系统不存在阴极钝化、膜污染、高盐再生剂二次污染等问题。总的来说,AE-ER-MC系统为低浓度NO3−水处理的节能和资源回收技术设计提供了有意义的范例。
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引用次数: 0
A gadolinium-doped polyphenol-boron nanodrug for improved boron neutron capture therapy 一种用于改进硼中子俘获治疗的掺钆多酚硼纳米药物
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-25 DOI: 10.1016/j.jcis.2026.139970
Gongde Lan , Yuchen Liu , Hongyuan Mao , Han Yu , Weicheng Huang , Pengxiang Chen , Xin Chen , Qingxu Song , Yufeng Cheng , Yuxia Luan
Boron neutron capture therapy (BNCT) is a promising strategy for selective tumor eradication. However, the clinical application of the boron delivery agent p‑boronophenylalanine (BPA) is limited by challenges such as poor solubility, suboptimal tumor accumulation, and lack of effective imaging capabilities. Here, we present a metal polyphenol-based boron nanodrug (EB@Gd NPs), designed to address these challenges and enhance the efficacy of BNCT. Self-assembled from epigallocatechin-3-gallate (EGCG), BPA, and gadolinium ions (Gd3+), the EB@Gd NPs exhibit significantly improved tumor targeting and enable real-time magnetic resonance imaging (MRI). These nanoparticles show enhanced tumor accumulation, with MRI providing dynamic insights into boron distribution, thus aiding in determining optimal timing for neutron irradiation. Furthermore, EGCG potentiates therapeutic effect of BNCT by inhibiting DNA repair and promoting efficient DNA double-strand breaks. Therefore, the EB@Gd NPs demonstrate potent tumor growth inhibition in BNCT, holding great potential for improving precision and efficacy of BNCT in cancer therapy.
硼中子俘获治疗(BNCT)是一种很有前途的选择性肿瘤根除策略。然而,硼递送剂对硼苯丙氨酸(BPA)的临床应用受到诸如溶解度差、非理想肿瘤积聚和缺乏有效成像能力等挑战的限制。在这里,我们提出了一种金属多酚基硼纳米药物(EB@Gd NPs),旨在解决这些挑战并提高BNCT的疗效。由表没食子儿茶素-3-没食子酸酯(EGCG)、BPA和钆离子(Gd3+)自组装而成的EB@Gd NPs具有显著提高的肿瘤靶向性,并可实现实时磁共振成像(MRI)。这些纳米颗粒显示出增强的肿瘤积聚,MRI提供了硼分布的动态信息,从而有助于确定中子照射的最佳时机。此外,EGCG通过抑制DNA修复和促进有效的DNA双链断裂来增强BNCT的治疗效果。因此,EB@Gd NPs在BNCT中表现出强大的肿瘤生长抑制作用,在提高BNCT在癌症治疗中的准确性和有效性方面具有很大的潜力。
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引用次数: 0
Biomimetic lipid nanoparticles for RNA delivery to breast cancer microenvironment cells by enhanced homotypic and heterotypic adhesion 通过增强同型和异型粘附,用于RNA递送到乳腺癌微环境细胞的仿生脂质纳米颗粒。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-24 DOI: 10.1016/j.jcis.2026.139972
Stefania Garbujo , Chiara Baioni , Andrea Banfi , Leonardo Bolis , Giulia Bonvini , Elena Del Favero , Paola Gagni , Alessandro Gori , Linda Barbieri , Marco Davide Giustra , Giulia Tomaino , Lucia Morelli , Clizia Chinello , Fulvio Magni , Lucia Salvioni , Miriam Colombo , Davide Prosperi
Lipid nanoparticles (LNPs) have emerged as a clinically validated nonviral RNA delivery system. However, their limited tumor targeting remains challenging in oncology. In this work, LNPs were functionally integrated with cancer cell membrane components to enhance their targeting capabilities. The natural composition of tumor membranes was leveraged to promote both homotypic and heterotypic adhesion, exploiting cancer cell self-recognition and interactions with stromal cells in the tumor microenvironment. A biomimetic nanocarrier was developed by cloaking RNA-loaded LNPs with nanoghosts obtained from the membrane of triple negative breast cancer cells. Nanoghosts were dye-labeled and comprehensively characterized in terms of size, surface charge, protein composition, and membrane sidedness. The functional orientation of nanoghost membrane-associated proteins mediated homotypic binding with 4 T1 cells and heterotypic recognition of functionally validated cancer-associated fibroblasts and exhibited higher affinity for the latter, as confirmed through flow cytometry and confocal microscopy. RNA-LNPs were incorporated into nanoghosts using ultrasound-assisted fusion, yielding stable biomimetic LNPs with a multilamellar mRNA-LNP core enveloped by a nanoghost shell, as confirmed by Small-Angle X-ray Scattering. While uncoated LNPs showed negligible interaction with heterotypic cells, biomimetic LNPs displayed strong affinity for cancer-associated fibroblasts, enabling efficient internalization and RNA transfection. Additionally, the biomimetic coating enhanced LNP uptake in homotypic 4 T1 cells, resulting in significantly improved biological activity compared to uncoated LNPs. This work provides proof of concept that RNA-LNPs can be effectively integrated into biomimetic carriers to enable dual targeting of tumor and stromal cells. The enhanced selectivity and delivery performance of biomimetic LNPs highlight their therapeutic potential for overcoming stromal barriers in desmoplastic tumors such as triple negative breast cancer.
脂质纳米颗粒(LNPs)已成为一种临床验证的非病毒RNA递送系统。然而,它们有限的肿瘤靶向性在肿瘤学领域仍然具有挑战性。在这项工作中,LNPs与癌细胞膜组分进行功能整合,以增强其靶向能力。利用肿瘤膜的天然成分来促进同型和异型粘附,利用癌细胞的自我识别以及与肿瘤微环境中的基质细胞的相互作用。利用从三阴性乳腺癌细胞膜中获得的纳米宿主包裹负载rna的LNPs,制备了一种仿生纳米载体。纳米宿主被染料标记,并在大小、表面电荷、蛋白质组成和膜侧性方面进行了全面表征。通过流式细胞术和共聚焦显微镜证实,纳米宿主膜相关蛋白的功能取向介导了与4 T1细胞的同型结合和功能验证的癌症相关成纤维细胞的异型识别,并对后者表现出更高的亲和力。小角度x射线散射证实,通过超声辅助融合将RNA-LNPs整合到纳米宿主中,得到了稳定的仿生LNPs,其多层mRNA-LNP核被纳米宿主壳包裹。虽然未包被LNPs与异型细胞的相互作用可以忽略不计,但仿生LNPs对癌症相关成纤维细胞表现出很强的亲和力,能够有效地内化和RNA转染。此外,与未包被LNPs相比,仿生包被增强了LNP在同型4 T1细胞中的摄取,从而显著提高了LNP的生物活性。这项工作证明了RNA-LNPs可以有效地整合到仿生载体中,从而实现肿瘤和基质细胞的双重靶向。仿生LNPs增强的选择性和递送性能突出了它们在克服间质屏障治疗结丝增生肿瘤(如三阴性乳腺癌)方面的潜力。
{"title":"Biomimetic lipid nanoparticles for RNA delivery to breast cancer microenvironment cells by enhanced homotypic and heterotypic adhesion","authors":"Stefania Garbujo ,&nbsp;Chiara Baioni ,&nbsp;Andrea Banfi ,&nbsp;Leonardo Bolis ,&nbsp;Giulia Bonvini ,&nbsp;Elena Del Favero ,&nbsp;Paola Gagni ,&nbsp;Alessandro Gori ,&nbsp;Linda Barbieri ,&nbsp;Marco Davide Giustra ,&nbsp;Giulia Tomaino ,&nbsp;Lucia Morelli ,&nbsp;Clizia Chinello ,&nbsp;Fulvio Magni ,&nbsp;Lucia Salvioni ,&nbsp;Miriam Colombo ,&nbsp;Davide Prosperi","doi":"10.1016/j.jcis.2026.139972","DOIUrl":"10.1016/j.jcis.2026.139972","url":null,"abstract":"<div><div>Lipid nanoparticles (LNPs) have emerged as a clinically validated nonviral RNA delivery system. However, their limited tumor targeting remains challenging in oncology. In this work, LNPs were functionally integrated with cancer cell membrane components to enhance their targeting capabilities. The natural composition of tumor membranes was leveraged to promote both homotypic and heterotypic adhesion, exploiting cancer cell self-recognition and interactions with stromal cells in the tumor microenvironment. A biomimetic nanocarrier was developed by cloaking RNA-loaded LNPs with nanoghosts obtained from the membrane of triple negative breast cancer cells. Nanoghosts were dye-labeled and comprehensively characterized in terms of size, surface charge, protein composition, and membrane sidedness. The functional orientation of nanoghost membrane-associated proteins mediated homotypic binding with 4 T1 cells and heterotypic recognition of functionally validated cancer-associated fibroblasts and exhibited higher affinity for the latter, as confirmed through flow cytometry and confocal microscopy. RNA-LNPs were incorporated into nanoghosts using ultrasound-assisted fusion, yielding stable biomimetic LNPs with a multilamellar mRNA-LNP core enveloped by a nanoghost shell, as confirmed by Small-Angle X-ray Scattering. While uncoated LNPs showed negligible interaction with heterotypic cells, biomimetic LNPs displayed strong affinity for cancer-associated fibroblasts, enabling efficient internalization and RNA transfection. Additionally, the biomimetic coating enhanced LNP uptake in homotypic 4 T1 cells, resulting in significantly improved biological activity compared to uncoated LNPs. This work provides proof of concept that RNA-LNPs can be effectively integrated into biomimetic carriers to enable dual targeting of tumor and stromal cells. The enhanced selectivity and delivery performance of biomimetic LNPs highlight their therapeutic potential for overcoming stromal barriers in desmoplastic tumors such as triple negative breast cancer.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"709 ","pages":"Article 139972"},"PeriodicalIF":9.7,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146083748","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Bioinspired tough, anti-freezing, and anti-drying organohydrogel via photocurable 3D printing for flexible electronics 生物灵感坚韧,防冻,防干燥的有机水凝胶通过光固化3D打印柔性电子产品
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-24 DOI: 10.1016/j.jcis.2026.139976
Hanqiang Zhang , Peiren Wang , Zhenning Di , Xin Zhou , Haibo Ding , Zhonglin Xu , Yupeng Xu , Lize Cai , Jiqing Chen , Zihuan Chen , Hua Xu , Ji Li
Conductive hydrogels hold great potential for applications in flexible electronics due to their excellent flexibility and conductivity. However, hydrogels typically have poor mechanical properties and are prone to freezing and drying under extreme conditions, while a lack of shaping approaches severely restricts their capacity to form complex geometries and customized functionalities for high-performance devices. Herein, inspired by the synergistic mechanisms observed in arctic brown algae, we propose a novel strategy integrating ionic crosslinking, ion hydration, and hydrogen bonding networks for one-step photocurable 3D printing of organohydrogels. The bioinspired design of the organohydrogel provides remarkable tensile strength (4.65 MPa), excellent transparency (97%), high ionic conductivity (0.34 S/m), and ultrawide temperature tolerance (down to −50 °C), and is enabled by the synergistic mechanism to achieve rapid 3D printing (<2 s/100 μm). The 3D-printed organohydrogel is capable of versatile sensing platform of stress, motion, respiration, and temperature with exceptional adaptability. Customized cryo-tolerant sensors enable encrypted Morse code communication via strain-responsive signals at −50 °C. Utilizing inherent triboelectric and piezoresistive properties, we developed smart insoles with spatial pressure mapping for real-time gait and posture monitoring. This work lays the foundation for advanced human-machine interactions, soft robotics, customizable flexible electronics, and health monitors for applications in extreme environments.
导电性水凝胶由于其优异的柔韧性和导电性,在柔性电子领域具有很大的应用潜力。然而,水凝胶通常具有较差的机械性能,并且在极端条件下容易冻结和干燥,而缺乏成型方法严重限制了其形成复杂几何形状和高性能设备定制功能的能力。在此,受在北极褐藻中观察到的协同机制的启发,我们提出了一种结合离子交联、离子水化和氢键网络的新策略,用于一步光固化有机水凝胶的3D打印。仿生设计的有机水凝胶具有卓越的抗拉强度(4.65 MPa)、优异的透明度(97%)、高离子电导率(0.34 S/m)和超宽的耐温性(低至- 50°C),并通过协同机制实现快速3D打印(<2 S/ 100 μm)。3d打印的有机水凝胶具有应力、运动、呼吸和温度的多功能传感平台,具有特殊的适应性。定制的耐寒传感器可以在- 50°C下通过应变响应信号加密莫尔斯电码通信。利用固有的摩擦电和压阻特性,我们开发了具有空间压力映射的智能鞋垫,用于实时监测步态和姿势。这项工作为先进的人机交互、软机器人、可定制的柔性电子设备和用于极端环境应用的健康监视器奠定了基础。
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引用次数: 0
Water-stable Bi-based perovskite for efficient photocatalytic hydrogen evolution in aqueous media 水稳定铋基钙钛矿在水介质中高效光催化析氢
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-24 DOI: 10.1016/j.jcis.2026.139975
Chun Sun , Jiazhi Cui , Zhengtao Qiu , Jiabao Bai , Chao Fan , Dan Huang , Guohua Jia
Perovskites have attracted considerable interest as potential photocatalysts for sustainable hydrogen generation. Nonetheless, their intrinsic instability in aqueous media significantly constrains their practical deployment in photocatalytic hydrogen evolution. To address this challenge, we propose a versatile strategy for stabilizing Cs3Bi2Br9 (CBB) perovskite photocatalysts through combining zwitterionic ligand encapsulation with Sn4+ doping. The zwitterionic ligand, synthesized by reacting 4-bromobutyric acid (BBA) with oleylamine (OLA), was employed to passivate the perovskite surface by anchoring to both Bi3+ and Br sites, effectively mitigating surface defects. Notably, Sn4+ doping is essential for aqueous stability, as the incorporation of Sn4+ not only enhances the intrinsic stability of CBB but also reinforces the binding affinity of surface ligands. As a result, the Sn4+-doped CBB (CBBSx) with ligand encapsulation demonstrates remarkable stability, retaining its structural integrity in water for over six months and withstanding more than three cycles of photocatalytic testing. Importantly, this strategy demonstrates considerable generality, as it can be readily extended to the synthesis of other halide perovskites. Specifically, the MoSx-loaded Sn4+:Cs3Bi2BrxI9-x (MoSx/CBBIS0.2) composite achieves a remarkable hydrogen evolution rate of 18.2 mmol h−1 g−1, which represents the highest performance reported to date among Bi-based perovskite photocatalysts.
钙钛矿作为可持续制氢的潜在光催化剂引起了人们的极大兴趣。然而,它们在水介质中的固有不稳定性极大地限制了它们在光催化析氢中的实际应用。为了解决这一挑战,我们提出了一种稳定Cs3Bi2Br9 (CBB)钙钛矿光催化剂的通用策略,即将两性离子配体包封与Sn4+掺杂相结合。由4-溴丁酸(BBA)与油胺(OLA)反应合成的阴离子配体通过锚定在Bi3+和Br -位点上来钝化钙钛矿表面,有效地减轻了表面缺陷。值得注意的是,Sn4+的掺杂对CBB的水稳定性至关重要,因为Sn4+的掺入不仅增强了CBB的固有稳定性,而且增强了表面配体的结合亲和力。结果表明,配体包封的Sn4+掺杂CBB (CBBSx)表现出显著的稳定性,在水中保持其结构完整性超过6个月,并经受了超过3次的光催化测试循环。重要的是,这种策略显示出相当大的普遍性,因为它可以很容易地扩展到其他卤化物钙钛矿的合成。具体而言,负载MoSx的Sn4+:Cs3Bi2BrxI9-x (MoSx/CBBIS0.2)复合材料的析氢速率为18.2 mmol h−1 g−1,是迄今为止报道的铋基钙钛矿光催化剂中性能最高的。
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引用次数: 0
Modulating mRNA carrier efficacy through the molecular catwalk of ionizable nitrogens in lipidic domains 通过脂质结构域中可电离氮的分子通道调节mRNA载体效能。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-24 DOI: 10.1016/j.jcis.2026.139973
Melina Grau , Nora Martini , Sophie Thalmayr , Miriam Höhn , Olivia M. Merkel , Benjamin Winkeljann , Ernst Wagner
Double pH-responsive lipo-xenopeptides (lipo-XPs) with varying lipo amino fatty acid (LAF) to succinoyl tetraethylene pentamine (Stp) ratios and two distinct bundle and U-shape topologies were identified as highly effective carriers for mRNA delivery. Physicochemical properties and transfection efficacies of the carriers are strongly influenced by the lipid tail length and position of the ionizable nitrogen within the LAF domain, defined as the “molecular catwalk”. Bundles containing short LAFs (8Oc, 12Bu) and U-shapes with medium-length LAFs (12Oc) and centrally placed tertiary amines exhibited strongest activity, while extreme catwalk variants (2Hd, 16Et) proved ineffective. These trends establish clear structure-activity relationships which were subjected to further mechanistic investigation. Mechanistic studies revealed topology- and LAF-specific differences in requirement for endosomal acidification and corresponding escape, indicating that different molecular arrangements trigger distinct biological mechanisms. All-atom molecular dynamics simulations at the water-octanol interface further contextualized these behaviors by resolving how protonation reshapes carrier polarity, hydration and interfacial localization. Protonation-induced relocation was more pronounced in bundles, consistent with their higher LAF content, whereas 12Oc-based U-shapes displayed more moderate shifts and retained greater octanol affinity at neutral pH. Variations in nitrogen placement modulated interfacial enrichment and hydrogen bonding, providing molecular comprehension for the experimentally observed activity profiles across the LAF-Stp carrier library.
具有不同脂质氨基酸(LAF)与琥珀酰四乙烯五胺(Stp)比率的双ph响应型脂质外肽(脂质xps)和两种不同的束状和u形拓扑结构被确定为mRNA递送的高效载体。载体的物理化学性质和转染效率受到脂质尾长度和LAF结构域内可电离氮的位置的强烈影响,这被定义为“分子天桥”。含有短LAFs (8Oc, 12Bu)和u型中长度LAFs (12Oc)和中心放置叔胺的束表现出最强的活性,而极端的t型变体(2Hd, 16Et)被证明无效。这些趋势建立了明确的结构-活性关系,有待进一步的机理研究。机制研究揭示了拓扑和af特异性对内体酸化和相应逃逸的需求存在差异,表明不同的分子排列触发不同的生物学机制。水-辛醇界面的全原子分子动力学模拟通过解析质子化如何重塑载流子极性、水合作用和界面定位,进一步将这些行为置于背景中。质子诱导的重定位在束中更为明显,这与LAF含量较高一致,而基于12oc的u形表现出更温和的位移,在中性ph下保持更大的正醇亲和力。氮放置的变化调节了界面富集和氢键,为实验观察到的LAF- stp载体库的活性谱提供了分子理解。
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引用次数: 0
Surface hydroxyl groups steer the degradation pathway for high-efficiency mineralization of toluene on BiOClBr: mechanistic insights from combined experimental and DFT studies 表面羟基引导降解途径,使甲苯在BiOClBr上高效矿化:来自实验和DFT联合研究的机制见解
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-24 DOI: 10.1016/j.jcis.2026.139974
Yang Li , Yiwen Zeng, Guanghua Cai, Xiaofei Li, Jian Yang, Ximei Fan
Toluene, a typical volatile organic compound (VOC), poses significant challenges in photocatalytic degradation due to low mineralization efficiency and the accumulation of hazardous intermediates. Here, we demonstrate that surface hydroxyls on BiOClBr solid solutions act as a molecular switch to steer the degradation pathway toward complete mineralization with high selectivity. Experimental results reveal that hydroxyl-rich BiOClBr samples, synthesized via a modified solvothermal method, exhibit a strengthened built-in electric field, enhanced charge separation efficiency, and facilitated generation of reactive oxygen species (ROS) such as ·O2 and ·OH compared to hydroxyl-deficient counterparts. In situ spectroscopic analysis combined with density functional theory (DFT) calculations indicate that surface hydroxyls introduce additional electron states, facilitating charge transfer and promoting the adsorption and activation of toluene at the methyl group. This pathway sequentially converts toluene to benzyl alcohol, benzaldehyde, and benzoic acid, ultimately leading to complete mineralization into CO2 while suppressing the formation of phenolic byproducts. This work provides mechanistic insights into surface hydroxyl-mediated charge dynamics and ROS balance, offering a strategic foundation for designing tailored catalysts for efficient aromatic VOC remediation.
甲苯是一种典型的挥发性有机化合物(VOC),由于矿化效率低和有害中间体的积累,给光催化降解带来了很大的挑战。在这里,我们证明了生物clbr固溶体上的表面羟基作为一个分子开关,以高选择性地引导降解途径走向完全矿化。实验结果表明,与缺乏羟基的样品相比,通过改进的溶剂热法合成的富含羟基的BiOClBr样品具有增强的内置电场,增强的电荷分离效率,并且促进了活性氧(ROS)的生成,如·O2−和·OH。原位光谱分析结合密度泛函理论(DFT)计算表明,表面羟基引入了额外的电子态,促进了电荷转移,促进了甲苯在甲基上的吸附和活化。该途径依次将甲苯转化为苯甲醇、苯甲醛和苯甲酸,最终完全矿化为CO2,同时抑制酚类副产物的形成。这项工作为表面羟基介导的电荷动力学和ROS平衡提供了机制见解,为设计适合芳香性VOC的高效修复催化剂提供了战略基础。
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引用次数: 0
Viscosity and dynamic surface tension measurement: A guideline for appropriate measurement 粘度和动态表面张力测量:适当测量的指南。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-23 DOI: 10.1016/j.jcis.2026.139929
Vivek Kumar , JSM Quintero , Aleksey Baldygin , Paul Molina , Thomas Willers , Prashant R. Waghmare
Dynamic surface tension measurements play a critical role in interfacial activities for liquids with varying viscosities. Understanding the rate at which the interface attains the equilibrium, for surface tension measurements, after the formation of a new interface is of significant interest. Although surface tension is independent of dynamic viscosity, the time required for a new surface to form (equilibrium/relaxation time) is influenced by viscosity. The measured surface tension value is accurate only once these viscous effects have subsided. Therefore, the relaxation time represents the minimum surface age value achievable during the measurement process. We experimentally established the minimum surface age needed to measure the dynamic and static surface tension of a fluid with a specific viscosity using three widely used methods: the Pendant drop method, the Wilhelmy plate method, and the Bubble pressure method. We propose a guideline with a phase plot that helps to choose the most suitable method and the youngest achievable surface age for an accurate measurement, independent of viscous effects. This guideline enables users in diverse applications such as 3D printed clothing, spray paint, coating, etc., to accurately measure dynamic and static surface tension without being influenced by viscosity effects.
动态表面张力测量对不同粘度液体的界面活性起着至关重要的作用。了解界面在形成新界面后达到平衡的速率,对于表面张力测量具有重要意义。虽然表面张力与动态粘度无关,但形成新表面所需的时间(平衡/松弛时间)受到粘度的影响。只有当这些粘性效应消退时,测量的表面张力值才准确。因此,松弛时间代表了测量过程中可以达到的最小表面年龄值。我们通过实验建立了测量具有特定粘度的流体的动态和静态表面张力所需的最小表面年龄,使用了三种广泛使用的方法:Pendant drop法、Wilhelmy plate法和Bubble pressure法。我们提出了一个相图的指导方针,有助于选择最合适的方法和最年轻的表面年龄,以进行准确的测量,独立于粘性效应。该指南使用户能够在3D打印服装,喷漆,涂层等不同应用中准确测量动态和静态表面张力,而不受粘度效应的影响。
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引用次数: 0
期刊
Journal of Colloid and Interface Science
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