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Direct Current Pulse Atmospheric Pressure Plasma Jet Treatment on Electrochemically Deposited NiFe/Carbon Paper and Its Potential Application in an Anion-Exchange Membrane Water Electrolyzer. 电化学沉积镍铁/碳纸上的直流脉冲大气压等离子体射流处理及其在阴离子交换膜水电解槽中的潜在应用。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-30 DOI: 10.1021/acs.langmuir.4c01169
Shuo-En Yu, Yu-Lun Su, I-Chih Ni, Yi-Cheng Chuang, Cheng-Che Hsu, Chih-I Wu, Yong-Song Chen, I-Chun Cheng, Jian-Zhang Chen

An atmospheric pressure plasma jet (APPJ) is used to process electrochemically deposited NiFe on carbon paper (NiFe/CP). The reactive oxygen and nitrogen species (RONs) of the APPJ modify the surface properties, chemical bonding types, and oxidation states of the material at the self-sustained temperature of the APPJ. The APPJ treatment further enhances the hydrophilicity and creates a higher disorder level in the carbon material. Moreover, the metal carbide bonds of NiFe/CP formed in the electrochemical deposition (ED) process are converted to metal oxide bonds after APPJ processing. The potential application of APPJ treatment on NiFe/CP in alkaline water electrolysis is demonstrated. With more oxygen-containing species and better hydrophilicity after APPJ treatment, APPJ-treated NiFe/CP is applied as the electrocatalyst for the oxygen evolution reaction (OER) in alkaline water electrolysis. APPJ-treated NiFe/CP is also used in a custom-made anion-exchange membrane water electrolyzer (AEMWE); this should contribute toward realizing the practical large-scale application of AEM for hydrogen production.

常压等离子体射流(APPJ)用于处理电化学沉积在碳纸上的镍铁(NiFe/CP)。在 APPJ 的自持温度下,APPJ 的活性氧和氮物种(RONs)会改变材料的表面性质、化学键类型和氧化态。APPJ 处理进一步增强了碳材料的亲水性,并产生了更高的无序度。此外,在电化学沉积(ED)过程中形成的 NiFe/CP 金属碳化物键在经过 APPJ 处理后会转化为金属氧化物键。APPJ 处理在碱性水电解中对 NiFe/CP 的潜在应用得到了证实。经过 APPJ 处理的 NiFe/CP 含氧物种更多,亲水性更好,因此可用作碱性水电解中氧进化反应(OER)的电催化剂。经 APPJ 处理的 NiFe/CP 还被用于定制的阴离子交换膜水电解槽(AEMWE),这将有助于实现 AEM 在制氢领域的实际大规模应用。
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引用次数: 0
Precise Control Light Emission of PVDF-CH3NH3PbBr3–xClx Nanocrystalline Films Using a Cl–(CH3OH)n System 利用 Cl-(CH3OH)n 系统精确控制 PVDF-CH3NH3PbBr3-xClx 纳米晶薄膜的光辐射
IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-29 DOI: 10.1021/acs.langmuir.4c01505
Rui Wang, Chengwei Wang, Yanan Liao, Kai Liu, Weian Wang, Fangfang Wang, Lei Wang, Chunxiang Xu, Feng Chen
Methylammonium lead halide perovskites with highly efficient pure-color or white-light generation have gained increasing scientific interest and promote the development of a great commercial opportunity in displays, lighting, and other applications. However, the poor stabilities, lead toxicity, and unfriendly solvents and ligands in the growth process severely restrict their commercial application. Here, we proposed a green method for preparing uniform and stable polymer-encapsulated photoluminescence (PL) tunable CH3NH3PbBr3–xClx NC thin films at room temperature. Utilizing the swelling effect between alcohol compounds and organic polymers and the ionization of NaCl in methanol solution, the anion exchange process can be achieved rapidly within 7 min. Moreover, the PL wavelengths of the CH3NH3PbBr3–xClx NCs films were precisely tuned with steps as fine as 2 nm. Experimental results showed that NaCl dissolved in methanol solution can form Cl(CH3OH)n, which brings ionized Cl into the polymer-encapsulated CH3NH3PbBr3 NCs film for CH3NH3PbBr3–xClx NCs film growth. Based on the swelling and anion exchange dynamics, a modified NaCl-CH3OH-MABr solution system was developed to trigger CH3NH3PbBr3–xClx NCs film PL emission tuning from 528 to 463 nm with several-fold intensity enhancement. The realization of precisely controlled photoluminescence from the perovskite nanocrystal film would have wide applications in the optical and imaging fields.
具有高效纯色或白光生成能力的甲基卤化铅铵盐过氧化物晶石已经获得了越来越多的科学兴趣,并在显示器、照明和其他应用领域带来了巨大的商业发展机遇。然而,生长过程中存在的稳定性差、铅毒性以及不友好的溶剂和配体等问题严重限制了它们的商业应用。在此,我们提出了一种在室温下制备均匀稳定的聚合物封装光致发光(PL)可调 CH3NH3PbBr3-xClx NC 薄膜的绿色方法。利用醇类化合物与有机聚合物之间的溶胀效应以及 NaCl 在甲醇溶液中的电离作用,阴离子交换过程可在 7 分钟内快速完成。此外,CH3NH3PbBr3-xClx NCs 薄膜的聚光波长可以精确地调整到 2 nm。实验结果表明,NaCl溶解在甲醇溶液中会形成Cl-(CH3OH)n,从而将电离的Cl带入聚合物封装的CH3NH3PbBr3-xClx NCs薄膜中,促进CH3NH3PbBr3-xClx NCs薄膜的生长。基于溶胀和阴离子交换动力学,开发了一种改良的 NaCl-CH3OH-MABr 溶液体系,以触发 CH3NH3PbBr3-xClx NCs 薄膜的光致发光从 528 纳米调谐到 463 纳米,强度增强了数倍。实现精确控制过氧化物纳米晶体薄膜的光致发光将在光学和成像领域得到广泛应用。
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引用次数: 0
Chiral Supramolecular Self-Assembly Catalysts with Enhanced Metal Ion Interaction for Higher Enantioselectivity. 增强金属离子相互作用的手性超分子自组装催化剂可提高对映选择性。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-28 DOI: 10.1021/acs.langmuir.4c01415
Cong Gao, Yemeng Sun, Zhengjie Miao, Shipeng Chen, Zheng Xi, Qingqing Sun, Jie Han, Rong Guo

Understanding the interaction between metal ions as catalytic centers and supramolecular scaffolds as chiral substrates plays an important role in developing chiral supramolecular catalysts with high enantioselectivity. Herein, we found that compared with l-norleucine chiral amphiphile (l-NorC16), l-methionine chiral amphiphile (l-MetC16) with the only heteroatom of S site difference in the hydrophilic group can form a similar supramolecular chiral nanoribbon (NR) with the bilayer structure through the self-assembly approach; yet, the interaction between the Cu(II) ion catalytic centers and supramolecular scaffolds is reinforced, favoring the chirality transfer and therefore enhancing their catalytic enantioselectivity of Diels-Alder reaction from 23% [l-NorC16-NR-Cu(II)] to 78% [l-MetC16-NR-Cu(II)]. Our work demonstrates a new strategy from the perspective of strengthening the metal ion-supramolecular scaffold interaction for the preparation of chiral supramolecular catalysts with good catalytic enantioselectivity.

了解作为催化中心的金属离子与作为手性底物的超分子支架之间的相互作用对于开发具有高对映选择性的手性超分子催化剂具有重要作用。在本文中,我们发现与 l-正亮氨酸手性双亲化合物(l-NorC16)相比,亲水基团中仅有 S 位点杂原子差异的 l-蛋氨酸手性双亲化合物(l-MetC16)可以通过自组装方法形成具有双层结构的类似超分子手性纳米带(NR);然而,Cu(II) 离子催化中心与超分子支架之间的相互作用得到了加强,有利于手性转移,从而提高了它们在 Diels-Alder 反应中的催化对映体选择性,从 23% [l-NorC16-NR-Cu(II)] 提高到 78% [l-MetC16-NR-Cu(II)]。我们的工作从加强金属离子-超分子支架相互作用的角度展示了制备具有良好催化对映选择性的手性超分子催化剂的新策略。
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引用次数: 0
Controlled Release of Amphoteric Surfactant from Mesoporous Nanosilica To Enhance Natural Gas Production at High Temperatures 从介孔纳米二氧化硅中控制两性表面活性剂的释放以提高高温下的天然气产量
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-28 DOI: 10.1021/acs.langmuir.4c01813
Jiang Yang*, Rongrong Fan, Yingcheng Li, Xiujuan He and Xiaolong Zhao*, 

Surfactants are widely used as foaming agents to remove liquid accumulation in gas wells, enhancing natural gas production. The surfactant used in traditional foam sticks was dissolved and released as foam in a short period, especially at elevated downhole temperatures. This often requires the addition of foam sticks to maintain foam. To solve this problem, this study studies the utilization of nano silica to incorporate the amphoteric surfactant, cocamidopropyl betaine (CAB), into the mesoporous structure of silica nanocomposite as foam sticks for controlled release of CAB. Mesoporous nano silica was prepared by a sol–gel acid-catalyzed process with a silica precursor. The formation of nanocomposite solid sticks containing the amphoteric surfactant was achieved by aging and drying. The composite was characterized by various techniques: infrared spectroscopy, thermogravimetric analysis, energy-dispersive spectrometry, scanning electron microscopy, transmission electron microscopy, and small-angle X-ray diffraction. Results showed that 49.3% of CAB was encapsulated within the mesoporous structure of 30–50 nm nano silica. CAB release over time in aqueous solution at 130 °C exhibited 10.1% surfactant left in the nanocomposite after 72 h, as determined by thermal analysis. Surfactant release was systematically evaluated through foam performance tests. The study revealed that CAB could be control-released over 168 h via CAB diffusion from mesoporous silica. This study provides a longer-lasting foam method to enhance gas production by utilizing mesoporous silica as a control release medium for gas well deliquification.

表面活性剂被广泛用作发泡剂,用于清除气井中的积液,提高天然气产量。传统泡沫棒中使用的表面活性剂会在短时间内溶解并以泡沫形式释放出来,尤其是在井下温度升高的情况下。这往往需要添加泡沫棒来维持泡沫。为解决这一问题,本研究利用纳米二氧化硅将两性表面活性剂椰油酰胺丙基甜菜碱(CAB)加入纳米二氧化硅复合材料的介孔结构中,作为泡沫棒控制 CAB 的释放。介孔纳米二氧化硅是用二氧化硅前驱体在溶胶-凝胶酸催化过程中制备的。通过老化和干燥,形成了含有两性表面活性剂的纳米复合固体泡沫棒。复合材料的表征采用了多种技术:红外光谱、热重分析、能量色散光谱、扫描电子显微镜、透射电子显微镜和小角 X 射线衍射。结果表明,49.3% 的 CAB 被包裹在 30-50 纳米的纳米二氧化硅介孔结构中。根据热分析测定,在 130 °C 的水溶液中,随着时间的推移,CAB 的释放量在 72 小时后显示,纳米复合材料中的表面活性剂残留量为 10.1%。通过泡沫性能测试系统地评估了表面活性剂的释放情况。研究表明,通过 CAB 从介孔二氧化硅中的扩散,CAB 可在 168 小时内得到控制释放。这项研究提供了一种更持久的泡沫方法,利用介孔二氧化硅作为气井脱液的控制释放介质,提高天然气产量。
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引用次数: 0
Optical and Chemical Measurements of Solvated Electrons Produced in Plasma Electrolysis with a Water Cathode 水阴极等离子电解过程中产生的溶解电子的光学和化学测量结果
IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-28 DOI: 10.1021/acs.langmuir.4c00639
Daniel C. Martin, Daniel T. Elg, Hernan E. Delgado, Hoang M. Nguyen, Paul Rumbach, David M. Bartels, David B. Go
It is known that glow discharges with a water anode inject and form solvated electrons at the plasma–liquid interface, driving a wide variety of reduction reactions. However, in systems with a water cathode, the production and role of solvated electrons are less clear. Here, we present evidence for the direct detection of solvated electrons produced at the interface of an argon plasma and a water cathode via absorption spectroscopy. We further quantify their yield using the dissociative electron attachment of chloroacetate, measuring a yield of 1.04 ± 0.59 electrons per incident ion, corresponding to approximately 100% faradaic efficiency. Additionally, we estimate a yield of 2.09 ± 0.93 hydroxyl radicals per incident ion. Comparison of this yield with other findings in the literature supports that these hydroxyl radicals are likely formed directly in the liquid phase rather than by diffusion from the vapor phase.
众所周知,带有水阳极的辉光放电会在等离子体-液体界面注入并形成溶电子,从而推动各种还原反应。然而,在带水阴极的系统中,溶电子的产生和作用却不太清楚。在这里,我们提出了通过吸收光谱直接检测氩等离子体和水阴极界面上产生的溶电子的证据。我们利用氯乙酸的离解电子附着进一步量化了电子的产率,测得每个入射离子的产率为 1.04 ± 0.59 个电子,相当于约 100%的法拉第效率。此外,我们估计每个入射离子产生 2.09 ± 0.93 个羟自由基。将这一产率与文献中的其他研究结果进行比较后发现,这些羟基自由基很可能是直接在液相中形成的,而不是通过气相扩散形成的。
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引用次数: 0
Effect of Mixed Morphology (Simple Cubic, Face-Centered Cubic, and Body-Centered Cubic)-Based Electrodes on the Electric Double Layer Capacitance of Supercapacitors. 混合形态(简单立方体、面心立方体和体心立方体)电极对超级电容器双电层电容的影响
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-28 DOI: 10.1021/acs.langmuir.4c00664
Ravi Nigam, Kamal K Kar

Supercapacitors store energy due to the formation of an electric double layer (EDL) at the interface of the electrodes and electrolyte. The present article deals with the finite element study of equilibrium electric double layer capacitance (EDLC) in the mixed morphology electrodes comprising all three fundamental crystal structures, simple cubic (SC), body-centered cubic (BCC), and face-centered cubic morphologies (FCC). Mesoporous-activated carbon forms the electrode in the supercapacitor with (C2H5)4NBF4/propylene carbonate organic electrolyte. Electrochemical interference is clearly demonstrated in the supercapacitors with the formation of the potential bands, as in the case of interference theory due to the increasing packing factor. The effects of electrode thickness varying from a wide range of 50 nm to 0.04 mm on specific EDLC have been discussed in detail. The interfacial geometry of the unit cell in contact with the electrolyte is the most important parameter determining the properties of the EDL. The critical thickness of the electrodes is 1.71 μm in all the morphologies. Polarization increases the interfacial potential and leads to EDL formation. The Stern layer specific capacitance is 167.6 μF cm-2 in all the morphologies. The maximum capacitance is in the decreasing order of interfacial geometry, as FCC > BCC > SC, dependent on the packing factor. The minimum transmittance in all the morphologies is 98.35%, with the constant figure of merit at higher electrode thickness having applications in the chip interconnects. The transient analysis shows that the interfacial current decreases with increasing polarization in the EDL. The capacitance also decreases with the increase of the scan rate.

超级电容器通过在电极和电解液界面上形成电双层(EDL)来储存能量。本文探讨了由简单立方(SC)、体心立方(BCC)和面心立方(FCC)三种基本晶体结构组成的混合形态电极中平衡双电层电容(EDLC)的有限元研究。介孔活性炭构成了超级电容器的电极,并带有 (C2H5)4NBF4/ 碳酸丙烯有机电解质。电化学干扰在超级电容器中得到了明显的体现,电位带的形成与干扰理论的情况一样,是由于填料系数的增加造成的。我们详细讨论了电极厚度从 50 纳米到 0.04 毫米不等对特定 EDLC 的影响。与电解质接触的单胞界面几何形状是决定 EDL 特性的最重要参数。在所有形态中,电极的临界厚度都是 1.71 μm。极化会增加界面电势并导致 EDL 的形成。在所有形态中,斯特恩层的比电容都是 167.6 μF cm-2。最大电容随界面几何形状的减小而减小,即 FCC > BCC > SC,这取决于堆积因子。所有形态的最小透射率均为 98.35%,在芯片互连中应用时,较高电极厚度下的性能指标不变。瞬态分析表明,界面电流随着 EDL 极化程度的增加而减小。电容也随着扫描速率的增加而减小。
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引用次数: 0
Reusable CS-Ca@PEI/CuMnO2 Hydrogel Beads for Peroxymonosulfate-Activated Degradation of Congo Red 可重复使用的 CS-Ca@PEI/CuMnO2 水凝胶珠用于过一硫酸盐激活降解刚果红
IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-28 DOI: 10.1021/acs.langmuir.4c00659
Jinyan Yang, Zhaoxing Hu, Wenhui Rao, Yijun Xie, Chuanbai Yu
Metal oxides can activate peroxymonosulfate (PMS) for the catalytic degradation of organic dyes. However, achieving high catalytic efficiency, structural stability, ease of recovery, and recyclability remains challenging for both research and practical applications. To address these requirements, a bimetallic oxide, CuMnO2, was synthesized using a simple hydrothermal approach and was encapsulated to create hydrogel beads, CS-Ca@PEI/CuMnO2. Subsequently, CS-Ca@PEI/CuMnO2 was used to activate PMS and establish a solid–liquid heterogeneous oxidation system (CS-Ca@PEI/CuMnO2/PMS) for the degradation of Congo red (CR). The effects of various parameters such as different systems, catalyst dosages, initial pH values, PMS concentrations, temperatures, and anion types on the catalytic degradation properties of CS-Ca@PEI/CuMnO2 for CR were systematically evaluated. The results indicated that CS-Ca@PEI/CuMnO2 has exceptional degradation capacity, achieving 91.0% degradation of CR at pH 7. After three degradation cycles, the catalyst maintained an 86.9% degradation efficiency compared to its original performance, highlighting its robust structural stability. The presence of reactive radicals, specifically 1O2 and O2, were confirmed through quenching experiments, X-ray photoelectron spectroscopy (XPS), and electron paramagnetic resonance spectroscopy (EPR). Liquid chromatography-tandem mass spectrometry (LC-MS) revealed ten proposed intermediates in the catalytic degradation process. Due to its exceptional catalytic performance, structural durability, recyclability, and ease of retrieval, the catalyst shows great potential for effectively removing organic pollutants from industrial wastewater.
金属氧化物可激活过氧单硫酸盐(PMS),对有机染料进行催化降解。然而,要实现高催化效率、结构稳定性、易回收性和可回收性,对于研究和实际应用来说仍然具有挑战性。为了满足这些要求,我们采用简单的水热法合成了双金属氧化物 CuMnO2,并将其封装成水凝胶珠 CS-Ca@PEI/CuMnO2。随后,CS-Ca@PEI/CuMnO2 被用于活化 PMS,并建立了一个用于降解刚果红(CR)的固液异构氧化体系(CS-Ca@PEI/CuMnO2/PMS)。系统评估了不同体系、催化剂用量、初始 pH 值、PMS 浓度、温度和阴离子类型等参数对 CS-Ca@PEI/CuMnO2 催化降解刚果红性能的影响。结果表明,CS-Ca@PEI/CuMnO2 具有优异的降解能力,在 pH 值为 7 时对 CR 的降解率达到 91.0%。通过淬灭实验、X 射线光电子能谱(XPS)和电子顺磁共振能谱(EPR)证实了活性自由基的存在,特别是 1O2 和 -O2-。液相色谱-串联质谱法(LC-MS)揭示了催化降解过程中的十种拟中间产物。由于该催化剂具有催化性能优异、结构耐用、可回收利用和易于回收等特点,因此在有效去除工业废水中的有机污染物方面显示出巨大的潜力。
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引用次数: 0
Wastewater Treatment Using High-Performance In Situ Formed Double-Heterojunction Janus Photocatalyst Microparticles Shaped via a Microfluidic Device 使用通过微流体设备成型的高性能原位形成双异质结 Janus 光催化剂微颗粒处理废水
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-27 DOI: 10.1021/acs.langmuir.4c01163
Hassanin M. Ali, Farzaneh Arabpour Roghabadi*, Vahid Ahmadi, Ahdieh Amjadi and Iraj Ghaedi, 

In this work, a heterogeneous photocatalysis system is fabricated for treating wastewater containing organic dyes and pharmaceutical substances. Double-heterojunction Janus photocatalysts are formed on the surface of size-tunable polydimethylsiloxane (PDMS) microparticles shaped via simple and low-cost coflow microfluidic devices. Ag0/Ag0-TiO2/TiO2 Janus-like photocatalysts are synthesized on the surface of porous PDMS microparticles as the support in which the metal–semiconductor heterojunction of Ag0/Ag0-TiO2 and the second heterojunction of Ag0-TiO2/TiO2 are created in situ, leading to the formation of Ag0/Ag0-TiO2/TiO2@PDMS photocatalysis systems. To form the heterojunctions on the PDMS surface, the polymer chain etching method is employed as a desired strategy to have half of the TiO2 nanoparticles on the surface of microparticles, which are treated by a Ag source. Using salt additives and the etching method, PDMS microparticles are made porous, providing more surface area for photoreactions. Surprisingly, the highest decomposition efficiencies of 94.4 and 91.1% are achieved for rhodamine B(RhB) and tetracycline (TC), respectively, under visible light for 60 min pH 11, a light source at a distance of 2 cm, 5 mM AgNO3, 10 wt % TiO2, 7 wt % NaCl, and 20 gm/L photocatalyst, which are conditions that result in the best performance for RhB degradation. Regarding the stability of the photocatalysts, no significant change is observed in the performance after five cycles.

这项研究制造了一种异相光催化系统,用于处理含有有机染料和药物的废水。通过简单、低成本的共流微流体装置,在尺寸可调的聚二甲基硅氧烷(PDMS)微颗粒表面形成了双异质结 Janus 光催化剂。Ag0/Ag0-TiO2/TiO2 类 Janus 光催化剂是在多孔 PDMS 微颗粒表面合成的,PDMS 微颗粒是 Ag0/Ag0-TiO2 的金属半导体异质结和 Ag0-TiO2/TiO2 的第二异质结的载体,从而形成 Ag0/Ag0-TiO2/TiO2@PDMS 光催化系统。为了在 PDMS 表面形成异质结,一种理想的策略是采用聚合物链蚀刻法,使一半的 TiO2 纳米颗粒位于经 Ag 源处理的微颗粒表面。利用盐添加剂和蚀刻方法,PDMS 微颗粒变得多孔,为光反应提供了更多的表面积。令人惊讶的是,在可见光 60 分钟、pH 值为 11、光源距离为 2 厘米、5 mM AgNO3、10 wt % TiO2、7 wt % NaCl 和 20 gm/L 光催化剂条件下,罗丹明 B(RhB)和四环素(TC)的最高分解效率分别达到 94.4% 和 91.1%,这也是 RhB 降解性能最好的条件。在光催化剂的稳定性方面,经过五个循环后,其性能没有明显变化。
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引用次数: 0
Capturing Enzyme-Loaded Diblock Copolymer Vesicles Using an Aldehyde-Functionalized Hydrophilic Polymer Brush 使用醛官能化亲水聚合物刷捕捉载酶二嵌段共聚物囊泡
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-27 DOI: 10.1021/acs.langmuir.4c01561
Georgios Karchilakis, Spyridon Varlas, Edwin C. Johnson*, Oleta Norvilaite, Matthew A. H. Farmer, George Sanderson, Graham J. Leggett and Steven P. Armes*, 

Compared to lipids, block copolymer vesicles are potentially robust nanocontainers for enzymes owing to their enhanced chemical stability, particularly in challenging environments. Herein we report that cis-diol-functional diblock copolymer vesicles can be chemically adsorbed onto a hydrophilic aldehyde-functional polymer brush via acetal bond formation under mild conditions (pH 5.5, 20 °C). Quartz crystal microbalance studies indicated an adsorbed amount, Γ, of 158 mg m–2 for vesicle adsorption onto such brushes, whereas negligible adsorption (Γ = 0.1 mg m–2) was observed for a control experiment conducted using a cis-diol-functionalized brush. Scanning electron microscopy and ellipsometry studies indicated a mean surface coverage of around 30% at the brush surface, which suggests reasonably efficient chemical adsorption. Importantly, such vesicles can be conveniently loaded with a model enzyme (horseradish peroxidase, HRP) using an aqueous polymerization-induced self-assembly formulation. Moreover, the immobilized vesicles remained permeable toward small molecules while retaining their enzyme payload. The enzymatic activity of such HRP-loaded vesicles was demonstrated using a well-established colorimetric assay. In principle, this efficient vesicle-on-brush strategy can be applied to a wide range of enzymes and functional proteins for the design of next-generation immobilized nanoreactors for enzyme-mediated catalysis.

与脂质相比,嵌段共聚物囊泡具有更强的化学稳定性,特别是在具有挑战性的环境中,因此可能成为酶的稳健纳米载体。在此,我们报告了顺式二元醇官能团二嵌段共聚物囊泡可在温和的条件下(pH 值为 5.5,温度为 20 °C)通过乙缩醛键的形成化学吸附到亲水性醛官能团聚合物刷上。石英晶体微天平研究表明,囊泡在这种刷子上的吸附量Γ为 158 mg m-2,而在使用顺式二元醇功能化刷子进行的对照实验中观察到的吸附量(Γ = 0.1 mg m-2)可以忽略不计。扫描电子显微镜和椭偏仪研究表明,刷表面的平均表面覆盖率约为 30%,这表明化学吸附的效率相当高。重要的是,利用水性聚合诱导的自组装配方,这种囊泡可以方便地装载模式酶(辣根过氧化物酶,HRP)。此外,固定化的囊泡在保留酶载荷的同时,对小分子仍具有渗透性。这种负载 HRP 的囊泡的酶活性已通过一种成熟的比色测定法得到证实。原则上,这种高效的刷上囊泡策略可应用于多种酶和功能蛋白,从而设计出用于酶介导催化的下一代固定化纳米反应器。
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引用次数: 0
Imidazolium-Based Polymeric Ionic Liquids with Short Alkyl Chains as Green Corrosion Inhibitors for Mild Steel in 1 M HCl: Experimental and Theoretical Investigations 具有短烷基链的咪唑基聚合物离子液体作为 1 M HCl 中低碳钢的绿色缓蚀剂:实验和理论研究。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-27 DOI: 10.1021/acs.langmuir.4c01633
Haidong Jia, Han Jia*, Qiuxia Wang, Yingbiao Xu, Bowen Wang, Qiang Wang, Xu Li, Zhe Wang, Kaihe Lv and Pan Huang, 

A novel polymeric ionic liquid (PDBA-IL-NH2) using imidazolium ionic liquids with short alkyl chains as monomers and two control ionic liquids (PDBA-IL-OH and PIL-NH2) were synthesized. Their inhibition properties and mechanisms were explored via surface analysis, weight loss tests, electrochemical studies, and adsorption isotherm analysis. The corrosion inhibition efficiency (CIE) of PDBA-IL-NH2 gradually increased with increasing concentration, and the largest efficiency was 94.67% at 100 ppm. At the same concentration (50 ppm), the corrosion inhibition abilities of inhibitors were in the order of PDBA-IL-NH2 > PDBA-IL-OH > PIL-NH2 > IL-NH2. Based on the experimental investigation, the synergistic effect of electrostatic interaction, protonation, and electron donor–acceptor interaction facilitated the intensive entanglement and coverage of PDBA-IL-NH2 with the reticulated form on the metal, and the generated densest films protected the metal from the corrosive media. Ultimately, the theoretical results of molecular dynamics simulations and quantum chemical study were in high agreement with the experimental data, which confirmed the proposed inhibition mechanisms on the microscopic scale. This study contributed valuable perspectives to the design of efficient and ecofriendly corrosion inhibitors.

以具有短烷基链的咪唑离子液体为单体,合成了一种新型聚合物离子液体(PDBA-IL-NH2),并合成了两种对照离子液体(PDBA-IL-OH 和 PIL-NH2)。通过表面分析、失重测试、电化学研究和吸附等温线分析,探讨了它们的缓蚀性能和机理。随着浓度的增加,PDBA-IL-NH2 的缓蚀效率(CIE)逐渐升高,当浓度为 100 ppm 时,缓蚀效率最高,达到 94.67%。在相同浓度(50 ppm)下,抑制剂的缓蚀能力依次为 PDBA-IL-NH2 > PDBA-IL-OH > PIL-NH2 > IL-NH2。实验结果表明,静电作用、质子化作用和电子供体-受体作用的协同效应促进了 PDBA-IL-NH2 在金属上以网状形式密集缠结和覆盖,生成的最致密薄膜保护金属免受腐蚀介质的侵蚀。最终,分子动力学模拟和量子化学研究的理论结果与实验数据高度吻合,证实了所提出的微观抑制机制。这项研究为设计高效、环保的缓蚀剂提供了宝贵的视角。
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