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Adsorber Charge Dominates over Hydrophobic or Fluorophilic Functionalization in Influencing Adsorption of PFCA onto Polystyrene Resins 在影响聚苯乙烯树脂对全氟辛烷磺酸的吸附方面,吸附剂电荷比疏水或亲氟官能度更重要
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-06-04 DOI: 10.1002/admi.202400199
Florian Junge, Philipp Wittwer, Thomas Sommerfeld, Lennart Gehrenkemper, Christian Zoister, Philip Nickl, Matthias Koch, Björn Meermann, Rainer Haag
A systematic series of industrial-relevant polystyrene-based anion exchange resins that are functionalized with hydro- or fluorocarbon chains are compared regarding their adsorption behavior toward perfluorocarboxylic acids (PFCA) in respect to their charge, chain length, and type of chain. The results clearly show the dominance of electrostatic interactions in the adsorption process as uncharged adsorber materials showed no adsorption at all. In contrast, the charged adsorber materials showed in general a PFCA removal of 80% to 30% over the experiment depending on effluent fraction. Unexpectedly, for perfluorobutanoic acid (PFBA) the highest removal rate is found with consistently >90%. Despite observing significant benefits in the adsorption of PFCA for fluoroalkylated adsorbers in comparison to their non-fluorinated counterparts, this effect of fluoroalkylation is comparatively small and can not be clearly attributed to fluorophilic interactions between the fluoroalkyl chains. These findings help clarifying that the introduction of fluorocarbon moieties in adsorber materials is not necessary in order to remove fluorocarbon molecules from the environment.
本研究比较了一系列与工业相关的聚苯乙烯基阴离子交换树脂,这些树脂具有功能化的碳氢链或碳氟化合物链,它们对全氟羧酸(PFCA)的吸附行为与电荷、链长和链类型有关。结果清楚地表明,静电作用在吸附过程中占主导地位,因为不带电的吸附剂材料根本没有吸附作用。相反,带电吸附剂材料在实验中对全氟甲烷的去除率一般在 80% 到 30% 之间,具体取决于流出物的馏分。出乎意料的是,全氟丁酸(PFBA)的去除率最高,一直达到 90%。尽管与未氟化的吸附剂相比,氟烷基化吸附剂对全氟辛酸的吸附效果显著,但氟烷基化的影响相对较小,不能明确归因于氟烷基链之间的亲氟相互作用。这些发现有助于说明,在吸附剂材料中引入碳氟化合物分子并不是从环境中去除碳氟化合物分子的必要条件。
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引用次数: 0
A Thioether-Bridging Surface Modification of Polymeric Microspheres Offers Nonbiological Protein A-Mimetic Affinity for IgG 对聚合物微球进行硫醚桥接表面改性,可提供非生物蛋白 A 对 IgG 的仿生亲和力
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-06-03 DOI: 10.1002/admi.202301028
Takanori Kishida
Surface modification of polymeric materials to control their interaction with proteins has been studied extensively, leading to widespread bio-applications. However, the development of nonbiological, smart polymer surfaces, mimicking the recognition ability of biomolecules, remains a challenge. The present study presents a thioether-bridging surface modification of polymeric microspheres as a new approach for mimicking protein A affinity for immunoglobulin G (IgG). The bridge-modified surface is created through an epoxide linking reaction of porous polymeric microspheres with potassium thioacetate in a 2:1 molar ratio, acting as a protein A ligand, which is essential for industrial IgG purification. This surface exhibits buffer responsiveness and selective high-affinity binding to the IgG Fc region. Remarkably, a comparison among the binding behaviors of a series of thioether-modified microspheres indicates that bridging structures composed of β,β′-dihydroxysulfide play a predominant role in IgG recognition. This straightforward approach can lead to the development of economical and practical nonbiological alternatives to protein A-conjugated materials, providing solutions for various applications such as biosensors and site-specific reagents utilizing the affinity of the IgG Fc region. The improved understanding of protein interactions at bridged/non-bridged interfaces can be valuable in various applications such as implant materials and biomaterials.
为控制聚合物材料与蛋白质的相互作用而对其进行表面改性的研究已十分广泛,并已在生物领域得到广泛应用。然而,开发模仿生物分子识别能力的非生物智能聚合物表面仍然是一项挑战。本研究提出了一种硫醚桥接聚合物微球表面改性的新方法,用于模拟蛋白 A 对免疫球蛋白 G (IgG) 的亲和力。桥接改性表面是通过多孔聚合物微球与硫代乙酸钾以 2:1 的摩尔比进行环氧化物连接反应而产生的,硫代乙酸钾可作为蛋白 A 的配体,而蛋白 A 是工业 IgG 纯化所必需的。这种表面具有缓冲响应性,可选择性地与 IgG Fc 区域高亲和性结合。值得注意的是,对一系列硫醚修饰微球的结合行为进行比较后发现,由 β,β′-二羟基硫醚组成的桥接结构在 IgG 识别中起着主导作用。这种直接的方法可以开发出经济实用的非生物替代品,替代蛋白 A 结合材料,为生物传感器和利用 IgG Fc 区域亲和力的位点特异性试剂等各种应用提供解决方案。加深对桥接/非桥接界面上蛋白质相互作用的了解,对植入材料和生物材料等各种应用都很有价值。
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引用次数: 0
Synthesis and Structural Design of Graphene, Silicon and Silicon-Based Materials Including Incorporation of Graphene as Anode to Improve Electrochemical Performance in Lithium-Ion Batteries 石墨烯、硅和硅基材料的合成与结构设计,包括加入石墨烯作为阳极以提高锂离子电池的电化学性能
IF 4.3 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-03 DOI: 10.1002/admi.202301062
Jawad Reslan, Mohamed Saadaoui, Thierry Djenizian

Silicon emerges as a candidate for advancing lithium ion batteries with important roles in various applications ranging from portable electronics to electric vehicles. However, despite its theoretical capacities silicon faces challenges such as unstable cycling and limited rate performance. This thorough review examines developments in improving the electrochemical performance of silicon and graphene within the context of lithium ion batteries. The focus lies on strategies for designing and synthesizing composite materials that incorporate silicon particularly when combined with graphene. Structural aspects like particle size, morphology and porosity are carefully optimized to harness the potential of silicon based anodes and graphene. The review highlights the effects resulting from these tailored design approaches, including key factors such as capacity retention, cycling stability and rate capability of the resulting anode materials. By exploring these design paradigms this review offers a comprehensive perspective on the transformative capabilities of silicon, graphene and silicon/graphene composites. It does not highlights recent advancements but also outlines future directions for innovation and practical applications. This compilation of progress contributes to the understanding of how silicon based anodes, in lithium ion batteries have evolved from small-scale implementations to catalyzing advancements in energy utilization.

硅已成为推动锂离子电池发展的候选材料,在从便携式电子产品到电动汽车等各种应用中发挥着重要作用。然而,尽管硅具有理论容量,它却面临着循环不稳定和速率性能有限等挑战。本综述深入探讨了在锂离子电池背景下提高硅和石墨烯电化学性能的发展情况。重点在于设计和合成含有硅(尤其是与石墨烯结合时)的复合材料的策略。对粒度、形态和孔隙率等结构方面进行了精心优化,以利用硅基阳极和石墨烯的潜力。综述重点介绍了这些量身定制的设计方法所产生的效果,包括所产生的阳极材料的容量保持率、循环稳定性和速率能力等关键因素。通过探讨这些设计范例,本综述从一个全面的角度介绍了硅、石墨烯和硅/石墨烯复合材料的变革能力。它不仅强调了最新进展,还概述了创新和实际应用的未来方向。这本进展汇编有助于人们了解锂离子电池中的硅基阳极如何从小规模应用发展到催化能源利用的进步。
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引用次数: 0
Nanoscale Investigation of the Effect of Annealing Temperature on the Polarization Switching Dynamics of Hf0.5Zr0.5O2 Thin Films 退火温度对 Hf0.5Zr0.5O2 薄膜极化转换动力学影响的纳米级研究
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-05-31 DOI: 10.1002/admi.202400156
Sang Won An, Seong Bin Bae, Beomjun Kim, Yoon Ki Kim, Jaeseung Kim, Tae Hyun Jung, Jae Heon Lee, Sang Woo Lee, Yu Bin Park, Hyunjung Kim, Hyobin Yoo, Sang Mo Yang
Recently, HfO2‐based ferroelectric thin films have attracted widespread interest in developing next‐generation nonvolatile memories. To form a metastable ferroelectric orthorhombic phase in HfO2, a post‐annealing process is typically necessary. However, the microscopic mechanism underlying the effect of annealing temperature on ferroelectric domain nucleation and growth is still obscure, despite its importance in optimizing the operation speed of HfO2‐based devices. In this study, the ferroelectric properties and polarization switching of Hf0.5Zr0.5O2 thin films annealed at different temperatures (550–700 °C) are systematically investigated. Evidently, the crystal structure, remnant polarization, and dielectric constant monotonically change with annealing temperature. However, microscopic piezoresponse force microscopy images as well as macroscopic switching current measurements reveal non‐monotonic changes in the polarization switching speed with annealing temperature. This intriguing behavior is ascribed to the difference in the ferroelectric‐domain nucleation process induced by the amount of oxygen vacancies in the Hf0.5Zr0.5O2 thin films annealed at different temperatures. This work demonstrates that controlling the defect concentration of ferroelectric HfO2 by tuning the post‐annealing process is critical for optimizing device performance, particularly polarization switching speed.
最近,基于二氧化铪的铁电薄膜在开发下一代非易失性存储器方面引起了广泛的兴趣。要在 HfO2 中形成稳定的铁电正交相,通常需要进行后退火处理。然而,尽管退火温度对优化基于 HfO2 的器件的运行速度非常重要,但退火温度对铁电畴成核和生长的影响的微观机制仍不清楚。本研究系统研究了在不同温度(550-700 °C)下退火的 Hf0.5Zr0.5O2 薄膜的铁电性质和极化转换。显而易见,晶体结构、残余极化和介电常数随退火温度的变化而单调变化。然而,微观压电响应力显微镜图像和宏观开关电流测量结果表明,极化切换速度随退火温度的变化是非单调变化。这种有趣的行为归因于在不同温度下退火的 Hf0.5Zr0.5O2 薄膜中氧空位的数量所引起的铁电畴成核过程的差异。这项研究表明,通过调整退火后工艺来控制铁电 HfO2 的缺陷浓度对于优化器件性能,尤其是极化切换速度至关重要。
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引用次数: 0
Formation of a Boron‐Oxide Termination for the (100) Diamond Surface 在 (100) 金刚石表面形成氧化硼端面
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-05-30 DOI: 10.1002/admi.202400208
Alex K. Schenk, Rebecca Griffin, Anton Tadich, Daniel Roberts, Alastair Stacey
A boron‐oxide termination of the diamond (100) surface has been formed by depositing molecular boron oxide B2O3 onto the hydrogen‐terminated (100) diamond surface under ultrahigh vacuum conditions and annealing to 950 °C. The resulting termination is highly oriented and chemically homogeneous, although further optimization is required to increase the surface coverage beyond the 0.4 monolayer coverage achieved here. This work demonstrates the possibility of using molecular deposition under ultrahigh vacuum conditions for complex surface engineering of the diamond surface, and may be a first step in an alternative approach to fabricating boron doped delta layers in diamond.
在超高真空条件下,将分子氧化硼 B2O3 沉积到氢封端的(100)金刚石表面,然后退火至 950 °C,形成了金刚石(100)表面的氧化硼封端。尽管要将表面覆盖率提高到 0.4 单层覆盖率以上还需要进一步优化,但所形成的终止层具有高度定向性和化学均匀性。这项工作证明了在超高真空条件下利用分子沉积对金刚石表面进行复杂的表面工程的可能性,并可能成为在金刚石中制造掺硼三角层的替代方法的第一步。
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引用次数: 0
Enhancing Capacitance of Carbon Cloth Electrodes via Highly Conformal PEDOT Coating Fabricated by the OCVD Method Utilizing SbCl5 Oxidant 利用 SbCl5 氧化剂通过 OCVD 方法制造高共形 PEDOT 涂层,从而提高碳布电极的电容量
IF 4.3 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-29 DOI: 10.1002/admi.202400118
Meysam Heydari Gharahcheshmeh, Kafil Chowdhury

Carbon cloth shows potential for flexible energy storage electrodes but encounters challenges such as low specific capacitance and limited wettability. This study addresses these limitations by fabricating a highly conformal coating of poly(3,4-ethylenedioxythiophene) (PEDOT) around 3D carbon fibers via the oxidative chemical vapor deposition (oCVD) method, employing antimony pentachloride (SbCl5) as the oxidant. The oCVD stands out as a robust manufacturing technique for fabricating highly conformal conducting polymer films on porous structures, ensuring the preservation of geometric features and the maintenance of active sites for redox reactions. The resulting PEDOT-coated carbon cloth electrodes exhibit improved pseudocapacitance and specific capacitance compared to their pristine counterparts. Particularly, oCVD PEDOT-coated carbon cloth fabricated at various deposition temperatures exhibit a substantial 1.5- to 2.3-fold enhancement in specific capacitance compared to pristine carbon cloth. The highest specific capacitance (170.94 F g⁻¹) is attained in the oCVD PEDOT-coated carbon cloth fabricated at a deposition temperature of 80 °C, representing a 2.3-fold enhancement over its pristine counterpart. The PEDOT-coated carbon cloths demonstrate lower charge transfer resistance compared to their pristine counterparts, further confirming their superior electrochemical performance. This investigation highlights oCVD's effectiveness in fabricating highly conformal PEDOT coating on carbon cloth electrodes for electrochemical energy storage devices.

碳布显示出柔性储能电极的潜力,但也遇到了一些挑战,如低比电容和有限的润湿性。本研究采用五氯化锑(SbCl5)作为氧化剂,通过氧化化学气相沉积(oCVD)方法在三维碳纤维周围制造出高保形性的聚(3,4-亚乙二氧基噻吩)(PEDOT)涂层,从而解决了这些局限性。氧化化学气相沉积法是在多孔结构上制造高保形导电聚合物薄膜的可靠制造技术,可确保保留几何特征并维持氧化还原反应的活性位点。与原始的碳布电极相比,PEDOT 涂层碳布电极具有更高的假电容和比电容。特别是,与原始碳布相比,在不同沉积温度下制造的 oCVD PEDOT 涂层碳布的比电容大幅提高了 1.5 至 2.3 倍。在沉积温度为 80 °C 时制造的 oCVD PEDOT 涂层碳布的比电容最高(170.94 F g-¹),比原始碳布提高了 2.3 倍。与原始碳布相比,PEDOT 涂层碳布的电荷转移电阻更低,进一步证实了其卓越的电化学性能。这项研究强调了 oCVD 在为电化学储能设备的碳布电极制造高度保形的 PEDOT 涂层方面的有效性。
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引用次数: 0
Reduction of Nitroarenes Using Efficient PdRu@mSiO2 Nanocatalyst Synthesized by a One-Pot Approach 利用单锅法合成的高效 PdRu@mSiO2 纳米催化剂还原硝基arenes
IF 4.3 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-28 DOI: 10.1002/admi.202400055
Eduardo Arenas-Sánchez, Carlos Eduardo Niño González, Valeria Resendiz-Bujaidar, Elena Smolentseva, Brenda Acosta

In the present work, PdRu@mSiO2 bimetallic core-shell nanoreactors (NRs) are synthesized for the first time by a fine-tuning one-pot method. The obtained NRs are evaluated in the reduction of nitroarenes using 4-nitrophenol (4-NP), 1-chloro-4-nitrobenzene (1-Cl-4-NB), 4-nitrotoluene (4-NT) and 2,4-dinitrophenol (2,4-DNP) as reagents. The mesoporous PdRu@mSiO2 NRs with a Pd1:Ru1 molar ratio present a homogenous spherical morphology with a single nucleus per capsule. Various techniques confirm the formation of Pd-Ru alloy. The bimetallic NRs show higher catalytic activity and stability compared with the reference catalysts (free and supported nanoparticles (NPs)) and with those reported in the literature. The order of catalytic activity for studied nitroarene compounds is 4-NP>1-Cl-4-NB>2,4-DNP>4-NT. The catalytic activity of NRs is affected by inter and intramolecular interactions between the reagent molecules. The one-pot method of NRs synthesis is low-cost and effective, with possible application in the catalytic reduction of various hazardous materials.

本研究首次采用微调一锅法合成了 PdRu@mSiO2 双金属核壳纳米反应器(NRs)。以 4-硝基苯酚(4-NP)、1-氯-4-硝基苯(1-Cl-4-NB)、4-硝基甲苯(4-NT)和 2,4-二硝基苯酚(2,4-DNP)为试剂,在硝基arenes 的还原过程中对所获得的 NR 进行了评估。Pd1:Ru1 摩尔比的介孔 PdRu@mSiO2 NR 呈现出均匀的球形形态,每个胶囊有一个单核。各种技术证实了 Pd-Ru 合金的形成。与参考催化剂(游离和支撑纳米粒子(NPs))和文献报道的催化剂相比,双金属 NRs 表现出更高的催化活性和稳定性。所研究的硝基烯烃化合物的催化活性顺序为 4-NP>1-Cl-4-NB>2,4-DNP>4-NT。NR 的催化活性受试剂分子间和分子内相互作用的影响。一锅法合成 NRs 成本低、效果好,可用于催化还原各种有害物质。
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引用次数: 0
Masthead: (Adv. Mater. Interfaces 15/2024) 刊头:(Adv. Mater. Interfaces 15/2024)
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-05-28 DOI: 10.1002/admi.202470040
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引用次数: 0
Antibacterial Plasma Coating with Aggregation-Induced Emission Photosensitizers to Prevent Surgical Site Infections (Adv. Mater. Interfaces 15/2024) 使用聚集诱导发射光敏剂进行抗菌等离子涂层以预防手术部位感染(Adv. Mater. Interfaces 15/2024)
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-05-28 DOI: 10.1002/admi.202470039
Resmarani Sahu, Neethu Ninan, Ngoc Huu Nguyen, Jianzhong Wang, Manh Tuong Nguyen, Krasimir Vasilev, Vi Khanh Truong, Youhong Tang

Surgical Site Infections

In article 2400053, Krasimir Vasilev, Vi Khanh Truong, Youhong Tang, and co-workers introduce a novel antibacterial coating that integrates plasma polymerization with aggregation-induced emission photosensitizers to selectively eradicate pathogenic bacteria through light-triggered reactive oxygen species generation, presenting a promising approach to combat antibiotic resistance and reduce the global burden of surgical site infections.

手术部位感染在第 2400053 号文章中,Krasimir Vasilev、Vi Khanh Truong、Youhong Tang 及其合作者介绍了一种新型抗菌涂层,该涂层将等离子聚合与聚集诱导发射光敏剂结合在一起,通过光触发活性氧的生成选择性地消灭病原菌,为抗击抗生素耐药性和减轻全球手术部位感染负担提供了一种前景广阔的方法。
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引用次数: 0
From Fundamental Interfacial Reaction Kinetics to Macroscopic Current–Voltage Characteristics: Case Study of Solid Acid Fuel Cell Limitations and Possibilities 从基本的界面反应动力学到宏观的电流-电压特性:固体酸性燃料电池的局限性和可能性案例研究
IF 4.3 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-28 DOI: 10.1002/admi.202400119
Louis S. Wang, Sossina M. Haile

The unique properties of solid acid electrolytes, in particular CsH2PO4, are in many ways ideal for fuel cell operation. However, the technology is constrained by high cathode overpotentials. Here a simplified cathode geometry is employed to obtain the fundamental electrochemical parameters (exchange current density and charge transfer coefficient) describing the oxygen reduction reaction (ORR) at the CsH2PO4-Pt-gas interface. The parameters are incorporated into a 1D model of the voltage–current characteristics of realistic SAFC cathodes, which reproduced the measured polarization behavior of such cathodes without recourse to fitting adjustable parameters. Following this validation, the model is utilized to evaluate the impact of changes to cathode properties, microstructure, and operating conditions. Of these, the charge transfer coefficient, measured to have a value of ≈0.6 for ORR on Pt in the SAFC cathode environment, is found to have the greatest impact on power output. Nevertheless, even without material modifications, a combination of microstructural and operational modifications are identified with projected performance metrics meeting Department of Energy targets (0.8 V at 300 mA cm−2, and peak power density of 1 W cm−2), albeit at high Pt loadings. However, the analysis indicates that truly meaningful advances will likely necessitate the discovery of alternative ORR catalysts.

固体酸性电解质(尤其是 CsH2PO4)的独特性质在许多方面都非常适合燃料电池的运行。然而,该技术受到阴极过电位过高的限制。本文采用简化的阴极几何形状来获得描述 CsH2PO4-Pt 气体界面氧还原反应 (ORR) 的基本电化学参数(交换电流密度和电荷转移系数)。这些参数被纳入了现实 SAFC 阴极电压-电流特性的一维模型,该模型再现了此类阴极的实测极化行为,而无需对可调参数进行拟合。经过验证后,该模型可用于评估阴极特性、微观结构和操作条件变化的影响。其中,电荷转移系数(在 SAFC 阴极环境中铂上 ORR 的测量值≈0.6)对功率输出的影响最大。尽管如此,即使不对材料进行改性,也能确定微结构和操作改性的组合,其预计性能指标符合能源部的目标(在 300 mA cm-2 时电压为 0.8 V,峰值功率密度为 1 W cm-2),尽管是在铂负载较高的情况下。不过,分析表明,要取得真正有意义的进步,可能需要发现替代的 ORR 催化剂。
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引用次数: 0
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