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Membrane-free sequential paired electrosynthesis of 1,4-hydroquinone from phenol over a self-supported electrocatalytic electrode 在自支撑电催化电极上以苯酚为原料进行无膜顺序配对电合成 1,4-氢醌
Pub Date : 2024-08-30 DOI: 10.1039/d4im00067f
Wei-Ling Zhang, Ya-Jing Li, Yingchun He, Shao Zhang, Haohong Li, Huidong Zheng, Qi-Long Zhu
Sequential paired electrosynthesis capable of the production of organic chemicals through a series of electrochemical reactions that occur consecutively and in pairs are of high significance. Herein, a three-dimensional porous carbon felt-loaded PbO2 electrode (PbO2/CF) with a self-supported nanostructure was fabricated using a double-cathode electrodeposition method, which served as an efficient electrocatalyst enabling the unique sequential paired electrosynthesis of 1,4-hydroquinone (1,4-HQ) from phenol in a membrane-free electrolytic cell. In such an exotic paired electrolysis system, phenol is first oxidized to p-benzoquinone at the anode, which is subsequently reduced to 1,4-HQ at the cathode. The as-obtained PbO2/CF electrode exhibited a remarkable electrochemical performance, achieving impressive conversion and selectivity of 94.5% and 72.1%, respectively, for the conversion of phenol to 1,4-HQ. This exceptional performance can be attributed to the open porous self-supported structure of the PbO2/CF electrode, which improves the active site exposure and substrate adsorption capability and reduces mass and charge transfer resistance. Furthermore, the catalyst electrode well maintained its structure integrity even after 140 hours of long-term use, further highlighting its promising application for the electrosynthesis of 1,4-HQ. Moreover, this sequential paired electrosynthesis strategy can be further extended to other substrates with electron-withdrawing/donating groups over the PbO2/CF electrode. The proof of concept in this innovative sequential paired electrosynthesis could provide a sustainable and efficient way to produce various desired organic compounds.
通过一系列成对连续发生的电化学反应生产有机化学品的顺序配对电合成具有重要意义。本文采用双阴极电沉积法制备了一种具有自支撑纳米结构的三维多孔碳毡负载 PbO2 电极(PbO2/CF),并将其作为一种高效电催化剂,在无膜电解池中以苯酚为原料进行了独特的 1,4-hydroquinone (1,4-HQ) 顺序配对电合成。在这种奇特的成对电解系统中,苯酚首先在阳极被氧化成对苯醌,然后在阴极被还原成 1,4-HQ。获得的 PbO2/CF 电极表现出卓越的电化学性能,将苯酚转化为 1,4-HQ 的转化率和选择性分别达到 94.5% 和 72.1%,令人印象深刻。这种优异的性能归功于 PbO2/CF 电极的开放式多孔自支撑结构,它改善了活性位点的暴露和底物吸附能力,降低了质量和电荷转移阻力。此外,催化剂电极在长期使用 140 小时后仍能很好地保持其结构完整性,这进一步凸显了其在 1,4-HQ 电合成中的应用前景。此外,这种顺序配对电合成策略还可进一步扩展到 PbO2/CF 电极上其他具有电子吸收/捐献基团的基质。这种创新的序贯配对电合成的概念验证可为生产各种所需有机化合物提供一种可持续的高效方法。
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引用次数: 0
Toward a low-cost uranium-adsorbing material based on nonwoven fabrics and photografting technology 基于无纺布和光固化技术的低成本铀吸附材料
Pub Date : 2024-08-07 DOI: 10.1039/d4im00034j
Zhiwei Zhong, Yanbin Huang, Wantai Yang
Amidoxime-functionalized polymeric adsorbents have attracted great interest for uranium extraction from seawater. However, the current graft polymerization method is time-consuming (2–6 h), wasteful in reagent, and hence not economical. Here, amidoxime-functionalized adsorbents based on low-cost polypropylene melt-blown nonwoven fabric (MBF) are produced by a simple, fast and also low-cost surface photografting technology, by which more than 80% of reagents can be saved and grafting time can be reduced to 3 min. The fabricated adsorbents retain their mechanical properties and exhibit excellent uranium adsorption properties, with a maximum uranium adsorption capacity of 400 mg g−1 when the monomer ratio of AN to AA is 8 : 2. Moreover, we showed that the adsorbents could be either reused or simply incinerated for uranium recovery. The photografting technology has great potential for low-cost, continuous industrial production of uranium-adsorbing material.
脒肟功能化聚合物吸附剂在从海水中提取铀方面引起了极大的兴趣。然而,目前的接枝聚合方法耗时长(2-6 小时)、浪费试剂,因此并不经济。本文采用简单、快速、低成本的表面光接枝技术,制备了基于低成本聚丙烯熔喷非织造布(MBF)的脒肟功能化吸附剂,可节省 80% 以上的试剂,并将接枝时间缩短至 3 分钟。当 AN 与 AA 的单体比为 8 : 2 时,最大铀吸附量为 400 mg g-1。此外,我们还发现这些吸附剂既可重复使用,也可直接焚烧以回收铀。光固化技术在低成本、连续工业化生产铀吸附材料方面具有巨大潜力。
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引用次数: 0
Depolymerization of PET with Ethanol by Homogeneous Iron Catalysts Applied for Exclusive Chemical Recycling of Cloth Waste 应用于布废料独家化学回收的均相铁催化剂用乙醇解聚 PET
Pub Date : 2024-08-06 DOI: 10.1039/d4im00081a
Nor Wahida Binti Awang, Muhammad Aidel Bin Ratno Hadiyono, Mohamed Abdellatif, Kotohiro Nomura
Acid-, base-free depolymerization of poly(ethylene terephthalate) (PET) with ethanol by FeCl3, FeBr3 (1.0-5.0 mol%) gave diethyl terephthalate (DET) and ethylene glycol (EG) exclusively (98->99 %, 160-180 ºC), and FeCl3 showed better catalyst performance in terms of the activity. The FeCl3 catalyst enabled to proceed exclusive, selective depolymerization of PET from the textile waste to afford DET (and recovered cotton waste), strongly suggesting the possibility of chemical recycling of cloth waste by the transesterification in this catalysis.
用 FeCl3、FeBr3(1.0-5.0 mol%)对聚对苯二甲酸乙二醇酯(PET)与乙醇进行无酸、无碱解聚,只得到对苯二甲酸乙二醇酯(DET)和乙二醇(EG)(98->99 %,160-180 ºC),FeCl3 的催化剂活性表现更好。FeCl3 催化剂能使纺织废料中的 PET 独家进行选择性解聚,生成 DET(和回收的棉花废料),这有力地说明了在该催化反应中通过酯交换反应对纺织废料进行化学回收利用的可能性。
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引用次数: 0
Introduction to the themed issue on liquid-based materials: novel concepts from fundamentals to applications 液基材料:从基础到应用的新概念》专题介绍
Pub Date : 2024-08-01 DOI: 10.1039/D4IM90008A
Xu Hou and Jungmok Seo

A graphical abstract is available for this content

本内容有图解摘要
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引用次数: 0
Recent advances on cellulose-based solid polymer electrolytes 纤维素基固体聚合物电解质的最新进展
Pub Date : 2024-07-29 DOI: 10.1039/d4im00066h
Xiaoqi Gong, Jiasheng Wang, Linfeng Zhong, Guangsheng Qi, Fujie Liu, Yaozheng Pan, Fan Yang, Xiaotong Wang, Jing Li, Longjie Li, Cong Liu, Dingshan Yu
Solid-state Li-metal batteries with solid-state electrolytes have attracted increasing attention due to their high energy density and intrinsically high safety. Among diverse available solid-state electrolytes, cellulose-based solid polymer electrolytes (CSPEs) are particularly attractive and have showcased great promise because of their multiple merits including abundant reserves, rich polar groups, chemical stability and high flexibility. This review surveys currently-developed solid electrolytes based on modified cellulose and their composites with diverse organic and inorganic fillers. Common preparation methods for solid electrolyte membranes are in-detail discussed, followed by a sequential overview of various modification and compositing strategies for improving Li-ion transport in CSPEs, and a summary of the current existing challenges and future prospects of CSPEs to achieve high-performance solid batteries.
采用固态电解质的固态锂金属电池因其高能量密度和固有的高安全性而受到越来越多的关注。在现有的各种固态电解质中,纤维素基固体聚合物电解质(CSPEs)因其储量丰富、极性基团丰富、化学性质稳定和灵活性高等多重优点而特别具有吸引力,并展现出广阔的前景。本综述介绍了目前开发的基于改性纤维素的固体电解质及其与各种有机和无机填料的复合材料。文章详细讨论了固体电解质膜的常见制备方法,随后依次概述了用于改善 CSPE 中锂离子传输的各种改性和复合策略,并总结了 CSPE 在实现高性能固体电池方面的现有挑战和未来前景。
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引用次数: 0
Outstanding Reviewers for Industrial Chemistry & Materials in 2023 2023 年《工业化学与材料》杰出审稿人
Pub Date : 2024-07-29 DOI: 10.1039/D4IM90007C

This article celebrates the Outstanding Reviewers for Industrial Chemistry & Materials in 2023.

本文旨在表彰 2023 年《工业化学与材料》的杰出审稿人。
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引用次数: 0
Improved Voltammetric Discrimination of Acetaminophen and Uric Acid in Urine Using CoO Biochar Nanocomposite 利用氧化钴生物炭纳米复合材料提高尿液中对乙酰氨基酚和尿酸的伏安法鉴别能力
Pub Date : 2024-07-18 DOI: 10.1039/d4im00069b
Yihan Zhang, Yiliyasi Baikeli, Zehong Gao, Xamxikamar Mamat, Longyi Chen
Overuse of acetaminophen (APAP) has become a severe societal burden in recent years. The rapid and reliable detection of urinal APAP concentration can offer certain guidance for better management of APAP usage. This study explored the electrochemical sensing application of a novel electrocatalyst prepared from the biomass of Elaeagnus Angustifolia gum. The biomass was first activated by ferric chloride to form a porous biomass carbon material (FBC). Then synthesized cobalt oxide cracked nanoplate by alkali precipitation and calcination approach were hybridized onto the biomass carbon via facile sonication process. The electrocatalyst of CoO-FBC was characterized by scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS), element mapping, transmission electron microscopy (TEM) and high resolution TEM, X-ray photoelectron spectroscopy (XPS), X-ray powder diffraction (XRD), thermo gravimetric analysis (TGA), Raman spectroscopy, and nitrogen adsorption/desorption analysis. CoO-FBC modified glassy carbon electrode (CoO-FBC/GCE) was characterized by various electrochemical methods including cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and differential pulse voltammetry (DPV). CoO-FBC/GCE sensor was used to measure APAP in pH 7.0, 0.1 M phosphate buffered saline (PBS) with two linear sensing range from 1 μM to 10 μM and 10 μM to 100 μM, sensitivity of 25.89 μA μM-1 cm-2 and 10.04 μA μM-1 cm-2, and limit of detection of 0.46 μM. The unavoidable inteference in measuring APAP is the inherent uric acid in urine. Uric acid and APAP exhibited adjacent and sometimes unseparable voltametric peak. This CoO-FBC/GCE sensor is capable to distinguish APAP from uric acid and to measure APAP in human urine sample with good recovery. This CoO-FBC/GCE sensor has promising application in clinical diagnosis and environmental detection.
近年来,对乙酰氨基酚(APAP)的过度使用已成为严重的社会负担。快速可靠地检测尿液中对乙酰氨基酚(APAP)的浓度可为更好地管理对乙酰氨基酚(APAP)的使用提供一定的指导。本研究探索了一种新型电催化剂的电化学传感应用,该催化剂由桉树胶生物质制备而成。首先用氯化铁对生物质进行活化,形成多孔生物质碳材料(FBC)。然后通过碱沉淀和煅烧方法合成氧化钴裂解纳米板,并通过简便的超声过程杂化到生物质碳上。通过扫描电子显微镜(SEM)和能量色散 X 射线光谱(EDS)、元素图谱、透射电子显微镜(TEM)和高分辨率 TEM、X 射线光电子能谱(XPS)、X 射线粉末衍射(XRD)、热重分析(TGA)、拉曼光谱和氮吸附/解吸分析,对 CoO-FBC 电催化剂进行了表征。CoO-FBC 修饰的玻璃碳电极(CoO-FBC/GCE)通过各种电化学方法进行了表征,包括循环伏安法(CV)、电化学阻抗谱法(EIS)和微分脉冲伏安法(DPV)。CoO-FBC/GCE 传感器用于测量 pH 值为 7.0、0.1 M 磷酸盐缓冲盐水(PBS)中的 APAP,其线性感应范围分别为 1 μM 至 10 μM 和 10 μM 至 100 μM,灵敏度分别为 25.89 μA μM-1 cm-2 和 10.04 μA μM-1 cm-2,检出限为 0.46 μM。测量 APAP 不可避免的干扰因素是尿液中固有的尿酸。尿酸和 APAP 的伏安峰相邻,有时甚至无法分隔。这种 CoO-FBC/GCE 传感器能够区分 APAP 和尿酸,并以良好的回收率测量人体尿样中的 APAP。这种 CoO-FBC/GCE 传感器有望应用于临床诊断和环境检测。
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引用次数: 0
Progress on fiber engineering for fabric innovation in ecological hydrophobic design and multifunctional applications 纤维工程在生态疏水设计和多功能应用织物创新方面的进展
Pub Date : 2024-07-11 DOI: 10.1039/D4IM00048J
Wei Li, Libing Yang, Jianying Huang, Chan Zheng, Yu Chen, Yunbo Li, Dapeng Yang, Shuhui Li, Zhong Chen, Weilong Cai and Yuekun Lai

The application of fluorinated coatings on textiles has garnered substantial research interest over the past years, owing to their ability to endow fabrics with exceptional hydrophobic characteristics, thereby mitigating issues associated with high moisture absorption and susceptibility to contamination. Nevertheless, the deployment of fluorinated substances has been proscribed due to concerns regarding their ecological impact and potential human toxicity. Consequently, there has been a burgeoning demand for hydrophobic textile alternatives derived from non-fluorinated, natural materials that are both sustainable and environmentally benign. This paper presents a thorough overview of the advancements in the development and functionalization of eco-friendly, hydrophobic textiles. Initially, the natural materials and their derivatives utilized in the creation of superhydrophobic textiles are delineated, including cellulose, lignin and chitosan, among others. Subsequently, methodologies for crafting efficient, stable, and resilient hydrophobic textiles are elucidated, encompassing conventional techniques as well as novel, inventive concepts. Furthermore, the current state of research and the obstacles faced in the evolution of multifunctional textiles based on superhydrophobic fabrics are examined. In conclusion, this discussion presents incisive insights into the impending direction of advancements in functional textiles.

Keywords: Eco-friendly; Superhydrophobic; Bioinspired; Multifunctional textiles; Natural materials.

由于含氟涂层能够赋予织物特殊的疏水特性,从而缓解与高吸湿性和易污染性相关的问题,因此在过去几年中,含氟涂层在纺织品上的应用引起了大量研究兴趣。然而,由于担心含氟物质对生态环境的影响和对人体的潜在毒性,含氟物质一直被禁止使用。因此,对由非含氟天然材料制成的、可持续发展且对环境无害的疏水性纺织品替代品的需求急剧增长。本文全面概述了在开发和功能化环保型疏水性纺织品方面取得的进展。首先,介绍了用于制造超疏水纺织品的天然材料及其衍生物,包括纤维素、木质素、壳聚糖等。随后,阐明了制作高效、稳定和弹性疏水性纺织品的方法,包括传统技术和新颖、创造性的概念。此外,还探讨了基于超疏水性织物的多功能纺织品的研究现状和发展过程中面临的障碍。总之,本讨论对功能性纺织品即将出现的发展方向提出了精辟的见解。
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引用次数: 0
Influence of surfactants on selective mechanical separation of fine active materials used in high temperature electrolyzers contributing to circular economy† 表面活性剂对促进循环经济的精细高温电解槽活性材料选择性机械分离的影响
Pub Date : 2024-07-09 DOI: 10.1039/D4IM00044G
Sohyun Ahn, Suvarna Patil and Martin Rudolph

As one of the promising hydrogen production technologies, the development of water electrolysis systems including recycling of their functional components is actively investigated. However, the focus lies on energy and chemical intensive metallurgical operations and less on mechanical separation processes in most studies. Here, an innovative surfactant-based separation process (using CTAB and SDS) is investigated to contribute to developing a selective physical separation process for ultrafine particles used in high temperature water electrolyzers (composed of NiO, LSM, ZrO2, and YSZ). Their different surface charge in alkaline solutions influences the adsorption of surfactants on particle surfaces as well as the modification of particulate wettability, which is a key separation feature. Through the observations of changes in surface charge and wetting behavior in the presence of surfactants, a feasibility of liquid–liquid particle separation (LLPS) is evaluated. The performance of LLPS with model particle mixtures shows the potential of selective separation with recovery of NiO in the organic phase, while the rest of the particles remain in the aqueous phase. Perovskite LSM is not considered in this system because it shows a high possibility of being recovered by magnetic separation. The proposed process can be further optimized by increasing the phase separation stages, and further research is needed on the NiO phase, which showed exceptional behavior in the presence of the surfactants.

Keywords: Fine particle separation; Solid oxide electrolyzer; Recycling; Particle surface modification.

作为前景广阔的制氢技术之一,水电解系统的开发(包括其功能部件的回收利用)正受到积极研究。然而,大多数研究的重点在于能源和化学品密集型冶金操作,而较少关注机械分离过程。在此,我们正在研究一种基于表面活性剂的创新分离工艺(使用 CTAB 和 SDS),以帮助开发一种选择性物理分离工艺,用于高温水电解槽中使用的超细颗粒(由 NiO、LSM、ZrO2 和 YSZ 组成)。它们在碱性溶液中的不同表面电荷会影响表面活性剂在颗粒表面的吸附以及颗粒润湿性的改变,而润湿性是关键的分离特征。通过观察表面活性剂存在时表面电荷和润湿行为的变化,评估了液-液颗粒分离(LLPS)的可行性。模型颗粒混合物的液-液颗粒分离性能表明,有机相中的氧化镍具有选择性分离的潜力,而其余颗粒则留在水相中。本系统中没有考虑包晶锂辉石,因为它很有可能被磁分离回收。建议的工艺可以通过增加相分离阶段来进一步优化,同时还需要对在表面活性剂存在下表现出特殊行为的氧化镍相进行进一步研究。
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引用次数: 0
Room-temperature rapid synthesis of hierarchically porous ZIF-93 for effective adsorption of volatile organic compounds 室温下快速合成分层多孔 ZIF-93 以有效吸附挥发性有机化合物
Pub Date : 2024-07-04 DOI: 10.1039/d4im00033a
Haiqi Zhang, Kaikai Zhao, Weibiao Guo, Kuan Liang, Jingjing Li, Xu Li, Qianjun Deng, Xuejun Xu, Huixia Chao, Hongxia Xi, ChongXiong Duan
Facile synthesis conditions, abundant hierarchical porosity, and high space-time yields (STYs) are prerequisites for the commercial application of zeolitic imidazolate frameworks (ZIFs). However, these prerequisites are rarely achieved simultaneously. Herein, a green and versatile strategy to rapidly synthesize hierarchically porous ZIFs (HP-ZIFs) was developed using an alkali as a deprotonating agent. The synthesis conditions were room temperature and ambient pressure in an aqueous solution, and the synthesis time could be reduced to 1 min. The produced HP-ZIFs had hierarchically porous structures with mesopores and macropores interconnected with micropores. The STY for HP-ZIFs was up to 9670 kg m-3 d-1, at least 712 times the previously reported values. In addition, the porosity and morphology of the produced HP-ZIFs could be fine-tuned by controlling the synthesis parameters (e.g., reaction time, molar ratios, metal source, and alkali source). Compared with conventional ZIFs, the adsorption performance of the as-synthesized HP-ZIFs for p-xylene and n-hexane was significantly improved. Positron annihilation lifetime spectroscopy (PALS) was utilized to study the pore properties, and the adsorption behavior of HP-ZIFs on guest molecules was investigated using density functional theory (DFT) simulations. This strategy shows significant promise for the large-scale industrial production of desirable HP-ZIFs for adsorption applications.
简便的合成条件、丰富的分层孔隙率和高时空产率(STYs)是沸石咪唑啉框架(ZIFs)商业化应用的先决条件。然而,这些先决条件很少能同时实现。在此,我们利用碱作为去质子剂,开发了一种快速合成分层多孔沸石咪唑啉框架(HP-ZIFs)的绿色多功能策略。合成条件为室温和环境压力下的水溶液,合成时间可缩短至 1 分钟。制得的 HP-ZIF 具有分层多孔结构,中孔和大孔与微孔相互连接。HP-ZIF 的 STY 高达 9670 kg m-3 d-1,是之前报道值的至少 712 倍。此外,还可以通过控制合成参数(如反应时间、摩尔比、金属源和碱源)对所制得的 HP-ZIF 的孔隙率和形态进行微调。与传统的 ZIF 相比,合成的 HP-ZIF 对对二甲苯和正己烷的吸附性能显著提高。正电子湮灭寿命光谱(PALS)被用来研究孔隙特性,密度泛函理论(DFT)模拟则研究了 HP-ZIFs 对客体分子的吸附行为。这一策略为大规模工业化生产理想的吸附应用 HP-ZIFs 带来了巨大希望。
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引用次数: 0
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Industrial Chemistry & Materials
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