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Microenvironment modulation of carbon-based single-atom catalysts for advanced oxidation processes 碳基单原子催化剂在高级氧化过程中的微环境调节
Pub Date : 2024-06-01 DOI: 10.1016/j.efmat.2025.01.002
Zhong-Shuai Zhu, Pengtang Wang, Ya Liu, Shuang Zhong, Xiaoguang Duan, Shaobin Wang
Advanced oxidation processes (AOPs) are among the most effective technologies for environmental remediation, particularly in removing recalcitrant organic pollutants from water. Carbon-based single-atom catalysts (CSACs) combine the strengths of both heterogeneous and homogeneous catalysts and maximize metal utilization via isolated metal active sites, thus fine-tuning the catalytic efficiency in AOPs via engineering molecular architecture. Atomically dispersed metal atoms are usually stabilized through ionic or covalent interactions with neighboring atoms, thus the geometric and electronic properties of CSACs are significantly affected by their local microenvironment. In this review, we explored recent advances in CSAC synthesis, emphasizing both bottom-up and top-down strategies, with a focus on microenvironment modulation. We also discussed the local microenvironment regulation of CSACs in AOPs, considering factors such as the first coordination sphere (metal center choice, site spacing/density and coordination structure) and the medium to long-range coordination (bimetallic doping, heteroatom doping/defect engineering and interface coupling). Finally, we outlined the challenges and prospects of CSAC microenvironment engineering, providing insights for advancing CSACs development in AOPs and beyond.
高级氧化工艺(AOPs)是环境修复中最有效的技术之一,特别是在去除水中难降解的有机污染物方面。碳基单原子催化剂(CSACs)结合了多相和均相催化剂的优点,通过分离的金属活性位点最大限度地利用金属,从而通过工程分子结构微调AOPs的催化效率。原子分散的金属原子通常通过与邻近原子的离子或共价相互作用来稳定,因此CSACs的几何和电子性质受到其局部微环境的显著影响。在这篇综述中,我们探讨了CSAC合成的最新进展,强调自下而上和自上而下的策略,重点是微环境调制。考虑到第一配位球(金属中心选择、位间距/密度和配位结构)和中远程配位(双金属掺杂、杂原子掺杂/缺陷工程和界面耦合)等因素,讨论了AOPs中CSACs的局部微环境调控。最后,我们概述了CSAC微环境工程的挑战和前景,为推进CSAC在AOPs及其他领域的发展提供了见解。
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引用次数: 0
Advancement factors in sludge dewatering technology for wastewater treatment from engineering and economic perspectives: A review 污泥脱水技术在污水处理中的工程与经济进展
Pub Date : 2024-06-01 DOI: 10.1016/j.efmat.2025.10.002
Ali Pirouzi, Mehdi Rahimi Asrami, Mohammad Mehdi Sabzehmeidani
The importance of the purifying municipal and industrial wastewater has increased due to a dramatically enhancing flow of sewage sludge in the last decades. There are various types of sludge including high water content, colloidal behavior, and compressibility. The sewage sludge contains about 1–5 ​wt% of solids and the remaining fraction of sludge is water (95–99 ​%). The huge amounts of sludge were produced in every year that confirmed the significant challenge in treatment of the sludge from sewage. Improving sludge dewatering reduces subsequent management and transport costs. To achieve this aim, it is necessary to investigate different sludge dewatering methods and indicators that affect sludge dewatering efficiency. In this review study, to clarify these two factors, existing technical understanding regarding sludge dewatering will be useful in practical applications, these two considerations will play a major role in the process of equipment selection and optimization measures. This study has investigated various techniques and devices for dewatering sewage sludge including mechanical, thermal, filtration, chemical, natural, and geotextile methods, and new methods that are the result of combining different processes. In the following, various parameters affecting the dewatering efficiency, including sludge characteristics, moisture content, costs, capacities, and environmental issues were examined, and at the end, challenges and limitations in dewatering processes were examined. Considering the very complex nature of sewage sludge, this study will help choose the sludge dewatering method and provide the conditions to increase the dewatering efficiency.
在过去的几十年里,由于污水污泥流量的急剧增加,净化城市和工业废水的重要性增加了。有各种类型的污泥,包括高含水量,胶体行为和可压缩性。污水污泥含有约1-5 wt%的固体,污泥的剩余部分是水(95 - 99%)。每年产生的大量污泥证实了污水污泥处理的重大挑战。改善污泥脱水可降低后续管理和运输成本。为了实现这一目标,有必要研究不同的污泥脱水方法和影响污泥脱水效率的指标。在本文的综述研究中,明确了这两个因素,现有的关于污泥脱水的技术认识将在实际应用中有所帮助,这两个考虑将在设备选择和优化措施的过程中发挥主要作用。本研究研究了各种脱水污泥的技术和设备,包括机械、热、过滤、化学、自然和土工布方法,以及结合不同工艺的新方法。下面,考察了影响脱水效率的各种参数,包括污泥特性、含水率、成本、容量和环境问题,最后考察了脱水过程中的挑战和限制。考虑到污泥的复杂性质,本研究将有助于污泥脱水方式的选择,为提高脱水效率提供条件。
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引用次数: 0
Strategies and applications of enhancing extracellular electron transfer in anaerobic digestion for wastewater resource recovery:A critical review 厌氧消化中加强细胞外电子转移的策略和应用:综述
Pub Date : 2024-06-01 DOI: 10.1016/j.efmat.2025.01.001
Longyi Lv , Xinyuan Wang , Duoying Zhang , Xinyang Liu , Jinsong Liang , Xiaoyang Liu , Wenfang Gao , Li Sun , Zhijun Ren , Guangming Zhang
Utilizing anaerobic digestion (AD) to treat wastewater while recovering the resources in the wastewater is research full of opportunities and challenges. Degradation of pollutants and the generation of resource recovery such as hydrogen and methane in AD relies on the crucial step of extracellular electron transfer (EET). However, the rate of EET in AD may be inhibited due to factors like pollutant toxicity, leading to slow resource recovery efficiency. Enhancing electron transfer process between microorganisms and pollutants through exogenous addition of electron shuttles can promote the degradation rate of pollutants and help the reaction system to detoxify rapidly. Exogenous addition of conductive materials can enhance electron transfer process between microorganisms and help improve the stability and efficiency of resource recovery process for hydrogen, methane, and high-value products. The review provided a comprehensive review of different types, mechanisms, and enhancement strategies of EET. The review summarized various approaches and mechanisms for promoting energy recovery in AD through the enhancement of EET and highlights limitations of current research. A discussion of the environmental and economic evaluation of exogenously added mediator-enhanced anaerobic resource recovery was presented in the review. Lastly, the review offered prospects for the application of strategies to enhance EET. The aim of the review is to further improve the applicability of enhancing EET in anaerobic wastewater treatment.
利用厌氧消化技术对废水进行处理,同时回收废水中的资源,是一项充满机遇和挑战的研究。AD中污染物的降解和氢、甲烷等资源回收的产生依赖于细胞外电子转移(EET)这一关键步骤。然而,由于污染物毒性等因素,AD中EET的速率可能受到抑制,导致资源回收效率缓慢。通过外源添加电子穿梭体增强微生物与污染物之间的电子传递过程,可以促进污染物的降解速度,帮助反应体系快速解毒。外源添加导电材料可以增强微生物之间的电子传递过程,有助于提高氢气、甲烷和高价值产品资源回收过程的稳定性和效率。本文对EET的不同类型、机制和增强策略进行了综述。综述了通过增强EET促进AD能量回收的各种方法和机制,并指出了目前研究的局限性。本文就外源添加介质强化厌氧资源回收的环境经济评价进行了综述。最后,展望了提高环境效应策略的应用前景。本文旨在进一步提高强化EET在厌氧废水处理中的适用性。
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引用次数: 0
Persulfate activation by Fe, N co-doped carbon: Effect of N-containing groups on electron structure of Fe-Nx sites 铁、氮共掺杂碳的过硫酸盐活化作用:含氮基团对 Fe-Nx 位点电子结构的影响
Pub Date : 2024-03-01 DOI: 10.1016/j.efmat.2024.09.001
Qin Wen , Fei Qi , Shizong Wang , Zequan Zeng , Zhanggen Huang
Iron and nitrogen co-doped carbon (Fe-N-C) with Fe-Nx and graphitic N sites shows great potential in persulfate (PS) activation for organic pollutants degradation. Fe-Nx and graphitic N sites were quantified by X-ray photoelectron spectroscopy (XPS) to determine their ratios. The interaction between Fe-Nx and graphitic N and the mechanism affecting the catalytic activity were systematically explored by combining experiments and theoretical calculations. The results indicated a significant synergistic effect between Fe-Nx and graphitic N. Especially, Fe-N-C with a 1:4 ratio of Fe-Nx to graphitic N owned the highest turnover frequency (TOF) value (1.59 ​× ​10−3 ​g ​m−2 min−1). The contributions of radical mechanism influenced TOF values of Fe-N-C-rx to a certain extent. Theoretical calculations proved that the coordination environment could regulate the electronic structure of active sites, thereby affecting catalytic activity. Fe-N-C with a ratio of 1:4 Fe-Nx to graphitic N had maximum adsorption energy (Eads), O-O bond length (lO-O) and the optimal d-band center value, which promoted adsorption and electron transfer with PS. The 2,4-Dichlorophenol (2,4-DCP) degradation behavior was also explored by combining Fukui functions and mass spectrometry analysis.
具有 Fe-Nx 和石墨 N 位点的铁氮共掺杂碳(Fe-N-C)在过硫酸盐(PS)活化降解有机污染物方面具有巨大潜力。通过 X 射线光电子能谱(XPS)对铁-氮和石墨 N 位点进行量化,以确定它们的比例。结合实验和理论计算,系统地探讨了 Fe-Nx 和石墨 N 之间的相互作用以及影响催化活性的机理。结果表明,Fe-Nx 与石墨 N 之间存在明显的协同效应,尤其是 Fe-Nx 与石墨 N 的比例为 1:4 的 Fe-N-C 具有最高的翻转频率(TOF)值(1.59 × 10-3 g m-2 min-1)。自由基机制的贡献在一定程度上影响了 Fe-N-C-rx 的 TOF 值。理论计算证明,配位环境可以调节活性位点的电子结构,从而影响催化活性。Fe-Nx 与石墨 N 的比例为 1:4 的 Fe-N-C 具有最大的吸附能(Eads)、O-O 键长度(lO-O)和最佳的 d 带中心值,从而促进了与 PS 的吸附和电子转移。此外,还结合福井函数和质谱分析,探讨了 2,4-DCP 的降解行为。
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引用次数: 0
Modified Titanium dioxide-based photocatalysts for water treatment: Mini review 用于水处理的改性二氧化钛基光催化剂:小型综述
Pub Date : 2024-03-01 DOI: 10.1016/j.efmat.2024.07.002
Xiaowen Yang, Ran Zhao, Hong Zhan, Hexiang Zhao, Yingnan Duan, Zhurui Shen
Titanium dioxide (TiO2), recognized for its affordability, low cost, high chemical stability, and eco-friendliness, has garnered extensive research attention in recent years. But because of the TiO2 band gap (>3.2eV) seriously limit the use of visible light, and fast electron-hole composite in TiO2 often lead to poor photocatalytic activity and low quantum yield. Therefore, TiO2 needs to be modified. Modification can change the broadband gap of TiO2, enhance light absorption, thus affect the important means of photocatalytic efficiency. In this review, we introduce the crystal form and photocatalytic mechanism of TiO2, and review some modification strategies of TiO2, including doping modification, construction of heterojunctions, crystal plane engineering and defect engineering. Furthermore, we review the application of modified TiO2-based photocatalytic materials in water treatment, including the removal of dye contaminants, antibiotics, advanced oxidative sterilization, and finally explore the challenges and prospects of modified TiO2-based photocatalysts.
二氧化钛(TiO2)因其经济实惠、成本低廉、化学稳定性高和环保等优点,近年来受到了广泛的研究关注。但由于 TiO2 的带隙(3.2eV)严重限制了其对可见光的利用,而且 TiO2 中快速的电子-空穴复合往往导致光催化活性差、量子产率低。因此,需要对 TiO2 进行改性。改性可以改变 TiO2 的宽带隙,增强光吸收,从而影响光催化效率的重要手段。在这篇综述中,我们介绍了 TiO2 的晶体形态和光催化机理,并综述了 TiO2 的一些改性策略,包括掺杂改性、构建异质结、晶面工程和缺陷工程。此外,我们还综述了改性 TiO2 基光催化材料在水处理中的应用,包括去除染料污染物、抗生素、高级氧化杀菌等,最后探讨了改性 TiO2 基光催化剂面临的挑战和发展前景。
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引用次数: 0
Advance of self-cleaning separation membranes for oil-containing wastewater treatment 用于含油废水处理的自清洁分离膜的进展
Pub Date : 2024-03-01 DOI: 10.1016/j.efmat.2024.06.001
The formidable challenge of membrane fouling by high-viscosity oils remains a primary impediment to the sustainable application of separation membranes in treating oil-contaminated wastewater. Consequently, there is an imperative for the development of oil-contaminated wastewater treatment membranes endowed with self-cleansing capabilities. The current review aims to delineate the landscape of self-cleansing membranes tailored for the treatment of oil-contaminated wastewater. Embarking from the foundational theories and benchmarks of self-cleansing, the self-cleansing functionalities were classified into active and passive modalities. We encapsulate the strides made in research, encompassing domains such as super-wettable surfaces, synchronously filtered self-cleansing, and post-filtration high-efficiency self-cleansing, while concurrently identifying extant constraints and prospective trajectories. By meticulously categorizing and dissecting self-cleansing functionalities, the aim of this work is delving into the fundamental tenets of self-cleansing within membranes intended for treating oil-contaminated wastewater, and furnishing guidance for the design and advancement of self-cleansing functionalities in oil-water separation membranes.
高粘度油对膜造成污垢的巨大挑战仍然是分离膜在处理油污染废水中可持续应用的主要障碍。因此,开发具有自清洁能力的油污染废水处理膜势在必行。本综述旨在描述专为处理油污染废水而定制的自清洁膜的发展前景。从自清洁的基础理论和基准出发,将自清洁功能分为主动和被动两种模式。我们总结了研究中取得的进展,包括超润湿表面、同步过滤自清洁和过滤后高效自清洁等领域,同时确定了现存的制约因素和未来的发展轨迹。通过对自清洁功能进行细致的分类和剖析,这项工作旨在深入研究用于处理油污染废水的膜内自清洁的基本原理,并为油水分离膜中自清洁功能的设计和发展提供指导。
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引用次数: 0
Progress of CO2 fixation using cycloaddition reaction 利用环化反应固定二氧化碳的进展
Pub Date : 2024-03-01 DOI: 10.1016/j.efmat.2024.07.001
Xing Chen , Ye Liu , Guoqiang Wang , Lei Zhang , Yubo Kuang , Haohan Tao , Xiaoqian Xiang , Guangran Di , Xiaojing Yin , Kaixin Wang , Qianqian Cai , Xiaojun Lv
Carbon dioxide, a significant greenhouse gas component, has been impacting the global climate. Photocatalytic CO2 reduction is a cost-effective and eco-friendly approach. Photocatalytic CO2 can combine with epoxides to produce cyclic carbonates, garnering considerable attention due to its full atom utilization and alignment with green chemistry principles. This review assesses the current state of research on photocatalytic CO2 cycloaddition with epoxides, examining factors influencing efficiency through pathways and enhancement methods like light absorption, separation and transfer of photogenerated charges, active site reaction, coupling reaction, and reaction device.
二氧化碳是重要的温室气体成分,一直影响着全球气候。光催化还原二氧化碳是一种具有成本效益且环保的方法。光催化二氧化碳可与环氧化物结合生成环状碳酸盐,因其原子的充分利用和符合绿色化学原则而备受关注。本综述评估了光催化二氧化碳与环氧化物环加成的研究现状,通过光吸收、光生电荷的分离和转移、活性位点反应、偶联反应和反应装置等途径和增强方法,探讨了影响效率的因素。
{"title":"Progress of CO2 fixation using cycloaddition reaction","authors":"Xing Chen ,&nbsp;Ye Liu ,&nbsp;Guoqiang Wang ,&nbsp;Lei Zhang ,&nbsp;Yubo Kuang ,&nbsp;Haohan Tao ,&nbsp;Xiaoqian Xiang ,&nbsp;Guangran Di ,&nbsp;Xiaojing Yin ,&nbsp;Kaixin Wang ,&nbsp;Qianqian Cai ,&nbsp;Xiaojun Lv","doi":"10.1016/j.efmat.2024.07.001","DOIUrl":"10.1016/j.efmat.2024.07.001","url":null,"abstract":"<div><div>Carbon dioxide, a significant greenhouse gas component, has been impacting the global climate. Photocatalytic CO<sub>2</sub> reduction is a cost-effective and eco-friendly approach. Photocatalytic CO<sub>2</sub> can combine with epoxides to produce cyclic carbonates, garnering considerable attention due to its full atom utilization and alignment with green chemistry principles. This review assesses the current state of research on photocatalytic CO<sub>2</sub> cycloaddition with epoxides, examining factors influencing efficiency through pathways and enhancement methods like light absorption, separation and transfer of photogenerated charges, active site reaction, coupling reaction, and reaction device.</div></div>","PeriodicalId":100481,"journal":{"name":"Environmental Functional Materials","volume":"3 1","pages":"Pages 13-24"},"PeriodicalIF":0.0,"publicationDate":"2024-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141715715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Adsorption of 2,4-dichlorophenoxyacetic acid and 4-chlorophenol using bio-based activated carbon: Thermodynamics, kinetics and cytotoxicity evaluation 使用生物基活性炭吸附 2,4-二氯苯氧乙酸和 4-氯苯酚:热力学、动力学和细胞毒性评估
Pub Date : 2024-03-01 DOI: 10.1016/j.efmat.2024.09.002
Rashda , Aaron Albert Aryee , Dai Kailu , Shumaila Kiran , Zhaohui Li , Runping Han
This study investigates the use of peanut husk biowaste (PH) activated carbon to remove 2,4-dichlorophenoxyacetic acid (2,4-D) and 4-chlorophenol (4-CP) from water. Acid activation of PH enhances its structure, creating pores in the activated carbon. SEM, TEM, and XRD confirm the effectiveness of this process. BET analysis shows the increase in surface area from 0.775 to 547 ​m2 ​g−1 for the PH and PH-AC samples. PH-AC tested against 2,4-D and 4-CP, optimizing pH, contact time, pollutant dose, PH-AC dose, and temperature for maximum adsorption efficiencies. Maximum adsorption capacity for 2,4-D and 4-CP is 165.9 and 99.4 ​mg ​g−1, respectively, higher than previous research. Kinetics, adsorption, and thermodynamic studies reveal the endothermic and spontaneous nature of the adsorption process. The adsorbent demonstrates stability and long-term applicability, with substantial adsorption capacities for four cycles. Cytotoxicity studies confirm non-toxicity and environmental friendliness of PH-AC material. These findings highlight the potential of PH-AC for wastewater treatment.
本研究调查了使用花生壳生物废料(PH)活性炭去除水中的 2,4-二氯苯氧乙酸(2,4-D)和 4-氯苯酚(4-CP)的情况。PH 的酸性活化可增强其结构,在活性炭中形成孔隙。SEM、TEM 和 XRD 证实了这一工艺的有效性。BET 分析表明,PH 和 PH-AC 样品的表面积从 0.775 m2 g-1 增加到 547 m2 g-1。PH-AC 针对 2,4-D 和 4-CP 进行了测试,优化了 pH 值、接触时间、污染物剂量、PH-AC 剂量和温度,以获得最大吸附效率。2,4-D 和 4-CP 的最大吸附容量分别为 165.9 mg g-1 和 99.4 mg g-1,高于之前的研究。动力学、吸附和热力学研究揭示了吸附过程的内热和自发性质。该吸附剂具有稳定性和长期适用性,在四个周期内都具有很强的吸附能力。细胞毒性研究证实了 PH-AC 材料的无毒性和环保性。这些研究结果突显了 PH-AC 在废水处理方面的潜力。
{"title":"Adsorption of 2,4-dichlorophenoxyacetic acid and 4-chlorophenol using bio-based activated carbon: Thermodynamics, kinetics and cytotoxicity evaluation","authors":"Rashda ,&nbsp;Aaron Albert Aryee ,&nbsp;Dai Kailu ,&nbsp;Shumaila Kiran ,&nbsp;Zhaohui Li ,&nbsp;Runping Han","doi":"10.1016/j.efmat.2024.09.002","DOIUrl":"10.1016/j.efmat.2024.09.002","url":null,"abstract":"<div><div>This study investigates the use of peanut husk biowaste (PH) activated carbon to remove 2,4-dichlorophenoxyacetic acid (2,4-D) and 4-chlorophenol (4-CP) from water. Acid activation of PH enhances its structure, creating pores in the activated carbon. SEM, TEM, and XRD confirm the effectiveness of this process. BET analysis shows the increase in surface area from 0.775 to 547 ​m<sup>2</sup> ​g<sup>−1</sup> for the PH and PH-AC samples. PH-AC tested against 2,4-D and 4-CP, optimizing pH, contact time, pollutant dose, PH-AC dose, and temperature for maximum adsorption efficiencies. Maximum adsorption capacity for 2,4-D and 4-CP is 165.9 and 99.4 ​mg ​g<sup>−1</sup>, respectively, higher than previous research. Kinetics, adsorption, and thermodynamic studies reveal the endothermic and spontaneous nature of the adsorption process. The adsorbent demonstrates stability and long-term applicability, with substantial adsorption capacities for four cycles. Cytotoxicity studies confirm non-toxicity and environmental friendliness of PH-AC material. These findings highlight the potential of PH-AC for wastewater treatment.</div></div>","PeriodicalId":100481,"journal":{"name":"Environmental Functional Materials","volume":"3 1","pages":"Pages 46-58"},"PeriodicalIF":0.0,"publicationDate":"2024-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142586855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The application of diatomic catalysts in advanced oxidation Fenton-like water treatment technology:A mini review 二原子催化剂在高级氧化 Fenton 类水处理技术中的应用:微型综述
Pub Date : 2024-03-01 DOI: 10.1016/j.efmat.2024.07.003
Ran Zhao , Xiao-Wen Yang , Tian-Hao Li , Tian-Miao Yu , Fang-Yuan Chen , Zhu-Rui Shen
In the past few years, there has been a widespread utilization of diatomic catalysts in the catalysis sector because of their distinct benefits. In this review, we specify the application of diatomic catalysts based on carbon and carbon nitride in the Fenton-like field. This paper focuses on the synthesis and characterization of homonuclear and heteronuclear diatomic catalysts and methods to improve the catalytic performance by optimizing d-band structure, tuning charge transfer, and constructing spin states. There is no doubt that diatomic catalysts have bright prospects in the Fenton-like field.
在过去几年中,由于二原子催化剂的独特优势,它们在催化领域得到了广泛应用。在这篇综述中,我们具体介绍了基于碳和氮化碳的二原子催化剂在类芬顿领域的应用。本文的重点是同核和异核二原子催化剂的合成和表征,以及通过优化 d 带结构、调整电荷转移和构建自旋态来提高催化性能的方法。毫无疑问,二原子催化剂在 Fenton-like 领域具有广阔的前景。
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引用次数: 0
Hydrophobic MOF-808 particles encapsulated melamine sponge for efficient oil-water separation 疏水性 MOF-808 粒子包裹三聚氰胺海绵,实现高效油水分离
Pub Date : 2024-03-01 DOI: 10.1016/j.efmat.2024.07.004
Shengquan Liu , Peng Li , Yuezhong Zhang , Xinli Gao , Guoyong Wang , Sufang Song , Xudong Zhao
Developing highly efficient adsorbents is one of the most feasible strategies to achieve oil-water separation. Herein, we exploited a new hydrophobic metal-organic framework (MOF) by a post-synthesis acid-exchange method. Pentadecafluorooctanoic acid (PFOA) was applied to substitute the acetic acid of MOF-808 to result in the fluorinated MOF-808-PFOA, which owns much larger water contact angle than the primary MOF-808. Further, we successfully loaded these sub-micron MOF-808-PFOA particles into a melamine (MA) sponge, via the crosslinking effect by polydimethylsiloxane (PDMS). The prepared MOF/PDMS/MA sponge shows a high contact angle of 151.9°, induced by the increased surface roughness of mesh filament and decreased surface energy. Meanwhile, it is found that this excellent hydrophobility remains well under different water media and pH values. Combining with the high hydrophobiclity, mechanical stability and porous structure, this sponge shows an excellent adsorption performance for various classes of organic oils, with the large saturated adsorption capacities (27–65 ​g ​g−1), short equilibrium time (∼3 ​s), and good recyclability. More interestingly, this sponge can serve as a filter cartridge to achieve the effective continuous oil-water separation, even under long-term use. Thus, our work provides a new sponge-based adsorbent for efficient oil-water separation, and proposes a feasible strategy to construct hydrophobic MOFs via post-synthesis methods.
开发高效吸附剂是实现油水分离的最可行策略之一。在此,我们采用合成后酸交换方法开发了一种新型疏水性金属有机框架(MOF)。用十五氟辛酸(PFOA)替代 MOF-808 的乙酸,得到氟化 MOF-808-PFOA,其水接触角远大于原生 MOF-808。此外,通过聚二甲基硅氧烷(PDMS)的交联作用,我们成功地将这些亚微米级的 MOF-808-PFOA 颗粒装载到了三聚氰胺(MA)海绵中。所制备的 MOF/PDMS/MA 海绵的接触角高达 151.9°,这是由于网状丝表面粗糙度增加和表面能降低所致。同时,研究还发现这种优异的疏水性在不同的水介质和 pH 值下都能保持良好。结合高疏水性、机械稳定性和多孔结构,该海绵对各类有机油具有优异的吸附性能,饱和吸附容量大(27-65 g-1),平衡时间短(∼3 s),可回收性好。更有趣的是,这种海绵可用作滤芯,即使长期使用也能实现有效的连续油水分离。因此,我们的研究为高效油水分离提供了一种新型海绵吸附剂,并提出了一种通过后合成方法构建疏水 MOFs 的可行策略。
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引用次数: 0
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Environmental Functional Materials
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