Engineering green MOF-based superhydrophobic sponge for efficiently synchronous removal of microplastics and pesticides from high-salinity water

IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2023-09-01 DOI:10.1016/j.watres.2023.120314
Xiaoxin Chen , Haobo Ma , Xiaoyu Ji , Ruimeng Han , Kyongjin Pang , Zemin Yang , Zhimin Liu , Shan Peng
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引用次数: 3

Abstract

Microplastics (MPs) and pesticides are becoming an intractable environmental issue due to their wide spreading and non-degradable nature, posing serious threat to ecosystem and human health. To settle such dilemma, this work reasonably designed a superhydrophobic MOF-based coated sponge (ODSOSS/TiO2/Ni-MOF/PDA@Sponge) through the combination of an environmentally friendly in-situ supersaturated coprecipitation and polysesiloxane modification method. Among them, (I) the introduction of polydopamine (PDA) not only improves the adhesion between coatings and sponge, but also enhances the growth of MOF structure through complexation. (II) The obtained Ni-MOF shows large-area microscale anthemy structure with multilayered flaky texture, forming heterogeneously hierarchical structure with the deposited TiO2 nanoparticles, which promotes photodegradation ability of TiO2 owing to great specific surface area of Ni-MOF. (III) The high specific large area Ni-MOF supplies sufficient action sites for linkage of PDA and polysesiloxane molecules with unique nanocage-like structure, thus further greatly increasing adsorption force for various pollutants. (IV) The superhydrophobicity protect the porous channels of MOF from contamination of various absorbed pollutants, while TiO2 nanoparticles effectively photodegrade the absorbed organic pollutants, endowing the sponge superior recyclability. The superhydrophobic sponge selectively rapidly and synchronously adsorbs various MPs (maintained almost 100% after 60 cycles) and pesticides (adsorption rates 71.6%–95.1%) from high-salinity water. The large-area sponge (9 cm × 6 cm × 1 cm) simultaneously removes almost 100% MPs (40 mg/L), Sudan Ⅲ (10 mg/L), kerosene (30 mL/L), and four pesticides (10 mg/L) within 1 min. Particularly, four pesticides are quickly photocatalytic degraded by the coated sponge. The free radical capture trials show that hydroxyl radicals (·OH) are the main active species of pesticide degradation. Furthermore, we reveal the negative centers where pesticide molecules are most vulnerable to ·OH attack, on basis of the charge distribution and molecular electrostatic potential (MEP) analysis. The adsorption mechanisms are carefully clarified through theoretical calculation and experimental data. This work not only provide an effective superhydrophobic candidate for MPs and pesticides removal in a broad applicable scope (especially in high-salinity wastewater), but also opens a new strategy for environmental remediation.

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工程绿色mof基超疏水海绵,高效同步去除高盐度水中的微塑料和农药
微塑料和农药由于其广泛分布和不可降解的特性,已成为一个棘手的环境问题,对生态系统和人类健康构成严重威胁。为了解决这一难题,本工作通过结合环保原位过饱和共沉淀法和聚硅氧烷改性法,合理设计了一种超疏水mof基包覆海绵(ODSOSS/TiO2/Ni-MOF/PDA@Sponge)。其中,(1)聚多巴胺(PDA)的引入不仅提高了涂层与海绵之间的附着力,而且通过络合作用促进了MOF结构的生长。(2)得到的Ni-MOF呈现出大面积的微细花状结构,具有多层片状纹理,与沉积的TiO2纳米颗粒形成非均匀的层次结构,由于Ni-MOF具有较大的比表面积,促进了TiO2的光降解能力。(三)高比大面积Ni-MOF为PDA与具有独特纳米笼状结构的聚硅氧烷分子的连锁提供了充足的作用位点,从而进一步大大提高了对各种污染物的吸附力。(四)超疏水性保护MOF的多孔通道不受各种被吸收污染物的污染,而TiO2纳米颗粒能有效地光降解被吸收的有机污染物,赋予海绵优越的可回收性。超疏水海绵选择性地快速、同步地吸附高盐度水中的各种MPs(60次循环后几乎保持100%)和农药(吸附率71.6% ~ 95.1%)。大面积海绵(9 cm × 6 cm × 1 cm)在1分钟内同时去除几乎100%的MPs (40 mg/L),苏丹Ⅲ(10 mg/L),煤油(30 mL/L)和四种农药(10 mg/L)。特别是四种农药被涂层海绵快速光催化降解。自由基捕获试验表明,羟基自由基(·OH)是农药降解的主要活性物质。此外,基于电荷分布和分子静电势(MEP)分析,我们揭示了农药分子最容易受到·OH攻击的负电荷中心。通过理论计算和实验数据详细阐明了吸附机理。本研究不仅为MPs和农药的去除提供了一种有效的超疏水候选材料,适用范围广泛(特别是在高盐度废水中),而且为环境修复开辟了新的策略。
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来源期刊
Water Research
Water Research 环境科学-工程:环境
CiteScore
20.80
自引率
9.40%
发文量
1307
审稿时长
38 days
期刊介绍: Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.
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