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JOURNAL OF SOILS AND SEDIMENTS · 2022 ·Vol. 23 ·期 3 ·1428-1438 · IF 3.536

Significantly bipolar immigration of PFOA and PFOS into macroaggregates and microaggregates in soils under simulated natural conditions

Li Yulong,He Liuyang,Chen Yulin,Xue Jianming,Zheng Li,Yang Shengmao,Wu Li,Chen Zhendong,Zhang Zulin,Yang Lie

Purpose Perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) in soils pose a severe threat to the soil ecosystem and human health. Soil aggregates play a critical role in the migration and transformation of pollutants. Materials and methods In this study, soil with different properties (Fluvisol and Planosol) spiked with PFOA/PFOS were incubated for 90 days, and then divided into five particle size fractions by wet sieving with low loss. The concentrations of PFOA and PFOS in soils and fractions were extracted using ultrasound-assisted extraction method with methanol as an extractant. The PFOA and PFOS were analyzed using high-performance liquid chromatography-tandem mass spectrometry (HPLC–MS/MS). Results and discussion The results showed that the ability of the soil aggregates to carry PFOA and PFOS initially decreased and then increased with decreasing particle sizes. Moreover, organic matter was the main factor influencing the PFOA and PFOS distribution in the soil aggregates, whereas soil types did not affect the accumulation capacity of PFOA and PFOS on soil particles. The macroaggregates (2000–250 µm) showed the highest accumulation capacity of PFOA and PFOS, suggesting high load of PFOA and PFOS. Additionally, the microaggregates (< 15 µm) played a dominant role in the PFOA and PFOS distribution due to the high proportion of this fraction in soil samples (51.73 ~ 62.47%). Conclusions Significantly bipolar immigrations of PFOA and PFOS into macroaggregates and microaggregates in soils were observed. This phenomenon can be explained by the fact that the particulate organic carbon (POM) can sorb the PFOA and PFOS in the macroaggregates, while the presence of SOC (highly humified) may increase the PFOA and PFOS contents in the microaggregates. Graphical Abstract

CAS / MDL: 335-67-1 1763-23-1
研究领域: 环境科学 · 土壤学 · 污染研究
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ACS Applied Energy Materials · 2020 · IF 4.473

High Proton Conductivity Achieved by the Self-Assembly of POM-Based Acid–Base Adduct in SBA-15 over a Wide Range from −40 to 85 °C

Xiuwei Sun,Shumei Liu,Shan Zhang,Tianyi Dang,Hongrui Tian,Ying Lu,Shuxia Liu

Almost all proton-conducting materials display poor conductivity at subzero temperatures, which significantly limits their application in cold regions. Thus, effective strategies to achieve high proton conductivity in a wide range from subzero to medium temperatures (−40 to 85 °C) need to be developed. Herein, we prepared proton-conductive materials by encapsulating the acid–base adduct based on Keggin-type H3PW12O40 (HPW) and aminoethanesulfonic acid (C2H7O3NS, HSN) in the linear channels of SBA-15 (named HPW-HSN@SBA-15). The result is the same as we expected: HPW-HSN@SBA-15 exhibits high proton conductivity over a wide temperature range (−40 to 85 °C). The proton conductivity of 75 wt % HPW-HSN@SBA-15 (3HPW-HSN@SBA-15) reaches 0.16 S cm–1 at 85 °C, 97% relative humidity (RH), and 6.8 × 10–5 S cm–1 at −40 °C. The excellent proton conductivity at subzero temperature of HPW-HSN@SBA-15 is mainly attributed to the ultrafast proton transfer with low energy barrier between proton donor (acid group) and proton acceptor (base group) in acid–base adduct without the attendance of water. Furthermore, the proton conductivity cycle test of 3HPW-HSN@SBA-15 demonstrates its good durability and stability.

研究领域: 材料科学 · 化学
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Radiative Cooling Electrostatic Spinning Fabric with Environmental Adaptability and Robustness

Lili Zhu,Dongxing Lu,Yibing Cai,Shiqin Liao,Qingqing Wang,Qufu Wei

Radiative cooling textiles are cooled by transferring the body’s metabolic heat to outer space and reflecting sunlight, without any energy input, providing a sustainable way for personal thermal management (PTM). However, current research on the environmental adaptability of fabrics is very scarce, and most of the research on PTM has a single application environment. Here, based on the Mie scattering theory and the design of micronanostructures, this work demonstrates an environmentally adaptive fabric (EAF) composed of polyformaldehyde (POM) with a high selectivity ratio and hollow SiO2. It not only achieves the selective emission of the atmospheric window (8–13 μm) but also shows the transmission of the entire band (2.5–25 μm) and reflect sunlight (0.3–2.5 μm). Remarkably, its optical properties remain outstanding after being subjected to acid, alkaline, and UV treatments, which match the daily garment use application requirements. As a result, the EAF achieves efficient radiative cooling both outdoors (under sunny and cloudy conditions) and indoors (1.5–12.2 °C lower than cotton and commercial cooling fabrics). The EAF with excellent environmental adaptability and robustness brings new possibilities for the rational design of next-generation smart thermal management textiles and other sustainable applications.

CAS / MDL: 100-42-5 920-66-1
研究领域: 材料科学 · 纳米技术 · 纺织工程 · 热管理 · 光学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Stacking of Tailored Chalcogenide Nanosheets around MoO2-C Conductive Stakes Modulated by a Hybrid POM⊂MOF Precursor Template: Composite Conversion–Insertion Cathodes for Rechargeable Mg–Li Dual-Salt Batteries

Chenglong Wu,Jiulin Hu,Jing Tian,Fulu Chu,Zhenguo Yao,Yongjian Zheng,Dongguang Yin,Chilin Li

Mg anode has pronounced advantages in terms of high volumetric capacity, resource abundance, and dendrite-free electrochemical plating, which make rechargeable Mg-based batteries stand out as a representative next-generation energy storage system utilized in the field of large-scale stationary electric grid. However, sluggish Mg2+ diffusion in cathode lattices and facile passivation on the Mg anode hinder the commercialization of Mg batteries. Exploring a highly electroactive cathode prototype with hierarchical nanostructure and compatible electrolyte system with the capability of activating both an anode and a cathode is still a challenge. Here, we propose a POM⊂MOF (NENU-5) core–shell architecture as a hybrid precursor template to achieve the stacking of tailored chalcogenide nanosheets around MoO2-C conductive stakes, which can be employed as conversion–insertion cathodes (Cu1.96S-MoS2-MoO2 and Cu2Se-MoO2) for Mg–Li dual-salt batteries. Li-salt modulation further activates the capacity and rate performance at the cathode side by preferential Li-driven displacement reaction in Cu+ extrusible lattices. The heterogeneous conductive network and conformal dual-doped carbon coating enable a reversible capacity as high as 200 mAh/g with a coulombic efficiency close to 100%. The composite cathode can endure a long-term cycling up to 400 cycles and a high current density up to 2 A/g. The diversity of MOF-based materials infused by functional molecules or clusters would enrich the nanoengineering of electrodes to meet the performance demand for future multivalent batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF CONTROLLED RELEASE · 2024 · IF 10.5

ATP-adenosine axis regulation combined with microneedle assisted photoimmunotherapy to boost the immunotherapy efficiency

Chaonan Shi,Minglong Chen,Xiaodie Li,Yanping Fu,Dan Yang,Ting Wen,Wanchen Zhao,Ying Sun,Wenhao Wang,Chao Lu,Qiaoli Wu,Chuanbin Wu,Xin Pan,Guilan Quan

Immunogenic cell death (ICD) is associated with the release of damage-associated molecular patterns, including ATP, to promote an effective immune cycle against tumors. However, tumors have evolved an effective strategy for degrading extracellular immunostimulatory ATP via the ATP-adenosine axis, allowing the sequential action of the ectonucleotidases CD39 to degrade accumulated immunostimulatory ATP into pleiotropic immunosuppressive adenosine. Here, an ingenious dissolving microneedle patch (DMNs) is designed for the intralesional delivery of CD39 inhibitor (sodium polyoxotungstate, POM-1) and ICD inducer (IR780) co-encapsulated solid lipid nanoparticles (P/I SLNs) for antitumor therapy. Upon insertion into the tumor site, IR780 induces ICD modalities with the release of damage-associated molecular patterns from endogenous tissues, which activates the antitumor immune cycle. Simultaneously, POM-1 promotes the liberation of immunostimulatory ATP and lowers the level of immunosuppressive extracellular adenosine, which supported immune control of tumors via recruiting CD39-expressing immune cells. In vivo antitumor studies prove that this platform can effectively eliminate mice melanoma (tumor growth inhibitory rate of 96.5%) and colorectal adenocarcinoma (tumor growth inhibitory rate of 93.5%). Our results shed light on the immunological aspects of combinatorial phototherapy and ATP-adenosine regulation, which will broaden the scope of synergistic antitumor immunotherapy .

CAS / MDL: 540-10-3
研究领域: 癌症免疫疗法 · 药学 · 生物医学工程 · 分子生物学
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ACS Sustainable Chemistry & Engineering · 2025 · IF 7.3

Interface Engineering and Heteroatom Doping Trigger Multisite Synergism in V-Incorporated MoP/Cu3P to Accelerate Alkaline Hydrogen Evolution

Xueting Li,Guimin Wang,Chunmei Lv,Xiuwen Wang,Yue Liu,Haijing Yan,Zilin Zhang,Yanqing Jiao

Efficient non-Pt electrocatalysts for the alkaline hydrogen evolution reaction (HER) are necessary for industrial water electrolysis. Cu-based materials are cheaper alternatives, but their performances are far from satisfactory due to slow water dissociation kinetics and weak Gibbs free energy of hydrogen adsorption (ΔGH*). Herein, we propose to construct multiple sites with different activation functions in response to sluggish alkaline HER kinetics. A multi-interfacial, ultrasmall V-doped MoP and Cu3P heterostructure (V-MoP/Cu3P) was successfully fabricated by confined conversion of a V–Mo bimetallic polyoxometalate (POM) cluster embedded in a Cu-based metal–organic framework (MOF). The spatial separation of each POM cluster by the MOF and the inherent structure of each [VO6] connecting four [MoO6] octahedrons enable precise V incorporation in the MoP lattice and multi-interface coupling of the MoP and Cu3P heterojunction. As a result, the interfacial charge redistribution occurs and the d-band centers are finely tuned, triggering a multisite synergism to encourage the adsorption and activation of H2O, H–OH* bond breaking, and H2 release. Consequently, V-MoP/Cu3P exhibits significantly enhanced HER activity, even superior to the commercial 20% Pt/C catalyst at current densities exceeding 155 mA cm–2, which indicates the feasibility of the V-MoP/Cu3P catalyst as cheaper alternatives to Pt-based catalysts in industrial applications. This work provides new insight for the design of low-cost, high-abundance HER catalysts via multi-interface engineering and heteroatom doping to trigger multisite synergies.

研究领域: 电化学 · 催化 · 材料科学 · 纳米技术 · 能量转换 · 表面科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2021 · IF 4.539

Biodegradable polyurethane based clay composite and their anti-biofouling properties

Abid Ali,Yue Xiao,Lina Song,Jiankun Hu,Qingqing Rao,Muhammad Shoaib,Bilal Ul Amin,Xiaoli Zhan,Qinghua Zhang

The colonization of tiny marine organisms on ship's hull which are connected directly from seawater , is a costly issue. Biofouling contributes to enhanced hydrodynamic drag, which leads to higher consumption of fuel and greenhouse gas emissions . Therefore, the environment-friendly solution is very necessary for anti-biofouling activity. For this purpose, we have synthesized biodegradable polyurethane (CL-PU) composed of ε-CL and 4,4′-methylenebis(cyclohexyl isocyanate) (H 12 MDI) and 1,4 butanediol (1,4 BD). The synthesized CL-PU was further modified with 4, 5-dicholoro-2-octyl-isothiazolone (DCOIT) and clay by mixing of the solution to make composites. Our study showed that CL-PU/DCOIT/clay composite degraded in the artificial seawater (ASW), enzymatic solution and seawater (through laboratory test) due to the contents of clay. Because the existence of clay reduced the size of the spherulite of polycaprolactone (PCL) in the composite, therefore remarkably improved the crystallinity as determined via the polarizing optical microscope (POM) and differential scanning calorimetry (DSC). The composite acted as carrier of antifoulant (DCOIT) and controlled their release rate. The anti-bacterial and anti-diatom experiments exhibited that the composite with DCOIT contents were effective in preventing the accretion of Escherichia coli ( E.coli) (region inhibition 14 mm) and marine diatom Navicula incerta (82.5% reduction). The degradable CL-PU/DCOIT/clay composite will have tremendous durability and excellent anti-fouling activity for marine biofouling owning to sustainability and tunability without being toxic to aquatic biota.

研究领域: 材料科学 · 海洋生物学 · 环境科学 · 化学工程
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