SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Lin Duan,Yiyuan Qin,Xin Meng,Yaqi Liu,Tong Zhang,Wei Chen
Microplastics in the environments can undergo various aging processes that alter their physicochemical properties and consequently their affinities for environmental contaminants. Here, we compare the effects of sulfide-induced aging (a common process in anoxic environments) and UV-induced aging on contaminant binding of polypropylene (PP), polystyrene (PS) and polyethylene terephthalate (PET) microplastics derived from commercial plastic products. The two aging processes differentially affect adsorption of pyrene (a model nonionic, nonpolar organic) and ciprofloxacin (CIP, a zwitterion under the conditions tested) by modulating the hydrophobicity , surface charges and polarity of the microplastics to different extents. The effects of the two treatments on Cd(II) adsorption correlate well with their modulation on ζ potential and surface (O + S)/C ratio of the microplastics. For all three microplastics sulfide treatment results in stronger adsorption of Cr(VI) and its subsequent conversion to Cr(III) than does UV treatment , as the thiol groups formed during sulfide treatment strongly regulate the complexation and reduction of Cr(VI). Notably, both sulfide and UV treatments result in the flattening of the PET microplastics, significantly enhancing the adsorption of all four contaminants, by increasing surface area for adsorption. The findings of this study further underline the importance of understanding environmental aging/weathering processes of microplastics, particularly, those readily occur in anoxic environments but were previously not well studied.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 8
·4319-4333
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IF 11.9
Chaojie Lyu,Jiarun Cheng,Yuquan Yang,Jiwen Wu,Kaili Wu,Yunguo Yang,Woon-Ming Lau,Ning Wang,Dawei Pang,Jinlong Zheng
Highly dispersed Pt NPs anchored in hierarchically N,F co-doped hollow carbon spheres (Pt@N,F-HCS) were synthesized through a template-assisted strategy followed by fluorination and wet chemical reduction. Due to the introduction of F heteroatoms into the carbon skeleton, the degree of d–π electron conjugation between Pt NPs and N,F-HCS can be enhanced. This will lead to higher Ptx+ content in Pt species, which is beneficial for the effective adsorption of *OOH intermediates and is conducive to O–O bond breaking and triggers the direct 4-electron transfer mechanism for the ORR. In particular, the onset potential and half-wave potential values for the ORR are more positive than Pt@N-HCS without F doping, even outperforming 20%Pt/C. Besides, the Pt@N,F-HCS catalyst also possesses the smallest onset potential and largest methanol oxidation current for the MOR. In alkaline media, abundant OH− will be adsorbed around the Ptx+ sites due to its higher positive valence, and the reaction intermediate COads generated in Ptx+ sites will be further oxidized to the final product, CO2, thus improving the MOR activity and CO tolerance capacity. This heteroatom-doping strategy is favorable for enhancing the interaction between Pt NPs and the carbon-based support, and also provides insight to promote the activity and selectivity for direct methanol fuel cells.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
·
2023
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IF 4.3
Huihui Wang,Xiaojiao Zheng,Jiadong Wang,Shu Qin,Jindong Li,Yanli Qi,Xiaowen Wang,Xu Jing
The risk of the hazardous pesticide dichlorvos (DDVP) entering the human body through aquatic products is causing concern as global demand for aquatic products increases. Herein, a novel approach ground on switchable hydrophilicity solvent-based microextraction coupled with fluorescent detection of DDVP in aquatic products was established. Sodium nonanoate , a switchable hydrophilic solvent, was converted into nonanoic acid in-situ for use as an extractant under acidic conditions to extract DDVP from aquatic products. Thereafter, DDVP was hydrolyzed to dichloroacetaldehyde (DCA) by adjusting the extraction solution to an alkaline condition. The fluorescent substances were generated due to the condensation reaction of DCA and resorcinol which can achieve the quantification of DDVP. The assay had a linear relationship between 40 and 280 μg kg −1 , with a limit of detection of 2.4 μg kg −1 . The assay has been used to determine the residual content of DDVP in grass carp, sea cucumber, and abalone samples. The recoveries ranged from 93.8% to 106%. The strategy integrating microextraction and detection offers insight into monitoring pesticides in food products.
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Nanomaterials
·
2023
·Vol. 13
·期 3
·455
·
IF 5.3
Xian Qi,Yaxian Du,Ziqiang Zhang,Xu Zhang
Janus particles for oil–water separation have attracted widespread attention in recent years. Herein, we prepared a bowl-shaped Janus particle that could rapidly separate oil and water through a thiol–ene click reaction and selective etching. Firstly, snowman-like composite microspheres based on silica and mercaptopropyl polysilsesquioxane (SiO2@MPSQ) were prepared by a hydrolytic condensation reaction and phase separation, and the effects of the rotational speed and molar ratios on their microscopic morphologies were investigated. Subsequently, bowl-shaped Janus particles with convex hydrophilic and concave oleophilic surfaces were prepared via a thiol–ene click reaction followed by HF etching. Our amphiphilic bowl-shaped Janus particles could remarkably separate micro-sized oil droplets from an n-heptane–water emulsion with a separation efficiency of >98% within 300 s. Based on the experimental and theoretical results, we proposed the underlying mechanism for the coalescence of oil droplets upon the addition of the amphiphilic bowl-shaped Janus particles.Keywords:Janus particles;bowl-shaped particles;thiol–ene click reaction;oil–water separation
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ACS Nano
·
2023
·
IF 17.1
Fenglian Qi,Lin Li,Zhiwei Li,Lili Qiu,Zihui Meng,Yadong Yin
Chiral plasmonic nanostructures have promising applications in optoelectronics due to their chiroptical responses. However, achieving active tuning of optical chirality remains challenging. Here, we develop stretchable chiroptical films with mechanically tunable extrinsic chirality by assembling hexagonal magnetic/plasmonic hybrid nanodisks in magnetic fields. The nanodisks, synthesized using a space-confined growth method, display three distinct plasmonic resonance modes at the UV–vis–NIR region, which red shift with increasing size as demonstrated by simulation and experimental results. The coupled magnetic and plasmonic anisotropy allows convenient control over the plasmonic resonance modes by altering the strength or direction of external magnetic fields. Further, magnetically aligning the nanodisks in a stretchable polymer film produces superstructures with extrinsic chirality, displaying selective absorption of circularly polarized light and inverted circular dichroism due to the linear dichroism-linear birefringence effect. Reversible mechanical stretching allows for continuous switching of circular dichroism in a wide range (from −1° to +1°). The efficient magnetic alignment of hybrid nanodisks in the hydrogel provides a simple and effective strategy for designing stretchable optical devices with tunable extrinsic chirality.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Haonan Wang,Chuyi Wang,Jiali Huang,Yunzhen Liu,Yang Wu,Ruiyun You,Jian-Han Zhang,Yudong Lu,Huiying Shen
As a widely used industrial additive of plastic products, phthalate ester (PAE) plasticizers can easily migrate into food, threatening human health. In this work, we proposed a rapid, precise, and reliable method to detect PAE plasticizers in edible oils by using surface-enhanced Raman spectroscopy (SERS) technology. A two-dimensional (2D) silver plate synergizing with a nanosilver sol was prepared as a substrate for SERS to detect potassium hydrogen phthalate (PHP), a hydrolysate of a PAE plasticizer. Detection conditions, such as pH values, drying times, and hydrolysate interference, were optimized. The working curve was well fitted with a linear parameter R 2 of 0.9994, and the minimum detection limit was evaluated as 10 −9 mol/L. Furthermore, the detection accuracy was supported by five edible oil samples. Therefore, using SERS technology to detect PHP is expected to provide an avenue for PAE plasticizer detection in oils and fats, and it features promising potential applications in food safety.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Hongru He,Pan Xu,Xi Wang,Shengqi Ma,Zhixiao Liu,Henan Peng,Daming Wang,Hongwei Zhou,Chunhai Chen
A novel thin film nanocomposite (TFN) membrane was prepared for efficient organic solvent nanofiltration (OSN) by doping hollow porous carbon spheres (HPCSs) nanoparticles in polyamide separating skin-layer through interfacial polymerization and solvent activation techniques. The undoped thin film composite (TFC) membrane was also prepared for comparison. In the interfacial polymerization process, the excellent adsorption properties of HPCSs lead to the unstable diffusion of m-phenylenediamine monomers from the aqueous phase to the oil phase, resulting in the formation of a ridge-valley morphology on the membrane surface. This ridge-valley morphology can effectively increase the contact area between the membrane and the solvent, which in turn improves the permeation capacity. The as-synthesized optimal TFN-HPCSs-200 membrane exhibits superior OSN performance. The methanol permeation capacity is 11.51 L m –2 h –1 bar –1 , which was 1.42 times of that of the TFC membrane. Meanwhile, the retention rate of RDB dye for TFN-HPCSs-200 membrane is maintained at a high level (97.50%). Furthermore, it is noteworthy that the prepared TFN-HPCSs-200 membrane maintained stable solvent resistance and long-term stability after immersion in a strong polar DMF solvent at 80 °C for 5 days, implying that TFN-HPCSs membranes have potential for long-term application in industrial OSN processing.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jiarun Cheng,Chaojie Lyu,Hangren Li,Jiwen Wu,Yue Hu,Bin Han,Kaili Wu,Mirabbos Hojamberdiev,Dongsheng Geng
An original strategy was reported to manipulate ORR selectivity of N-doped hollow mesoporous carbon spheres (N-HMCS) via heteroatom (P and S) doping. Heteroatom doping can not only modulate electronic structure of N-HMCS and proportion/configuration of doped N, but also regulate ORR pathway. Specifically, rich-graphitic N sites and electron-rich C–P bond domains in N,P-HMCS act as electron donors, making *OOH more unstable and easier to desorb into H 2 O 2 . This severely distorts the sp 2 lattice of graphene, catalyzing a two-electron ORR synergistically. Conversely, a strong interaction between electron-deficient C–S bond domain and *OOH intermediate due to the introduction of highly electronegative S hinders the desorption of *OOH, leading to the breakage of the O–O bond and promoting four-electron ORR along with the rich-pyridinic N receptor site. The reaction activity and kinetics mechanism present a positive correlation with proportion of graphitic N, revealing graphitic N is the primary active site with a much faster electron transfer capacity.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Shujing Zhao,Xin Zhang,Gang Wei,Zhiqiang Su
Interfacial solar-driven water evaporation is considered as an economic and efficient strategy to address the shortage of freshwater resources, which however suffers from severe salt pollution and poor long-term stable performance of seawater evaporation. Here, we design and construct a three-dimensional all-weather solar evaporator by zeolite-chitosan-TiO 2 @PPy aerogel (ZCTP), with an internally oriented pore arrangement structure by zeolite and chitosan assistance, which can efficiently enhance solar-driven water purification. Most importantly, long-term operation of the ZCTP aerogels using carbon fiber heating wires to fully utilize the solar energy that collected during the daytime to improve the efficiency of solar utilization and water purification. Benefiting from novel structural and functional design, the ZCTP aerogels exhibit high broadband light absorption (96 %), fast water transport (13 ms), and good thermal management properties (thermal conductivity of 0.1969 W m −1 K −1 in wet state). The obtained results show that the water evaporation rate of the ZCTP aerogel is 1.66 kg m -2 h −1 under 1 sun illumination. The integrated system of photothermal and electrothermal energy conversion mechanisms obtains an ultra-high water evaporation rate of 11.70 kg m -2 h −1 of 5 V voltage under 1 sun irradiation, achieving the purpose of continuous purification water around the clock. In addition, excellent salt resistance also enables perfect stability and reusability of ZCTP aerogel, even in the water with 20 % salt having minimal impact on the evaporation process and energy efficiency. Based on its excellent mechanical stability and highly ductility, simple and scalable manufacturing process, ZCTP aerogel may have great potential for all-weather efficient photothermal material for large-scale applications such as wastewater treatment, seawater desalination, and solar steam generation.
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OPTICAL MATERIALS
·
2023
·
IF 3.9
Han Kang,Ze Zhang,Wei Zhou
Rhodamine B(RhB) was encapsulated in Tb(btc) (btc = 1,2,4-benzene tricarboxylic acid) frameworks by “one-pot” method, and the complex RhB@Tb(btc) with host-guest dual fluorescence emissions was synthesized. Compared with the stability of Tb 3+ emission, the characteristic emission of RhB at 620 nm showed a more sensitive response to ambient temperature. By integrating the different temperature dependence of Tb 3+ and RhB emissions, the temperature sensing of RhB@Tb(btc) was determined with relative sensitivity ranging from 0.43 to 0.59% K −1 (temperature range 298–353 K). Among several common antibiotics, RhB@Tb(btc) showed fluorescence quenching response to metronidazole (MDZ) and color transition to levofloxacin (LOFX) respectively with stable reusability. The combination of photoinduced electron transfer and internal filtration effect was confirmed as the contributor to MDZ induced fluorescence quenching. Furthermore, hydrogels and milk, which were added antibiotics on purpose for simulating unsafe foods, were detected at in situ temperature by RhB@Tb(btc) test paper, which achieved highly sensitive and highly selective detection to MDZ and LOFX with limit of detection reaching 10 −6 M.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Ruixue Yangcheng,Yuntong Cui,Shuang Luo,Jiansu Ran,Jianjian Wang
Developing an efficient and stable catalyst for the aqueous hydrodeoxygenation (HDO) of lignin derivatives at ambient temperature is highly desirable. Here, a novel Pd/PHS catalyst with the hierarchical structure was facilely constructed. Taking HDO of vanillin (VAN, a typical molecule of lignin derivatives) to 2-methoxy-4-methyl phenol (MMP) as a model reaction, >99% VAN conversion and 98.2% MMP yield can be achieved over Pd/PHS at ambient temperature in a water solvent, outperforming the recent works reported in the literature. We found that the hierarchal zeolitic structure could immobilize acidic P species in Pd/PHS via trapping and hydrogen-bonding, and these P species could greatly accelerate the conversion of reaction intermediate, enhancing the yield of MMP product. Pd/PHS also showed excellent activities in HDO of other lignin derivatives. We think this work will provide a new route to guide the design of stable catalyst for the efficient aqueous HDO of lignin derivatives to high value-added chemicals and biofuels at ambient temperature.
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ACS Nano
·
2023
·
IF 17.1
Weitao Yang,Cuijun Deng,Xiudong Shi,Yan Xu,Chenyu Dai,Hui Wang,Kexin Bian,Tianming Cui,Bingbo Zhang
Enhanced imaging techniques using contrast agents enable high-resolution structural imaging to reveal space-occupying lesions but rarely provide detailed molecular information. To this end, we report a structural and molecular fusion magnetic resonance imaging (MRI) nanoprobe for differential diagnosis between benign and malignant tumors. This fusion nanoprobe, termed FFT NPs, follows a working mechanism involving a T1-/T2-weighted magnetic resonance tuning effect (MRET) between a magnetic Fe3O4 core and a paramagnetic Fe-tannic acid (Fe-TA) shell. The FFT NPs with an “always-on” inert T2 signal provide structural MRI (sMRI) contrast of tumors while affording an activated T1 signal in the presence of ATP, which is overproduced during the rapid growth of malignant tumors to enable molecular MRI (mMRI) of tumor lesions. We propose the use of the ratiometric mMRI:sMRI intensity to assist in the differential diagnosis of malignant 4T1 tumors from benign L929 fibroblast tumors. Furthermore, the dissociated FFT NPs were found to be able to catalyze H2O2 conversion in 4T1 tumors to generate excess reactive oxygen species (ROS) for chemodynamic therapy. The described fusion nanoprobe strategy enables the differential diagnosis of tumors from a combined spatial and molecular perspective with one-stop MRI imaging with potential applications in precision intervention.
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