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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Machine learning screening based strategy for the synthesis of a molecularly imprinted ionic liquid polymer for specific adsorption of perfluorooctanoic acid

Yiwei Zhang,Yingjie Luo,Jie Tong,Xuesong Liu,Yong Chen,Tengfei Xu

Perfluorooctanoic acid (PFOA) is a persistent organic pollutant that poses a significant environmental threat due to its resistance to degradation in both aquatic and terrestrial environments. Ionic liquids (ILs) are a type of salt that is liquid at or near room temperature and have been widely used in separation science, as well as showing great potential in environmental applications. However, the large number and variety of ILs make them impractical to assess the suitability of all possible ILs for PFOA adsorption using purely experimental methods. To address this issue, a high-throughput machine learning method was employed in this study to screen more than a thousand ILs and identify the most appropriate molecular for designing IL based molecularly imprinted polymer (MIP) with high affinity and selectivity of PFOA. The synthesized MIP, (Vim)C 3 (L-Pro)@MIP, has been proven to effectively and specifically recognize and adsorb PFOA in water. It has a maximum adsorption capacity of 568.18 mg g −1 and removal efficiency of over 99%, making it a highly efficient and selective option for PFOA removal in environmental remediation applications. This study showcases the promising potential of integrating high-throughput computer screening with experimental verification in the initial stages of MIP material design and development. By doing so, it is possible to create MIP materials that can effectively remove various pollutants, and potentially extend to other IL doped materials and applications.

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INDUSTRIAL CROPS AND PRODUCTS · 2023 · IF 5.9

Novel natural deep eutectic solvent-based supramolecular solvents designed for extracting phytochemicals from pigeon pea leaves and its scale-up and recovery process

Zi-Hui Cai,Lin Liu,Qi Gu,Jian-Dong Wang,Guo-Sheng Liu,Quan Zhou,Xin-Yue Dong,Su Zhang,Yu-Jie Fu

In this study, a novel green natural deep eutectic solvent-based supramolecular solvent/equilibrium solution (NADES-SUPRAS/EqS) system was designed. The microstructure and formation processes were characterized, revealing the formation and extraction mechanism of this novel solvent. In combination with vortex-assisted extraction, NADES-SUPRAS/EqS was used to efficiently extract and enrich representative active ingredients of different polarities in Cajanus cajan (Linn.) Millsp leaves. The influencing factors, including auxiliary extraction methods, the type of NADES, the proportion of NADES and ethanol for synthesis, the solid-to-liquid ratio, and the vortex time, were then adjusted utilizing single-factor optimization and response surface methodology . Under ideal extraction parameters, the extraction rates obtained were higher than other conventional organic solvents and had an excellent enrichment effect with only 90 s of vortex-shaking. Ultimately, an integrated multi-stage counter-current extraction and recovery unit was developed, capable of reducing costs and easily recovering solvents and target compounds, exploring the possibility of large-scale applications in the industry. A complete set of extraction, isolation, and recovery from plant material to chemical components offers a new perspective for the development of a high-value industry for plant secondary metabolites .

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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Interface-Induced Crystallinity Enhancement of Perovskite Quantum Dots for Highly Efficient Light-Emitting Diodes

Kaiyu Yang,Jinping Zheng,Jinliang Mao,Haobing Zhao,Songman Ju,QingKai Zhang,Zhihan Lin,Yongshen Yu,Fushan Li

Perovskite quantum dot light-emitting diodes (QLEDs) with high color purity and wide color gamut have good application prospects in the next generation of display technology. However, colloidal perovskite quantum dots (PQDs) may introduce a large number of defects during the film-forming process, which is not conducive to the luminous efficiency of the device. Meanwhile, the disordered film formation of PQDs will form interfacial defects and reduce the device performance. Here, we report an interface-induced crystallinity enhancement (IICE) strategy to increase the crystallinity of PQDs at the hole transport layer (HTL)/PQD interface. As a result, both the Br– vacancies in the PQD film and the interfacial defects were well passivated and the leakage current was also suppressed. We achieved QLEDs with a maximum external quantum efficiency (EQE) of 16.45% and current efficiency (CE) of 61.77 cd/A, showing improved performance to more than twice that of the control devices. The IICE strategy paves a new way to enhance the crystallinity of PQD films, so as to improve the performance of QLEDs for application in the future display field.

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Journal of Materials Chemistry C · 2023 ·Vol. 11 ·期 29 ·9996-10003 · IF 6.4

Trap states engineering toward all-inorganic CsPbBr3 perovskite nanocrystals for highly efficient light-emitting diodes

Xudong Jin,Yanqin Miao,Jianhua Dong,Jingkun Wang,Qiqing Lu,Min Zhao,Bingshe Xu,Junjie Guo

The room-temperature triple-ligand surface engineering strategy demonstrates the advantages of low-cost and high-yield in the preparation of perovskite nanocrystals (PeNCs). However, conventional octanoic acid (OTAc) with short-chain length shows weak binding energy with Pb2+, resulting in higher trap states density and inferior stability of PeNCs. Here, we prepare CsPbBr3 PeNCs capped with 4-dodecylbenzene sulfonic acid (DBSA) to maintain lower trap states density, a higher photoluminescence quantum yield of 91%, larger yield production and better stability compared to OTAc-PeNCs. Consequently, DBSA-PeNCs based PeLEDs with a peak external quantum efficiency (EQE) of 8.95% and a maximum luminance of 4452 cd m−2 are achieved, which constitute about 3-fold and 2-fold enhancement compared to OTAc-PeNCs based PeLEDs, respectively. These results demonstrate that introducing DBSA as the surface ligand is an effective way to realize highly efficient PeLEDs.

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MICROCHEMICAL JOURNAL · 2023 · IF 4.8

Hexafluoroisopropanol-based supramolecular solvent for liquid phase microextraction of triazole fungicides in drinking water and beverages

Ruiyu Fu,Tingze Ren,Yanhui Zhang,Qingxin Lu,Xiaoli Guo,Xin Di

A new supramolecular solvent (SUPRAS) was synthesized using hexafluoroisopropanol (HFIP) as hydrogen bond donor and undecanol as hydrogen bond acceptor. Then SUPRAS was used as extraction solvent to enrich triazole fungicides in drinking water and beverages by liquid phase microextraction (LPME). Additionally, several variables that influence extraction efficiency were optimized, and the significant factors were investigated by Box-Behnken design. At optimum condition, the method shows desirable precision (RSDs less than 19.4%) and acceptable recovery (63.4%-112.1%). The low limits of detection and limits of quantitation of this method were found to be in the range of 1.0–5.0 μg/L and 5.0–20 μg/L, respectively. Compared with other analytical techniques, the method demonstrated comparable sensitivity, consumed less extractant (750 μL) and a shorter pre-treatment time (10 min). The formation mechanism of SUPRAS was investigated by density functional theory. The proposed methodology was green, sensitive, time-saving and successfully applied to determine triazole fungicides in drinking water and beverages, making it an alternative technique for the analysis of trace analytes with satisfactory sensitivity.

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FOOD CHEMISTRY · 2023 · IF 8.8

The potential of hydroxytyrosol fatty acid esters to enhance oral bioavailabilities of hydroxytyrosol and fatty acids: Continuous and slow-release ability in small intestine and blood

Xinmiao Wang,Qian Wang,Jinghan Yu,Xu Guo,Peiyong Tong,Fawen Yin,Xiaoyang Liu,Dayong Zhou

HPLC-UV analysis in rat everted gut sac and in vitro simulated digestion models indicated that hydroxytyrosol fatty acid esters (HTy-Es) could be hydrolyzed by pancreatic lipase to slow-release of free fatty acids (FAs) and HTy. Meanwhile, the HTy-Es, the liberated FAs and the HTy could cross the membrane and were transported into blood circulation. HTy-Es were further hydrolyzed by carboxylesterase in in vitro rat plasma hydrolysis model, which also showed slow-release of FAs (C1-C4) and HTy. Especially, the rates of hydrolysis and transport initially increased and then decreased with the increasing alkyl chain length. Besides, the above rates of the HTy-Es with a straight chain were greater than those of its isomer with a branched chain. Therefore, the above-mentioned continuous and slow-release of FAs and HTy in small intestine and blood clearly demonstrated that HTy-Es would be an effective approach to enhance oral bioavailabilities of free fatty acids and hydroxytyrosol.

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ACS Applied Nano Materials · 2023 · IF 5.9

Perovskite Quantum Dot Light-Emitting Memcapacitor

Songman Ju,Chaomin Mao,Jinping Zheng,Kaiyu Yang,Lihua Lin,Tailiang Guo,Hailong Hu,Fushan Li

Perovskite quantum dots (PQDs) are promising in the field of light-emitting diodes (LEDs) due to their adjustable band gap, high photoluminescence quantum yield, and high color purity. However, ion migration is prone to occur in the device due to the structural instability of PQDs, resulting in the degradation of external quantum efficiency. In this work, we proposed a strategy to realize a perovskite quantum dot light-emitting memcapacitor (PQLEM) so as to enhance the electroluminescent performance of PQDs. By varying the pre-bias voltage and time, the ion distribution and trap density in the PQD film could be modified, thereby affecting the capacitance value and luminous efficiency of the device. Under the memcapacitive effect, the external quantum efficiency (EQE) of the device increases from an initial 2.81 to 7.95%. This work provides a route for achieving perovskite quantum dot light-emitting devices with high luminous efficiency.

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Food Chemistry-X · 2023 · IF 6.1

Magnetic deep eutectic solvent-based dispersive liquid–liquid microextraction for determination of strobilurin fungicides in water, juice, and vinegar by high-performance liquid chromatography

Min Wang,Luyao Zhao,Yu Niu,Shu Qin,Lixin Zhang,Liyan Jia,Xu Jing

In this study, a magnetic deep eutectic solvent coupled with dispersive liquid–liquid microextraction using high-performance liquid chromatography (MDES-DLLME-HPLC) was developed to detect strobilurin fungicides. The green hydrophobic MDES synthesized by methyltrioctylammonium chloride, ferric chloride, and heptanoic acid was used as an extraction solvent, which was dispersed by vortex and separated by an external magnetic field. The use of toxic solvents was avoided, and the separation time was reduced. The best experimental results were obtained through single factor and response surface optimization. The method had a good linear relationship with R 2  > 0.996. The limit of detection (LOD) ranged from 0.001 to 0.002 mg L −1 . The extraction recoveries were 81.9–108.9%. The proposed method was rapid and green, and it has been successfully applied to detection of strobilurin fungicides in water, juice, and vinegar.

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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Cationic COF nanosheets engineered positively charged polyamide membranes for efficient divalent cations removal

Guangzhe Wang,Tao Wu,Junhui Zhao,Benbing Shi,Tianrun Gu,Runnan Zhang,Xiaoyao Wang,Roni Kasher,Yanlei Su,Zhongyi Jiang

Ionic covalent organic frameworks (COFs) hold great promise in regulating the structure of polyamide nanofiltration membranes for divalent ions removal. In this work, we demonstrate cationic COF (cCOF) nanosheets engineered polyamide membrane with excellent divalent cations rejection. cCOF nanosheets as versatile regulator and an interlayer accelerate the self-sealing and self-termination of interfacial polymerization between polyethyleneimine and trimesoyl chloride, endowing membranes with dense network and small thickness. Meanwhile, the quaternary ammonium groups on cCOF nanosheets increase positive charges on membranes. Through synergistic intensification of electrostatic repulsion and size sieving, the resulting cCOF-PA membranes display excellent rejection for divalent cations (MgCl 2 , 99.3%), superior to most reported polyethyleneimine-based polyamide membranes. This work highlights the significance of ionic COF materials in developing positively charged membranes for efficient ionic and molecular separations.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Lead-free halide perovskite hollow nanospheres to boost photocatalytic activity for CO2 reduction

Yan-Fei Mu,Jin-Shuang Zhao,Li-Yuan Wu,Ke-Ying Tao,Zhao-Lei Liu,Fu-Quan Bai,Di-Chang Zhong,Min Zhang,Tong-Bu Lu

Strong photoresponse, efficient charge separation, and high surface activity are three important requirements for an ideal photocatalyst, while few photocatalysts can fully meet these requirements. Herein, we report such a photocatalyst based on lead-free halide perovskite hollow nanospheres (H-Cs 3 Sb 2 Br 9 ) by a facile antisolvent-assisted method. The hollow structure of H-Cs 3 Sb 2 Br 9 improves the light-harvesting performance; The formation of surface shallow trap states contributes to promoting the excited-carrier separation; The ligand-free termination surface of H-Cs 3 Sb 2 Br 9 facilitates the exposure of Br vacancies and active sites, thus strengthens the CO 2 adsorption and accelerates surface reactivity dynamics. As a result, with a dinuclear Co(II) complex as the co-catalyst, H-Cs 3 Sb 2 Br 9 exhibits a record-high photocatalytic activity for CO 2 reduction, with a CO yield of 15,010.4 ± 550.4 μmol g −1 after 8 h of illumination under simulated solar light (100 mW cm −2 ). This research presents a new way to develop cost-effective photocatalysts for CO 2 reduction.

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BIOTECHNOLOGY AND APPLIED BIOCHEMISTRY · 2023 ·Vol. 70 ·期 6 ·1806-1816 · IF 2.8

Quantitative determination of rhamnolipid using HPLC-UV through carboxyl labeling

Jing Zhou,Si-Jia Miao,Shi-Zhong Yang,Jin-Feng Liu,Hong-Ze Gang,Bo-Zhong Mu

Rhamnolipid, as a low-toxic, biodegradable and environmentally friendly biosurfactant, has broad application prospects in many industries. However, the quantitative determination of rhamnolipid is still a challenging task. Here, a new sensitive method for the quantitative analysis of rhamnolipid based on a simple derivatization reaction was developed. In this study, 3-[3′-( l -rhamnopyranosyloxy) decanoyloxy] decanoic acid (Rha-C10-C10) and 3-[3′-(2′- O -α- l -rhamnopyranosyloxy) decanoyloxy] decanoic acid (Rha-Rha-C10-C10) were utilized as the representative rhamnolipids. Liquid chromatography–mass spectrometry and high-performance liquid chromatography-ultra violet results showed that these two compounds were successfully labeled with 1 N1-(4-nitrophenyl)-1,2-ethylenediamine. There was an excellent linear relationship between rhamnolipid concentration and peak area of labeled rhamnolipid. The detection limits of the Rha-C10-C10 and Rha-Rha-C10-C10 were 0.018 mg/L (36 nmol/L) and 0.014 mg/L (22 nmol/L), respectively. The established amidation method was suitable for the accurate analysis of rhamnolipids in the biotechnological process. The method had good reproducibility with the relative standard deviation of 0.96% and 0.79%, respectively, and sufficient accuracy with a recovery of 96%–100%. This method was applied to quantitative analysis of 10 rhamnolipid homologs metabolized by Pseudomonas aeruginosa LJ-8. The single labeling method was used for the quantitative analysis of multiple components, which provided an effective method for the quality evaluation of other glycolipids with carboxyl groups.

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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Improving Perovskite Green Quantum Dot Light-Emitting Diode Performance by Hole Interface Buffer Layers

Qiangqiang Wang,Xuanyu Zhang,Lei Qian,Chaoyu Xiang

Perovskite quantum dot light-emitting diodes (QLEDs) are potential candidates for next-generation displays due to their high color purity and wide color gamut. Due to the strong electron-accepting ability of poly[bis(4-phenyl) (2,4,6-trimethylphenyl) amine] (PTAA), quantum dot (QD) films are prone to be charged, which leads to the imbalance of charge injection and the increase of nonradiative recombination, ultimately affecting the performance of the QLEDs. Here, we compared and studied two polymers, poly(methyl methacrylate) (PMMA) and poly(vinyl pyrrolidone) (PVP), as the hole interface buffer layers of QD films, which effectively reduced the defect density, suppressed nonradiative recombination, and greatly improved the efficiency and stability of QLEDs. The devices with PMMA achieved a maximum external quantum efficiency of 20.71%.

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