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ACS Applied Nano Materials · 2020 · IF 0

Bowl-like Nanoreactors Composed of Packed Gold Nanoparticles Surrounded with Silica Nanosheets for a Photothermally Enhancing Enzymatic Reaction

Jiao Sun,Chen Cao,Jun Chen,Wenli Zhao,Qin Tang,Bohong Jiang,Fan Xu,Yehao Zhang,Qingmin Ji

Using controllable gold sputtering and a hydrothermal process on silica particles, we fabricated a bowl-like plasmonic nanoreactor, which is composed of loosely packed gold nanoparticles surrounded with thin silica nanosheets. The open-end bowl-like spheres have the advantages of facile mass transfer, large binding surface, and high photothermal conversion at the same time. An extremely high photo-induced heating conversion efficiency can be achieved for the bowl-like spheres, which can adjust the temperature over a wide range from 50 to 270 °C under 532 nm laser irradiation with a power of 10–150 mW at a short exposure time (< 2 s). When used in an enzymatic reaction (cholesterol oxidase), the system showed much improved enzymatic catalysis performance due to the light-induced thermal effect on the activity of cholesterol oxidase.

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SCIENCE OF THE TOTAL ENVIRONMENT · 2020 · IF 6.551

Sustainable recycling of LiCoO2 cathode scrap on the basis of successive peroxymonosulfate activation and recovery of valuable metals

Hao Guo,Zijun Min,Ying Hao,Xu Wang,Jinchen Fan,Penghui Shi,Yulin Min,Qunjie Xu

Increasing demand and waste of lithium-ion batteries (LIBs) has adversely affected resources and the environment. Multistage utilization of spent LIBs is essential to their sustainable development. Here, we propose a simple recycling method of LiCoO 2 cathode scrap, based on the first use of the cathode scrap as a catalyst to degrade organic pollutants via peroxymonosulfate activation , and subsequent recovery of valuable metals from the used catalyst. Compared with pristine LiCoO 2 , the LiCoO 2 cathode scrap exhibits excellent catalytic performance due to the active sites generated, such as the vacancy generation and electronic structure modulation by the degradation of LiCoO 2 during the continuous lithiation and delithiation processes. The removal efficiency of cathode scrap to the o -phenylphenol exceeds 98% within 60 min, and the degradation efficiency is still above 95% after the 10th use because its unique sandwich and porous structure ensure the stability and recyclability . After multiple catalytic reactions, due to the generation of crack, the separation of the sandwich structure, and further degradation of active materials, the leaching efficiency of transition metals from the cathode scrap in deep eutectic solvent is promoted. 86% of lithium and 95% of cobalt are leached from the used catalyst respectively. This study provides a promising strategy for the sustainable development of LIBs and promotes the utilization of spent LIBs in multiaspect.

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LUMINESCENCE · 2020 ·Vol. 36 ·期 2 ·431-442 · IF 1.855

Mussel-inspired polydopamine-encapsulated carbon dots with dual emission for detection of 4-nitrophenol and Fe3+

Qian Liu,Feifei Zhao,Bingfeng Shi,Changli Lü

Carbon dots (CDs) with excellent optical properties are widely used in biomedicine, fluorescence sensing, and light-emitting diodes (LEDs). However, it is still a challenge to prepare CDs that can stably emit red fluorescence in the water environment. In this study, polydopamine-encapsulated luminescent carbon dots (CDs@PDA) with an encapsulating structure were synthesized at room temperature from p -phenylenediamine-derived red-light CDs as the core and using mussel-inspired chemical properties of polydopamine (PDA). In the binary system of water:ethanol = 1: 3 (volume ratio), the as-prepared CDs@PDA had a dual emission of ultraviolet light (330 nm) and red light (640 nm) with the fluorescence quantum yields of 8.0 and 15.5%, respectively, at the same time under 285 nm light excitation. The as-prepared CDs@PDA could be directly used for fluorescence selective sensing of 4-nitrophenol (4-NP) and Fe 3+ through simultaneously quenching of ultraviolet and red fluorescence based on the internal filtration effect mechanism with detection limits of 3.44 and 3.75 μM, respectively. This research showed that PDA-coated CDs can significantly improve the photoluminescence stability of CDs with new optical features. This means that the encapsulated structure of mussel chemistry is very helpful for expanding the application range of CDs in the water environment.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Factors affecting UV/persulfate treatment of phenacetin and its disinfection byproduct formation potential

Yu-qiong Gao,Jin-qiang Zhou,Jia Zhang,Cong Li,Nai-yun Gao,Da-qiang Yin

The pollution of aquatic bodies in the natural environment by pharmaceuticals has become a matter of increasing concern. In this study, we investigated the effects of the various influencing factors on the degradation of phenacetin (PNT) and its disinfection byproduct formation potentials (DBPFPs) by UV/persulfate (UV/PS) treatment. We first examined the effects of factors such as the PS concentration, pH, HCO 3 – , NO 3 – , NO 2 – , and natural organic matter (NOM) on the PNT degradation kinetics. The PNT degradation rate exhibited a positive correlation with the PS concentration. The PNT degradation rate was also pH-dependent, and it was highest under mild-alkalinity conditions. The presence of NO 3 – , NO 2 – , and NOM all inhibited PNT degradation, whereas HCO 3 – slightly accelerated PNT degradation. We next adopted LC/MS/MS to identify the degradation products of PNT, and the possible degradation pathways were proposed accordingly. The effects of UV/PS pretreatment on the DBPs from chlorination exhibit a close relationship with the abovementioned factors influencing the PNT degradation performance. Upon prolonging the pretreatment time and increasing the PS concentration, it was observed that trichloromethane (TCM) formation continuously decreased, while dichloroacetonitrile (DCAN) and trichloronitromethane (TCNM) exhibited patterns of increase and subsequent decrease in concentration. Mild alkalinity enhanced TCM formation and largely restrained DCAN and TCNM formation. Additionally, the presence of NOM enhanced TCM formation, while HCO 3 – hardly affected DBP formation. Meanwhile, NO 2 – profoundly affected the formation of TCNM. Therefore, these factors influencing PNT degradation by UV/PS should be carefully considered when integrating such technology as an alternative pretreatment for PNT-polluted water before disinfection.

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JOURNAL OF ORGANIC CHEMISTRY · 2021 · IF 4.354

Transition-Metal-Free and Base-Promoted Carbon–Heteroatom Bond Formation via C–N Cleavage of Benzyl Ammonium Salts

Long Liu,Yuanyuan Tang,Kunyu Wang,Tianzeng Huang,Tieqiao Chen

A facile and general method for constructing carbon–heteroatom (C–P, C–O, C–S, and C–N) bonds via C–N cleavage of benzyl ammonium salts under transition-metal-free conditions was reported. The combination of t-BuOK and 18-crown-6 enabled a wide range of substituted benzyl ammonium salts to couple readily with different kinds of heteroatom nucleophiles, i.e. hydrogen phosphoryl compounds, alcohols, thiols, and amines. Good functional group tolerance was demonstrated. The scale-up reaction and one-pot synthesis were also successfully performed.

CAS / MDL: 64-17-5 108-95-2
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Analytical Methods · 2021 ·Vol. 13 ·期 11 ·1404-1411 · IF 2.896

Determination of phenolic compounds in estuary water and sediment by solid-phase isotope dansylation coupled with liquid chromatography-high resolution mass spectrometry

Wenxue Xu,Yufeng Hu,Minghuo Wu,Enming Miao,Hao Zhou,Xuwang Zhang,Jingjing Zhan

A method consisting of solid-phase isotope dansylation (derivatization with dansyl chloride) and liquid chromatography-high resolution mass spectrometry (LC-HRMS) was developed for the quantitative analysis of phenolic compounds (phenols) in environmental samples. A magnetic-HLB (hydrophilic lipophilic balanced) material was synthesized and applied as an adsorbent in magnetic solid-phase extraction (MSPE) for the enrichment of the analytical targets. Furthermore, with the solid-phase isotope labeling, the desalting and removal of labeling residuals could be simplified over conventional in-solution labeling. In addition to overcoming the matrix effect by isotope dansylation, the sensitivity for the analysis of phenols by LC-HRMS was remarkably improved by over 100-fold. The method was systematically verified, and good accuracy (86.5–104.9%) and precision (<8.6% and <11.4% for intra- and inter-day, respectively) were achieved for the tested 15 phenols. The limits of detection (LODs) of this method were estimated to be 0.2–5 ng L−1 and 5–100 ng kg−1 in estuary water and sediment samples, respectively. With this method, samples collected from the Daliao River estuary (Panjin, China) were analyzed. It was found that all of the targeted phenols were detected at concentrations ranging from unquantifiable to 485 ng L−1 (the total concentration of analytes found in each sample were in the range 822–957 ng L−1) and unquantifiable to 1368 ng kg−1 (the total concentration of analytes found in each sample were in the range 2251–2992 ng kg−1) in water and sediment, respectively.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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ENVIRONMENTAL POLLUTION · 2021 · IF 8.071

Rapid formation of pyrogenic char (biochar) with high and low sorption capacity towards organic chemicals

Zaiming Chen,Jianfei Wang,Yuefeng Wang,Bing Li,Meizhen Wang

Pyrogenic char (biochar) with a high sorption capacity (B-HSC) can sequester hazardous chemicals (e.g., phenanthrene). However, when sorption inhibits bioavailability of some functional chemicals (e.g., the herbicidal efficacy of diuron in soil), biochar with a low sorption capacity (B-LSC) is required to prevent sorption effects. The pyrolytic B-HSC generation has been reported, but information on B-LSC formation is scarce. How fast B-HSC and B-LSC could be generated is unknown until now. Here, biochars were rapidly prepared (the shortest heating time reached 5 min and the cooling time reached < 30 min) by a direct-pyrolysis method by directly exposing packaged rice straw and pine wood to 350 °C, 500 °C and 700 °C and out-of-furnace cooling at room temperature. The sorption of diuron, phenanthrene , and twelve other chemicals was investigated. B–HSCs were obtained within 30 min of rice straw pyrolysis , and the biochar K d values quickly increased to 7-730-fold that of the raw biomass as –OH and C–O–C in (hemi)cellulose of rice straw rapidly degraded, increasing hydrophobic interactions between the char and chemicals (solubility ≤ 82.8 g/L). In contrast, B-LSCs were generated within 30 min of PW pyrolysis, and the K d values of the biochars were 0.2–3.0-fold that of the raw biomass, as the surface area development and hydrophobicity-driven sorption were probably delayed by the late degradation of lignin aromatic C–O and phenolic –OH. Biochar amendment revealed an enhancement effect of B-HSC but not of B-LSC on soil sorption. The fast formation of B-LSC and B-HSC provides a guide to develop time- and cost-effective technique in pyrolytically producing weakly or strongly sorbing biochars for organic chemical management.

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CHEMISTRY OF MATERIALS · 2021 · IF 9.811

Multiresponse Shape-Memory Nanocomposite with a Reversible Cycle for Powerful Artificial Muscles

Chi Chen,Yangyuanchen Liu,Ximin He,Hua Li,Yujie Chen,Ying Wei,Yusen Zhao,Yanfei Ma,Zhen Chen,Xu Zheng,Hezhou Liu

In the field of bionic soft robots and microrobots, artificial muscle materials have exhibited unique potential for cutting-edge applications. However, current mainstream thermal-responsive artificial muscles based on semicrystalline polymers (SCPs), despite their excellent physical properties, suffer from the limitation of environmental stimuli in practice, while their photodriven counterparts adopting liquid crystal elastomers (LCEs) lack ductility. Herein, a novel multifunctional programmable artificial muscle with a unique patch-sewing structure formed by π–π stacking between azobenzene groups was designed, which combined the advantages of SCPs and LCEs. The nanocomposite demonstrated a unique combination between artificial muscle performance (46.5 times the energy density and 26.6 times the power density of human skeletal muscles) and programmability (274.84% strain and 100% shape-memory recovery rate within 1 s). Meanwhile, coupling the photoisomerization of azobenzene and the photothermal conversion of gold nanorods, the cycle of deformation triggered by ultraviolet light and restoring by infrared light could be accomplished rapidly within 30 s. A COMSOL Multiphysics model was established and the corresponding finite element analysis verified the photoactuation and captured the general principle of light initiation in elastomers. These demonstrate that the multifunctional programmable elastomer is promising for artificial muscle applications, especially for photoinduced actuation.

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Analytical Methods · 2021 ·Vol. 13 ·期 7 ·925-932 · IF 2.896

Preparation and evaluation of photo-responsive hollow SnO2 molecularly imprinted polymers for the selective recognition of kaempferol

Yun Sun,Xiaoying Yin,Lin Zhang,Menghui Cao

Novel photo-responsive hollow structured molecularly imprinted polymers (PHMIPs) were developed as a selective sorbent to recognize and separate analytes in complex samples. The PHMIPs were prepared using kaempferol (KAE) as the template, 4-[(4-methacryloyloxy) phenylazo] benzenesulfonic acid as a photo-responsive functional monomer, and hollow SnO2 (Ho-SnO2) as the support via free radical polymerization. The structure and physical properties of the developed polymers were characterized using different nano structural techniques and spectroscopy. Under alternating irradiation at 365 and 440 nm, the PHMIPs could release and uptake KAE, indicating that the template molecules can be easily bound to recognition sites and released back into solution. From adsorption experiments, the binding properties were evaluated, and the maximal adsorption capacity of the PHMIPs was 11.04 mg g−1. Furthermore, the developed PHMIPs showed high selectivity towards KAE compared to other compounds. Subsequently, the materials were successfully applied to the photo-controlled extraction of KAE from sea buckthorn leaves. The recoveries for KAE were higher than 90% and relative standard deviation values were between 1.81% and 2.53%, indicating the potential of the developed materials for use in extracting KAE from complex samples.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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ACS Omega · 2021 · IF 3.512

Development of a New Route for Separating and Purifying 4-Ethyl-2-methoxyphenol Based on the Reaction Mechanism between the Chemical and Calcium Ion

Junjun Yin,Duo Wang,Zhifeng Zheng,Yueyuan Ye,Shuirong Li,Xingyong Jia

Based on the characteristic that Ca2+ can react with 4-ethyl-2-methoxyphenol (EMP) to form a complexation with a phenol–calcium ratio of 4:1, a new extraction and purification method of EMP is developed for the first time in this work. At an optimum purification condition, 99.60% purity of EMP can be obtained through a reaction and decomposition operation. By combining a variety of characterizations, which consist of in situ Fourier transform infrared spectrometer (FTIR), nuclear magnetic resonance (NMR), inductively coupled plasma optical emission spectrometer (ICP-OES), gas chromatography–mass spectrometry (GC–MS)/flame ionization detector (FID), elemental analysis, and thermogravimetric analysis, the reaction mechanism of the coordination process is studied. It is demonstrated that there are three stages of the coordination reaction between Ca2+ and EMP. A neutralization reaction occurs in the first stage, while the second stage is a mixing reaction stage including neutralization and coordination reaction. When the reaction proceeds to the third stage, another coordination reaction occurs. Furthermore, phenol and ethanol are added as impurities in EMP. EMP with a purity of more than 99.50% can be obtained using this purification method. It confirms that this efficient method can achieve a good purification effect even for EMP solutions with complicated components.

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ACS Omega · 2020 · IF 2.87

Selective Conversion of Scenedesmus into Lactic Acid over Amine-Modified Sn-β

Zheng Shen,Yishan Gao,Ling Kong,Minyan Gu,Meng Xia,Wenjie Dong,Wei Zhang,Xuefei Zhou,Yalei Zhang

Amine-modified Sn-β was synthesized to improve the yield of lactic acid produced from Scenedesmus. After studying the growth of Scenedesmus, we selected Scenedesmus with the highest sugar content of 46.7% after 8 days of culture as the reaction substrate. The results showed that the yield of lactic acid from Scenedesmus was greatly increased after being catalyzed by 3-aminopropyltrimethoxysilane (APTMS)-modified Sn-β. After the pretreatment of Scenedesmus in an ice bath ultrasound, under the optimal reaction conditions (190 °C and 5 h), the yield of lactic acid reached the highest (37%). The acid–base characterization results of the catalyst confirmed that there are both Lewis acidic sites and medium-strength basic sites in the catalyst. Both of these sites can promote the hydrolysis of Scenedesmus, while the Lewis acidic sites can promote the production of lactic acid and the basic sites can effectively inhibit the production of the byproduct 5-hydroxymethylfurfural (HMF). This study proved that this amination catalyst is a useful strategy to increase the yield of lactic acid.

CAS / MDL: 108-95-2
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MACROMOLECULES · 2020 · IF 5.918

A Microporous Polymer with Suspended Cations for Anion Exchange Membrane Fuel Cells

Ziqin Li,Jing Guo,Jifu Zheng,Tauqir A. Sherazi,Shenghai Li,Suobo Zhang

A novel microporous anion exchange membrane containing a spirobiindane segment and cardo moiety is successfully synthesized through superacid-catalyzed Friedel–Crafts-type polymerization. The developed polymer showed good solubility in common polar aprotic solvent and exhibited excellent ionic conductivity (163 mS cm–1 at 80 °C). A series of poly(spirobiindane-aryl ether sulfone) copolymers P(SBI/AES)-X with variable SBI/AES molar ratios were synthesized, and each copolymer exposed different free volumes that increases by increasing the content of spirobiindane in the copolymers. In turn, this free volume of copolymer causes the construction of well-developed ion channels in the developed anion exchange membranes (AEMs). The resulting QP(SBI/AES)-0.5 AEM, with an ion exchange capacity (IEC) of 1.59 mmol g–1, exhibited a high hydroxide conductivity of 110 mS cm–1 at 80 °C as well as good mechanical robustness. The peak power density achieved using a single cell fuel cell test is 593 mW cm–2. The results depicted the excellent potential of the resultant microporous anion exchange membrane in the progress of anion exchange membrane fuel cells.

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