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JOURNAL OF MOLECULAR STRUCTURE · 2023 · IF 3.8

Extraction of quinoline from toluene solution of wash oil using 1‑butyl‑3-methylimidazolium hexafluorophosphate ([BMIM] [PF6]): Experimental and molecular dynamics simulations

Yuxiu Fu,Xiaoli Song,Yaming Pang,Yinan Zheng,Liguo Gao

In this paper, a green solvent [BMIM] [PF 6 ] ionic liquid was selected for the extraction and separation of quinoline from simulated wash oil. The effects of extraction temperature, extraction time, and solvent oil ratio on the extraction of quinoline from wash oil were studied. The optimal process parameters were obtained by changing single factor conditions and optimizing the experiment using response surface methodology. When the temperature is 71 ℃, the time is 60 min, and the solvent oil ratio is 3:5, the extraction efficiency can reach 67%. The ionic liquids were recovered and their properties were investigated by infrared spectroscopy. The mechanism of quinoline extraction by ionic liquids was analyzed using infrared spectroscopy and GROMACS kinetic simulation calculations.

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ACS Catalysis · 2022 · IF 13.7

Development of a Metal- and Oxidant-Free Enzyme–Photocatalyst Hybrid System for Highly Efficient C-3 Acylation Reactions of Indoles with Aldehydes

Yuan Yu,Ru-De Lin,Yao Yao,Ming-Liang Shi,Wei-Fan Lu,Na Wang,Xiao-Qi Yu

An enzyme–photocatalyst hybrid system has been developed for aldehyde-based indole C-3 acylation. The concept of this process is to form a C–N bond through the three-component Mannich reaction of aldehydes, amines, and indoles, thereby introducing an aminomethyl group on the indole ring. Next, this system catalyzed the formation of the corresponding imide ion from the Mannich product, followed by rapid hydrolysis to give the final C-3 carbonyl indole product. More than 30 indole C-3 acylated products (up to 93% yield) were successfully synthesized under mild conditions, and indole derivatization of two bioactive substances (probenecid and cholesterol) was realized. The mechanistic study provides theoretical support for the construction of photoenzyme catalytic systems. This is an example of enzyme–light-activated C-3 acylation of indoles under very mild reaction conditions, without the use of transition metal catalysts, metal salts, and additional oxidants. This efficient enzyme–photocatalyst hybrid system provides a strategy for the development of photoenzyme catalysis fields.

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Energy & Environmental Science · 2022 ·Vol. 15 ·期 12 ·5379-5390 · IF 39.714

Realizing record-high output power in flexible gelatin/GTA-KCl-FeCN4−/3− ionic thermoelectric cells enabled by extending the working temperature range

Yuchen Li,Qikai Li,Xinbo Zhang,Jiajia Zhang,Shuaihua Wang,Liuqin Lai,Kang Zhu,Weishu Liu

Quasi-solid-state ionic thermoelectric (i-TE) cells have attracted increasing interest due to their high thermopower and easy solution processability for flexible and wearable thermoelectric devices. However, many i-TE gels have drawbacks of a narrow working temperature range (ΔTmax) and low power density. In this study, we introduced glutaraldehyde into the gelatin-KCl-FeCN4−/3− matrix, forming strong covalent bonds and interconnected porous structures, which significantly improve ΔTmax from 9 °C to 23 °C. The formed gelatin/GTA polymer network increases the entropy difference between the redox couples of FeCN4−/3−, thereby enhancing its thermopower. For the first time, a high thermopower of 24.7 mV K−1, a record-high power density of 9.6 mW m−2 K−2 and a 2 h energy density (E2h) of 198 J m−2 are achieved simultaneously in a quasi-solid-state i-TE cell. The i-TE cell exhibits good cycling performance in long-term power generation, corresponding to an average E2h value of 175 J m−2 after the whole cycling process. A flexible and wearable device consisting of 16 i-TE cells can generate a high voltage of 3.6 V and an output power of 115 μW by harvesting body heat. This work provides a general route to increase the working temperature range and output power density of gel-based i-TE cells through a molecular-level approach.

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CORROSION SCIENCE · 2022 · IF 7.72

Insight into synergistic corrosion inhibition of 3-amino-1,2,4-triazole-5-thiol (ATT) and NaF on magnesium alloy: Experimental and theoretical approaches

Youmin Qiu,Jie Li,Yifeng Bi,Xiaopeng Lu,Xiaohui Tu,Junjie Yang

A novel mixture, comprising sodium fluoride (NaF) and 3-amino-1,2,4-triazole-5-thiol (ATT), was reported as an effective hybrid corrosion inhibitor for magnesium alloy in pH neutral NaCl solution. The highest efficiency (95.8%) was achieved when 50 mM NaF and 5 mM ATT were mixed. Both experimental and theoretical approaches were employed for addressing the synergism. The synergism was proposed as the formation of a double-layered inhibitors film, in which the lower layer is a uniform fluoride-enriched precipitate layer and the upper one is a hydrophobic adsorption layer. These two layers were mutually strengthened to produce an excellent inhibition effect as a whole.

CAS / MDL: 1310-73-2
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Translational Oncology · 2022 · IF 4.803

Human β-defensin-3 and nuclear factor-kappa B p65 synergistically promote the cell proliferation and invasion of oral squamous cell carcinoma

Yongxiu Du,Yanlan Yang,Wenbo Zhang,Chenxi Yang,Pu Xu

Oral squamous cell carcinoma (OSCC) is a usual oral cancer. Therefore, it's essential to identify targets for its early diagnosis and therapy. This research aimed to explore the roles of human β-defensin-3 (hBD-3) and nuclear factor-kappa B (NF-κB) p65 in the pathogenesis and progression of OSCC. The connection between NF-κB p65 and the carcinogenesis of oral cancer was analyzed by immunohistochemical staining. The relative expressions of hBD-3 and NF-κB p65 in OSCC cells were evaluated by qRT-PCR and Western blot. Afterward, hBD-3 was knocked down, and NF-κB p65 was overexpressed. The cell viability and invasion were tested via CCK-8 and Transwell experiment, and the expression of hBD-3, NF-κB p65, and its downstream molecules was evaluated by Western blot. The expression of NF-κB p65 was increased with the aggravation of the oral submucosal fibrosis. HBD-3 and NF-κB p65 were high-expressed in OSCC cells. The viability and invasion abilities of OSCC cells that knocked down hBD-3 were markedly decreased, while they were restored by the overexpression of NF-κB p65. The expressions of NF-κB p65 and c-myc were diminished while IκB and p21 were raised with the knockdown of hBD-3. After overexpression of NF-κB p65, the expression of hBD-3 and IκB did not change markedly, while c-myc was increased and p21 was decreased dramatically. HBD-3 and NF-κB p65 facilitate the proliferation and invasion of OSCC cells, and hBD-3 may promote this process by governing the expression of NF-κB p65 and its downstream c-myc and p21.

CAS / MDL: 548-62-9
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Corrosion resistance and mechanisms of Nd(NO3)3 and polyvinyl alcohol organic-inorganic hybrid material incorporated MAO coatings on AZ31 Mg alloy

Lei Cai,Xiang Song,Cheng-Bao Liu,Lan-Yue Cui,Shuo-Qi Li,Fen Zhang,M. Bobby Kannan,Dong-Chu Chen,Rong-Chang Zeng

This work reports the design and preparation of novel organic (polyvinyl alcohol, PVA)-inorganic (neodymium nitrate, Nd(NO 3 ) 3 ) hybrid coatings on micro-arc oxidation (MAO) coating for magnesium (Mg) alloy corrosion protection . X-ray diffractometer , X-ray photoelectron spectroscopy, fourier transform infrared spectroscopy , field emission scanning electron microscope , Energy Dispersive X-ray spectrometer and surface roughness were applied to characterize the chemical composition and surface morphology of the coatings. The corrosion resistance of the coatings was evaluated by electrochemical and salt spray tests. The results suggested that the formation of PVA-Nd 3+ and PVA-Mg 2+ complexes promoted the enrichment of Nd 3+ on the surface, and thereby improved the sealing quality and compactness of the coating. Interestingly, when the coating was damaged, the Nd 3+ ions were transformed to their carbonates and covered the active sites, and thus exhibiting self-healing function. Further, the corrosion resistance of PVA-Nd 3+ modified MAO composite coating on AZ31 Mg alloy was improved.

CAS / MDL: 16454-60-7
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REACTIVE & FUNCTIONAL POLYMERS · 2022 · IF 4.966

Bio-based poly(vinyl benzoxazine) derived from 3-hydroxycinnamic acid— An intrinsically green flame-retardant polymer free of both halogen and phosphorus

Zhi-Ming Wu,Yu Cao,Jin-Han Guo,Xiu-Qin Fang,Cheng-Mei Liu

A novel bio-based benzoxazine monomer (VBOZ-7, 7-vinyl-3-phenyl-3,4-dihydro- 2H -1,3-benzoxazine) bearing polymeriable vinyl and 1,3-benzoxazine functionalities was synthesized from 3-hydroxycinnamic acid through successive decarboxylation reaction and Mannich condensation .The styrene-like bifunctional monomer underwent radical polymerization to obtain soluble P(VBOZ-7) which still remainining polymeriable benzoxazien pendent groups. The reactive P(VBOZ-7) possessed excellent solubility just like polystyrene , and also showed excellent thermal stability under 220 °C verified by differential scanning calorimeter (DSC) results. When the linear P(VBOZ-7) was heated over 240 °C, the remaining benzoxazines polymerized rapidly to form crosslinked structure. Thermogravimetric analysis (TGA) results showed that both linear and crosslinked P(VBOZ-7) possessed high char-formability at 800 °C. Cone calorimeter test (Cone test) proved that in situ crosslinking reaction strikingly improved the flame-retardancy of P(VBOZ-7). The total heat release of the crosslinked P(VBOZ-7) was only 6.7 MJ/m 2 , far below the value of polystyrene (109.4 MJ/m 2 ). Undoubtedly, the P(VBOZ-7) consisting of C, H, O, N atoms is an intrinsically green flame-retardant polymer with excellent solution processibility.

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Materials Today Physics · 2022 · IF 11.021

Spectrally stable and efficient pure-blue light-emitting diodes based on CsPb(Br/Cl)3 nanocrystals with surface passivation by organic sulfonate

Siqi Sun,Pei Jia,Qizhang Huang,Min Lu,Po Lu,Feisong Qin,Guang Sun,Yanbo Gao,Xue Bai,Zhennan Wu,Yu Zhang

Despite rapid development of perovskite nanocrystal (PeNC) light-emitting diodes (LEDs), it remains challenging to achieve efficient and stable blue PeLEDs , especially for pure-blue PeLEDs required for displays. Mixed halide CsPb(Br/Cl) 3 NC is a common strategy to achieve pure-blue emission, but suffers from low photoluminescence quantum yield (PLQY) and spectra instability. Here, a facile approach for the synthesis of high-quality pure-blue emitting CsPb(Br/Cl) 3  NCs is reported by introducing an organic sulfonate, phenyl trifluoromethanesulfonate (PTFMS), which works as an efficient surface passivator. As a result, the optimized PeNCs achieve a high PLQY of 85% and enhanced conductivity. Furthermore, the LED based on the optimized PeNCs is developed with pure-blue emission at 469 nm, which yields an external quantum efficiency (EQE) of 1.20% and luminance of 355 cd m −2 . More impressively, the device shows excellent spectra and operation stability under voltage bias , resulting from the suppressed ion migration channels by efficient defect passivation .

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EUROPEAN POLYMER JOURNAL · 2022 · IF 5.546

Synthesis of poly(1,2-butylene oxide-stat-tetrahydrofuran) by controllable polymerization over Sc(OTf)3 for use in high-performance lubricating oil

Xianqiang Zeng,Liguo Wang,Yan Cao,Chen Liu,Ziqiang Han,Peng He,Huiquan Li

Aliphatic polyethers are synthesized byring-opening polymerization (ROP) of the most common epoxide monomers, such as ethylene oxide (EO) and propylene oxide (PO). 1,2-Butylene oxide (BO) and tetrahydrofuran (THF) are potentially extended ROP monomers, which can give polyether unique properties. In this work, a series of poly(1,2-butylene oxide- stat -tetrahydrofuran)s (PBO- stat -PTHFs) with M n of 900–3700 g·mol −1 were synthesized by cationic ring-opening polymerization (CROP) of BO with THF using strong Lewis acid Rare Earth triflates (RE(OTf) 3 ) as catalysts and diols as an initiator at room temperature. PBO- stat -PTHFs product with yield up to 90 %, narrow polydispersity of Đ <1.30, and molar ratio of PBO to PTHF 1:1 were obtained. The copolymerization process was studied by in-situ IR and 1 H NMR spectroscopy analysis, and the results showed that PBO- stat -PTHF is a statistical copolymer. The early stage of the polymerization reaction was dominated by the activated chain end mechanism (ACEM), which incorporates a large amount of THF into the polymer chains. However, the late stage of the polymerization reaction was dominated by the activated monomer mechanism (AMM), which incorporates a large amount of BO into the polymer chains. Most PBO- stat -PTHFs have a suitable M n range, super high viscosity index (≥198) and low pour point (≤-53 °C), which can be used as a lubricant base oil and additives. In addition, PBO- stat -PTHFs have excellent miscibility with polyalphaolefin (PAO), which could significantly improve the PAO viscosity index. This study provides a mild route to construct high-performance copolyether materials through cationic ring-opening controllable polymerization.

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JOURNAL OF CATALYSIS · 2022 · IF 8.047

Selective conversion of 2-methylfuran to 3-acetyl-1-propanol in water over Pd@HZSM-5 catalyst with balanced metal-acid cooperation

Xin-Xin Fu,Jian-Peng Li,Zhuo-Qian Li,Yan Liu,Chen-Xiao Feng,Hai-Yang Wang,Zhi-Peng Zhao,Qiao-Yun Liu,Zhong-Yi Liu,Zhi-Kun Peng

Biomass is a promising renewable carbon resource, and bio-based platform molecules such as furan derivatives play an important role in the green manufacturing of high value-added chemicals. Of these, the conversion of 2-methylfuran (2-MF) to 3-acetyl-1-propanol (3-AP) over a bifunctional catalyst has attracted significant interest. However, bifunctional catalysts prepared by traditional method suffer from poor catalytic performance and limited stability due to the agglomeration of metal NPs. Here, Pd@HZSM-5, in which Pd NPs were encapsulated in HZSM-5 in situ showed improved stability and 3-AP yield. The highest yield of 3-AP (90.6%) to date was obtained with a nearly 100% conversion of 2-MF. The catalytic performance over a series of Pd@Zeolite confirms the superiority of the encapsulation effect, which is ascribed to the optimal adjustment of metal/acid balance. The Pd@HZSM-5 catalyst displayed excellent stability due to the encapsulation structure, which restricts the Pd NPs agglomeration. The highest yield of 3-AP was obtained at a high concentration of 2-MF (60%), which implies a promising strategy for the green industrial manufacture of 3-AP. This work reports a new bifunctional catalytic system for the green synthesis of 3-AP from 2-MF, thus stimulating the downstream biomass market.

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FOOD CHEMISTRY · 2022 · IF 9.231

Encapsulation of indole-3-carbinol in Pickering emulsions stabilized by OSA-modified high amylose corn starch: Preparation, characterization and storage stability properties

Wenxiu Zheng,Lin Ren,Wenzhuo Hao,Lei Wang,Changhong Liu,Lei Zheng

The stability of hydrophobic bioactive compound indole-3-carbinol (I3C) is a challenge for application. In this work, Pickering emulsions were prepared to encapsulate I3C. As the emulsifier, high amylose corn starch was pretreated by acid hydrolysis, afterwards modified by different concentrations of octenyl succinic anhydride (OSA), and their emulsions were evaluated. The XRD, SEM and FTIR results indicated the successful modification. ζ-potential, mean droplet size and emulsification index (EI) of the emulsions confirmed that modified starch with a higher degree of substitution (DS) was more effective for enhancing the storage stability. The results of encapsulation efficiency (EE) and retention degree of I3C after 14 d also proved the assumption. Moreover, the Pickering emulsions protected I3C against ultraviolet light and achieved controlled release in vitro . The food-grade Pickering emulsion loading I3C is promising to be used as a nutrient or dietary supplement for food applications.

CAS / MDL: 700-06-1
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ORGANIC PROCESS RESEARCH & DEVELOPMENT · 2022 · IF 3.858

Efficient Synthesis of (S)-1-Boc-3-aminopiperidine in a Continuous Flow System Using ω-Transaminase-Immobilized Amino-Ethylenediamine-Modified Epoxide Supports

Xiangxiang Wang,Youyu Xie,Zhicai Wang,Ke Zhang,Hualei Wang,Dongzhi Wei

We developed a continuous flow system using ω-transaminase covalently immobilized on an epoxy resin modified with ethylenediamine (EDA) to synthesize (S)-1-Boc-3-aminopiperidine, which is a key intermediate for several novel inhibitors. A second functional group (−NH3+) was introduced to rapidly adsorb ω-transaminase, which was further rigidified by multipoint covalent attachment to the modified resin with high binding efficiency (>95%) and activity recovery (75%). The resulting immobilized ω-transaminase was stable with 90% residual activity after 15 reuse cycles. We synthesized (S)-1-Boc-3-aminopiperidine using this continuous flow system, and 95% conversion was obtained within 10 min of residence. The system was continuously operated for 24 h and achieved a space–time yield of 930.73 g·L–1·day–1, indicating outstanding reaction efficiency. This efficient continuous bioprocess has potential for large-scale production of (S)-1-Boc-3-aminopiperidine.

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