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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

α-Fe2O3 nanospindles as an efficient catalyst for optical and magnetic fields co-assisted Li-O2 cells

Daming Yang,Guiru Sun,Xinru Wang,Fengyang Li,Ze Gao,Pingli Zhang,Wei Lu,Ming Feng

The photo-assisted lithium-oxygen (Li-O 2 ) cell is widely concerned due to its low overpotential. However, rapid recombination rate of photogenerated electrons and holes remains a fundamental challenge for photo-assisted Li-O 2 cells. Herein, we design an optical and magnetic fields co-assisted Li-O 2 cell based on α-Fe 2 O 3 nanospindles. We employed PL spectrum and I-t curve confirm that under the magnetic field, the photogenerated electrons and holes are driven via the opposite Lorentz forces in photo-assisted Li-O 2 cells, which is beneficial to accelerating the formation and decomposition of Li 2 O 2 . The optical and magnetic fields co-assisted Li-O 2 cell based on α-Fe 2 O 3 nanospindles achieves an ultra-high discharge platform of 3.47 V and a low charge platform of 3.57 V, as well as a surprising energy efficiency of 97.2%. In addition, the optical and magnetic fields co-assisted Li-O 2 cell can stably cycle for over 25 cycles. This study offers a reference for improving the electrochemical kinetics of photo-assisted Li-O 2 cell by introducing magnetic field, which opens up a new avenue for the development of high-performance Li-O 2 cells.

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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-10 · IF 16.6

Selective nucleophilic α-C alkylation of phenols with alcohols via Ti=Cα intermediate on anatase TiO2 surface

Du Xinze,Fan Hongjun,Liu Shenglin,Zhang Z. Conrad

C−C bond forming reaction by alkylation of aryl rings is a main pillar of chemistry in the production of broad portfolios of chemical products. The dominant mechanism proceeds via electrophilic substitution of secondary and tertiary carbocations over acid catalysts, forming multiple aryl alkylation products non-selectively through all secondary and tertiary carbons in the alkyl chains but producing little α-C alkylation products because primary carbocations are poorly stable. Herein, we report that anatase TiO 2 (TiO 2 -A) catalyzes nucleophilic α-C alkylation of phenols with alcohols in high selectivity to simply linear alkylphenols. Experimental and computational studies reveal the formation of Ti=C− bond with the α-carbon of the alkyl group at oxygen vacancies of the TiO 2 -A surface. The subsequent α-C alkylation by selective substitution of phenol ortho- C−H bond is verified by deuterium exchanged substrate and DFT calculations.

CAS / MDL: 1344-28-1 13463-67-7
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PHYTOTHERAPY RESEARCH · 2023 · IF 7.2

Angelica sinensis polysaccharide ameliorates nonalcoholic fatty liver disease via restoring estrogen-related receptor α expression in liver

Li Luo,Huafeng Zhang,Weiliang Chen,Ziming Zheng,Zihao He,Haoyu Wang,Kaiping Wang,Yu Zhang

Angelica sinensis polysaccharide (ASP) showed increasingly recognized hepatoprotective effects and lipid regulation. Because polysaccharides are typically degraded into fragments or short-chain fatty acids in the gut, rather than being absorbed in their intact form, it is worth pondering why ASP can regulate hepatic lipid metabolism and protect the liver from damage caused by lipid accumulation. In vivo and in vitro nonalcoholic fatty liver disease (NAFLD) models with lipid accumulation were established to investigate the effect and potential mechanisms of ASP on hepatic fat accumulation. Our results showed that ASP remodeled the composition and abundance of the gut microbiota in high-fat diet-fed mice and increased their levels of propionate (0.92 ± 0.30 × 10 7 vs. 2.13 ± 0.52 × 10 7 ) and butyrate (1.83 ± 1.31 × 10 7 vs. 6.39 ± 1.44 × 10 7 ). Sodium propionate significantly increased the expression of estrogen-related receptor α (ERRα) in liver cells (400 mM sodium propionate for 2.19-fold increase) and alleviated the progress of NAFLD in methionine–choline-deficient diet model. Taken together, our study demonstrated that ASP can regulate hepatic lipid metabolism via propionate/ERRα pathway and ultimately relieving NAFLD. Our findings demonstrate that ASP can be used as a health care product or food supplement to prevent NAFLD.

CAS / MDL: 112-80-1
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2023 · IF 4.2

Temperature-Responsive Ratiometric Au Nanoclusters (NCs) Fabricated through α-Cyclodextrin-Protected Au NCs and Au@GSH NCs

Guojuan Qu,Tao Jiang,Tao Liu,Xiang Ma

Low color rendering indices (CRIs), distorted chromaticity, and monotonous luminescence seriously hinder the application of luminescent nanomaterials. In this case, Au nanoclusters (Au NCs) are promising candidates for the fabrication of luminescent sensing systems attributed to their excellent luminescent properties and ultrafine size. Here, we synthesized Au@α-CD NCs with blue fluorescence emission adopting the host macrocyclic molecule (6-SH-α-CD) as the ligand and matched it elaborately with orange phosphorescence-emissive Au@GSH NCs to fabricate multicolor tunable ratiometric Au NC luminescent systems. Accordingly, a standard white-light emission was successfully achieved with Commission Internationale de L’Éclairage located at (0.33, 0.33) and a CRI as high as 93. In view of the difference in temperature sensitivity between the lowest excited states of the two Au NCs, the ratiometric blending Au NCs moved from the 3500 K warm light region to 14400 K cold light region when the temperature varied from 0 to 70 °C, which played a role in monitoring temperature changes with the naked eye.

CAS / MDL: 70-18-8
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Chemical Engineering and Processing-Process Intensification · 2023 · IF 4.3

α-aminonitriles synthesis and kinetic investigation via photooxidative cyanation of amines in a visible LED-based photomicroreactor

Mohsin Pasha,Minjing Shang,Yuhan Wang,Saier Liu,Xiao Xue,Yuanhai Su

α-aminonitriles (AN) are valuable intermediates and building blocks with versatile applications in organic synthesis. Herein, we presented a visible LED-based photomicroreactor for the AN synthesis with three amine substrates, i.e., dibenzylamine (DBA), pyrrolidine (PYR) and piperidiene (PIP), using meso‑tetraphenylporphyrin (m-TPP) and trimethylsilyl cyanide (TMSCN) as photosensitizer and cyanide source, respectively. The results showed that the photooxidative cyanation is a chromoselective and wavelength-selective photochemical transformation with the optimum AN yield and selectivity of 98.2% and 99.5% at a residence time of 2.69 min. Computational studies indicated that a high energy gap between the molecular orbitals of PYP, PIR and their imine intermediates potentially led to their higher reactivity than DBA and formation of by-products with larger molecular weight. Kinetic investigation showed that the apparent rate constants of the DBA photooxidative cyantaion were improved by rising the LED input power, and the applied photosensitizer exhibited high photostability. The overall photonic efficiency of this photomicroreactor was found to be 54.3% within the wavelength range of 400–440 nm, which is higher than previously used photoreactors. Finally, linear correlations were developed between the input power of LED and apparent rate constants of DBA photooxidative cyanation, which would be beneficial for the design, optimization, and scale-up of this photochemical process.

CAS / MDL: 109-99-9
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2023 · IF 8.2

Rapid and ultrasensitive activity detection of α-amylase based on γ-cyclodextrin crosslinked metal-organic framework nanozyme

Liangqiang Chen,Wanqiu Huang,Mengdi Hao,Fan Yang,Hao Shen,Shaoning Yu,Li Wang

α-Amylase plays a significant part in fermentation and the food industry, as this enzyme effectively regulates the content of different sugars in brewing systems and affects the yield and quality of alcoholic beverages. Nevertheless, current strategies suffer from unsatisfactory sensitivity and are time-consuming or are indirect methods which demand the assistance of tool enzymes or inhibitors. Therefore, they are unsuitable for the low bioactivity and non-invasive detection of α-amylase in fermentation samples. Rapid, sensitive, facile, and direct detection method of this protein remains challenging in actual applications. In this work, a nanozyme-based α-amylase assay was constructed. The colorimetric assay used the interaction between α-amylase and γ-cyclodextrin (γ-CD) which crosslinks MOF-919-NH 2 . The determination mechanism bases on the hydrolysis of γ-CD by α-amylase, resulting in increased peroxidase-like bioactivity of the released MOF nanozyme. The detection limit was 0.12 U L −1 with a wide linear range (0–200 U L −1 ) and excellent selectivity. Additionally, the proposed detection method was successfully utilized in distilled yeasts to verify analytical capability in fermentation samples. The exploration of this nanozyme-based assay not only provides a convenient and effective strategy for enzyme activity determination in food industry, but also has promotion significance in clinical diagnosis and pharmaceutical production.

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BIOMASS & BIOENERGY · 2023 · IF 6

One-pot conversion of α-pinene into biomass high energy density fuel over a bifunctional zeolite catalyst

Benqiang Zhu,Xiuxiu Zhao,Yingchao Zhang,Bing Yuan,Fengli Yu,Congxia Xie,Shitao Yu

A shape-selective bifunctional catalyst (Ru x /SOT-Hβ) was furnished by loading Ru onto the Hβ zeolite prepared via seed organic template (SOT) method using the seeds obtained via steam-assisted conversion (SAC) method. The Ru x /SOT-Hβ catalyst exhibited both favorable acid-catalytic performance and hydrogenation performance in the two-stage one-pot conversion of α-pinene, enabling an energy-efficient process for producing biomass blended high energy density fuels (HEDF). The effect of preparation conditions of Hβ zeolite carrier, metal type, loading amount, and loading method on the catalytic performance of the bifunctional catalyst was investigated. After the optimization of the catalytic process over Ru 1.2 /SOT-Hβ using pinane as the reaction medium, the resulting liquid reaction mixture without undergoing further distillation and other operations was found to possess good biomass HEDF properties. Feasible recyclability of Ru 1.2 /SOT-Hβ catalyst in α-pinene one-pot conversion was also demonstrated by a 3-run recycling test.

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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2023 · IF 6.1

Biotransformation of Tyrosol into a Novel Valuable α-Galactoside with Increased Solubility and Improved Anti-inflammatory Activities

Tong Sun,Yan Liu,Ke Wang,Feiyu Duan,Lili Lu

Herein, tyrosol [2-(4-hydroxyphenyl) ethanol], which is rich in olive oil and red wine, was converted to a novel bioactive galactoside by enzymic glycosylation. The gene of α-galactosidase from Geobacillus stearothermophilus 23 was cloned and expressed in Escherichia coli as catalytically active inclusion bodies. The catalytically active inclusion bodies efficiently catalyzed the galactosylation of tyrosol using either melibiose or raffinose family oligosaccharides as glycosyl donors, resulting in a glycoside with 42.2 or 14.2% yields. The glycoside product was purified and identified as p-hydroxyphenethyl α-d-galactopyranoside by mass spectrometry and NMR analyses. The inclusion bodies can be recycled and reused for at least 10 batch reactions of galactoside synthesis. Moreover, the galactoside showed 11-fold increased water solubility and reduced cytotoxicity as compared to tyrosol. Also, it exhibited higher antioxidative and anti-inflammatory activities than tyrosol based on lipopolysaccharide-induced activated BV2 cells. These results provided important insights into the application of tyrosol derivatives in functional foods.

CAS / MDL: 501-94-0 585-99-9
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MICROCHEMICAL JOURNAL · 2023 · IF 4.8

AuNPs and CNTs embellished three-dimensional bloom-like α-Fe2O3 nanocomposites for highly sensitive electrochemical pesticides detection

Congyi Zhao,Yaxu Zhao,Lianqi Wang,Ke Lu,Wei Guo,Xiong Lu,Faming Gao

In this experimental study, a highly sensitive electrochemical acetylcholinesterase (AChE) biosensor for the detection of organophosphorus pesticides (OPs) based on three-dimensional α-Fe 2 O 3 nanoflowers decorated with Au nanoparticles (AuNPs) and carbon nanotube (CNTs) (α-Fe 2 O 3 NFs-AuNPs-CNTs) was developed. With the blooms structure, the α-Fe 2 O 3 NFs not only provided an excellent microenvironment for the loading of AChE, but also increased the contact specific surface area. Meanwhile, AuNPs dispersed uniformly on the α-Fe 2 O 3 nanosheets and CNTs further enhanced the conductivity of the nanocomposites. Under the optimized conditions, the biosensor was made to exhibit favorable linear relationship with the logarithm of the concentration of omethoate from 1 × 10 −13 -1 × 10 −7 M, with the detection limit of 1.9 × 10 −15 M. In addition, the biosensor also possessed good repeatability, stability and practicality, proved to be a valuable tool for the detection of pesticides in environment.

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Molecular Catalysis · 2023 · IF 4.6

Harvesting alkyl phenols from lignin monomers via selective hydrodeoxygenation under ambient pressure on Pd/α-MoC catalysts

Haoquan Guo,Xinyu Lu,Yue Yang,Jinhe Wei,Lizhi Wu,Li Tan,Yu Tang,Xiaoli Gu

Alkyl phenol is an essential chemical intermediate that is in high demand in the chemical industry. The synthesis of alkyl phenols from lignin-derived molecules is one of the most promising routes for utilizing biomass resources. Herein, we report the catalytic hydrodeoxygenation (HDO) of dihydroeugenol (DHE) to alkyl phenols over a highly dispersed Pd/α-MoC catalyst with a substrate conversion of 98% and a selectivity of 96% to alkyl phenols. The Pd/α-MoC catalyst prepared by co-precipitation and temperature-programmed carbonization exhibits exceptional HDO activity under mild conditions with a low H 2 pressure (1–10 bars). The characterizations of the catalyst suggest that Pd are highly dispersed on the α-MoC matrix. The reaction mechanism was investigated using the substrate scope experiments. Under ambient pressure, the abundant oxygen vacancies and acidity sites on Pd/α-MoC enable the selective hydrodeoxygenation of lignin monomers.

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Materials Today Bio · 2023 · IF 8.2

Non-viral gene therapy using RNA interference with PDGFR-α mediated epithelial-mesenchymal transformation for proliferative vitreoretinopathy

Jiahao Wang,Peiyi Zhao,Zhirong Chen,Hui Wang,Yajia Wang,Quankui Lin

Fibrotic eye diseases, a series of severe oculopathy, that will destroy normal ocular refractive media and imaging structures. It is characterized by the transformation of the epithelial cells into mesenchyme cells. Proliferative vitreoretinopathy (PVR) is one of these representative diseases. In this investigation, polyethylene glycol grafted branched Polyethyleneimine (PEI- g -PEG) was used as a non-viral gene vector in gene therapy of PVR to achieve anti-fibroblastic effects in vitro and in vivo by interfering with platelet-derived growth factor alpha receptor (PDGFR-α) in the epithelial-mesenchymal transition (EMT) of retinal pigment epithelium (RPE) cells. The plasmid was wrapped by electrostatic conjugation. Physical characterization of the complexes indicated that the gene complexes were successfully prepared. In vitro, cellular experiments showed excellent biocompatibility of PEI-g-PEG, efficient cellular uptake of the gene complexes, and successful expression of the corresponding fragments. Through gene silencing technique, PEI-g-PEG/PDGFR-α shRNA successfully inhibited the process of EMT in vitro. Furthermore, in vivo animal experiments suggested that this method could effectively inhibit the progression of fibroproliferative membranes of PVR. Herein, a feasible and promising clinical idea was provided for developing non-viral gene vectors and preventing fibroblastic eye diseases by RNA interference (RNAi) technology.

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ANALYTICAL SCIENCES · 2023 ·Vol. 39 ·期 7 ·1171-1178 · IF 1.6

Label-free photoelectrochemical immunosensing of α-fetoprotein based on Eu-TiO2 nanocomposites sensitized with dye-encapsulated HMA

Wang Kun,Gao Xue,Chen Jianfeng,Yang Xiaoyan

Abstract In this study, a sensitive photoelectrochemical immunosensor with dye-enhanced anodic photocurrent response was proposed for sensitive detection of α-fetoprotein (AFP). Specifically, europium-doped TiO 2 (Eu-TiO 2 ) was used as the photoelectrochemical functional material and coated onto indium tin oxide (ITO) electrode. Doxorubicin (DOX) as an excellent fluorescent dye was encapsulated in the hydrophobically modified alginate (HMA). Then the dye-loaded HMA was modified onto the surface of Eu-TiO 2 to further sensitize the photocurrent response. The results showed that the photoelectrical signal was enhanced and stabilized due to the effect of sensitization of DOX on Eu-TiO 2 material. The constructed PEC sensor revealed a good linear response to AFP antigen ranging from 0.5 to 100 ng/mL with a detection limit of 0.41 pg/mL. The clinical patient’s serum test results obtained from the proposed PEC immunosensor were consistent with those obtained from the commercial electrochemilunescence assay. The proposed PEC sensing method could be a promising analytical tool for the detection of AFP in clinical analysis. Graphical abstract

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