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Chemosensors · 2023 ·Vol. 11 ·期 8 ·431 · IF 4.2

Ratio-Metric Fluorescence/Colorimetric and Smartphone-Assisted Visualization for the Detection of Dopamine Based on Cu-MOF with Catecholase-like Activity

Yushuang Guo,Mingli Chen,Ting Yang,Jianhua Wang

As the most abundant catecholamine neurotransmitter in the brain, dopamine plays an important role in the normal physiological process, and its level in urine also changes during human pathological processes. In clinic, the detection of dopamine in urine is a potential marker for the diagnosis and the treatment of endocrine-related diseases. In this work, a copper metal organic framework with catecholase-like activity was prepared via the precipitation of Cu2+and imidazole, simulating the N-Cu coordination environment in the active site of catecholase. Cu-MOF (the copper–metal organic framework) can catalyze the oxidation of DA (dopamine) to dopaquinone using O2in the air. The oxidation product can further react with 1,3-dihydroxynaphthalene to produce a fluorophore product. Based on the above reaction, a multimodal sensing platform with three signal outputs, including ratio-metric fluorescence, absorbance and digital information extracted from smartphone images for simple and sensitive determination of DA, was proposed, with detection limits of 0.0679, 0.3206, and 0.3718 μM, respectively. This multimodal sensing platform was able to detect DA in body fluid in a self-correcting way, as demonstrated by the successful determination of DA in normal human urine samples, and samples with a high level of interference.

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PROCESS BIOCHEMISTRY · 2023 · IF 4.4

Production of hydroxytyrosol from tyrosol via controllable oxidation with immobilized tyrosinase: A comparative study

Chenchen Zhao,Yu Sha,Wei Zhuang,Yuan Rao,Jihang Zhang,Jinglan Wu,Tao Shen,Zhuotao Tan,Chenjie Zhu,Hongman Zhang,Hanjie Ying

Hydroxytyrosol (HT) is a novel functional pharmaceutical or food ingredient that can be prepared using tyrosinase (TYR) as the catalyst. In this study, cross-linked agarose resin (AG-NTA-Ni 2+ ) was selected as the carrier for the one-step immobilization and purification of the enzyme via specific adsorption of the His-tag on the protein and metal ions on the carrier particles. The immobilized TYR exhibited excellent thermal and pH stabilities and retained 82.3% of its relative activity after seven cycles. Using different reduction methods, immobilized TYR was used as a catalyst to synthesize HT via the controlled oxidation of tyrosol. The enzymatic cascade reaction of co-immobilized TYR and glucose dehydrogenase (GDH) as a biocatalyst served as a bioreduction method with an HT yield of 88%. For the chemical reduction using ascorbic acid (AA) as the reducing agent, an 80% HT yield was achieved. These results indicate that the immobilization method, which relies on the specific coordination between transition metal ions and certain protein amino acids , is a potential strategy for the effective co-immobilization of TYR and GDH. The proposed affinity co-immobilization technique is among the potential strategies for the efficient production of HT.

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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Regulation of the band structure and water solubility of perylene imide derivatives based on bay-substitution to accelerate the transport of photogenerated carriers with TiO2

Yunning Chen,Zhengkai Wu,Renquan Guan,Xueying Cheng,Qingkun Shang,Yingnan Sun

Improving the efficiency of photogenerated charge separation and transport is the primary goal of designing and constructing efficient composite photocatalysts. The matching of energy bands and the formation of chemical bond between the two components are very conducive to the separation and transmission of photogenerated charges. Herein, three perylene diimide derivatives (PDIs) are synthesized by introducing sulfonic acid group (PDI-SA) and benzenesulfonic acid (PDI-BSA) respectively into the amide bond and further chlorine bay-substituting (Cl-PDI-BSA). The good water solubility of Cl-PDI-BSA ensures its forms a stable chemical bond with TiO 2 through the sulfonic acid group in the single molecular state, coupled with the matching of energy band structure, TiO 2 @Cl-PDI-BSA exhibited excellent performance upon visible light photocatalytic degradation to phenol and trenbolone acetate (TBA). It can remove 100% of phenol in 15 min and 100% trenbolone acetate (TBA) in 30 min, which is 14.3 times that of TiO 2 . Combining to DFT calculation, Kelvin probe force microscope and EPR analysis prove that bay chlorine substitution has a greater impact on the energy band structure and electron cloud distribution of PDIs than N-sulfonation, thereby seriously affecting the transport of photogenerated carriers with TiO 2 .

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JOURNAL OF APPLIED PHYCOLOGY · 2023 · IF 3.3

Efficient preparation and production of ulvan oligosaccharides by using a new PL25 family ulvan lyase from Alteromonas sp. 76–1

Tang Tiancheng,Li Chen,Zhu Benwei,Yao Zhong

Ulvan lyase is a useful tool which can degrade ulvan into oligosaccharides with a range of biological activities. In this study, the ulvan lyase ULA-3 from Alteromonas sp. 76–1, which was a 1467-bp encoded 489-amino acid residue protein, has been cloned, heterologously expressed and biochemically characterized. ULA-3 showed the maximum activity at 45 ˚C and pH 9.0. The K m is 1.879 mg mL −1 and V max is 2.597 µmol min −1  mL −1 . Its enzyme activity was outstanding at 11.754 U mg −1 . Moreover, its metal ion stability is exceptionally good and most metal ions at a concentration of 1 mM have no inhibitory effect on its activity. It can endolytically degrade ulvan into oligosaccharides with a degree of polymerization (Dp) of 2–4 and with unsaturated double bond through the β -elimination reaction, which mainly cleaves the glycosidic bond between rhamnose and uronic acids. All in all, our study has increased the ulvan lyase database and offers the opportunity to fully utilize ulvan, a green biomass resource from marine algae.

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CHEMISTRY OF MATERIALS · 2023 · IF 8.6

Construction of Actively Targeted and High Drug Content Polyprodrug Amphiphiles to Perform Synergistic Chemo–Photo-Anti-Tumor Therapy and Immune-Activated Investigation

Guangwei Yang,Longxiang Tao,Guijie Kang,Jinhao Yan,Kewu He,Xuefu Wang,Jun Yin

Chemotherapy is one of the most employed strategies in clinical treatment of cancer, but the low content of drug molecules caused by the inadequate accumulation of drug carriers in the lesion locations has an adverse impact on the therapeutic effect. To solve this issue, a kind of high drug content prodrug monomers with topological structures of AB2 and AB3 were designed and utilized to construct a series of polyprodrug amphiphiles, P[GMA(-l-RGD/-PEG)-CPTn] (n = 2 or 3), with both targeting peptides (l-RGD) and high drug content. Depending on the structure of prodrug monomers, the content of drug molecules could be achieved as high as 60 wt % (n = 2) and 65 wt % (n = 3), respectively. These polyprodrug amphiphiles could self-assemble with photothermal conversion reagents (IR780) in water to form spherical nanoparticles, which could expose original hidden l-RGD through the removal of hydrophilic PEG coronas under the trigger of a tumor microenvironment and thus promote the endocytosis of nanoparticles. Once in the presence of intracellular glutathione (GSH), high content drug molecules could be efficiently released by a cascade amplification reaction to kill cancer cells, this process could be further enhanced by the synergistic effect of local hyperthermia induced by near-infrared light irradiation. The results from in vitro simulation and in vivo mouse solid tumor models showed that these nanoreagents had a highly inhibitory effect on the tumor. Not only that, the immune response after chemical–optical synergistic therapy was also systematically conducted, the results demonstrated that the maturation of dendritic cells and proliferation of T cells could be successfully activated, accompanied by the increase of high mobility group protein B1 and decrease of immunosuppressive regulatory T cells. We believe this proof-of-concept could effectively solve the bottleneck problem in chemotherapy and provide a continuous immune protection to the body after anti-tumor treatment.

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Advanced Healthcare Materials · 2022 ·Vol. 12 ·期 1 ·2200807 · IF 11.092

Zwitterionic Polymer/Polydopamine Coating of Electrode Arrays Reduces Fibrosis and Residual Hearing Loss after Cochlear Implantation

Anning Chen,Dongxiu Chen,Kai Lv,Guowei Li,Jing Pan,Dong Ma,Jie Tang,Hongzheng Zhang

Since the first surgery 50 years ago, cochlear implantation (CI) is the major treatment for patients with severe sensorineural hearing loss. However, unexpected foreign body reactions (FBRs) after surgery are reported in 90% of CI recipients, resulting in the formation of fibrosis in the cochlea and progressive residual hearing loss. Zwitterion modification is universally used to reduce bio-fouling and suppress FBRs but never for CI. In the present study, a zwitterionic coating is developed, which is composed of poly sulfobetaine methacrylate (PSB) and polydopamine (PDA) for cochlear implants. The PSB-PDA coating shows a series of characters for an ideal anti-FBRs material, including super-hydrophilicity, low protein and cell adsorption, long-term stability, and high biocompatibility. Compared to the uncoated controls, PSB-PDA coating inhibits the activation of macrophages and reduces the release of inflammatory factors (TNF- α , IL-1 β , NO) and fibrosis-related factors (TGF- β 1, α -SMA, collagen I). PSB-PDA coated electrode arrays suppress fibrosis completely and preserve residual hearing significantly in rat CI models. These results suggest that PSB-PDA coating is a novel strategy for anti-fibrosis to improve the outcomes of CI.

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Algal Research-Biomass Biofuels and Bioproducts · 2022 · IF 5.276

Biochemical characterization and elucidation the action mode of a new PL25 family ulvan lyase from marine bacterium Alteromonas sp. TK-45 (2)

Tiancheng Tang,Benwei Zhu,Zhong Yao

Ulvan , extracted from the marine green algae belonging to the genus Ulva , is a complex water-soluble sulfated polysaccharide which mainly composed of four monosaccharides consisting of rhamnose , xylose , glucuronic acid and iduronic acid . Its complex monosaccharide composition gives ulvan great potential for application in the fields of food, pharmaceuticals, and chemistry. And it can be degraded by ulvan lyases mainly from Polysaccharide Lyases (PL) family of PL24, PL25 and PL28 through β -elimination mechanism, which cleaves the β -glycosidic bond between sulfated rhamnose and glucuronic acid or iduronic acid, thereby producing an Ulva oligosaccharide with unsaturated bond. In this study, we have identified a putative ulvan lyase from Alteromonas sp. TK-45 (2). We heterologously expressed, purified, and biochemically characterized the ulvan lyase, which has removed signal peptide . The results show that ULA-1 had best activity at 45 °C and pH 8.0. The K m and V max values were 13.25 μg·mL −1 and 1.719 μmol·min −1 ·mL −1 , respectively. The thermostability of ULA-1 was excellent, and its activity hardly decreased after incubation at 45 °C for 1 h. ESI-MS analysis showed that the primary end-product were disaccharides to tetrasaccharides . In conclusion, our research has expanded the database of ulvan lyase, and provided the possibility to make full use of ulvan, a huge marine biomass resource .

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INTERNATIONAL JOURNAL OF MASS SPECTROMETRY · 2022 · IF 1.934

A MALDI-TOF MS based method for the fast screening of recombinant protein high-yield strains

Xiaoyan Liu,He Zhu,Yanan Li,Hongqiang Qin,Mingliang Ye

In this study, we presented a MALDI-TOF MS based approach for the screening of recombinant protein high-yield strains. It relies on the MALDI MS analysis of the affinity tag containing peptide that released from the targe t recombinant proteins expressed in host strains. This approach was illustrated by quantifying the His-tag containing target peptide which was removed from the recombinant protein of Src Homology 2 superbinder by tobacco etch virus protease . After the specific enrichment and detection of target peptide with the theoretical molecular weight of 1895.09 Da, we could achieve the identification of strains with different expression levels of Src Homology 2 superbinder. Furthermore, the screening of strains at the absolute quantitative level was realized by adding the synthesized heavy labeled peptide as internal standards, and the quantitative results have a good linear correlation. In general, based on the virtue of high speed, accuracy and sensitivity of MALDI-TOF MS, this approach has the potential to achieve high throughput detection, and then provide powerful technical support for the screening of recombinant protein high-yield strains.

CAS / MDL: 288-32-4
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Journal of CO2 Utilization · 2022 · IF 8.321

Synthesis of highly effective [Emim]IM applied in one-step CO2 conversion to dimethyl carbonate

Fei Chen,Wensheng Wei,Yunsheng Gao,Yuxin Wang,Zizhen Yan,Zhanguo Zhang,Haiming Yu,Guangwen Xu,Lei Shi

Ionic liquid 1-ethyl-3-methylimidazolium ([Emim]IM) with high thermal stability and strong basicity was successfully synthesized. Using [Emim]IM as catalyst, dimethyl carbonate (DMC) was directly synthesized from epoxy propane (PO), CO 2 , and methanol under mild reaction conditions. A continuous two-stage DMC synthesis process was developed. The cycloaddition of CO 2 and PO was first conducted to produce propylene carbonate (PC), and then methanol was introduced into the system to synthesize DMC. During the cycloaddition process, 97.40% PO conversion and 97.40% PC yield were achieved with TON of 99.49. In the subsequent transesterification stage, DMC yield attained 83.63% with selectivity higher than 99% and TON of 70.15. [Emim]IM was reused for seven times without obvious deactivation, exhibiting good stability. The effects of reaction temperature, reaction time, the initial pressure of CO 2 , and catalyst weight on cycloaddition and transesterification reactions were systematically investigated. The kinetic study showed that the activation energies (E a ) of cycloaddition and transesterification reactions were 28.02 and 38.53 KJ·mol −1 , respectively, much lower than those of catalysts reported in the literatures. In addition, [Emim]IM displayed superior catalytic activity for the cycloaddition of CO 2 with various epoxy compounds .

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Arabian Journal of Chemistry · 2022 · IF 6.212

Simultaneous determination of four sedative-hypnotics in human urine based on dendritic structured magnetic nanomaterials

Jing An,Xin Wang,Haojing Song,Tangjuan Zhao,Hongyan Ren,Weijun Kang,Zhanjun Dong,Lingmei Niu,Hongmei Shi

A magnetic solid-phase extraction technique based on magnetic dendritic structured nanoparticles (Fe 3 O 4 @SiO 2 -NH 2 -G5) as adsorbent coupled with ultra-high performance liquid chromatography tandem mass spectrometry (UHPLC-MS/MS) has been developed to detect diazepam, midazolam, zolpidem, and zaleplon in human urine. With Fe 3 O 4 @SiO 2 -NH 2 as the central core, dendrimer (G5) grafted alternately with cyanuric chloride and imidazole were bonded to the surface of the core to synthesize Fe 3 O 4 @SiO 2 -NH 2 -G5. The morphology and structure of the magnetic materials were characterized by transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), vibrating sample magnetometer (VSM), and dynamic light scattering (DLS). The key parameters affecting the extraction efficiency were optimized. A satisfactory performance was obtained under the optimum extraction conditions. The proposed method was validated, and the limits of detection of zaleplon, diazepam, zolpidem, and midazolam were 0.05, 0.05, 0.02, and 0.02 ng mL −1 , respectively. The linear correlation coefficients r of the four analytes were > 0.996, the intra-day precision was between 2.4 % and 9.4 % with the recoveries between 88.3 % and 104.8 %, and the inter-day precision ranged from 3.9 % to 15.2 % with the recovery in the range of 94.1 %−108.3 %. The magnetic dendritic structure nanomaterial Fe 3 O 4 @SiO 2 -NH 2 -G5 was successfully used to extract sedative-hypnotic drugs from human urine samples. The Fe 3 O 4 @SiO 2 -NH 2 -G5-based magnetic solid-phase extraction method eliminates centrifugation and filtration steps as in conventional extraction. Only one step of vortex dispersion extraction could achieve the separation and purification of the target compounds. The proposed method was simple, rapid, environment-friendly, and suitable for the analysis of sedative-hypnotic drugs in human urine.

CAS / MDL: 288-32-4
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POLYMERS FOR ADVANCED TECHNOLOGIES · 2022 ·Vol. 34 ·期 1 ·419-429 · IF 3.348

Thermosetting epoxidized polybutadiene/low-molecular weight polyphenylene oxide compatible system with quite low-dielectric constant and loss prepared through co-curing reaction

Tianwen Dai,Xinyue Jiang,Ying Ge,Huawei Zou,Pengbo Liu

Through the redistribution reaction of PPO, the hydroxyl-terminated low molecular weight PPO (PPO-OH) was prepared. Furthermore, after the reacting of PPO-OH with methacrylic anhydride, the double-bond-terminated low-molecular weight PPO (R-PPO) were synthesized, its M n was 2631 g/mol. The R-PPO were co-cured with epoxidized polybutadiene (JP-100) to prepare JP-100/R-PPO cured systems. The JP-100/R-PPO cured systems showed single-phase morphology. The co-curing reaction with R-PPO could effectively improve the thermal performance of JP-100, the glass transition temperature ( T g ) of cured JP-100/R-PPO systems raised greatly. For the cured JP-100/R-PPO (100/30) system, its T g was 192°C. The dielectric constant and dissipation factor of cured JP-100/R-PPO systems were both decreased and showed good frequency stability. The dielectric constant and dissipation factor at 1 MHz of cured JP-100/R-PPO (100/30) system were 2.61 and 0.0038, respectively, were obviously lower than those of cured JP-100 system (which were 3.10 and 0.0099, respectively). The JP-100/R-PPO systems exhibited an excellent thermal stability. The 5% weight loss temperature ( T 5% ) of cured JP-100/R-PPO system was around 340°C.

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ChemistrySelect · 2022 ·Vol. 7 ·期 36 ·e202203100 · IF 2.307

Regulation of Structure and Magnetic Properties for Nickel(II)/Cobalt(II) Coordination Polymers with 1,4-Bis(imidazole-1-ylmethyl)benzene Ligand

Yanhong Wang,Duming Gong,Hongcheng Lu

Graphical Two new three-dimensional coordination polymers based on same semi-flexible ligand 1,4-bis(imidazole-1-ylmethyl)benzene (bix) have been successfully synthesized under hydrothermal condition. Both of them have similar local coordination environments but different magnetic properties due to their different topological structures and spin number S . Two new coordination polymers Ni(bix) 3 ⋅ 2(NO 3 ) ⋅ (H 2 O) 1 and Co(bix) 2 ⋅ 2(NO 3 ) 2 (bix=1,4-bis(imidazole-1-ylmethyl)benzene) have successfully been synthesized via hydrothermal reactions. These two compounds have similar local coordination environments but different topological networks due to the flexibility of the bix ligand. Additionally, magnetic studies reveal that 1 and 2 also exhibit different magnetic behaviors. Although magnetic exchange pathways are same as M II -bix-M II (M=Ni 1 , Co 2 ), 1 shows purely paramagnetic state almost down to 2 K with weak antiferromagnetic interaction; while stronger antiferromagnetic interaction in 2 is suggested. Meanwhile, an anomaly around 38 K in zero-field-cooled mode is observed but suppressed in field-cooled mode, which may be suggesting the spin canting for 2 . The field dependent magnetizations show magnetization of 2.17 μ B and 2.44 μ B at 7 T for 1 and 2 , respectively. Also, the magnetic interaction J / k B of −3.3 K is estimated for 2 .

CAS / MDL: 288-32-4
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