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NUCLEIC ACIDS RESEARCH · 2022 ·Vol. 50 ·期 17 ·9858-9872 · IF 19.16

Formation and removal of 1,N6-dimethyladenosine in mammalian transfer RNA

You Xue-Jiao,Zhang Shan,Chen Juan-Juan,Tang Feng,He Jingang,Wang Jie,Qi Chu-Bo,Feng Yu-Qi,Yuan Bi-Feng

RNA molecules harbor diverse modifications that play important regulatory roles in a variety of biological processes. Over 150 modifications have been identified in RNA molecules. N6-methyladenosine (m6A) and 1-methyladenosine (m1A) are prevalent modifications occurring in various RNA species of mammals. Apart from the single methylation of adenosine (m6A and m1A), dual methylation modification occurring in the nucleobase of adenosine, such as N6,N6-dimethyladenosine (m6,6A), also has been reported to be present in RNA of mammals. Whether there are other forms of dual methylation modification occurring in the nucleobase of adenosine other than m6,6A remains elusive. Here, we reported the existence of a novel adenosine dual methylation modification, i.e. 1,N6-dimethyladenosine (m1,6A), in tRNAs of living organisms. We confirmed that m1,6A is located at position 58 of tRNAs and is prevalent in mammalian cells and tissues. The measured level of m1,6A ranged from 0.0049% to 0.047% in tRNAs. Furthermore, we demonstrated that TRMT6/61A could catalyze the formation of m1,6A in tRNAs and m1,6A could be demethylated by ALKBH3. Collectively, the discovery of m1,6A expands the diversity of RNA modifications and may elicit a new tRNA modification-mediated gene regulation pathway.

CAS / MDL: 13010-53-2
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ENZYME AND MICROBIAL TECHNOLOGY · 2023 · IF 3.4

Rational design of tryptophan hydroxylation 1 for improving 5-Hydroxytryptophan production

Feifei Song,Tao Gu,Lin Zhang,Jiaxing Zhang,Shengping You,Wei Qi,Rongxin Su

5-Hydroxytryptophan (5-HTP) is a chemical precursor of serotonin, which synthesizes melatonin and serotonin in animals and regulates mood, sleep , and behavior. Tryptophan hydroxylase (TPH) uses tetrahydrobiopterin (BH4) as a cofactor to hydroxylate L -tryptophan ( L -Trp) to 5-HTP, and the low catalytic activity of TPH limits the rate of hydroxylation of L -Trp. In this study, the catalytic mechanism and structural features of L -Trp-TPH1-BH4 were investigated, and the catalytic activity was improved using a rational design strategy. Then the S337A/F318Y beneficial mutation was obtained. Molecular dynamics simulations showed that the S337A/F318Y mutant formed a salt bridge with TPH1 while forming an additional hydrogen bond with the substrate indole ring, stabilizing the indole ring and enhancing the binding affinity of the variant to L -Trp. As a result, the yield of 5-HTP was increased by 2.06-fold, resulting in the production of 0.91 g/L of 5-HTP. The rational design of the TPH structure to improve the hydroxylation efficiency of L -Trp offers the prospect of green production of 5-HTP.

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Antioxidants · 2021 ·Vol. 10 ·期 11 ·1733 · IF 6.313

Chlorophyllin Inhibits Mammalian Thioredoxin Reductase 1 and Triggers Cancer Cell Death

Shibo Sun,Yici Zhang,Weiping Xu,Yue Zhang,Rui Yang,Jianli Guo,Shui Guan,Qiang Ma,Kun Ma,Jianqiang Xu

Food colorants are widely used by humans in food production and preparation; however, their potential toxicity requires an in-depth analysis. In this study, five out of 15 commercial food colorants, namely, lutein, betanin, caramel, crocin and chlorophyll, significantly inhibited wild type selenoprotein thioredoxin reductase 1 (TrxR1, TXNRD1) in vitro. The hyperactive Sec498residue of TrxR1 was targeted by those five colorants, which was confirmed by the site-directed mutagenesis of TrxR1. Furthermore, two colorants, chlorophyll and betanin, triggered the oligomerization of TrxR1. A chlorophyll-derived compound, chlorophyllin, irreversibly inhibited the 5,5′-dithiobis-2-nitrobenzoic acid (DTNB) reducing activity of TrxR1 withKinact= 6.96 × 10−3± 0.49 × 10−3µM−1min−1. Moreover, chlorophyllin reduced the cellular TrxR activity, leading to reactive oxygen species (ROS) accumulation and, subsequently, promoting cancer cell death. In conclusion, this study might contribute to understand the food safety of commercial colorants and provide chemotherapeutic compounds by targeting TrxR1.Keywords:food colorants;thioredoxin reductase;chlorophyllin;cell death;selenocysteine;SecTRAPs (selenium compromised thioredoxin reductase-derived apoptotic proteins)

CAS / MDL: 11006-34-1
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CATALYSIS LETTERS · 2021 ·Vol. 152 ·期 1 ·162-171 · IF 3.186

Magnesium Pyrophosphate-Catalyzed Epoxidation of 1-Octene with Aqueous Hydrogen Peroxide

Yang Xingyu,Li Xu,Dong Jinxiang

The epoxidation of terminal olefins (e.g., 1-octene) presents an enormous challenge owing to their electron-deficient nature, whereas the vicinal diols that are derived from epoxides are highly desirable as fine chemicals. We report the facile preparation of magnesium pyrophosphate via the thermal decomposition of commercially available newberyite and the first use of magnesium pyrophosphate as a solid catalyst for terminal olefin epoxidation. The as-synthesized magnesium pyrophosphate was characterized by XRD, FTIR, SEM–EDS, and CO 2 -TPD techniques. The CO 2 -TPD results proved that the medium base was dominant in magnesium pyrophosphate. Magnesium pyrophosphate exhibited an effective catalytic activity in the liquid-phase epoxidation of 1-octene with a 94.2% selectivity of epoxide using aqueous hydrogen peroxide as oxidant in the presence of acetonitrile solvent. The influences of various reaction parameters, including solvent, temperature, H 2 O 2 to 1-octene molar ratio, amount of magnesium pyrophosphate, reaction time, and solvent amount were investigated. According to the reaction mechanism, the perhydroxyl ion that originated from H 2 O 2 heterocracking formed in the presence of magnesium pyrophosphate and reacted with acetonitrile to generate active intermediate peroxycarboximidic acid. The epoxide and amide formed when active oxygen was transferred from peroxycarboximidic acid to the olefin. Therefore, magnesium pyrophosphate was an appropriate catalyst for 1-octene epoxidation. Graphic Abstract

CAS / MDL: 75-05-8 111-66-0
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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Particle-bound PAHs induced glucose metabolism disorders through HIF-1 pathway

Siqi Wu,Zhongli Chen,Li Yang,Yulin Zhang,Xiaohe Luo,Jinsong Guo,Ying Shao

Vehicle exhaust, as one of the most important compositions of air pollution, induced various adverse health effects, especially diabetes, on human beings. Even though monitoring and epidemiological data indicates that particle-bound polycyclic aromatic hydrocarbons (PAHs) is an inducing factor of diabetes, the specific causative mechanisms are still unclear. In the current study, the concentration of particulate matters (PMs, including PM 1.0 , PM 2.5 and PM 10.0 ) and PAHs was investigated at rush hour of weekday in three urban underground parking garages (UPGs). To evaluate the impacts of particle-bound PAHs on human beings, analysis of non-target metabolomics and unmetabolized PAHs were conducted for UPG and non-UPG worker urine samples. The results showed that the highest concentrations of PMs and total PAHs were found at the UPG entrance. The concentrations of unmetabolized 5-6 rings PAHs in the UPG worker urine were significantly higher than that in non-UPG worker urine samples, which induced glucose metabolism disorders through hypoxia-inducible factor 1 (HIF-1) signaling pathway. This could be a reason for particle-bound PAHs induced-diabetes on road workers, drivers and garage staff. These findings can serve as a step towards air pollution management and the pathological mechanism analysis of environmental factor induced-diseases.

CAS / MDL: 7778-77-0
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Journal of Environmental Chemical Engineering · 2020 · IF 4.3

Thiol-functionalized PIM-1 for removal and sensing for mercury (II)

Junwen Xu,Shujuan Ma,Ya Li,Xiaowei Li,Junjie Ou,Mingliang Ye

Polymers of intrinsic microporosity (PIMs) are a class of microporous polymers with rigid and contorted molecular structures. The special structures lead to incomplete space occupation, and the pores of PIMs originate from the formed void. In this work, we made attempts to expand the applications of PIMs to the aspect of heavy metal removal. First, PIM-1 was synthesized using tetrafluoroterephthalonitrile (TFTPN) and 5,5′,6,6′-tetrahydroxy-3,3,3′,3′-tetramethyl-1,1′-spirobisindane (TTSBI) as precursors. The primary PIM-1 was quite hydrophobic, and thus could not be evenly dispersed in water, resulting in low adsorption capacity for mercury ions (Hg 2+ ). A conversion of nitrile group in PIM-1 to thiol group was then carried out by two steps, namely carboxylation and introduction of thiol groups. The carboxylation made the polymers more active, and the final thiol-functionalization provided the polymers with hydrophilicity and affinity for Hg 2+ . The thiolethyl modified PIM-1 (assigned as PIM-G) and thiophenyl modified (assigned as PIM-B) possessed maximum Hg 2+ adsorption capacity of 136 mg g −1 and127 mg g −1 at pH 5, respectively. Besides, the thiol-functionalized PIMs had fluorescence property and showed potential in sensing for Hg 2+ .

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Nature Communications · 2021 ·Vol. 12 ·期 1 ·1-20 · IF 14.919

Boosting anti-PD-1 therapy with metformin-loaded macrophage-derived microparticles

Wei Zhaohan,Zhang Xiaoqiong,Yong Tuying,Bie Nana,Zhan Guiting,Li Xin,Liang Qingle,Li Jianye,Yu Jingjing,Huang Gang,Yan Yuchen,Zhang Zelong,Zhang Bixiang,Gan Lu,Huang Bo,Yang Xiangliang

The main challenges for programmed cell death 1(PD-1)/PD-1 ligand (PD-L1) checkpoint blockade lie in a lack of sufficient T cell infiltration, tumor immunosuppressive microenvironment, and the inadequate tumor accumulation and penetration of anti-PD-1/PD-L1 antibody. Resetting tumor-associated macrophages (TAMs) is a promising strategy to enhance T-cell antitumor immunity and ameliorate tumor immunosuppression. Here, mannose-modified macrophage-derived microparticles (Man-MPs) loading metformin (Met@Man-MPs) are developed to efficiently target to M2-like TAMs to repolarize into M1-like phenotype. Met@Man-MPs-reset TAMs remodel the tumor immune microenvironment by increasing the recruitment of CD8 + T cells into tumor tissues and decreasing immunosuppressive infiltration of myeloid-derived suppressor cells and regulatory T cells. More importantly, the collagen-degrading capacity of Man-MPs contributes to the infiltration of CD8 + T cells into tumor interiors and enhances tumor accumulation and penetration of anti-PD-1 antibody. These unique features of Met@Man-MPs contribute to boost anti-PD-1 antibody therapy, improving anticancer efficacy and long-term memory immunity after combination treatment. Our results support Met@Man-MPs as a potential drug to improve tumor resistance to anti-PD-1 therapy.

CAS / MDL: 5505-63-5
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International Journal of Chemical Engineering · 2020 · IF 1.877

Thermophysical Properties of 1-Octyl-3-Methylimidazolium Acetate with Organic Solvents

Fuxin Yang,Peng Feng

Ionic liquid (IL) usually possesses high viscosity. In this work, the selected organic solvents, namely, dimethyl sulfoxide, N,N-dimethylacetamide, and N,N-dimethylformamide, were used as the diluents to lower IL viscosity. The thermophysical properties of the densities and viscosities for the binary mixtures of IL (i.e., 1-octyl-3-methylimidazolium acetate) with solvents were studied at normal pressure in the temperature ranges of 303.15 K to 348.15 K. The effects of the organic solvents on lowering IL viscosity were quantitatively evaluated. The excess properties of the mixtures were calculated to analyze the interactions between IL and solvents. The hard-sphere model was employed to reproduce the viscosity behavior of the pure substances and binary mixtures.

CAS / MDL: 67-64-1
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AIP Advances · 2020 ·Vol. 10 ·期 12 · IF 1.337

Hydrotalcite-assisted rapid synthesis of HKUST-1 toward efficient benzene capture

Xu Feng,Lv Daofei,Xu Weicheng,Yang Xixian,Sun Huili,Yuan Wenbin,Yan Jian,Chen Xin

Volatile organic compounds (VOCs) have been recognized as one of the major environmental hazards in the air. Metal organic frameworks (MOFs) and their associated materials have offered an excellent strategy for the adsorption removal of VOCs. In this work, we develop a facile and rapid synthesis method of HKUST-1, a typical and ideal Cu-based MOF, for VOC adsorption by using hydrotalcite as the intermediate for efficient crystallization at room temperature. The results show that HKUST-1 can be successfully synthesized within 10 s at room temperature. The as-synthesized HKUST-1 has a Brunauer-Emmett-Teller surface area of 2170.7 m 2 g −1 and a total pore volume of 0.977 cm 3 g −1 , which are among the highest reported values for such material. When tested for its benzene adsorption performance, the material can achieve a saturated adsorption capacity of 7.3 mmol g −1 at 35 °C. Based on the temperature-programmed desorption result, it is shown that the activation energy for the benzene desorption is 68.23 kJ mol −1 . The material can demonstrate a relatively constant saturated adsorption capacity after several adsorption/desorption cycles, which indicates good regenerative performance.

CAS / MDL: 554-95-0
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Biomolecules & Therapeutics · 2020 · IF 3.47

Contributions of HO-1-Dependent MAPK to Regulating Intestinal Barrier Disruption

Zhenling Zhang,Qiuping Zhang,Fang Li,Yi Xin,Zhijun Duan

The mitogen-activated protein kinase (MAPK) pathway controls intestinal epithelial barrier permeability by regulating tight junctions (TJs) and epithelial cells damage. Heme oxygenase-1 (HO-1) and carbon monoxide (CO) protect the intestinal epithelial barrier function, but the molecular mechanism is not yet clarified. MAPK activation and barrier permeability were studied using monolayers of Caco-2 cells treated with tissue necrosis factor α (TNF-α) transfected with FUGW-HO-1 or pLKO.1-sh-HO-1 plasmid. Intestinal mucosal barrier permeability and MAPK activation were also investigated using carbon tetrachloride (CCl 4 ) administration with CoPP (a HO-1 inducer), ZnPP (a HO-1 inhibitor), CO releasing molecule 2 (CORM-2), or inactived-CORM-2-treated wild-type mice and mice with HO-1 deficiency in intestinal epithelial cells. TNF-α increased epithelial TJ disruption and cleaved caspase-3 expression, induced ERK, p38, and JNK phosphorylation. In addition, HO-1 blocked TNF-α-induced increase in epithelial TJs disruption, cleaved caspase-3 expression, as well as ERK, p38, and JNK phosphorylation in an HO-1-dependent manner. CoPP and CORM-2 directly ameliorated intestinal mucosal injury, attenuated TJ disruption and cleaved caspase-3 expression, and inhibited epithelial ERK, p38, and JNK phosphorylation after chronic CCl 4 injection. Conversely, ZnPP completely reversed these effects. Furthermore, mice with intestinal epithelial HO-1 deficient exhibited a robust increase in mucosal TJs disruption, cleaved caspase-3 expression, and MAPKs activation as compared to the control group mice. These data demonstrated that HO-1-dependent MAPK signaling inhibition preserves the intestinal mucosal barrier integrity by abrogating TJ dysregulation and epithelial cell damage. The differential targeting of gut HO-1-MAPK axis leads to improved intestinal disease therapy.

CAS / MDL: 56-23-5
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Advanced Optical Materials · 2023 ·Vol. 11 ·期 15 ·2203140 · IF 9

2-in-1 Optimization for High Performance Semitransparent Perovskite Solar Cells

Jing Yang,Ziyu Wang,Lu Liu,Le Wang,Zhen Chang,Jianxun Li,Kai Wang,Shengzhong (Frank) Liu

Organic lead halide perovskites are regarded as qualified candidates for the photoactive layers of semitransparent solar cells. The critical aspect of boosting the performance of semitransparent perovskite solar cells (PSCs) to a higher level lies in preparing perovskite films with both excellent photoelectric properties and high transmittance. Herein, it is realized that, through theoretical analysis, perovskite materials with bandgap of 2.00–2.30 eV are suitable for the preparation of semitransparent PSCs that can simultaneously achieve low thermal-energy loss, allow transmission of light for high photopic response, and provide acceptable transmittance for photovoltaic greenhouses. Then the study aims at improving the crystallinity and morphology of wide-bandgap perovskite films by using additive engineering. As such, PSCs with absorber bandgaps of 2.02, 2.16, and 2.32 eV deliver maximum power-conversion efficiencies of 12.08%, 9.17%, and 8.42%, respectively. Then the corresponding semitransparent PSCs are crafted with average transmittance of light detectable by the human eye of 9.41%, 23.26%, and 43.47%, respectively. Furthermore, the crop growth factors are predicted to be 21.25%, 29.48%, and 37.07%, respectively. This work gives full play to bandgap modulation in the fabrication of semitransparent PSCs, which will broaden the application of semitransparent solar cells in the field of building integrated photovoltaics.

CAS / MDL: 7550-45-0
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TENSIDE SURFACTANTS DETERGENTS · 2023 ·Vol. 60 ·期 4 ·368-375 · IF 1

CuCl2-modified ionic liquids for alkylation of benzene with 1-dodecene

Yarou Yang,Xu Li,Jinxiang Dong

Benzene and 1-dodecene are often alkylated to produce linear alkylbenzene (LAB). LAB is the raw material for the production of linear alkylbenzene sulfonate (LAS), a very important anionic surfactant used in both industrial cleaning and commercial laundry processes, as well as in household laundry detergents. In the present study, we investigated the use of [Et 3 NH]Cl–2AlCl 3 modified with CuCl 2 as a catalyst for the alkylation of benzene with 1-dodecene, specifically looking at the effect of reaction conditions on product activity. The results showed that a conversion of 1-dodecene of 100.0 % and a selectivity of LAB of 93.79 % could be obtained when the following ideal reaction conditions were present: molar ratio of benzene/1-dodecene = 6, reaction temperature = 25 °C, reaction time = 10 min, stirring speed of 1000 rpm and addition of 5.0 mol % CuCl 2 ). The catalyst concentration was 7.0 mol %. FTIR and 31 P-TMPO-NMR measurements were performed to characterise the ionic liquid before and after the addition of CuCl 2 . After the addition of CuCl 2 , it was found that the acidity of the ionic liquid had decreased. The regeneration of the catalyst was also investigated and the cause of inactivation of the catalyst was determined. The results showed that CuCl 2 modified the ionic liquids and decreased the benzene/1-dodecene ratio, but the high product selectivity was maintained.

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