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(+)/(-)-Gerbeloid A,a pair of unprecedented coumarin-based polycyclic meroterpenoid enantiomers from Gerbera piloselloides:Structural elucidation,semi-synthesis,and lipid-lowering activity

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Acta Pharmaceutica Sinica B 2024年第6期14卷 2657-2668页

作者： chenxu zhao Jingrong Li Yue Hu Lingyu Li Meng Yu Yunfeng Huang Tao Zhang Hai Shang Zhongmei Zou State Key Laboratory of Bioactive Substance and Function of Natural Medicines Institute of Medicinal Plant DevelopmentChinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing 100193China Institute of Chinese Medicine Resources Guangxi Institute of Chinese Medicine&Pharmaceutical ScienceNanning 530000China

A pair of coumarin-based polycyclic meroterpenoid enantiomers(+)/(-)-gerbeloid A[(+)-1a and(-)-1b]were isolated from the medicinal plant Gerbera piloselloides,which have a unique caged oxatricyclo[4.***.2.0^(3,8)]decene scaffold.Their planar and three-dimensional structures were exhaustively characterized by comprehensive spectroscopic data and X-ray diffraction analysis.Guided by the hypothetical biosynthetic pathway,the biomimetic synthesis of racemic 1 was achieved using 4-hydroxy-5-methylcoumarin and citral as the starting material via oxa-6πelectrocyclization and intramolecular[2+2]photocycloaddition.Subsequently,the results of the biological activity assay demonstrated that both(+)-1a and(-)-1b exhibited potent lipid-lowering effects in 3T3-L1 adipocytes and the high-fat diet zebrafish model.Notably,the lipid-lowering activity of(+)-1a is better than that of(-)-1b at the same concentration,and molecular mechanism study has shown that(+)-1a and(-)-1b impairs adipocyte differentiation and stimulate lipolysis by regulating C/EBPα/PPARγsignaling and Perilipin signaling in vitro and in vivo.Our findings provide a promising drug model molecule for the treatment of obesity.

关键词： Gerbera piloselloides Natural products Coumarin meroterpenoid Structural elucidation Biomimetic synthesis Lipid-lowering activity 3T3-L1 adipocytes High-fat diet zebrafish model

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Turning the V site in V@2D-BC_(3)N_(2)complex to high curvature state for efficient CO_(2)electroreduction to hydrocarbons

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中国化学快报:英文版 2023年第8期34卷 328-332页

作者： Chaozheng He Yue Yu chenxu zhao Jinrong Huo Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi’an Technological UniversityXi’an 710021China School of Sciences Xi’an Technological UniversityXi’an 710021China

Hydrocarbons are promising products for CO_(2)electroreduction(CRR)while is impeded by the low selectivity.Turning the curvature of the active site is an effective strategy to change the adsorption properties and further regulate the product distribution and reactivity.Herein,we have designed a novel V single atom catalyst(SAC)based on rolled two-dimensional(2D)BC_(3)N_(2)substrate with different curvatures.The results have demonstrated that increased curvature can enhance the adsorption strength of CRR intermediates,which follows different mechanisms for systems with low and high curvature.This character eventually leads to the deviation away from the scaling line between Ead[CO]∼Ead[COOH]based on transition metals for V@2D-BC_(3)N_(2)systems.3-3 system is screened as the optimal candidate for hydrocarbons production due to the enhanced binding ability of adsorbates,which can increase the reactivity for hydrocarbons production and hinder the production of H2 and HCOOH simultaneously.

关键词： V doped 2D BC_(3)N_(2) Curvature effect CO_(2)electroreduction Hydrocarbons production d-band center theory Geometric and electronic properties

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Computational design of BC_(3)N_(2) based single atom catalyst for dramatic activation of inert CO_(2) and CH4 gasses into CH_(3)COOH with ultralow CH_(4) dissociation barrier

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Chinese Chemical Letters 2023年第1期34卷 493-498页

作者： chenxu zhao Menghui Xi Jinrong Huo Chaozheng He Ling Fu Institute of Environment and Energy Catalysis School of Materials Science and Chemical EngineeringXi’an Technological UniversityXi’an 710021China School of Sciences Xi’an Technological UniversityXi’an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

The production of CH_(3)COOH from CO_(2)and CH_(4) has stimulated much interest due to the high energy density of C2 species.Various kinds of catalysts have been developed while the high dissociation barrier of CH_(4) and low selectivity still hinders the efficiency of the reaction.We have herein proposed a novel catalyst with single metals loaded on 2D BC_(3)N_(2) substrate(M@2D-BC_(3)N_(2))based on density functional theory.Among numerous candidates,Pt@2D-BC_(3)N_(2) possesses the most favorable reactivity with an ultralow barrier of CH_(4) splitting(0.26 e V),which is due to the efficient capture ability of CH_(4) on Pt site.Besides,the selectivity for CH_(3)COOH is also very high,which mainly stems from the unique electronic properties of molecules and substrate:The degenerated states,including s,px,pyand pz,in CO_(2)reflects the existence of delocalizedπbonds between C and O.This can interact with states of Pt(s),Pt(pz),Pt(dxz),Pt(dyz),and Pt(z2)in Pt@2D-BC_(3)N_(2).The kinetics model also proves that our system can promote CH_(3)COOH production via simply increasing the temperature or the coverage of CH_(4) and CO_(2).Our results provide a reasonable illustration in clarifying mechanism and propose promising candidates with high reactivity for further study.

关键词： Density functional theory CO_(2)/CH4 coactivation 2D BC_(3)N_(2)substrate CH_(3)COOH production

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Associative vs. dissociative mechanism: Electrocatalysis of nitric oxide to ammonia

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Chinese Chemical Letters 2022年第2期33卷 1051-1057页

作者： Chaozheng He Jia Wang Ling Fu chenxu zhao Jinrong Huo Institute of Environment and Energy Catalysis Shaanxi Key Laboratory of Optoelectronic Functional Materials and DevicesSchool of Materials Science and Chemical EngineeringXi’an Technological UniversityXi’an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China School of Sciences Xi’an Technological UniversityXi’an 710021China

Nitric oxide reduction to ammonia by electrocatalysis is the potential application in the elimination of smog and energy conversion. In this work, the feasibility of the application of two-dimensional metal borides(MBenes) in nitric oxide electroreduction reaction(NOER) was investigated through density functional theory calculations. Including the geometry and electronic structure of five kinds of MBenes, the adsorption of NO on the surface of these substrates, the selective adsorption of hydrogen protons during the hydrogenation process, and the overpotential in the electrocatalytic ammonia synthesis process. As a result, Mn B exhibited the most favorable catalytic performance according to the associative pathways,which is thermodynamically performed spontaneously, and WB has a minimum overpotential of 0.37 V vs. RHE in the process of ammonia production according to the dissociative pathway. Overall, our work is the first to explore the electrocatalytic NO through the dissociative mechanism to synthesize ammonia in-depth and proves that MBenes are efficient NO electrocatalytic ammonia synthesis catalysts. These research results provide a new direction for the development of electrocatalytic ammonia synthesis experimentally and theoretically.

关键词： MBenes Nitric oxide NOER First-principles calculation Ammonia

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Highly active Fe_(36)Co_(44) bimetallic nanoclusters catalysts for hydrolysis of ammonia borane: The first-principles study

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Chinese Chemical Letters 2023年第2期34卷 550-556页

作者： Jinrong Huo Haocong Wei Ling Fu chenxu zhao Chaozheng He School of Sciences Xi'an Technological UniversityXi'an 710021China Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

In this paper,Fe_(36)Co_(44)nanocluster structure is used to catalyze the hydrolysis reaction of ammonia borane to produce H_(2).Firstly,we complete the construction of Fe_(36)Co_(44)cluster structure and calculate the electronic properties of the cluster.By comparing the adsorption process of Ammonia Borane (AB) in active sites of the cluster,which have different Effective Coordination Number (ECN),the qualitative relationship between ECN and the catalytic activation of AB is clarified,and the optimal catalytic active site is obtained.Then,from the perspective of different reaction paths,we study the hydrolysis reaction of AB in multiple paths,and obtain 5 different reaction paths and energy profiles.The calculation results show that in the case of N–H bond priority break (path 5),the reaction has the minimum rate-determining step (RDS) barrier (about 1.02 e V) and the entire reaction is exothermic (about 0.40 e V).So,path 5 is an optimal catalytic reaction path.This study will have an important guiding significance for the study of the AB hydrolysis reaction mechanism.

关键词： The first-principles NH_(3)BH_(3) Hydrolysis reaction FeCo cluster Catalyst

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Wip1 inhibits neutrophil extracellular traps to promote abscess formation in mice by directly dephosphorylating Coronin-1a

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Cellular & Molecular Immunology 2023年第8期20卷 941-954页

作者： Yifang Chen chenxu zhao Han Guo Weilong Zou zhaoqi Zhang Dong Wei Hezhe Lu Lianfeng Zhang Yong zhao State Key Laboratory of Membrane Biology Institute of ZoologyChinese Academy of SciencesBeijingChina University of Chinese Academy of Sciences BeijingChina Beijing Institute for Stem Cell and Regeneration BeijingChina Department of Hepatobiliary Surgery The Affiliated Hospital of Guizhou Medical UniversityGuiyangGuizhouChina Shenzhen Institute of Advanced Technology Chinese Academy of SciencesShenzhenChina Key Laboratory of Human Diseases Comparative Medicine Ministry of Health Institute of Laboratory Animal Science Chinese Academy of Medical SciencesBeijingChina

Neutrophil extracellular traps (NETs) participate in the rapid inhibition and clearance of pathogens during infection;however, the molecular regulation of NET formation remains poorly understood. In the current study, we found that inhibition of the wild-type p53-induced phosphatase 1 (Wip1) significantly suppressed the activity of Staphylococcus aureus (S. aureus) and accelerated abscess healing in S. aureus-induced abscess model mice by enhancing NET formation. A Wip1 inhibitor significantly enhanced NET formation in mouse and human neutrophils in vitro. High-resolution mass spectrometry and biochemical assays demonstrated that Coro1a is a substrate of Wip1. Further experiments also revealed that Wip1 preferentially and directly interacts with phosphorylated Coro1a than compared to unphosphorylated inactivated Coro1a. The phosphorylated Ser426 site of Coro1a and the 28–90 aa domain of Wip1 are essential for the direct interaction of Coro1a and Wip1 and for Wip1 dephosphorylation of p-Coro1a Ser426. Wip1 deletion or inhibition in neutrophils significantly upregulated the phosphorylation of Coro1a-Ser426, which activated phospholipase C and subsequently the calcium pathway, the latter of which promoted NET formation after infection or lipopolysaccharide stimulation. This study revealed Coro1a to be a novel substrate of Wip1 and showed that Wip1 is a negative regulator of NET formation during infection. These results support the potential application of Wip1 inhibitors to treat bacterial infections.

关键词： Wild-type p53-induced phosphatase 1(Wip1) Coro1a Calcium pathway Neutrophils Neutrophil extracellular trap(NET) Abscess

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Principles for designing CO_(2) adsorption catalyst: Serving thermal conductivity as the determinant for reactivity

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Chinese Chemical Letters 2022年第2期33卷 990-994页

作者： Chaozheng He Haotian Wang Ling Fu Jinrong Huo Zhiheng Zheng chenxu zhao Meng An Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi’an Technological UniversityXi’an 710021China College of Mechanical and Electrical Engineering Shaanxi University of Science and TechnologyXi’an 710021China School of Sciences Xi’an Technological UniversityXi’an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China School of Energy and Materials Shanghai Polytechnic UniversityShanghai 201209China Shanghai Engineering Research Center of Advanced Thermal Functional Materials Shanghai Polytechnic UniversityShanghai 201209China

CO_(2)is a representative prototype model in energy and environmental fields.Many factors for CO_(2)capture and activation have been investigated extensively but the research on the influence of thermal conductivity is still absence.We herein have calculated many properties,including dipole moment,electric structure,and adsorption energies,on Pt doped graphene and 2D BC_(3)N_(2)substrates and served the thermal conductivity as the bridge.Our results have demonstrated that the lower (higher) thermal conductivity for 2D BC_(3)N_(2)(graphene) corresponds to larger (lower) dipole moment,which is beneficial for CO_(2)activation (capture) process.Our research have not only revealed the dominant role of heat conductivity for CO_(2)capture and activation,but also paved the way for further catalyst design of various areas.

关键词： 2D materials Absorption Thermal conductivity Polarization bonding Molecular dynamics simulations Density functional theory

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Defect engineering for high-selection-performance of NO reduction to NH3 over CeO_(2)(111)surface:A DFT study

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Chinese Chemical Letters 2022年第1期33卷 527-532页

作者： Chaozheng He Risheng Sun Ling Fu Jinrong Huo chenxu zhao Xiuyuan Li Yan Song Sumin Wang Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China School of Sciences Xi'an Technological UniversityXi'an 710021China

To reduce the greenhouse effect caused by the surgery of nitrogen-oxides concentration in the atmosphere and develop a future energy carrier of renewables,it is very critical to develop more efficient,controllable,and highly sensitive catalytic materials.In our work,we proposed that nitric oxide(NO),as a supplement to N_(2) for the synthesis of ammonia,which is equipped with a lower barrier.And the study highlighted the potential of CeO_(2)(111)nanosheets with La doping and oxygen vacancy(OV)as a high-performance,controllable material for NO capture at the site of Vo site,and separation the process of hydrogenation.We also reported that the E_(ads) of-1.12 eV with horizontal adsorption and the Bader charge of N increasing of 0.53|e|and O increasing of 0.17|e|at the most active site of reduction-OV predicted.It is worth noting thatΔG of NORR(NO reduction reaction)shows good performance(thermodynamically spontaneous reaction)to synthesize ammonia and water at room temperature in the theoretical calculation.

关键词： La-doping CeO_(2) Bader analysis Oxygen vacancy(OV) Single atom catalysis Synergistic effect NO reduction reaction(NORR)

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Identification of niclosamide as a novel antiviral agent against porcine epidemic diarrhea virus infection by targeting viral internalization

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Virologica Sinica 2023年第2期38卷 296-308页

作者： Yue Wang Huimin Huang Dongliang Li chenxu zhao Shuai Li Panpan Qin Yaqin Li Xia Yang Wenjuan Du Wentao Li Yongtao Li College of Veterinary Medicine Henan Agricultural UniversityZhengzhou450002China State Key Laboratory of Agricultural Microbiology College of Veterinary MedicineHuazhong Agricultural UniversityWuhan430070China Faculty of Veterinary Medicine Utrecht UniversityUtrecht3584 CLthe Netherlands Hubei Hongshan Laboratory Wuhan430070China

Porcine epidemic diarrhea virus(PEDV),an enteropathogenic coronavirus,has catastrophic impacts on the global pig industry.However,there remain no effective drugs against PEDV infection.In this study,we utilized a recombinant PEDV expressing renilla luciferase(PEDV-Rluc)to screen potential anti-PEDV agents from an FDAapproved drug library in Vero cells.Four compounds were identified that significantly decreased luciferase activity of PEDV-Rluc.Among them,niclosamide was further characterized because it exhibited the most potent antiviral activity with the highest selectivity index.It can efficiently inhibit viral RNA synthesis,protein expression and viral progeny production of classical and variant PEDV strains in a dose-dependent manner.Time of addition assay showed that niclosamide exhibited potent anti-PEDV activity when added simultaneously with or after virus infection.Furthermore,niclosamide significantly inhibited the entry stage of PEDV infection by affecting viral internalization rather than viral attachment to cells.In addition,a combination with other small molecule inhibitors of endosomal acidification enhanced the anti-PEDV effect of niclosamide in vitro.Taken together,these findings suggested that niclosamide is a novel antiviral agent that might provide a basis for the development of novel drug therapies against PEDV and other related pathogenic coronavirus infections.

关键词： Coronavirus Porcine epidemic diarrhea virus(PEDV) Niclosamide(NIC) Antiviral Virus entry Endocytosis Host-targeted antivirals

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Effects of perinatal stress on the metabolites and lipids in plasma of dairy goats

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Stress Biology 2023年第1期3卷 126-144页

作者： Yan Huang Yezi Kong Bowen Li chenxu zhao Juan J.Loor Panpan Tan Yang Yuan Fangyuan Zeng Xiaoyan Zhu Simeng Qi Baoyu zhao Jianguo Wang College of Veterinary Medicine Northwest A&F UniversityYangling 712100ShaanxiChina LipidALL Technologies Company Limited Changzhou 213022JiangsuChina Department of Animal Sciences Division of Nutritional SciencesUniversity of IllinoisUrbanaIL 61801USA

Dairy goats experience metabolic stress during the peripartal period,and their ability to navigate this stage of lactation is related to the occurrence and development of metabolic diseases.Unlike dairy cows,there is a lack of comprehensive analysis of changes in the plasma profiles of peripartal dairy goats,particularly using high-throughput techniques.A subset of 9 clinically-healthy dairy goats were used from a cohort of 96 primiparous Guanzhong dairy goats(BCS,2.75±0.15).Blood samples were collected at seven time points around parturition(d 21,14,7 before parturition,the day of kidding,and d 7,14,21 postpartum),were analyzed using untargeted metabolomics and targeted lipidomics.The orthogonal partial least squares discriminant analysis model revealed a total of 31 differential metabolites including p-cresol sulfate,pyruvic acid,cholic acid,and oxoglutaric acid.The pathway enrichment analysis identified phenylalanine metabolism,aminoacyl-tRNA biosynthesis,and citrate cycle as the top three significantly-altered pathways.The Limma package identified a total of 123 differentially expressed lipids.Phosphatidylserine(PS),free fatty acids(FFA),and acylcarnitines(ACs)were significantly increased on the day of kidding,while diacylglycerols(DAG)and triacylglycerols(TAG)decreased.Ceramides(Cer)and lyso-phosphatidylinositols(LPI)were significantly increased during postpartum period,while PS,FFA,and ACs decreased postpartum and gradually returned to antepartum levels.Individual species of FFA and phosphatidylcholines(PC)were segregated based on the differences in the saturation and length of the carbon chain.Overall,this work generated the largest repository of the plasma lipidome and metabolome in dairy goats across the peripartal period,which contributed to our understanding of the multifaceted adaptations of transition dairy goats.

关键词： Dairy goat Transition period Untargeted metabolomics Lipidomics

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