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Metal-N_(4)model single‐atom catalyst with electroneutral quadri‐pyridine macrocyclic ligand for CO_(2)electroreduction

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Carbon Energy 2024年第8期6卷 122-133页

作者： Jian‐Zhao Peng Yin‐Long Li Yao‐Ti Cheng Fu‐Zhi Li Bo Cao Qing Wang xian Yue Guo‐tao Lai Yang‐Gang Wang Jun Gu Department of Chemistry Southern University of Science and TechnologyShenzhenGuangdongChina Institute for Catalysis Hokkaido UniversitySapporoJapan

Metal–N–C single‐atom catalysts,mostly prepared from pyrolysis of metalorganic precursors,are widely used in heterogeneous *** metal sites with diverse local structures coexist in this type of material and it is challenging to characterize the local structure,a reliable structure–property relationship is difficult to *** macrocyclic complexes adsorbed on carbon support are well‐defined models to mimic the singleatom ***–N_(4)site with four electroneutral pyridine‐type ligands embedded in a graphene layer is the most commonly proposed structure of the active site of single‐atom catalysts,but its molecular counterpart has not been *** this work,we synthesized the conjugated macrocyclic complexes with a metal center(Co,Fe,or Ni)coordinated with four electroneutral pyridinic ligands as model catalysts for CO_(2)*** comparison,the complexes with anionic quadri‐pyridine macrocyclic ligand were also *** Co complex with the electroneutral ligand expressed a turnover frequency of CO formation more than an order of magnitude higher than that of the Co complex with the anionic *** ab initio molecular dynamics simulations based on the well‐defined structures of the model catalysts indicate that the Co complex with the electroneutral ligand possesses a stronger ability to mediate electron transfer from carbon to CO_(2).

关键词： ab initio molecular dynamics CO_(2)reduction electrocatalysis model catalyst single‐atom catalyst

中国13个城市经皮冠状动脉介入治疗的成本疗效分析

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中华心血管病杂志 2010年第6期38卷 484-487页

作者：宋现涛杜梦阳苑飞吕树铮无首都医科大学附属北京安贞医院心内科 100029 代表冠心病介入治疗现状及医疗保险基金支付办法研究协作组

目的对经皮冠状动脉介入治疗（PCI）进行成本疗效分析.方法连续收集2006年1月至6月在中国13个城市行PCI的冠心病患者资料.利用SF-36健康调查量表对患者住院期间及出院9个月后的生命质量进行问卷调查,并依此进行成本疗效分析.结果（1... 详细信息

目的对经皮冠状动脉介入治疗（PCI）进行成本疗效分析.方法连续收集2006年1月至6月在中国13个城市行PCI的冠心病患者资料.利用SF-36健康调查量表对患者住院期间及出院9个月后的生命质量进行问卷调查,并依此进行成本疗效分析.结果（1）51.8%接受PCI的冠心病患者年龄在60岁以下.（2）患者住院成本中材料成本占82.5%、西药费占6.8%、手术费占5.9%,这3项共占总住院成本的95.2%,其中支架费用占材料成本的69.8%.（3）术后1年内患者再次入院成本：44例由于发生不良反应事件而再次入院患者的平均再次住院成本为17 841.5元.（4）术后1年内的药物费用：以使用频率最高的5种药（阿司匹林、氯吡格雷、美托洛尔、阿托伐他汀和辛伐他汀）的使用量和价格为依据,通过对患者术后1、3、6、9、12个月的随访调查显示,患者在术后平均每个月的药费为831.5元,每个月药费为400.0元的患者最多.（5）患者治疗后的生命质量显著提高,平均得分提高20.59分;每提高一个分值的生命质量需花费3975.7元;每获得一个质量调整生命年花费59 898.3元.结论我国PCI的成本疗效比在一个较为理想的范围内.

关键词：血管成形术,经腔,经皮冠状动脉费用效益分析质量校正寿命

Promotion and Mechanism of Acupotomy on Chondrocyte Autophagy in Knee Osteoarthritis Rabbits

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Chinese Journal of Integrative Medicine 2024年第9期30卷 809-817页

作者： LU Man MENG De-hong SHE Ze-yu WU xian XIA Shuai YANG Kai-ning LIU Cun-bin LI tao YANG Yong-hui The First Affiliated Hospital of Anhui University of Chinese Medicine Hefei230031China The Second Affiliated Hospital of Anhui University of Chinese Medicine Hefei230038China Department of Acupotomy Rehabilitation Anhui Provincial Hospital of Integrated Traditional Chinese and Western MedicineHefei230031China

Objective:To explore the effect of acupotomy intervention on autophagy of chondrocytes in rabbits with knee osteoarthritis(KOA),and to determine the possible mechanisms of acupotomy to alleviate cartilage ***:The modified Videman method was used to construct a KOA rabbit *** modeling,40 rabbits were randomly divided into 4 groups by a random number table:control;KOA(model);KOA+acupotomy(acupotomy),and KOA+sham acupotomy(sham),10 in each *** a 3-week treatment course,the knee joint activity was determined by the modified Lequesne MG ***-eosin staining staining was used to examine the morphological changes of *** of chondrocytes was observed by transmission electron *** surface morphology of cartilage tissue was observed by scanning electron *** mRNA and protein levels of AMP kinase/mammalian target of rapamycin/Unc-51(AMPK/mTOR/ULK1)signal pathway key proteins,autophagy-related factor Beclin-1 and microtubule-associated protein 1A/1B light chain 3(LC3)in rabbit knee cartilage were assessed by real-time fluorescence quantitative polymerase chain reaction and Western blot,***:The modified Lequesne MG score of acupotomy group was significantly lower than that of model group(P<0.05).Pathological results showed that chondrocyte autophagy decreased and cartilage surface was rough in the model group,which recovered after acupotomy *** mRNA expressions of AMPK,ULK1,Beclin-1 and the protein levels of p-AMPK,p-ULK1,Beclin-1,and LC3Ⅱ/LC3Ⅰwere decreased in the model group,while the mRNA and protein expressions of mTOR were increased(P<0.01).However,acupotomy treatment reversed these abnormal changes(P<0.05).Conclusions:Acupotomy could effectively up-regulate the expressions of AMPK,ULK1 and Beclin1,reduce the expression of mTOR,promote autophagy,and alleviate joint *** is a promising complementary and alternative therapy for KOA.

关键词： acupotomy knee asteoarthritis autophagy AMPK/mTOR/ULK1 signaling pathway rabbit

A mixed-valence polyoxometalate-based 3D inorganic framework cathode material for high-efficiency rechargeable AZIBs

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Rare Metals 2024年第8期43卷 3677-3691页

作者： Qing Han Hao-Ran Xiao tao Zhou Bing-Chuan Li Liu Yang Ling-Ling Xie Xue-Jing Qiu xian-Yong Wu Li-Min Zhu Xiao-Yu Cao School of Chemistry and Chemical Engineering Henan University of TechnologyZhengzhou 450001China Key Laboratory of High Specific Energy Materials for Electrochemical Power Sources of Zhengzhou City Zhengzhou 450001China College of Materials Engineering Henan University of EngineeringZhengzhou450007China School of Environmental Engineering Henan University of TechnologyZhengzhou 450001China Department of Chemistry University of Puerto Rico-Rio Piedras CampusSan JuanPR 00925USA

The global trend towards new energy storage systems has stimulated the development of electrochemical energy storage *** these technologies,rechargeable aqueous zinc-ion batteries(AZIBs)have attracted considerable interest as a potential alternative to lithium-ion batteries(LIBs)due to their affordable cost,environmental compatibility and high safety *** this study,a high-quality electrode for AZIBs has been successfully developed using a dehydrated mixed-valence polyoxometalate-based three-dimensional(3D)inorganic framework material known as[H_6Mn_(3)V^Ⅳ_(15)V-^Ⅴ_(4O)_(46)(H_2O)_(12)](3D-MnVO).This innovative 3D-MnVO material is built from the alternate connections of{V_(19)O_(46)}"sphere-shaped"clusters andμ_(2)-{Mn(H_(2)O)_(4)}bridges,where each{V_(19)O_(46)}cluster is surrounded by three pairs of vertically distributed{Mn(H_(2)O)_(4)}units,thus resulting in the 3D interpenetrating grid-like network from the infinite[-{V_(19)O_(46)}-μ_(2)-Mn(H_(2)O)_(4)-{V_(19)O_(46)}]_∞chains in three mutually perpendicular *** 3D framework structure of 3D-MnVO possesses abundant oxygen vacancies,spacious and multi-level interconnected channels for ion transport,which facilitates the efficient intercalation/deintercalation of hydrated Zn^(2+)into the pores of the primary structure via the intercalation capacitance *** a result,the 3D-MnVO electrode exhibits excellent diffusion rates and minimal interfacial *** a current density of 0.1 A·g^(-1),the 3D-MnVO cathode delivers a commendable discharge capacity of170.5 mAh·g^(-1)with 81.6%capacity retention after100 charge/discharge ***,even at a high current density of 1.0 A·g^(-1),the 3D-MnVO electrode delivers a remarkable reversible capacity of198.9 mAh·g^(-1).Our research results provide valuable insights into the development of advanced polyoxometalate-based 3D inorganic framework electrode materials for high-performance rechargeable AZIBs.

关键词： Cathode Polyoxometalate 3D inorganic framework Zinc-ion batteries Energy storage mechanism

Antibacterial and cytotoxic metabolites produced by Streptomyces tanashiensis BYF-112 isolated from Odontotermes formosanus

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Chinese Journal of Natural Medicines 2024年第9期22卷 822-830页

作者： WU Jun song tao ZHANG Le HUANG Zhongdi HUANG Fang YIN Caiping ZHANG Shuxiang LIU Xinhua ZHANG Yinglao School of Life Science Anhui Agricultural UniversityHefei 230036China School of Pharmacy Anhui Medical UniversityHefei 230036China

Chemical investigations of the termite-associated Streptomyces tanashiensis BYF-112 resulted in the discovery of four novel alkaloid derivatives: vegfrecines A and B(1 and 2), exfoliazone A(3), and venezueline H(7), in addition to nine known metabolites(4-6, 8-13). The structures of these compounds were elucidated through comprehensive spectroscopic analysis and comparison with existing literature data. Antibacterial assays revealed that viridomycin A(11) exhibited potent antibacterial activity against Staphylococcus aureus, with a zone of inhibition(ZOI) of 12.67 mm, in comparison to a ZOI of 17.67 mm for the positive control gentamicin sulfate. Viridomycin A(11) showed moderate activity against Micrococcus tetragenus and Pseudomonas syringae pv. actinidae, with ZOI values of 15.50 and 14.33 mm, respectively, which were inferior to those of gentamicin sulfate(34.67 and 24.00mm). Viridomycin F(12) also exhibited moderate antibacterial effects against S. aureus, M. tetragenus, and P. syringae pv. actinidae,with ZOI values of 8.33, 16.50, and 10.83 mm, respectively. Cytotoxicity assays demonstrated that viridobruunine A(5), exfoliazone(6), viridomycin A(11), and X-14881E(13) exhibited significant cytotoxicity against human malignant melanoma(A375), ovarian cancer(SKOV-3), and gastric cancer(MGC-803) cell lines, with IC_(50) values ranging from 4.61 to 19.28 μmol·L^(-1). Furthermore, bioinformatic analysis of the complete genome of S. tanashiensis suggested a putative biosynthetic gene cluster(BGC) responsible for the production of compounds 1-12. These findings indicate that the secondary metabolites of insect-associated S. tanashiensis BYF-112hold promise as potential sources of novel antibacterial and anticancer agents.

关键词： Odontotermes formosanus Streptomyces tanashiensis Alkaloid Cytotoxic activity Antibacterial activity Biosynthetic pathway

Coronary artery plaque imaging:Comparison of black-blood MRI and 64-multidetector computed tomography

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Chronic Diseases and Translational Medicine 2016年第3期2卷 -页

作者： Yi He Qin-Yi Da Jing An xian-tao song De-Biao Li Department of Radiology Beijing Institute of Heart Lung and Blood Vessel Disease Beijing Anzhen Hospital Capital Medical University Beijing 100029 China Siemens Healthcare MR Collaboration NE Asia Beijing 100102 China Department of Cardiology Beijing Institute of Heart Lung and Blood Vessel Disease Beijing Anzhen Hospital Capital Medical University Beijing 100029 China Cedars-Sinai Medical Center University of California Los Angeles USA

Objective: To comparatively evaluate black-blood coronary arterial wall MRI and 64-multidetector computed tomography (64-MDCT) for detection and classification of coronary artery plaques. Methods: We included 15 patients with confirmed coronary artery plaques in the proximal or middle segments of coronary arteries by 64-MDCT, who underwent black-blood coronary wall MRI at 1.5 T within 10 days. Cross-sectional coronary wall images were acquired using a 2D double-inversion-recovery, electrocardiograph-triggered, navigator-gated, fat-suppressed, turbo-spin-echo sequence on the coronary arteries with lesions from the ostium to the middle segment continuously without gap. The vessel cross-sectional area (CSA), luminal CSA, maximal wall thickness, plaque burden, contrast-to-noise ratio (CNR), and signal-to-noise ratio (SNR) were measured in each slice and subsequently compared with computed tomography angiography (CTA) images. CTA images were divided into 5-mm segments for side-by-side comparison with MRI. Results: Of the 15 patients, 12 were enrolled in the study. Coronary plaques were found in 46 slices on both CTA and MRI. Plaques were classified to 3 groups based on CTA:calcified plaques (n ? 11), soft plaques (n ? 23), and mixed plaques (n ? 12). In MRI, the plaque burden, maximal wall thickness, SNR, and CNR in the coronary walls containing plaques were greater than in the normal coronary walls (0.83 ± 0.08 vs. 0.73 ± 0.08, 1.88 ± 0.51 vs. 1.51 ± 0.26 mm, 12.95 ± 2.78 vs. 9.93 ± 2.31, and 6.76 ± 2.52 vs. 3.89 ± 1.54, respectively;P<0.05). The luminal CSA at the plaque was smaller than in normal coronary walls (2.50 ± 1.50 vs. 4.72 ± 2.28 mm2;P<0.05). The SNR in the soft plaque was significantly greater than in calcified and mixed plaques (P<0.05). Conclusions: Coronary wall MRI can identify coronary plaques in the proximal and middle segments and has the potential to differentiate plaque types based on signal intensity.

关键词： Magnetic resonance imaging Coronary artery Wall imaging Atherosclerosis Plaques

Metal-organic nanosheet assembly ions sieving membrane for precise lithium ion and anion/solvent separation toward robust lithium metal battery

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Science China Chemistry 2024年第10期67卷 3320-3327页

作者： Jian-Qiang Shen Tian-Tian Zhao Ying-Li song Lingjuan Zhang Ya-Nan Gao Xiao-Nan Cui Peng Zhao xian-Ming Zhang Key Laboratory of Magnetic Molecules&Magnetic Information Materials Ministry of EducationSchool of Chemistry&Material ScienceShanxi Normal UniversityTaiyuan 030031China College of Chemistry and Chemical Engineering Taiyuan University of TechnologyTaiyuan 030024China

Metal-organic nanosheets(MONs)as a novel material with tunable pore structures and low mass transfer resistance,have emerged as molecular sieves for the separation of gases and *** theory,they can also serve as ion sieves for lithium metal batteries(LMBs),realizing the high-energy and dendritic free ***,there are rarely relevant reports,because it is difficult to simultaneously balance efficient ion sieving ability,high ion passing rate and high electrochemical ***,we synthesized a stable ultrathin MON[Zn_(2)(Bim)_(4)]([Zn_(2)(Bim)_(4)]Nanosheet,HBim=benzimidazolate),which can achieve both efficient lithium ion sieving ability,high lithium ion passing rate and high electrochemical stability at the same *** separator assembled by this MON exhibits high Li^(+)transfer number of 0.81 due to the accurate lithium ion and anion/solvent *** battery containing such separator shows high lithium ionic conductivity of 0.74 m S cm^(-1)and low activation energy of 0.099 eV,which can be attributed to the nanometer level thickness and the ion sieving *** is more,we realized the application of MONs-based ion sieves in LMBs with intercalation cathodes for the first *** the LiFePO_(4)|Li battery with as-assembled separator demonstrates improved Coulombic efficiency(>99%)and significantly extended cycling life(>1600 cycles)with 80%capacity retention.

关键词： lithium sieving membrane metal-organic nanosheets lithium metal battery lithium ion and anion separation lithium ion and solvent separation

Re-estimating China's lake CO_(2)flux considering spatiotemporal variability

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Environmental Science and Ecotechnology 2024年第3期19卷 152-160页

作者： Zhidan Wen Yingxin Shang Lili Lyu Hui tao Ge Liu Chong Fang Sijia Li Kaishan song Northeast Institute of Geography and Agroecology Chinese Academy of SciencesChangchun130102China School of Environment and Planning Liaocheng UniversityLiaocheng252000China

The spatiotemporal variability of lake partial carbon dioxide pressure(pCO_(2))introduces uncertainty into CO_(2)fluxestimates at the lakewater-air *** the variationpattern of pCO_(2)isimportant for obtaining accurate global *** we examine seasonal and trophic variations in lake pCO_(2)based on 13 field campaigns conducted in Chinese lakes from 2017 to *** found significant seasonal fluctuations in pCO_(2),with decreasing values as trophic states intensify within the same *** lakes exhibit lower pCO_(2)levels thanfreshwater *** pCO_(2)dynamics result invariable areal CO_(2)emissions,withlakes exhibiting different trophic states(oligotrophication>mesotrophication>eutrophication)and saline lakes differing from freshwater lakes(-23.1±17.4 vs.19.3±18.3 mmol m^(-2)d^(-1)).These spatiotemporal pCO_(2)variations complicate total CO_(2)emission *** area proportions of lakes with varying trophic states and salinity in China,we estimate China's lake CO_(2)flux at 8.07 Tg C yr^(-1).In future studies,the importance of accounting for lake salinity,seasonal dynamics,and trophic statesmust be noticed to enhance the accuracy of large-scale carbon emission estimates from lake ecosystems in the context of climate change.

关键词： Carbon dioxide Eutrophication Saline lakes Overestimation Carbon budget

Upcycling of Poly(butylene adipate-co-terephthalate)into Dual Covalent Adaptable Networks through Chain Breaking-Crosslinking Strategy

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Chinese Journal of Polymer Science 2024年第10期42卷 1505-1513,I0011页

作者： Bin-Bo Wang Rong Huang Xin Wang tao Jiang Yi Wang Shuai Du Fa-Lin Li Jin Zhu song-Qi Ma Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi214122China Key Laboratory of Bio-based Polymeric Materials Technology and Application of Zhejiang Province Divisions of Polymers and CompositesNingbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo315201China University of Chinese Academy of Sciences Beijing100049China

Poly(butylene adipate-co-terephthalate)(PBAT),a widely studied biodegradable material,has not effectively addressed the problem of plastic *** into consideration the cost-effectiveness,upcycling PBAT should take precedence over direct composting *** present work adopts a chain breaking-crosslinking strategy,upcycling PBAT into dual covalent adaptable networks(CANs).During the chainbreaking stage,the ammonolysis between PBAT and polyethyleneimine(PEI)established the primary crosslinked ***,styrene maleic anhydride copolymer(SMA)reacted with the hydroxyl group,culminating in the formation of dual covalent adaptable *** contrast to PBAT,the PBAT-dual-CANs exhibited a notable Young's modulus of 239 MPa,alongside an inherent resistance to creep and *** to catalysis from neighboring carboxyl group and excess hydroxyl groups,the PBAT-dual-CANs exhibited fast stress ***,they could be recycled through extrusion and hot-press reprocessing,while retaining their *** straightforward strategy offers a solution for dealing with plastic waste.

关键词： Poly(butylene adipate-co-terephthalate) Dynamic crosslinked networks Chain breaking-crosslinking strategy Upcycle Recycle