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以重水为氘源的钴催化脱卤氘代反应

Chinese Journal of Catalysis 2024年第4期59卷 250-259页

作者：陈炳志季定纬周博超王小雨刘恒万伯顺胡向平陈庆安中国科学院大连化学物理研究所辽宁大连116023 中国科学院大学北京100049

自2017年氘代丁苯那嗪获得美国食品药品监督管理局批准以来,氘代化合物在药物开发领域的潜力受到越来越多的重视.开发高效实用的有机分子选择性氘化方法成为有机和药物化学家的研究热点.有机卤化物是性质稳定且来源广泛的化学品,其脱卤... 详细信息

自2017年氘代丁苯那嗪获得美国食品药品监督管理局批准以来,氘代化合物在药物开发领域的潜力受到越来越多的重视.开发高效实用的有机分子选择性氘化方法成为有机和药物化学家的研究热点.有机卤化物是性质稳定且来源广泛的化学品,其脱卤氘代反应已经发展成为构建氘代化合物的有效策略.然而,已报道的制备方法普遍存在氘代试剂昂贵、底物适用范围较窄或需要使用特殊的反应设备(光催化或电化学)等诸多问题.因此,开发简单普适的廉价金属催化体系,实现以廉价重水为氘源的脱卤氘代反应,具有重要的研究意义.相较于钯、铑等贵金属,储量丰富且毒性较低的钴金属催化剂对水分敏感度较低,且对C(sp2)-X和C(sp3)-X键活化都表现出较好的反应活性.基于此,本文开发了制备简单、普适性较好的钴催化体系,实现了位点选择性氘代化合物的构建.反应以锰金属为还原剂,重水为氘源,对各种类有机卤化物或类卤化合物,如芳基、烯基、苄基、烯丙基或烷基卤化物,均获得较好的收率和氘代率.值得注意的是,对于炔丙基乙酸酯类化合物,该催化体系也展现出较好的适用性,可以专一的选择性得到氘代联烯类化合物.在此基础上,成功将该方法应用于一系列药物类似物的选择性脱卤氘代.利用简单的C-O偶联和脱溴氘代反应,即可实现氘代的N-甲基度洛西汀的合成.鉴于药物分子直接进行氢-氘同位素交换时位点选择性控制的挑战,本文发展了卤代-氘代的两步策略.该策略成功应用于生育酚、萘普生、黄毒素、萘丁美酮等多个药物分子的位点选择性氢-氘同位素交换,充分展现出该催化合成方法在药物开发领域的应用潜力.为了验证反应机理,开展了一系列对照实验.结果表明,反应可能是由一价钴物种催化启动的.此外,自由捕获和抑制实验结果表明,反应并非通过自由基反应过程进行.基于以上实验结果提出了一个反应机理,它涉及Co(I)到Co(III)再回到Co(I)的催化循环.具体来说,首先,一价钴络合物与底物发生氧化加成生成三价钴络合物;随后,三价钴物种与重水络合,并通过还原消除的方式生成氘代化合物和一价钴物种.最后,为了验证这一机理,还利用密度泛函理论进行了计算,结果进一步证明了该机理的合理性.综上,本文利用钴催化体系,以廉价重水为氘源,实现芳基、烯基、苄基、烯丙基或烷基等卤化物,以及炔丙基乙酸酯类类卤化合物的选择性氘代反应.该反应表现出较好的底物适用性,为相关氘代有机化合物的制备提供了新思路.

关键词：钴催化脱卤氘代位点选择性氘代有机卤代物氘代药物

Long non-coding RNA BANCR promotes pancreatic cancer lymphangiogenesis and lymphatic metastasis by regulating the HIF-1α/VEGF-C/VEGFR-3 pathway via miR-143-5p

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Genes & Diseases 2024年第4期11卷 57-60页

作者： Shaolong Hao Yu ji weixuan Pan Hao Sun Fang Nie Jonathan Ray Warren Yuchuan ding wei Han Department of General Surgery Beijing Luhe HospitalCapital Medical UniversityTongzhouBeijing 101149China Department of Central Laboratory Beijing Luhe HospitalCapital Medical UniversityTongzhouBeijing 101149China Department of Neurosurgery Wayne State University School of MedicineJohn D.Dingell VA Medical CenterDetroitMI 48201USA

Pancreatic cancer is one of the most aggressive malignant tumors of the digestive system.Lymph node metastasis(LNM),as the main way of invasion and metastasis,can occur in the early stage of pancreatic cancer and be considered the most important factor affecting the clinical treatment and prognosis of patients with pancreatic cancer.

关键词： metastasis cancer invasion

Enhanced organic degradation and microbial community cooperation by inoculating Bacillus licheniformis in low temperature composting

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Journal of Environmental Sciences 2024年第9期143卷 189-200页

作者： jing Su Kaiyun Zhou Wenjie Chen Shaoqi Xu Ziwei Feng Yuan Chang Xiaoyan ding Yi Zheng Xingling Tao Ake Zhang Yue Wang ji Li Guochun ding Yuquan wei Nanjing Institute of Environmental Sciences Ministry of Ecology and EnvironmentNanjing 210042China College of Resources and Environmental Science Beijing Key Laboratory of Biodiversity and Organic FarmingChina Agricultural UniversityBeijing 100193China Organic Recycling Institute(Suzhou)of China Agricultural University Wuzhong DistrictSuzhou 215128China Fuyang Academy of Agricultural Sciences Fuyang 236065China

Microbial activity and interaction are the important driving factors in the start-up phase of food waste composting at low temperature.The aim of this study was to explore the effect of inoculating Bacillus licheniformis on the degradation of organic components and the potential microbe-driven mechanism from the aspects of organic matter degradation,enzyme activity,microbial community interaction,and microbial metabolic function.The results showed that after inoculating B.licheniformis,temperature increased to 47.8℃ on day2,and the degradation of readily degraded carbohydrates(RDC)increased by 31.2%,and the bioheat production increased by 16.5%.There was an obvious enhancement of extracellular enzymes activities after inoculation,especially amylase activity,which increased by 7.68 times on day 4.The inoculated B.licheniformis colonized in composting as key genus in the start-up phase.Modular network analysis and Mantel test indicated that inoculation drove the cooperation between microbial network modules who were responsible for various organic components(RDC,lipid,protein,and lignocellulose)degradation in the start-up phase.Metabolic function prediction suggested that carbohydrate metabolisms including starch and sucrose metabolism,glycolysis/gluconeogenesis,pyruvate metabolism,etc.,were improved by increasing the abundance of related functional genes after inoculation.In conclusion,inoculating B.licheniformis accelerated organic degradation by driving the cooperation between microbial network modules and enhancing microbial metabolism in the start-up phase of composting.

关键词： Microbial agent Organic matter degradation Microbial interaction Food waste Low temperature composting

Synergistic effects of chemical additives and mature compost on reducing H_2S emission during kitchen waste composting

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Journal of Environmental Sciences 2024年第5期139卷 84-92页

作者： Yongdi Liu Haihou Wang Hao Zhang Yueyue Tao Rui Chen Sheng Hang Xiaoyan ding Meidi Cheng Guochun ding Yuquan wei Ting Xu ji Li College of Resources and Environmental Science Beijing Key Laboratory of Biodiversity and Organic FarmingChina Agricultural UniversityBeijing 100193China Organic Recycling Institute(Suzhou)of China Agricultural University Wuzhong DistrictSuzhou 215128China Suzhou Academy of Agricultural Sciences Institute of Agricultural Sciences in Taihu Lake DistrictSuzhou 215155China Technical Centre for Soil Agriculture and Rural Ecology and EnvironmentMinistry of Ecology and EnvironmentBeijing 100012China College of Chemistry and Chemical Engineering Yantai UniversityYantai 264005China

Additives could improve composting performance and reduce gaseous emission,but few studies have explored the synergistic of additives on H_(2)S emission and compost maturity.This research aims to make an investigation about the effects of chemical additives and mature compost on H_(2)S emission and compost maturity of kitchen waste composting.The results showed that additives increased the germination index value and H_(2)S emission reduction over 15 days and the treatment with both chemical additives and mature compost achieved highest germination index value and H_(2)S emission reduction(85%).Except for the treatment with only chemical additives,the total sulfur content increased during the kitchen waste composting.The proportion of effective sulfur was higher with the addition of chemical additives,compared with other groups.The relative abundance of H_(2)S-formation bacterial(Desulfovibrio)was reduced and the relative abundance of bacterial(Pseudomonas and Paracoccus),which could convert sulfur-containing substances and H_(2)S to sulfate was improved with additives.In the composting process with both chemical additives and mature compost,the relative abundance of Desulfovibrio was lowest,while the relative abundance of Pseudomonas and Paracoccus was highest.Taken together,the chemical additives and mature compost achieved H_(2)S emission reduction by regulating the dynamics of microbial community.

关键词： Kitchen waste composting Sulfur conversion Chemical additives Mature compost Microbial community

Soft coarse-grained particle model for particle-fluid systems

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Particuology 2024年第1期84卷 178-193页

作者： Yanhao Ye ji Xu wei Ge State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing100190China

By modeling a group of neighboring real particles as a single coarse-grained particle(CGP),discrete particle method(DPM)is now capable of simulating industrial-scale particle-fluid systems.However,a systematic approach to determine the CGP properties and develop their interaction models is still lacking,which casts uncertainty on the predictivity of the method.In this study,collisions between predefined particle groups are analyzed to construct kernel functions for modeling the CGPs and then the model parameters are determined by equating the statistical properties of the CGPs and the real particles in the physical process studied.This approach is implemented for homogeneous cooling of granular gas,then demonstrated effective in simulating experimental fluidized beds.

关键词： Coarse-grain(CG) Discrete particle method(DPM) Fluidized bed Multi-scale simulation

A review on g-C_(3)N_(4)decorated with silver for photocatalytic energy conversion

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Chinese Chemical Letters 2024年第2期35卷 187-196页

作者： Ziyu Pan Wufan ding Hanchun Chen Haodong ji Eco-environment and Resource Efficiency Research Laboratory School of Environment and EnergyPeking University Shenzhen Graduate SchoolShenzhen 518055China

Artificial photocatalytic energy conversion is considered as the most potential strategy for solving the increasingly serious energy crisis and environmental pollution problems by directly capturing solar energy.Therefore,high efficiency photocatalyst has drawn significant research attention in recent years.Due to the excellent electronic,optical,structural,and physicochemical performances,silver-based g-C_(3)N_(4)have become promising photocatalysts.This review emphasizes the recent progresses and challenges on g-C_(3)N_(4)decorated with silver for photocatalytic energy conversion.The extensive use of g-C_(3)N_(4)decorated with silver in diverse photocatalytic reactions,including hydrogen evolution,pollutant degradation and carbon dioxide reduction,is also fully introduced.In addition,we propose the perspectives of g-C_(3)N_(4)decorated with silver on photocatalytic applications.We hope that this review will shed some light on the photocatalytic energy conversion of g-C_(3)N_(4)decorated with silver.

关键词： g-C_(3)N_(4) Silver-modified g-C_(3)N_(4) Photocatalytic energy conversion H_(2)evolution Pollutant degradation CO_(2)reduction

Sedimentary and Heavy Mineral Records for the Oligocene-Miocene Exhumation of the Easternmost Tianshan

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Journal of Earth Science 2024年第2期35卷 449-461页

作者： Yan ding Tianyi Shen Guocan Wang Junliang ji School of Earth Sciences Center for Global TectonicsChina University of GeosciencesWuhan430074China State Key Laboratory of Geological Processes and Mineral Resources China University of GeosciencesWuhan430078China Hubei Key Laboratory of Critical Zone Evolution School of Geography and Information EngineeringChina University of GeosciencesWuhan430074China

The topography of the Harlik Mountain has a strong impact on the formation of current arid climate in the Turpan-Hami Basin.However,it is still controversial if Harlik Mountain experienced significant exhumation during the Middle to Late Cenozoic according to the previous thermochronology studies.The features of the Oligocene to Miocene sediments in the foreland basin could provide productive information for resolving the debates.The peak ages of detrital apatite fission track analysis of the Oligocene–Miocene sandstone in the Turpan-Hami Basin are well comparable with the cooling age records of the Harlik Mountain rocks,indicating that the Oligocene–Miocene Taoshuyuanzi Formation in the basin was mostly derived from the Harlik Mountain.The stratigraphic sequence exhibits coarsening upward,reflecting that the source area was in a tectonically active period during the deposition process.Heavy mineral assemblages also suggest that the unstable minerals in the sediment increased significantly at the end of the deposition.Moreover,the proportion of apatite increased up-section,while the garnet content decreased significantly,indicating that the Carboniferous metamorphic rocks have been gradually eroded out and more intrusive rocks have been exposed to the surface.These observations suggest that the Harlik Mountain experienced exhumation during the Oligocene to Miocene,and the denudation depth afterward was probably less than 2.5 km according to the previously apatite(U-Th)/He data.The Oligocene–Miocene exhumation probably acted as one of the triggers for the heavy drought of the Turpan-Hami Basin during the Middle–Late Neogene.

关键词： Turpan-Hami Basin Harlik Mountain Taoshuyuanzi Formation Oligocene–Miocene uplift sedimentology structural geology

A Hybrid Signal Processing Method Combining Mathematical Morphology and Walsh Theory for Power Quality Disturbance Detection and Classification

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CSEE Journal of Power and Energy Systems 2024年第2期10卷 584-592页

作者： Zhi ding Tianyao ji Mengshi Li Q.H.Wu School of Electric Power Engineering South China University of Technology(SCUT)Guangzhou 510641China

In this paper, a novel signal processing method combining mathematical morphology (MM) and Walsh theory is proposed, which uses Walsh functions to control the structuring element (SE) and MM operators. Based on the Walsh-MM method, a scheme for power quality disturbances detection and classification is developed, which involves three steps: denoising, feature extraction and morphological clustering. First, various evolution rules of Walsh function are used to generate groups of SEs for the multiscale Walsh-ordered morphological operation, so the original signal can be denoised. Next, the fundamental wave of the denoised signal is suppressed by Hadamard matrix;thus, disturbances can be extracted. Finally, the Walsh power spectrum of the waveform extracted in the previous step is calculated, and the parameters of which are taken by morphological clustering to classify the disturbances. Simulation results reveal the proposed scheme can effectively detect and classify disturbances, and the Walsh-MM method is less affected by noise and only involves simple calculation, which has a potential to be implemented in hardware and more suitable for real-time application.

关键词： Hadamard matrix mathematical morphology morphological clustering power quality disturbance Walsh theory

Protective mechanism of quercetin in alleviating sepsis-related acute respiratory distress syndrome based on network pharmacology and in vitro experiments

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World Journal of Emergency Medicine 2024年第2期15卷 111-120页

作者： weichao ding wei Zhang Juan Chen Mengmeng Wang Yi Ren jing Feng Xiaoqin Han Xiaohang ji Shinan Nie Zhaorui Sun Department of Emergency Medicine Jinling HospitalAffiliated Hospital of Medical SchoolNanjing UniversityNanjing 210002China Department of Emergency Medicine Jinling Clinical Medical College of Nanjing University of Chinese MedicineNanjing 210002China Department of Emergency Medicine the Affiliated Hospital of Xuzhou Medical UniversityXuzhou 221002China Department of Emergency Medicine Xuzhou Municipal Hospital Affiliated to Xuzhou Medical UniversityXuzhou 221000China

BACKGROUND:Sepsis-related acute respiratory distress syndrome(ARDS)has a high mortality rate,and no effective treatment is available currently.Quercetin is a natural plant product with many pharmacological activities,such as antioxidative,anti-apoptotic,and anti-inflammatory effects.This study aimed to elucidate the protective mechanism of quercetin against sepsis-related ARDS.METHODS:In this study,network pharmacology and in vitro experiments were used to investigate the underlying mechanisms of quercetin against sepsis-related ARDS.Core targets and signaling pathways of quercetin against sepsis-related ARDS were screened and were verified by in vitro experiments.RESULTS:A total of 4,230 targets of quercetin,360 disease targets of sepsis-related ARDS,and 211 intersection targets were obtained via database screening.Among the 211 intersection targets,interleukin-6(IL-6),tumor necrosis factor(TNF),albumin(ALB),AKT serine/threonine kinase 1(AKT1),and interleukin-1β(IL-1β)were identified as the core targets.A Gene Ontology(GO)enrichment analysis revealed 894 genes involved in the inflammatory response,apoptosis regulation,and response to hypoxia.Kyoto Encyclopedia of Genes and Genomes(KEGG)enrichment analysis identified 106 pathways.After eliminating and generalizing,the hypoxia-inducible factor-1(HIF-1),TNF,nuclear factor-κB(NF-κB),and nucleotide-binding and oligomerization domain(NOD)-like receptor signaling pathways were identified.Molecular docking revealed that quercetin had good binding activity with the core targets.Moreover,quercetin blocked the HIF-1,TNF,NF-κB,and NODlike receptor signaling pathways in lipopolysaccharide(LPS)-induced murine alveolar macrophage(MH-S)cells.It also suppressed the inflammatory response,oxidative reactions,and cell apoptosis.CONCLUSION:Quercetin ameliorates sepsis-related ARDS by binding to its core targets and blocking the HIF-1,TNF,NF-κB,and NOD-like receptor signaling pathways to reduce inflammation,cell apoptosis,and oxidative stress.

关键词： Quercetin Sepsis-related acute respiratory distress syndrome Network pharmacology