作者机构：
[Hao, Ge-Fei; Li, Xiao-Hong; Gao, Yang-Yang] Guizhou Univ, Ctr Res & Dev Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang, Peoples R China.;[Li, Jing-Yi; Liu, Chun-Rong; Hao, Ge-Fei; Li, Meng-Zhao; Li, JY] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan, Peoples R China.
通讯机构：
[Liu, CR; Li, JY] C;[Hao, GF ] G;Guizhou Univ, Ctr Res & Dev Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang, Peoples R China.;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan, Peoples R China.
关键词：
wearable sensors;in-situ and continuous;monitoring;plant health information;precision agriculture
摘要：
Plant health is intricately linked to crop quality, food security and agricultural productivity. Obtaining accurate plant health information is of paramount importance in the realm of precision agriculture. Wearable sensors offer an exceptional avenue for investigating plant health status and fundamental plant science, as they enable real-time and continuous in-situ monitoring of physiological biomarkers. However, a comprehensive overview that integrates and critically assesses wearable plant sensors across various facets, including their fundamental elements, classification, design, sensing mechanism, fabrication, characterization and application, remains elusive. In this study, we provide a meticulous description and systematic synthesis of recent research progress in wearable sensor properties, technology and their application in monitoring plant health information. This work endeavours to serve as a guiding resource for the utilization of wearable plant sensors, empowering the advancement of plant health within the precision agriculture paradigm.
摘要：
With increasingly stringent regulations, the reduction of NOx emissions during vehicle cold start is a major challenge. Pd-modified zeolites are considered as the most promising passive NOx adsorber (PNA) for cold start NOx control. Nevertheless, the scarcity and the high cost of Pd limit its practical application. Herein, a non-precious metal modified Co/Na-SSZ-13 zeolite for low-temperature NOx adsorption is reported. This one-pot synthesized Co/Na-SSZ-13 exhibits an extraordinary NOx storage capacity (212 mu mol g(cat)(-1)) under humid conditions (3% H2O v/v), which is more than double that of conventional Co or Pd-modified SSZ-13. This is attributed to the absence of the inert cobalt phyllosilicate commonly found in conventional Co-SSZ-13, as well as the highly dispersed Co and Na ions as the effective NOx adsorption sites in Co/Na-SSZ-13. Moreover, the presence of Na ions shields the negative charge generated by the Al center and weakens the local electric field strength of the Al and Co centers. This lowers the H2O adsorption energy and improves the zeolite hydrophobicity, which enhances the NO storage capacity of the Co/Na-SSZ-13 under humid conditions. This work highlights the Co/Na-SSZ-13, synthesize via a simple and high-efficiency method, as a promising substitute for noble metal PNA materials.
作者机构：
[Dong, Suwei] Peking Univ, State Key Lab Nat & Biomimet Drugs, Beijing 100191, Peoples R China.;[Dong, Suwei] Peking Univ, Sch Pharmaceut Sci, Beijing 100191, Peoples R China.;[Tang, Shan; Zheng, Ji-Shen] Univ Sci & Technol China, Div Life Sci & Med, Hefei 230027, Peoples R China.;[Li, Yiming] Hefei Univ Technol, Engn Res Ctr Bioproc, Sch Food & Biol Engn, Minist Educ, Hefei 230009, Peoples R China.;[Wang, Huan] Nanjing Univ, Sch Chem & Chem Engn, Nanjing 210023, Peoples R China.
通讯机构：
[Liu, L ] T;Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China.
关键词：
chemical protein synthesis;solid-phase peptide synthesis;ligation reactions;post-translational modifications;mirror-image proteins;peptide drugs
摘要：
The central dogma of modern biology underscores the pivotal roles proteins play in diverse biological processes, the study of which necessitates advanced methods to produce proteins with precision and versatility. Chemical protein synthesis, a powerful approach utilizing chemical reactions for the de novo construction of structurally accurate proteins, has emerged as a transformative tool for studying proteins and generating protein derivatives/mimics inaccessible by natural biological machinery, including post-translationally modified proteins, proteins comprised of unnatural amino acids, as well as mirror-image proteins. This review summarizes recent strides in synthetic method developments for chemical protein synthesis, including innovative techniques in solid-phase peptide synthesis, the challenges presented by difficult sequences in either synthesis or folding and the exploration of novel ligation reactions using both chemical and enzymatic methods. Furthermore, the review also delves into newly developed protocols for site-selective protein modifications and the generation of stapled or macrocyclized peptides/mini-proteins, highlighting the power of chemical methods to make structurally diverse proteins. Recent applications of synthetic proteins in investigating post-translational modifications (phosphorylation, lipidation, glycosylation, ubiquitination, etc.), mirror-image biological processes and drug development are further discussed. Together, these topics provide a comprehensive overview of the current landscape of chemical protein synthesis.
摘要：
Viruses are ubiquitous in human life. Some viruses can be used as vectors of genetic engineering and specific pesticides. Other viruses trigger a variety of diseases in humans, animals and plants, resulting in high infection rates and mortality. Therefore, convenient, accurate and rapid detection of viruses is of great significance for the diagnosis and treatment of subsequent diseases. In contrast to traditional methods of detection, which rely on time-consuming and complex techniques such as polymerase chain reaction (PCR), fluorescent probes and imaging methods generate real-time results, with high specificity, and have been widely used in viral detection. In this review, the application of viral fluorescent probes in analyzing the molecular structure, detection and biological imaging is discussed. In particular, we catego-rized the probes based on their specificity for human and plant viruses, reviewing the latest findings and analyzing their limitations. The potential of fluorescent molecular probes in the treatment of viral dis-ease and environmental analysis, and their possible combinations with protein and immune technology are discussed.(c) 2023 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
期刊：
CHEMISTRY OF MATERIALS,2024年36(4):1975-1981 ISSN：0897-4756
通讯作者：
Cheng, Jing;Li, HB
作者机构：
[Cheng, Jing; Li, Guang; Xu, Weiwei; Li, Haibing; Ma, Cuiguang; Li, HB; He, Qiang; Zhang, Haifan; Qu, Haonan] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Cheng, J; Li, HB ] C;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
Chiral fungicides have been widely used for disease control in agricultural cultivation due to their advantages of high efficiency, low toxicity, high selectivity, and low residue. However, the enantiomers of chiral fungicides in the chiral environment often exhibit different physiological and biochemical properties and sometimes even diametrically opposite effects. This work modified the chiral alanine-functionalized pillar[5]arene within PET nanochannels. The binary hybridized nanochannel exhibits high selectivity for the chiral fungicide Propranolol, with a selectivity coefficient of 7.36, which is seven times higher than that of the LAP[5] nanochannel membrane. The mechanism of chiral selectivity was explored by COMSOL finite element simulation, which proves the high selectivity of the binary hybrid nanochannel originated from the high surface charge density of the nanochannel. This study provides a novel and effective method for the selective enrichment and release of chiral pesticides in green agriculture.
期刊：
Journal of Hazardous Materials,2024年465:133009 ISSN：0304-3894
通讯作者：
Jia, FL
作者机构：
[Zhang, Lizhi; Jia, Falong; Guo, Furong; Li, Donglei; Zhang, Yuhang; She, Liang; Ai, Zhihui; Liu, Xiao] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Jia, FL ] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
关键词：
Cu(II)-EDTA;Decomplexation;Ferrous formate shell;Oxidative degradation;Zero-valent iron
摘要：
Heavy metal complexes in industrial wastewater are challenging to be removed by conventional methods arising from their stable chelating structure. In this study, zero-valent iron (ZVI) was ball-milled with tiny formic acid (FA), and the as-prepared sample (FA-ZVI(bm)) was attempted to eliminate a model heavy metal complex of Cu(II)-ethylenediaminetetraacetic acid (Cu(II)-EDTA). The addition of FA to ball-milling could dramatically enhance the performance of ball-milled ZVI (ZVI(bm)) towards Cu(II)-EDTA removal and increase the removal rate constant by 80 times. This conspicuous improvement of Cu(II)-EDTA elimination was attributed to the ferrous formate (Fe(HCOO)(2)) shell formed on the surface of FA-ZVI(bm). Results revealed that the Fe(HCOO)(2) shell facilitated the activation of O(2) to reactive oxygen species (ROS) and the leaching of Fe(3+). Cu(II)-EDTA was decomplexed through both oxidative destruction and Fe(3+) replacement, and the released Cu(2+) was reduced by FA-ZVI(bm) and immobilized synchronously. Meanwhile, the ligands underwent oxidative degradation by ROS, thus avoiding the re-chelation ecological risk. Impressively, FA-ZVI(bm) could achieve cyclic treatment of actual copper complex wastewater and possessed promising advantage in treatment cost. This study would offer a promising approach for eliminating Cu(II)-EDTA through EDTA ligands degradation and synchronous Cu(II) removal, moreover to shed light on the decomplexation mechanism.
作者机构：
[Chen, Shuibing; Pan, Fong Cheng; Feng, Lingling; Evans, Todd; Pan, FC; Duan, Xiaohua; de Silva, Neranjan; Greenspun, Benjamin; Chandwani, Rohit] Weill Cornell Med, Dept Surg, 1300 York Ave, New York, NY 10065 USA.;[Chen, Shuibing; Evans, Todd; Duan, Xiaohua; Greenspun, Benjamin] Weill Cornell Med, Ctr Genom Hlth, 1300 York Ave, New York, NY 10065 USA.;[Zhang, Tuo] Weill Cornell Med, Genom Resources Core Facil, New York, NY 10065 USA.;[Feng, Lingling] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Wang, Xing; Moyer, Jenna; Elemento, Olivier; Martin, M. Laura] Weill Cornell Med, Caryl & Israel Englander Inst Precis Med, New York, NY USA.
通讯机构：
[Evans, T; Chen, SB; Chen, SB ; Pan, FC ] W;Weill Cornell Med, Dept Surg, 1300 York Ave, New York, NY 10065 USA.;Weill Cornell Med, Ctr Genom Hlth, 1300 York Ave, New York, NY 10065 USA.
关键词：
KRAS;SREBP2;cholesterol biosynthesis;colon cancer organoids;lung cancer organoids;orthotopic transplantation;pancreatic organoid;perhexiline maleate;targeted therapy
摘要：
KRAS mutations, mainly G12D and G12V, are found in more than 90% of pancreatic ductal adenocarcinoma (PDAC) cases. The success of drugs targeting KRAS(G12C) suggests the potential for drugs specifically targeting these alternative PDAC-associated KRAS mutations. Here, we report a high-throughput drug-screening platform using a series of isogenic murine pancreatic organoids that are wild type (WT) or contain common PDAC driver mutations, representing both classical and basal PDAC phenotypes. We screened over 6,000 compounds and identified perhexiline maleate, which can inhibit the growth and induce cell death of pancreatic organoids carrying the Kras(G12D) mutation both invitro and invivo and primary human PDAC organoids. scRNA-seq analysis suggests that the cholesterol synthesis pathway is upregulated specifically in the KRAS mutant organoids, including the key cholesterol synthesis regulator SREBP2. Perhexiline maleate decreases SREBP2 expression levels and reverses the KRAS mutant-induced upregulation of the cholesterol synthesis pathway.
作者机构：
[Yang, Wenchao; Yang, WC; Lu, Mengjiao; Pang, Yida] Guizhou Univ, Ctr R&D Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang 550025, Peoples R China.;[Sun, Yao; Pang, Yida] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Kim, Jong Seung; Kim, JS; Rha, Hyeonji] Korea Univ, Dept Chem, Seoul 02841, South Korea.;[Sharma, Amit; Sharma, A] CSIR Cent Sci Instruments Org, Sect 30C, Chandigarh 160030, India.;[Kim, Jong Seung; Kim, JS] TheranoChem Inc, Seoul 02856, South Korea.
通讯机构：
[Yang, WC ] G;[Kim, JS ] K;[Sun, Y ; Sharma, A ] C;Guizhou Univ, Ctr R&D Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang 550025, Peoples R China.;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
Fluorescence imaging is a non-invasive and highly sensitive bioimaging technique that has shown remarkable strides in plant science. It enables real-time monitoring and analysis of biological and pathological processes in plants by labeling specific molecular or cellular structures with fluorescent probes. However, tissue scattering and phytochrome interference have been obstacles for conventional fluorescence imaging of plants in the ultraviolet and visible spectrum, resulting in unsatisfactory imaging quality. Fortunately, advances in near-infrared (NIR) fluorescence imaging technology (650-900 nm) offer superior spatial-temporal resolution and reduced tissue scattering, which is sure to improve plant imaging quality. In this review, we summarize recent progress in the development of NIR fluorescence imaging probes and their applications for in vivo plant imaging and the identification of plant-related biomolecules. We hope this review provides a new perspective for plant science research and highlights NIR fluorescence imaging as a powerful tool for analyzing plant physiology, adaptive mechanisms, and coping with environmental stress in the near future.
通讯机构：
[Zhang, ZH; Lei, HH ] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;Wuhan Inst Photochem & Technol, Wuhan 430083, Hubei, Peoples R China.
摘要：
Regioselective C-H amination of simple arenes is highly desirable, but accessing meta-sites of ubiquitous arenes has proven challenging due to the lack of both electronic and spatial preference. This study demonstrates the successful use of various privileged nitrogen-containing functionalities found in pharmaceutical compounds to direct meta-C-H amination of arenes, overcoming the long-standing requirement for a redundant directing group. The remarkable advancements in functional group accommodation for precise regiochemical control were achieved through the discovery of an unprecedented organo-initiator and the strategic utilization of non-covalent interactions. This protocol has been successfully applied in the concise synthesis and late-stage derivatization of drug molecules, which would have been otherwise challenging to achieve.
摘要：
In the pursuit of advancing materials for methane storage, a critical consideration arises given the prominence of natural gas (NG) as a clean transportation fuel, which holds substantial potential for alleviating the strain on both energy resources and the environment in the forthcoming decade. In this context, a novel approach is undertaken, employing the rigid triptycene as a foundational building block. This strategy is coupled with the incorporation of dichloromethane and 1,3-dichloropropane, serving as rigid and flexible linkers, respectively. This combination not only enables cost-effective fabrication but also expedites the creation of two distinct triptycene-based hypercrosslinked polymers (HCPs), identified as PTN-70 and PTN-71. Surprisingly, despite PTN-71 manifesting an inferior Brunauer-Emmett-Teller (BET) surface area when compared to the rigidly linked PTN-70, it showcases remarkably enhanced methane adsorption capabilities, particularly under high-pressure conditions. At a temperature of 275 K and a pressure of 95 bars, PTN-71 demonstrates an impressive methane adsorption capacity of 329 cm(3) g(-1). This exceptional performance is attributed to the unique flexible network structure of PTN-71, which exhibits a pronounced swelling response when subjected to elevated pressure conditions, thus elucidating its superior methane adsorption characteristics. The development of these advanced materials not only signifies a significant stride in the realm of methane storage but also underscores the importance of tailoring the structural attributes of hypercrosslinked polymers for optimized gas adsorption performance.
期刊：
JOURNAL OF NATURAL PRODUCTS,2024年87(1):141-151 ISSN：0163-3864
通讯作者：
Ruan, HL
作者机构：
[Ruan, Han-Li; Hu, Jia-Yun; Qin, Chun-Lun; Chang, Jin-Ling; Pei, Jiao; Ouyang, Qian-Xi; Ruan, HL; Zhou, Yin-Hui] Huazhong Univ Sci & Technol, Tongji Med Coll, Sch Pharm, Hubei Key Lab Nat Med Chem & Resource Evaluat, Wuhan 430030, Peoples R China.;[Meng, Xiang-Gao] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Ruan, HL ] H;Huazhong Univ Sci & Technol, Tongji Med Coll, Sch Pharm, Hubei Key Lab Nat Med Chem & Resource Evaluat, Wuhan 430030, Peoples R China.
摘要：
Twelve new austalide meroterpenoids (1-12) were isolated from the endophytic fungus Diaporthe sp. XC1211. Their structures were elucidated by extensive spectroscopic analysis. The absolute configurations of compounds 1, 3, 4, and 6 were established by single-crystal X-ray diffraction, whereas those for the others were established by experimental electronic circular dichroism (ECD) data analysis. Compounds 1-12 represent a rare class of austalides with a 24α-CH(3). Compounds 2 and 5 demonstrated potent proliferation inhibitory effects against LPS-induced B cells with IC(50) values of 6.7 (SI = 3.6) and 3.8 (SI > 13) μM, respectively. Compounds 2 and 5 decreased the secretion of IL-6 in LPS-induced B cells in a dose-dependent manner.
摘要：
Two new Zn(II)/Cd(II) luminescent coordination polymers (CPs) based on the V-shaped bis(imidazole) ligand 3,6-bis (1H-benzo[d]imidazol-1-yl)-9-methyl-9H-carbazole (bbimc) with [1,1'-biphenyl]-4,4'-dicarboxylic acid ligand (H(2)bpdc) have been synthesized under solvothermal conditions: {[Zn(bbimc)(bpdc)]·DMF·2.5H(2)O} (CP 1), {[Cd(bbimc)(bpdc)]·2DMF} (CP 2). CP 1 and CP 2 both display a uninodal 4-c unimodal sql topology 2D framework with vertex symbols of {4(4)·6(2)}. In addition, the two identical 2D nets of CP 2 were interpenetrated each other to form a 2D+2D→3D and generate a 2-fold interpenetrating architecture. Moreover, sensing investigations of CP 1 and CP 2 revealed that both of compounds can be used as a highly sensitive and selective multi-responsive luminescent sensor for sensing Cr(2)O(7)(2-), CrO(4)(2-) and antibiotics (TC: Tetracycline; CTC: Chlortetracycline) in H(2)O by exhibiting fluorescence quenching with significant quenching constants (K(sv)=1.369×10(4) M(-1) (Cr(2)O(7)(2-)), 2.003×10(4) M(-1) (CrO(4)(2-)), 5.343×10(4) M(-1) (TC), 8.706×10(4) M(-1) (CTC) for CP 1 and 4.452×10(4) M(-1) (Cr(2)O(7)(2-)), 2.119×10(4) M(-1) (CrO(4)(2-)), 4.175×10(4) M(-1) (TC), 1.257×10(5) M(-1) (CTC) for CP 2). The detection limit are 0.67μM (Cr(2)O(7)(2-)), 0.48μM (Cr(2)O(7)(2-)), 0.23μM (TC), 0.14μM (CTC) for CP 1 and 0.28μM (Cr(2)O(7)(2-)), 0.54μM (CrO(4)(2-)), 0.31μM (TC), 0.098μM (CTC) for CP 2, respectively. In addition, the probable fluorescence quenching mechanism was studied through experiment and theoretical calculation and the co-existance of competitive absorption (CA) and photoinduced electron transfer (PET) progress contributed to such sensing processes.
关键词：
Cancer biomarkers;Liquid biopsy;Microfluidics;Digital assay;Single molecule detection
摘要：
The current paradigm of cancer management relies on imaging modalities and tissue biopsy to characterize the tumor landscape and devise treatment. As a complementary approach to non-invasive cancer detection, liquid biopsy is gaining interest through the detection of biomarkers circulating in body fluids. However, the wider use of liquid biopsy in the clinical setting is often hindered by limited technologies that can reliably and sensitively detect trace biomarkers in bodily fluids. As one of the most promising emerging technologies, digital single-molecule platforms (DSMPs) offer unparalleled sensitivity using digital read-out that is poised to improve current cancer management. This review provides an overview of the recent development in DSMPs based on digital ELISA, digital flow cytometry, digital surface-enhanced Raman scattering, and other emerging DSMPs for circulating cancer biomarker detection, especially for those that were evaluated on clinical cancer cohorts. DSMPs are well-positioned to address the challenges of studying cancer heterogeneity and trace biomarker discovery with outcomes expected to deliver new tools for cancer screening, treatment monitoring, and tumor recurrence detection.
摘要：
As a hotspot issue of global concern, the abuse of environmental and biological related molecules, including antibiotics, small organic molecules and inorganic anions poses a severe threat to the biological health and ecological environment. Accurate and effective monitoring of these species is of great significance. In this study, one novel nickel(II)-based coordination polymer [Ni(H(2)edda)(2)(Hbmoe)(2)] (Ni-CP) has been successfully designed and synthesized by using the mixed ligands 5,5 '-(ethane-1,2-diylbis(oxy)) diisophthalic acid (H(4)edda) and 1,1 '-bis(1H-benzimidazolyl) oxydiethane (bmoe). Significantly, this framework reveals great thermal and chemical stability and can retain its structural integrity when immersed in water or even in a certain acid/base aqueous solution (pH = 2-13) for a period of time. As expected, this material also exhibits strong fluorescence. Further investigations indicate that as-synthesized Ni-CP can be served as a multi-responsive sensing platform for the highly selective and sensitive detection of nitrofurazone (NFZ), acetylacetone (ACAC), MnO4- and Cr(VI) in aqueous media. The mechanisms for fluorescence quenching have been disclosed through thorough experimental and computational investigations.
作者机构：
[Duan, Gui-Yun; Li, Hong-Shuang; Zhao, Jun; Tian, Kai-Qiang] Shandong First Med Univ & Shandong Acad Med Sci, Natl Key Lab Adv Drug Delivery & Release Syst, Sch Pharmaceut Sci, Jinan 250117, Peoples R China.;[Duan, Gui-Yun; Li, Hong-Shuang; Zhao, Jun; Tian, Kai-Qiang] Shandong First Med Univ & Shandong Acad Med Sci, Inst Mat Med, Jinan 250117, Peoples R China.;[Zhang, Shi-Jiao] Qingdao Univ, Pharm Intravenous Admixture Serv, Affiliated Taian City Cent Hosp, Tai An 271000, Peoples R China.;[Cui, Guo-Hao; Guo, R; Wang, Qiao-Ling; Guo, Rui] Cent China Normal Univ CCNU, Int Joint Res Ctr Intelligent Biosensing Technol &, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol,Minist Educ,Coll Ch, Wuhan 430079, Peoples R China.
通讯机构：
[Guo, R ] C;[Li, HS ] S;Shandong First Med Univ & Shandong Acad Med Sci, Natl Key Lab Adv Drug Delivery & Release Syst, Sch Pharmaceut Sci, Jinan 250117, Peoples R China.;Shandong First Med Univ & Shandong Acad Med Sci, Inst Mat Med, Jinan 250117, Peoples R China.;Cent China Normal Univ CCNU, Int Joint Res Ctr Intelligent Biosensing Technol &, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol,Minist Educ,Coll Ch, Wuhan 430079, Peoples R China.
摘要：
The regio- and diastereoselective alkene isomerization and hydrofunctionalization sequence enabled by transition-metal complexes allows rapid activation and assembly of the C-(sp(3))-H bond that is either adjacent or distal to the initial double bond, which has been a longstanding challenge in this field. Herein, we develop unusual rhodium-catalyzed isomerization of alkylidenecyclobutanes with subsequent hydroacylation reaction to provide multisubstituted cyclobutanes with continuous stereocenters. Note that this tandem process features a good regio- and diastereoselectivity profile. Isotopic labeling experiments support the "exo to endo" migration of the double bond to a coordinated cyclobutene that is responsible for the deuterium incorporation observed in the cyclobutane product.
摘要：
Herein, a novel fluorescent coordination polymer [Cu2(edda)(bpy)2]Greek ano teleia6H2O (Cu-CP; H4edda = 5,5 '-(ethane-1,2-diylbis(oxy)) diisophthalic acid; bpy = 2,2 '-bipyridine) was designed and successfully architected using semi-rigid tetracarboxylic acid ligand H4edda combined with N,N '-donor linker bpy through a hydrothermal method. Single-crystal structural analysis reveals that the adjacent Cu1 centers are linked by 3 '- and 5-carboxyl groups of edda4-linker to form a one-dimensional Cu(II)-edda4-chain, which is further strutted by 3-and 5 '- carboxyl groups in edda4-ligand to generate a two-dimensional (2D) network with sql topology. Notably, bpy molecules do not actually dedicate to the formation of this 2D network, which merely saturate the configuration of Cu ions. Apart from the great thermal and acid/base stabilities, the pi-conjugated nature of H4edda endows Cu-CP with the traits of strong fluorescent emission in both solid state and aqueous solution. Interestingly, Cu-CP can act as a multifunctional platform for effectively detecting nitrofurazone (NFZ), nitrofurantoin (NFT), Cr2O72-, CrO42-and MnO4- via fluorescence quenching effects in an aqueous system. The fabricated Cu-CP fluorescent sensor shows distinguished sensitivity and anti-interference performance as well as low detection limits (3.55 nM for NFZ; 1.02 nM for NFT; 0.58 mu M for Cr2O72-, 0.68 mu M for CrO42-and 4.59 mu M for MnO4 -). The underlying quenching mechanisms have been studied through in-depth experimental and computational researches.
期刊：
JOURNAL OF ORGANIC CHEMISTRY,2024年89(4):2505-2515 ISSN：0022-3263
通讯作者：
Wu, AX
作者机构：
[Wang, Can; Zhao, Peng] Taizhou Univ, Sch Pharmaceut Sci, Inst Adv Studies, Taizhou 318000, Zhejiang, Peoples R China.;[Wu, An-Xin; Zhou, You; Zhao, Peng] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Wu, AX ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
A novel iodine-promoted difunctionalization of alpha-C sites in enaminones was demonstrated as a means of synthesizing a variety of fully substituted thiazoles by constructing C-C(CO), C-S, and C-N bonds. This transformation allows the realization of enaminones as unusual aryl C2 synthons and simultaneously allows the thioylation and dicarbonylation of alpha-C sites. A preliminary mechanistic study was performed and indicated that the cleavage of C=C bonds in enaminones involves a bicyclization/ring-opening and oxidative coupling sequence.
摘要：
A mild strategy for the synthesis of boron‐handled pyrazoles through photocatalytic cascade radical cyclization of LBRs (Lewis base‐boryl radicals) with vinyldiazo reagents is described here. The reaction starts with the addition of LBRs at diazo site, followed by intramolecular radical cyclization to access a wide range of important boron‐handled pyrazoles in good to excellent yields. Control experiments, together with detailed mechanism studies well explain the observed reactivity. Abstract Vinyldiazo compounds are one of the most important synthons in the construction of a cyclic ring. Most photochemical transformations of vinyldiazo compounds are mainly focusing on utilization of their C═C bond site, while reactions taking place at terminal nitrogen atom are largely unexplored. Herein, a photocatalytic cascade radical cyclization of LBRs with vinyldiazo reagents through sequential B─N/C─N bond formation is described. The reaction starts with the addition of LBRs (Lewis base–boryl radicals) at diazo site, followed by intramolecular radical cyclization to access a wide range of important boron‐handled pyrazoles in good to excellent yields. Control experiments, together with detailed mechanism studies well explain the observed reactivity. Further studies demonstrate the utility of this approach for applications in pharmaceutical and agrochemical research.
摘要：
The development of efficient, bright, and stable narrowband light-emitting electrochemical cells (LECs) has remained a challenge. Here, intrinsically ionic multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters are reported as guest emitters for narrowband LECs, which are developed by attaching an imidazolium cation onto a typical MR-TADF emitter. In solution, the emitters show green-blue emission peaked at 486-497 nm with small full widths at half-maximum (FWHMs) at 24-26 nm. In doped films, they show narrowband green-blue emission with high luminescent efficiencies at approximate to 90%. LECs using an ionic exciplex host and the ionic MR-TADF guest emitters show green-blue emission peaked at 494-503 nm with small FWHMs at 31-34 nm, and afford high external quantum efficiencies (EQEs) up to 10% under constant-voltage driving. With ionic TADF small-molecule hosts, the narrowband LECs show high EQEs up to 13.0% under constant-voltage driving, which is the highest among all reported narrowband LECs, and afford peak brightness/EQE/half lifetime at 780 cd m-2/5.6%/62.2 h under constant-current driving. A long half-lifetime of approximate to 630 h has further been achieved at 136 cd m-2. The work demonstrates the great potential for the use of intrinsically ionic MR-TADF guest emitters and ionic TADF hosts to develop efficient, bright, and stable narrowband LECs. Narrowband light-emitting electrochemical cells (LECs) are fabricated with ionic multi-resonance thermally- activated delayed fluorescence (TADF) guest emitters, which show high external quantum efficiencies (EQEs) up to 13.0% under constant-voltage driving and peak brightness/EQE/half-lifetime at 780 cd m-2/5.6%/62.2 h under constant-current driving. A half-lifetime of approximate to 630 h is further achieved at 136 cd m-2. image
摘要：
The role of AXL in various oncogenic processes has made it an attractive target for cancer therapy. Currently, kinase selectivity profiles, especially circumventing MET inhibition, remain a scientific issue of great interest in the discovery of selective type II AXL inhibitors. Starting from a dual MET/AXL-targeted lead structure from our previous work, we optimized a 1,6-naphthyridinone series using molecular modeling-assisted compound design to improve AXL potency and selectivity over MET, resulting in the potent and selective type II AXL-targeted compound 25c. This showed excellent AXL inhibitory activity (IC(50)=1.1nM) and 343-fold selectivity over the highly homologous kinase MET in biochemical assays. Moreover, compound 25c significantly inhibited AXL-driven cell proliferation, dose-dependently suppressed 4T1 cell migration and invasion, and induced apoptosis. Compound 25c also showed noticeable antitumor efficacy in a BaF3/TEL-AXL xenograft model at well-tolerated doses. Overall, this study presented a potent and selective type II AXL-targeted lead compound for further drug discovery.
