作者机构：
[Xu Zhang; Xing Peng] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, PR China;[Zixin Yao; Yan Gao; Wenjuan Shen] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China;[Shuang Yan] School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, PR China
通讯机构：
[Xing Peng] K;[Wenjuan Shen] S;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, PR China<&wdkj&>School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China
摘要：
The inhibition of electron transfer by the iron oxide passivation layer and the competition of oxygen for electrons limited the efficiency of heavy metal removal by zero-valent iron reduction. Herein we synthesized micron zero-valent iron modified with boric acid by mechanical ball milling, and demonstrated its enhanced copper ions removal performance. Compared to pristine ZVI, B-ZVI is approximately 2.6 times more efficient in the removal of copper. Interestingly, copper removal was significantly inhibited under air atmosphere for pristine ZVI. However, for B-ZVI, copper removal efficiency was almost insignificantly different between air and argon atmosphere conditions. Furthermore, the modification of ZVI with boric acid promoted the Cu(II) reduction proportion. Boronated modification effectively inhibited oxygen competition for electrons in removing heavy metals by zero-valent iron, which was conducive to the improvement of the heavy metal removal efficiency and the electron utilization of zero-valent iron. This study elucidated the importance of surface modification on the reactivity of micron-sized zero-valent iron and provided an efficient heavy metal removal strategy with zero-valent iron for environmental remediation.
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.
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.
摘要：
Ten previously unreported [11]-chaetoglobosins, chaepseubakerins A-J (1-10), were characterized from the solid rice-based culture of Pseudeurotium bakeri P1-1-1, an endophyte harbored in the roots of Macrocoma tenue subsp. sullivantii Vitt. (Orthotrichaceae). Their structures were determined by spectroscopic analysis, single -crystal X-ray diffraction (Cu K alpha radiation), and chemical methods. Chaepseubakerin A (1) exhibited signifi-cant cytotoxic effects against seven human cancer cell lines, A549, A427, HCT116, HT-29, HeLa, HepG2, and MCF-7, with IC50 values of 2.9, 3.0, 4.0, 4.4, 7.1, 6.7, and 8.9 mu M, respectively. Mechanistically, 1 induced G2/M cell cycle arrest and apoptosis in A549, Hela, and HCT116 cells in a dose dependent manner.
摘要：
We developed a facile bottom‐up strategy to synthesize Ni(II)‐incorporated covalent organic framework (LZU‐713@Ni) as heterogeneous all‐in‐one metallaphotoredox catalyst. LZU‐713@Ni showed excellent activity and recyclability in photoredox/nickel‐catalyzed C−O, C−S, and C−P cross‐coupling reactions. The superiority of bottom‐up strategy was exemplified by the increased activity of LZU‐713@Ni compared to both the dual catalyst system and LZU‐713/Ni prepared via post‐synthetic modification. Abstract The construction of an all‐in‐one catalyst, in which the photosensitizer and the transition metal site are close to each other, is important for improving the efficiency of metallaphotoredox catalysis. However, the development of convenient synthetic strategies for the precise construction of an all‐in‐one catalyst remains a challenging task due to the requirement of precise installation of the catalytic sites. Herein, we have successfully established a facile bottom‐up strategy for the direct synthesis of Ni(II)‐incorporated covalent organic framework (COF), named LZU‐713@Ni, as a versatile all‐in‐one metallaphotoredox catalyst. LZU‐713@Ni showed excellent activity and recyclability in the photoredox/nickel‐catalyzed C−O, C−S, and C−P cross‐coupling reactions. Notably, this catalyst displayed a better catalytic activity than its homogeneous analogues, physically mixed dual catalyst system, and, especially, LZU‐713/Ni which was prepared through post‐synthetic modification. The improved catalytic efficiency of LZU‐713@Ni should be attributed to the implementation of bottom‐up strategy, which incorporated the fixed, ordered, and abundant catalytic sites into its framework. This work sheds new light on the exploration of concise and effective strategies for the construction of multifunctional COF‐based photocatalysts.
作者机构：
[Suwei Dong] State Key Laboratory of Natural and Biomimetic Drugs, and School of Pharmaceutical Sciences, Peking University, Beijing, China;[Ji-Shen Zheng; Shan Tang] Division of Life Sciences and Medicine, University of Science and Technology of China, Hefei, China;[Yiming Li] School of Food and Biological Engineering, Engineering Research Center of Bio-process, Ministry of Education, Hefei University of Technology, Hefei, China;[Huan Wang] School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China;[Gong Chen] State Key Laboratory of Elemento-Organic Chemistry, Nankai University, Tianjin, China
通讯机构：
[Lei Liu] D;Department of Chemistry, Tsinghua University, Beijing, China
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.
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.
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：
[Lin, Fengcai; Li, Xiaoqing; Zhu, Jide; Zheng, Xiaoxiao; Xu, Yanlian; Chen, Jipeng] Fujian Engineering and Research Center of New Chinese Lacquer Materials, College of Materials and Chemical Engineering, Minjiang University, Fuzhou, Fujian 350108, P. R. China;[Shen, Lijuan; Zhu, Jide; Zheng, Xiaoxiao; Chen, Xiaoping; Jiang, Lilong] National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, P. R. China;[Chen, Xiaoping] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan, Hubei 430079, P. R. China;[Shen, Lijuan] College of Environmental and Resource Sciences, College of Carbon Neutral Modern Industry, Fujian Key Laboratory of Pollution Control & Resource Reuse, Fujian Normal University, Fuzhou, Fujian 350007, P. R. China
摘要：
The development of stable and effective catalysts to convert toxic H(2)S into high value-added sulfur is essential for production safety and environmental protection. However, the inherent defects of traditional iron- and zirconium-based catalysts, such as poor activity, high oxygen consumption, and low sulfur selectivity, limit their further developments and applications. Herein, the Fe-Zr bimetallic organic framework FeUIO-66(x) with different cubic morphologies was synthesized via a facile solvothermal method. The results indicate that the introduction of Fe not only increases the specific surface area and weak L-sites of the catalyst without changing its crystal structure, which provides enough reaction space and more active sites for the adsorption and activation of H(2)S, but also reduces the activation energy of the reaction, significantly promoting the selective oxidation of H(2)S. As a result, the as-obtained FeUIO-66(1) catalyst exhibits the highest desulfurization activity and superior durability and water resistance stability, and its H(2)S conversion and sulfur selectivity within 50 h are 100 and 88%, respectively. More importantly, the structure of the catalyst after the desulfurization reaction is consistent with that of the fresh counterpart. The study offers new insights into the development of effective and stable bimetallic catalysts to eliminate H(2)S and recycle sulfur.
摘要：
A pair of new chiral molecules, (S)-4 and (R)-4, has been designed and synthesized by introducing two valine-containing groups at symmetrical positions on the periphery of an indolo[3,2-b]carbazole unit. They show aggregation-induced circular dichroism (AICD) properties in DMF/water mixtures, and a mixture with 99 % water fraction exhibits strong, mirror-image, blue circularly polarized luminescence (CPL) signals with glum of +1.1 × 10−2 and −1.0 × 10−2, respectively. The results demonstrate that we have devised a simple self-assembly strategy to achieve desirable chirality.
作者机构：
[Zhang, Xiangqian; Chen, Yu; Deng, GZ; Feng, Huili; Deng, Ganzhen; Zhou, Qingqing] Huazhong Agr Univ, Coll Vet Med, State Key Lab Agr Microbiol, Wuhan 430070, Peoples R China.;[Liu, Shuang] Wuhan Univ Technol, Sch Mat Sci & Engn, 122 Luoshi Rd, Wuhan 430070, Peoples R China.;[Li, JR; Li, Junrong; Li, Chonglu] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticides, Wuhan 430079, Peoples R China.;[Guan, Xiaofang] Wuhan Univ Sci & Technol, Hubei Prov Key Lab Occupat Hazard Identificat & C, Wuhan 430081, Peoples R China.;[Deng, Yun; Fu, Cheng] Jianghan Univ, Key Lab Optoelect Chem Mat & Devices, Minist Educ, Wuhan 430056, Peoples R China.
通讯机构：
[Liu, S ] W;[Li, JR ] C;[Deng, GZ ] H;Huazhong Agr Univ, Coll Vet Med, State Key Lab Agr Microbiol, Wuhan 430070, Peoples R China.;Wuhan Univ Technol, Sch Mat Sci & Engn, 122 Luoshi Rd, Wuhan 430070, Peoples R China.
摘要：
High efficiency, stability, long emission wavelength (NIR-II), and good biocompatibility are crucial for photosensitizers in phototherapy. However, current Food and Drug Administration (FDA)-approved organic fluorophores exhibit poor chemical stability and photostability as well as short emission wavelength, limiting their clinical usage. To address this, we developed Se-IR1100, a novel organic photosensitizer with a photostable and thermostable benzobisthiadiazole (BBTD) backbone. By incorporating selenium as a heavy atom and constructing a D-A-D structure, Se-IR1100 exhibits a maximum fluorescence emission wavelength of 1100 nm. Compared with FDA-approved indocyanine green (ICG), DSPE-PEGylated Se-IR1100 nanoparticles exhibit prominent photostability and long-lasting photothermal effects. Upon 808 nm laser irradiation, Se-IR1100 NPs efficiently convert light energy into heat and reactive oxygen species (ROS), inducing cancer cell death in cellular studies and living organisms while maintaining biocompatibility. With salient photostability and a photothermal conversion rate of 55.37%, Se-IR1100 NPs hold promise as a superior photosensitizer for diagnostic and therapeutic agents in oncology. Overall, we have designed and optimized a multifunctional photosensitizer Se-IR1100 with good biocompatibility that performs NIR-II fluorescence imaging and phototherapy. This dual-strategy method may offer novel approaches for the development of multifunctional probes using dual-strategy or even multi-strategy methods in bioimaging, disease diagnosis, and therapy. High efficiency, stability, long emission wavelength (NIR-II), and good biocompatibility are crucial for photosensitizers in phototherapy.
作者机构：
[Yonghui Xu; Yufei Liu; Wei Zhan; Dingle Zhang; Yiyun Liu; Yi Xu; Zhengshun Wu] Chemistry College, Central China of Normal University, Wuhan, 430079, China
通讯机构：
[Zhengshun Wu] C;Chemistry College, Central China of Normal University, Wuhan, 430079, China
摘要：
This study explores the transformation of peanut shells, an abundant agricultural waste, into high-efficiency activated carbon for CO2 capture using a two-step pyrolysis and K2CO3 activation method. Observations indicated that with an increasing impregnation ratio, the activated carbon demonstrates remarkable improvements in structural properties, achieving specific surface areas and pore volumes of 1150.02 m2/g and 0.46 cm3/g, respectively. Among the prepared samples, the activated carbon obtained with a peanut shell to K2CO3 impregnation mass ratio of 1:2 exhibits superior CO2 adsorption capacity at 1 bar, with values of 3.76 mmol/g at 25 °C and 5.70 mmol/g at 0 °C. The CO2 adsorption isotherms of the activated carbon conform to the Langmuir and Freundlich models. These results demonstrate the potential of this method in addressing environmental concerns, particularly in mitigating CO2 emissions, and highlight the broader application prospects of biomass-derived activated carbon in environmental management.
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.
作者机构：
[Shu, C; Deng, Zhengxi; Xuan, Chenglong; Zhu, Zhiming; Shu, Chao] Cent China Normal Univ CCNU, Coll Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control &, CCNU uOttawa Joint Res Ctr,Natl Key Lab Green Pest, Wuhan 430070, Hubei, Peoples R China.;[Shu, C; Deng, Zhengxi; Xuan, Chenglong; Zhu, Zhiming; Shu, Chao] Anhui Normal Univ, Key Lab Funct Mol Solids, Minist Educ, Wuhu 241000, Anhui, Peoples R China.
通讯机构：
[Shu, C ] C;Cent China Normal Univ CCNU, Coll Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control &, CCNU uOttawa Joint Res Ctr,Natl Key Lab Green Pest, Wuhan 430070, Hubei, Peoples R China.;Anhui Normal Univ, Key Lab Funct Mol Solids, Minist Educ, Wuhu 241000, Anhui, Peoples R China.
摘要：
A thermoinduced radical homolytic substitution cyclization of alkenyl tethered sulfinate esters was displayed under mild metal-free conditions, enabling the functionalization of alkenes and leading to structurally diverse value-added sultine products. The process utilizes readily available substrates using inexpensive 5% benzoyl peroxide (BPO) as an initiator to generate functionalized sultines with broad functional group tolerance in medium to excellent yields in a highly atom-economical manner. In addition, the obtained sultines could be further readily functionalized toward valuable sultone frameworks in one pot. A thermo-catalytic radical chain process was proposed based on mechanistic studies.
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.
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.
摘要：
In this study, PGM free metal oxide based nanorod array (nanoarray) forests have been conformally integrated onto the millimeter-sized channel walls and microscale pores of SiC diesel particulate filter (DPF) substrates using scalable microwave-assisted hydrothermal and dip-coating methods. High-efficiency and robust low temperature soot oxidation is successfully achieved using such a new type of cDPFs as a result of i) promoted tight soot-catalyst contact through spontaneous soot deposits in-between nanorods, ii) highly dispersed loading of LaSrCoO3 perovskite oxidation catalysts onto ZnO nanorod arrays, effectively mitigating active site blockage by soot deposition. The light-off temperature of soot oxidation was lowered to 250 degrees C in oxygen, a 250 degrees C decrease compared to that of the commercial Pt based catalyst, due to the abundant oxygen vacancies enabled by the LaSrCoO3/ZnO (LSCO/ZnO) nanorod array catalysts. The performance of the catalyst was further enhanced to initiate the soot oxidation at similar to 150 degrees C with co-fed gas of NO, due to the LSCO catalyzed NO2 formation and its favorable oxidation with soot at low temperature. Furthermore, the nanoarray supported perovskite catalyst shows excellent stability and activity after 120 h of hydrothermal aging at 650 degrees C. Soot oxidation Tmax is lowered from 542 degrees C to 510 degrees C under 6 % water steam condition due to the formation and promotion effect of oxidative-OH species. In situ DRIFTS study reveals that such-OH species form at various catalyst surfaces and interfaces, pointing to a potentially generic water promotion effect for solid/solid interfacial catalytic oxidation under humidity condition. Finally, the mechanistic soot oxidation pathways under O-2, NO2, and H2O feeds are pro-posed for understanding the low-temperature soot oxidation behaviors over the nanoarray supported perovskite catalysts.
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024年 ISSN：0002-7863
作者机构：
[Tu, Le; Li, Meiqin; Li, Junrong; Sun, Yao; Li, Chonglu] National Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensor Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, China;[Li, Chonglu] State Key Laboratory of Chemo/Biosensing and Chemometrics, Hunan University, Changsha 410082, China;[Kim, Jong Seung; Ding, Qihang] Department of Chemistry, Korea University, Seoul 02841, Korea;[Sharma, Amit] Amity School of Chemical Sciences, Amity University Punjab, Sector 82A, Mohali, Punjab 140306, India
摘要：
Though immunogenic cell death (ICD) has garnered significant attention in the realm of anticancer therapies, effectively stimulating strong immune responses with minimal side effects in deep-seated tumors remains challenging. Herein, we introduce a novel self-assembled near-infrared-light-activated ruthenium(II) metallacycle, Ru1105 (λ(em) = 1105 nm), as a first example of a Ru(II) supramolecular ICD inducer. Ru1105 synergistically potentiates immunomodulatory responses and reduces adverse effects in deep-seated tumors through multiple regulated approaches, including NIR-light excitation, increased reactive oxygen species (ROS) generation, selective targeting of tumor cells, precision organelle localization, and improved tumor penetration/retention capabilities. Specifically, Ru1105 demonstrates excellent depth-activated ROS production (∼1 cm), strong resistance to diffusion, and anti-ROS quenching. Moreover, Ru1105 exhibits promising results in cellular uptake and ROS generation in cancer cells and multicellular tumor spheroids. Importantly, Ru1105 induces more efficient ICD in an ultralow dose (10 μM) compared to the conventional anticancer agent, oxaliplatin (300 μM). In vivo experiments further confirm Ru1105's potency as an ICD inducer, eliciting CD8(+) T cell responses and depleting Foxp3(+) T cells with minimal adverse effects. Our research lays the foundation for the design of secure and exceptionally potent metal-based ICD agents in immunotherapy.
