期刊：
Journal of Carbohydrate Chemistry,2024年 ISSN：0732-8303
通讯作者：
Guo, J
作者机构：
[Zhang, Ru-Yan; Liu, Yan-Ling; Ding, Dong; Guo, J; Wen, Yu; Guo, Jun; Zhou, Shi-Hao; Zou, Yong-Ke] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Guo, J ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
关键词：
Cancer vaccine;c-GAMP;MUC1;MUC1 glycopeptide;poly(I:C);ternary adjuvant system
摘要：
The highly glycosylated mucin 1 (MUC1) serves as a promising target for cancer vaccines. However, the weak immunogenicity of MUC1 greatly impedes its application. Here, we covalently linked a MUC1 glycopeptide to carrier protein bovine serum albumin (BSA), and the resulting BSA-MUC1 conjugate was integrated with a ternary adjuvant system comprising TLR3 agonist poly(I:C), STING agonist c-GAMP, and Alum adjuvant. Compared to adjuvant-free and Alum-adjuvanted groups, the ternary adjuvant group induced 18.3- and 10.9-fold increases in MUC1-specific IgG titers, and effectively suppressed tumor growth. These findings may propose a straightforward yet highly effective strategy for designing vaccines, offering promising prospects in cancer treatment.
摘要：
Engineering isolated metal sites resembling the primary coordination sphere of metallocofactors enables atomically dispersed materials as promising nanozymes. However, most existing nanozymes primarily focus on replicating specific metallocofactors while neglecting other supporting cofactors within active pockets, leading to reduced electron transfer (ET) efficiency and thus inferior catalytic performances. Herein, we report a metal–organic framework UiO-67 nanozyme with atomically dispersed iron sites, which involves multiple tailored enzyme-like nanocofactors that synergistically drive the ET process for enhanced peroxidase-like catalysis. Among them, the linker-coupled atomic iron site plays a critical role in substrate activation, while bare linkers and zirconia nodes facilitate the ET efficiency of intermediates. The synergy of three nanocofactors results in a 4.29-fold enhancement compared with the single effort of isolated metal site-based nanocofactor, holding promise in immunoassay for sensitive detection of chlorpyrifos. This finding opens a new way for designing high-performance nanozymes by harmonizing various nanocofactors at the atomic and molecular scale.
摘要：
Cancer cells need a greater supply of glucose mainly due to their aerobic glycolysis, known as the Warburg effect. Glucose transport by glucose transporter 1 (GLUT1) is the rate-limiting step for glucose uptake, making it a potential cancer therapeutic target. However, GLUT1 is widely expressed and performs crucial functions in a variety of cells, and its indiscriminate inhibition will cause serious side effects. In this study, we designed and synthesized a photocaged GLUT1 inhibitor WZB117-PPG to suppress the growth of cancer cells in a spatiotemporally controllable manner. WZB117-PPG exhibited remarkable photolysis efficiency and substantial cytotoxicity toward cancer cells under visible light illumination with minimal side effects, ensuring its safety as a potential cancer therapy. Furthermore, our quantitative proteomics data delineated a comprehensive portrait of responses in cancer cells under glucose deprivation, underlining the mechanism of cell death via necrosis rather than apoptosis. We reason that our study provides a potentially reliable cancer treatment strategy and can be used as a spatiotemporally controllable trigger for studying nutrient deprivation-related stress responses.
作者机构：
[Li, Guang; Xu, Weiwei; Hameed, Muhammad Salman; Yang, Qinglin; Li, Haibing; Qu, Haonan] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Quan, Jiaxin; Quan, JX] Hanjiang Normal Univ, Dept Chem Biol & Environm Engn, Shiyan 442000, Peoples R China.;[Zhang, J; Zhang, Jin] Yunnan Normal Univ, Coll Chem & Chem Engn, Kunming 650092, Peoples R China.;[Sun, Zhongyue] Hubei Univ Chinese Med, Sch Lab Med, Wuhan 430065, Peoples R China.
通讯机构：
[Quan, JX ; Sun, ZY ] H;[Li, HB ] C;[Zhang, J ] Y;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Hanjiang Normal Univ, Dept Chem Biol & Environm Engn, Shiyan 442000, Peoples R China.
关键词：
arginine;biomimetic;mimic Cyt C transport;nanochannel;pH
摘要：
Proteins are vital components in cells, biological tissues, and organs, playing a pivotal role in growth and developmental processes in living organisms. Cytochrome C (Cyt C) is a class of heme proteins found in almost all life and is involved in cellular energy metabolic processes such as respiration, mainly as electron carriers or terminal reductases. It binds cardiolipin in the inner mitochondrial membrane, leading to apoptosis. It is a challenge to design a simple and effective artificial system to mimic the complex Cyt C biological transport process. In this paper, an asymmetric biomimetic pH-driven protein gate is described by introducing arginine (Arg) at one end of an hourglass-shaped nanochannel. The nanochannel shows a sensitive protonation-driven protein gate that can be "off" at pH = 7 and "on" at pH = 2. Further studies show that differences in the binding of Arg and Cyt C at different levels of protonation lead to different switching behaviors within the nanochannels, which in turn lead to different surface charges within the nanochannels. It can be used for detecting Cyt C and as an excellent and robust gate for developing integrated circuits and nanoelectronic logic devices.
摘要：
Fosmidomycin (FOS) is a natural product inhibiting the DXR enzyme in the MEP pathway and has stimulated interest for finding more suitable FOS analogues. Herein, two series of FOS analogue hydroxamate-containing bisphosphonates as proherbicides were designed, with bisphosphonate replacing the phosphonic unit in FOS while retaining the hydroxamate (BPF series) or replacing it with retro-hydroxamate (BPRF series). The BPF series were synthesized through a three-step reaction sequence including Michael addition of vinylidenebisphosphonate, N-acylation, and deprotection, and the BPRF series were synthesized with a retro-Claisen condensation incorporated into the reaction sequence. Evaluation on model plants demonstrated several compounds having considerable herbicidal activities, and in particular, compound 8m exhibited multifold activity enhancement as compared to the control FOS. The proherbicide properties were comparatively validated. Furthermore, DXR enzyme assay, dimethylallyl pyrophosphate rescue, and molecular docking verified 8m to be a promising proherbicide candidate targeting the DXR enzyme. In addition, 8m also displayed good antimalarial activities.
作者机构：
[Kong, Sheng; Yi, Beibei; Guo, R; Ma, Yujiao; Guo, Rui; Zhang, Guozhu; Du, Qianqian; Zhang, He; Zhang, GZ; Zheng, Jialian] 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, Hubei, Peoples R China.
通讯机构：
[Guo, R ; Zhang, GZ] C;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, Hubei, Peoples R China.
关键词：
Amines;Silylation;Copper catalysis;Hydrogen atom transfer;C−H activation
摘要：
The development of a general and selective method for alpha-C-(sp(3))-H silylation of feedstock amines has been a long-standing challenge. In this paper, we disclose a mild, general, practical, and highly regio- and diastereoselective alpha-C-(sp(3))-H silylation of various readily available acyclic, cyclic, and aromatic amines with silylboranes through a copper-catalyzed intramolecular 1,5-hydrogen atom transfer (HAT) strategy. The mild activation of 2-iodobenzamide to generate an aryl radical enabled by a ligand-coordinated silyl copper complex without additional heating or photoinduced conditions, as well as the intramolecular selective 1,5-HAT process to produce the crucial alpha-aminoalkyl radical species, is the key to the success of this chemistry. This silylation protocol has demonstrated its potential utility in the late-stage modification of structurally complex drugs and bioactive molecules. Therefore, it is expected that this method will find applications in synthetic chemistry and drug discovery.
摘要：
An electrochemcial synthesis of indoline‐fused polycycles by constructing both the five‐ and six‐membered heterocyclic rings in a single step from arylamide‐tethered ynones has been developed, which provides facile access to various indoline‐based tetracyclic 6/5/6/6 skeletons with highly regioselective control in a sustainable, metal‐ and oxidant‐free condition. Abstract Indoline‐fused polycyclic scaffolds are virtually universal in biological and pharmaceutical. Here we demonstrate a facile electrooxidative cascade cyclization for indoline‐based derivatives, employing amidyl radicals with ynones under mild conditions. The efficient method enables the formation of two new C−N and C−C bonds in a single step with high regioselectivity. Various indoline‐based tetracyclic 6/5/6/6 skeletons can be achieved through a biscyclization/dehydrogenation cascade process. Additionally, this electrochemical strategy proceeds in a sustainable metal‐ and oxidant‐free condition, with H2 being the solely byproduct.
摘要：
Regioselective 1,2-dichalcogenation of alkenes has attracted significant attention in modern organic synthetic chemistry. While there are a plethora of methods to access alkene dichalcogenated architectures, sulfonylsulfination of alkenes is extremely challenging due to the inherent characteristics of the sulfur atom. Herein, a multicomponent fragment coupling of alkenes, sulfinates, and DABSO was developed to construct densely functionalized sulfonylsulfinated products, which are otherwise challenging to access, with broad substrate scope and group tolerance under mild and operationally simple conditions, using an inexpensive 100-1000 ppm organic photocatalyst. In addition, the protocol was applied to the late-stage functionalization of complex molecules, and the obtained products were converted into diverse downstream transformations to demonstrate their synthetic potential. Experimental and theoretical mechanistic investigations suggest that these reactions proceed through sequential sulfonyl and sulfinyl oxygen radical mutual transformations and radical-polar crossover coupling. This strategy provides access to previously inaccessible alkene sulfonylsulfinated products in good-to-high regio- and stereoselectivity, along with opening up previously unexplored synthetic directions.
关键词：
Photocatalysis;H2O2;g-C3N4;Excitons dissociation;Reactive oxygen species
摘要：
Solar-driven hydrogen peroxide (H2O2) production offers a sustainable strategy to address the ever-growing demand of eco-friendly oxidant and clean fuel, while its efficiency highly relies on the generation of desired reactive oxygen species (ROSs). Herein, we demonstrate that introducing boron-nitrogen vacancy (B-N-V) associates in g-C3N4 enables to weaken the robust excitonic effect and promote bound excitons spontaneously dissociating into free charge carriers under ambient conditions. Specifically, the doped B atoms introduced a donor state below the conduction band of g-C3N4, which disturbs charge distribution around heptazine rings and further destabilizes excitons. The concomitant N-V, serving as an accepter state locating above the valence band, cooperates with the doped B atoms to form B-N-V associates that simultaneously downshifts the conduction band and valence band of g-C3N4. Distinct from the counterpart preferring to activate O-2 into O-1(2) via an energy-transfer-involved pathway, g-C3N4 featuring with B-N-V associates displayed a superior photoactivity of visible-light-driven two-electron oxygen reduction reaction for H2O2 production with a yield of 182 mu mol h(-1) and selectivity of 100%. The produced H2O2 could effectively degrade organic contaminants and kill typical bacteria. This study highlights the importance of ROSs generation in two-dimensional photocatalysts for sustainable solar-to-chemical conversion and on site environmential governance.
作者机构：
[Liu, Ying; Yang, Shu; Hou, Shenghuai; Bai, Yuxuan; Qiao, Zhaoyu; Zhen, Shuang] Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079, China;[Xu, Hui] Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079, China. Electronic address: huixu@ccnu.edu.cn
通讯机构：
[Xu, Hui] K;Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079, China. Electronic address:
关键词：
Fipronil and its metabolites;Soil;Spherical fluorinated covalent organic polymers;μ-Matrix cartridge extraction-online-μ-solid phase extraction
摘要：
Covalent organic polymers (COPs) have garnered considerable attention as promising adsorbents of online solid phase extraction (online SPE). Morphology modulation provides an appealing solution to enhance adsorption efficiency and reduce back-pressure in the absorbent. However, the synthesis of COPs with regular geometric shapes and specific adsorption selectivity remains challenging. In this study, a uniform spherical fluorinated COP (F-sCOP, average diameter: 2.14μm) was successfully synthesized by Schiff base reaction of 1,3,5-triformylphoroglucinol (TP) and 2,2(')-bis(trifluoromethyl)benzidine (TFMB). The F-sCOP had a large surface area (BET: 346.2m(2)g(-1)), remarkable enrichment capacity (enrichment factors: 186-782), high selectivity toward fipronil and its metabolites (adsorption efficiency >93.1%), and admirable service life (>60 times). Based on the adsorbent, a novel μ-matrix cartridge extraction-online-μ-solid phase extraction-high performance liquid chromatography-mass spectrometry (μ-MCE-online-μ-SPE-HPLC-MS) method was constructed and used to track trace fipronil and its metabolites in soil. The proposed method exhibited a wide linear range (0.05-1000ngg(-1)), low quantitation limits (LOQs: 0.0027-0.011ngg(-1)), high recoveries (90.1-119.6%) and good repeatability (RSD ≤10.5%, n=3) for fipronil analysis. This study paves the way for pesticide analysis in soil risk assessment.
作者机构：
[Ling, Cancan; Zhang, Lizhi; Zhan, Guangming] School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China;[Ling, Cancan; Zhan, Guangming] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, China;[Liang, Chuan; Liu, Xiufan; Sun, Hongwei; Zhao, Jincai; Zhou, Bing; Li, Yaling; Li, Meiqi] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, China;[Li, Hao] School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China. Electronic address: hao_li@sjtu.edu.cn;[Zhang, Lizhi] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, China. Electronic address: zhanglizhi@sjtu.edu.cn
通讯机构：
[Hao Li; Lizhi Zhang] S;School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
期刊：
Journal of Colloid and Interface Science,2024年653(Pt A):540-550 ISSN：0021-9797
通讯作者：
Yang, Guohai;Qu, Lu-Lu
作者机构：
[Luo, Siyu; Chen, Yu; Guo, Yuxin; Rong, Chengyu; Gu, Yingqiu] School of Chemistry & Materials Science, Jiangsu Normal University, Xuzhou 221116, PR China;[Gao, Wenhui] School of Life Science, Jiangsu Normal University, Xuzhou, 221116, PR China;[Yang, Guohai] School of Chemistry & Materials Science, Jiangsu Normal University, Xuzhou 221116, PR China. Electronic address: yangguohai@jsnu.edu.cn;[Xu, Weiqing; Zhu, Chengzhou] National Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan, Hubei 430079, PR China;[Qu, Lu-Lu] School of Chemistry & Materials Science, Jiangsu Normal University, Xuzhou 221116, PR China. Electronic address: luluqu@jsnu.edu.cn
通讯机构：
[Qu, Lu-Lu; Yang, Guohai] S;School of Chemistry & Materials Science, Jiangsu Normal University, Xuzhou 221116, PR China. Electronic address:
摘要：
Reactive oxygen species (ROS) are ideal alternative antibacterial reagents for rapid and effective sterilization. Although a variety of ROS-based antimicrobial strategies have been developed, many are still limited by their inefficiency. Herein, we report the synthesis of the Ag-MXene nanozyme, which have superior peroxidase-like activity for antibacterial applications. As a result, Ag-MXene nanozyme can efficiently increase the level of intracellular ROS, converting H(2)O(2) into hydroxyl radicals that effectively kill both Gram-negative and Gram-positive bacteria and disrupting the bacterial biofilm formation. Moreover, a sensitive and selective colorimetric biosensor was constructed for assaying cholesterol based on the Ag-MXene's prominent peroxidase-mimicking activity and the cholesterol oxidase cascade reaction. The biosensor exhibits high performance with a linear cholesterol detection range of 2-800μM, and a detection limit of 0.6μM. Ag-MXene nanozyme can be used for the rapid detection of cholesterol in serum without complicated sample pretreatment. Collectively, it is conceivable that the proposed Ag-MXene nanozyme could be used as a biocide and as a cholesterol sensor. This study provides a broad prospect for the rapid detection and sterilization of MXene nanozymes in the biomedical field.
摘要：
Organic molecules bearing chiral sulfur stereocenters exert a great impact on asymmetric catalysis and synthesis, chiral drugs, and chiral materials. Compared with acyclic ones, the catalytic asymmetric synthesis of thio-heterocycles has largely lagged behind due to the lack of efficient synthetic strategies. Here we establish the first modular platform to access chiral thio-oxazolidinones via Pd-catalyzed asymmetric [3+2] annulations of vinylethylene carbonates with sulfinylanilines. This protocol is featured by readily available starting materials, and high enantio- and diastereoselectivity. In particular, an unusual effect of a non-chiral supporting ligand on the diastereoselectivity was observed. Possible reaction mechanisms and stereocontrol models were proposed.
期刊：
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY,2024年72(13):7021-7032 ISSN：0021-8561
通讯作者：
Feng, LL
作者机构：
[Zuo, Lingzi; Fan, Yuxuan; Feng, LL; Feng, Lingling; He, Yanlin; Cheng, Cai; Zhang, Liexiong; Guo, Xiaoliang; Cheng, Guonian; Yu, Jie; Tang, Guangmei; Huang, Shi; Chen, Ruiqing] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;[Liu, Yanyang; Feng, LL; Feng, Lingling] Wuhan Inst Photochem & Technol, Wuhan 430083, Hubei, Peoples R China.;[Feng, LL; Feng, Lingling] Cent China Normal Univ, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Feng, LL ] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;Wuhan Inst Photochem & Technol, Wuhan 430083, Hubei, Peoples R China.;Cent China Normal Univ, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
关键词：
Active substructure splicing;DFT;Harmful cyanobacteria blooms;SAR;algicide;thioacetamide derivatives
摘要：
Lakes and reservoirs worldwide are experiencing a growing problem with harmful cyanobacterial blooms (HCBs), which have significant implications for ecosystem health and water quality. Algaecide is an effective way to control HCBs effectively. In this study, we applied an active substructure splicing strategy for rapid discovery of algicides. Through this strategy, we first optimized the structure of the lead compound S5, designed and synthesized three series of thioacetamide derivatives (series A, B, C), and then evaluated their algicidal activities. Finally, compound A3 with excellent performance was found, which accelerated the process of discovering and developing new algicides. The biological activity assay data showed that A3 had a significant inhibitory effect on M. aeruginosa. FACHB905 (EC(50) = 0.46 μM) and Synechocystis sp. PCC6803 (EC(50) = 0.95 μM), which was better than the commercial algicide prometryn (M. aeruginosa. FACHB905, EC(50) = 6.52 μM; Synechocystis sp. PCC6803, EC(50) = 4.64 μM) as well as better than lead compound S5 (M. aeruginosa. FACHB905, EC(50) = 8.80 μM; Synechocystis sp. PCC6803, EC(50) = 7.70 μM). The relationship between the surface electrostatic potential, chemical reactivity, and global electrophilicity of the compounds and their activities was discussed by density functional theory (DFT). Physiological and biochemical studies have shown that A3 might affect the photosynthesis pathway and antioxidant system in cyanobacteria, resulting in the morphological changes of cyanobacterial cells. Our work demonstrated that A3 might be a promising candidate for the development of novel algicides and provided a new active skeleton for the development of subsequent chemical algicides.
作者机构：
[Feng, Guoqiang; Gong, Shengyi; Gui, Zhisheng] Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan 430079, China
摘要：
Dual-state emissive (DSE) materials exhibit fluorescence in both solid and solution states and have become an emerging material in the fields of materials science and sensing in recent years. However, due to the lack of effective and universal preparation methods, DSE materials, especially those with long emission wavelengths, are still scarce. Developing an effective method for constructing such DSE molecules is urgently needed. In this study, we constructed three DSE molecules (NRP-Boc, DCIP-Boc, and DCMP-Boc) with far-red to near-infrared fluorescence by simply modifying three traditional aggregation-caused quenching (ACQ) fluorophores with tert-butyloxycarbonyl (Boc) groups. Density functional theory (DFT) calculations and crystal data revealed the reasons for the bright fluorescence of these three molecules in solution and solid, demonstrating that this Boc protection method is a simple and effective strategy for constructing DSE molecules. We also found that these three DSE molecules have the potential to target and visualize lipid droplets (LDs). Among them, DCIP-Boc shows advantages of a large Stokes shift, long emission wavelength, low fluorescence background, and good photostability in cells, providing a powerful new molecular tool with DSE property for high-fidelity imaging of LDs.
摘要：
Fe-SSZ-13 (Fe -13) is an effectual catalyst for NOx abatement with extensive application potential in the selective reduction of NOx by NH3 (NH3-SCR). It is necessary to further research and expand the fundamental knowledge of Fe -13 catalysts. In this research, Fe -13 zeolites possessing Si/Al ratios of 6.9, 12.0, and 17.5 were prepared. Fe13(6.9) showed excellent catalytic activity because it had a larger number of isolated Fe3+ ions and welldispersed Fe species. Upon hydrothermal aging, the Fe -13(6.9) catalyst diminished significantly in catalytic activity. Among the three, Fe -13(17.5) exhibited the best hydrothermal stability. It is because Fe -13, possessing a higher Si/Al ratio, had fewer Si-OH-Al bonds but more Si(0Al) structures. Thus, Fe -13(17.5) suffered less structural collapse during hydrothermal aging, leading to a smaller decrease in active isolated Fe3+ ions and acid sites, as well as a lower aggregation of Fe species. Moreover, above 200 degrees C, Fe -13(6.9) exhibited a higher reaction rate compared to Fe -13(12.0) and Fe -13(17.5), and the SCR reaction route of Fe -13(6.9) was distinctly different from that of the other two catalysts.
作者机构：
[Qiu, Xiaofeng; Zheng, Juan; Zhu, Xiaoxiao; Zhang, Qian; Guo, Yanbing; Zhu, Yuhua; Chen, Wei; Zhang, Baojian; Guo, YB; Luo, Zhu; Li, Weihao; Pan, Chuanqi; Fang, Yarong; Wang, Jinlong] Cent China Normal Univ, Inst Environm & Appl Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control &, Minist Educ,Coll Chem,Key Lab Pesticide & Chem Bio, Wuhan 430079, Peoples R China.;[Guo, Yanbing; Guo, YB; Luo, Zhu; Wang, Jinlong] Wuhan Inst Photochem & Technol, Wuhan 430082, Peoples R China.;[Wu, Jinsong; Wang, Yutao] Wuhan Univ Technol, Nanostruct Res Ctr, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China.;[Hu, Jinpeng; Wang, Sibo] Fujian Longxin 3D Array Technol Co Ltd, Longyan 364000, Peoples R China.;[Cui, Shuang] SINOPEC Beijing Res Inst Chem Ind Co Ltd, Div Anal, Beijing 100013, Peoples R China.
通讯机构：
[Guo, YB ; Luo, Z] C;Cent China Normal Univ, Inst Environm & Appl Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control &, Minist Educ,Coll Chem,Key Lab Pesticide & Chem Bio, Wuhan 430079, Peoples R China.;Wuhan Inst Photochem & Technol, Wuhan 430082, Peoples R China.
关键词：
(Pt−S−O)-Ti active structure;C3H8 catalytic oxidation;C−H bond activation;Pt-based catalysts;SO2 promotion
摘要：
Typically, SO(2) unavoidably deactivates catalysts in most heterogeneous catalytic oxidations. However, for Pt-based catalysts, SO(2) exhibits an extraordinary boosting effect in propane catalytic oxidation, but the promotive mechanism remains contentious. In this study, an in situ-formed tactful (Pt-S-O)-Ti structure was concluded to be a key factor for Pt/TiO(2) catalysts with a substantial SO(2) tolerance ability. The experiments and theoretical calculations confirm that the high degree of hybridization and orbital coupling between Pt 5d and S 3p orbitals enable more charge transfer from Pt to S species, thus forming the (Pt-S-O)-Ti structure with the oxygen atom dissociated from the chemisorbed O(2) adsorbed on oxygen vacancies. The active oxygen atom in the (Pt-S-O)-Ti active structure is a robust site for C(3)H(8) adsorption, leading to a better C(3)H(8) combustion performance. This work can provide insights into the rational design of chemical bonds for high SO(2) tolerance catalysts, thereby improving economic and environmental benefits.
期刊：
JOURNAL OF MEDICINAL CHEMISTRY,2024年67(8):6822-6838 ISSN：0022-2623
通讯作者：
Guo, J
作者机构：
[Bian, Miao-Miao; Zhang, Ru-Yan; Cui, Hong-Ying; Ding, Dong; Guo, J; Wen, Yu; Guo, Jun; Zhou, Shi-Hao; Zou, Yong-Ke] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Guo, J ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
摘要：
Weak antigens represented by MUC1 are poorly immunogenic, which greatly constrains the development of relevant vaccines. Herein, we developed a multifunctional lipidated protein as a carrier, in which the TLR1/2 agonist Pam(3)CSK(4) was conjugated to the N-terminus of MUC1-loaded carrier protein BSA through pyridoxal 5'-phosphate-mediated transamination reaction. The resulting Pam(3)CSK(4)-BSA-MUC1 conjugate was subsequently incorporated into liposomes, which biomimics the membrane structure of tumor cells. The results indicated that this lipidated protein carrier significantly enhanced antigen uptake by APCs and obviously augmented the retention of the vaccine at the injection site. Compared with the BSA-MUC1 and BSA-MUC1 + Pam(3)CSK(4) groups, Pam(3)CSK(4)-BSA-MUC1 evoked 22- and 11-fold increases in MUC1-specific IgG titers. Importantly, Pam(3)CSK(4)-BSA-MUC1 elicited robust cellular immunity and significantly inhibited tumor growth. This is the first time that lipidated protein was constructed to enhance antigen immunogenicity, and this universal carrier platform exhibits promise for utilization in various vaccines, holding the potential for further clinical application.
作者机构：
[Liu, Lijuan; Zhang, Lizhi; Gong, JM; Meng, Mingxia; Gong, Jingming; Yao, Qingfeng; Cai, Zheng; Sun, Hongwei; Jiang, Fang] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol, Coll Chem,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Gong, JM ] C;Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol, Coll Chem,Minist Educ, Wuhan 430079, Peoples R China.
摘要：
As emerging contaminants in the environment, antibiotic resistance genes (ARGs) have aroused a global health crisis and posed a serious threat to ecological safety and human health. Thus, efficient and accurate onsite detection of ARGs is crucial for environmental surveillance. Here, we presented a colorimetric-photoelectrochemical (PEC) dual-mode bioassay for simultaneous detection of multiple ARGs by smartly incorporating rolling circle amplification (RCA) into a stimuli-responsive DNA nanoassembly, using the tetracycline resistance genes tetA and tetC as models. The tailored DNA nanoassembly containing RCA amplicons hybridized with specific signal probes: CuO nanoflowers-anchored signal DNA1 and HgO nanoparticles-anchored signal DNA2, respectively. Upon exposure to an acidic stimulus, numerous Cu(2+) and Hg(2+) were released, serving as the reporting agent of colorimetric/PEC dual-mode assay. The released Cu(2+) and Hg(2+) induced localized surface plasmon resonance shifts in Au nanorods and triangular Ag nanoplates through an etching process, respectively, enabling visual analysis of ARGs with distinguishing color changes. Meanwhile, numerous Cu(2+) and Hg(2+) triggered the amplified PEC variations via reacting with the photoactive layers of CuS/CdS and ZnS, respectively. Thus, a rapid and ultrasensitive colorimetric/PEC dual-mode detection of multiple ARGs was achieved with the detection limit down to 17.2 aM. Furthermore, such dual-mode bioassay could discriminate single-base mismatch and successfully determine ARGs in E. coli plasmids and sludge samples, holding great promise for point-of-care genetic diagnostics.
