作者机构：
[Xu, Yuling; Luo, Lishi; Sun, Yao; Pang, Yida; Yang, Jingfang; Li, Chonglu] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Luo, Lishi] Hunan Univ, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Peoples R China.;[Sharma, Amit] Amity Univ Punjab, Amity Sch Chem Sci, Dept Phys, Mohali 140306, India.;[Liu, Shuang] Wuhan Univ Technol, Sch Mat Sci & Engn, Wuhan 430070, Peoples R China.;[Zhan, Jianbo] Hubei Prov Ctr Dis Control & Prevent, Inst Hlth Inspect & Testing, Wuhan, Hubei, Peoples R China.
通讯机构：
[Sun, Y ] 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：
Albeit sonodynamic therapy (SDT) has achieved encouraging progress in microbial sterilization, the scarcity of guidelines for designing highly effective sonosensitizers and the intricate biofilm microenvironment (BME), substantially hamper the therapeutic efficacy against biofilm infections. To address the bottlenecks, we innovatively design a Ru(II) metallacycle-based sonosensitizer/sonocatalyst (named Ru-A3-TTD) to enhance the potency of sonotherapy by employing molecular engineering strategies tailored to BME. Our approach involves augmenting Ru-A3-TTD’s production of ultrasonic-triggered reactive oxygen species (ROS), surpassing the performance of commercial sonosensitizers, through a straightforward but potent π-expansion approach. Within the BME, Ru-A3-TTD synergistically amplifies sonotherapeutic efficacy via triple-modulated approaches: (i) effective alleviation of hypoxia, leading to increased ROS generation, (ii) disruption of the antioxidant defense system, which shields ROS from glutathione consumption, and (iii) enhanced biofilm penetration, enabling ROS production in deep sites. Notably, Ru-A3-TTD sono-catalytically oxidizes NADPH, a critical coenzyme involved in antioxidant defenses. Consequently, Ru-A3-TTD demonstrates superior biofilm eradication potency against multidrug-resistant Escherichia coli compared to conventional clinical antibiotics, both in vitro and in vivo. To our knowledge, this study represents the pioneering instance of a supramolecular sonosensitizer/sonocatalyst. It provides valuable insights into the structure-activity relationship of sonosensitizers and paves a promising pathway for the treatment of biofilm infections.
期刊：
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY,2024年311:123979 ISSN：1386-1425
通讯作者：
Liu, SH;Zhang, J
作者机构：
[Peng, Zhen; Liu, Sheng Hua; Liu, SH] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Zhang, Jing; Feng, Na; Zhang, J] Southern Med Univ, Nanfang Hosp, Dept Lab Med, Guangzhou 510515, Peoples R China.;[Zhang, Jianyu] Hong Kong Univ Sci & Technol, Hong Kong Branch, Chinese Natl Engn Res Ctr Tissue Restorat & Recons, Dept Chem,Kowloon, Clear Water Bay, Hong Kong 999077, Peoples R China.;[Zhang, Jianyu] Hong Kong Univ Sci & Technol, Inst Adv Study, Kowloon, Clear Water Bay, Hong Kong 999077, Peoples R China.
通讯机构：
[Liu, SH ] C;[Zhang, J ] S;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Southern Med Univ, Nanfang Hosp, Dept Lab Med, Guangzhou 510515, Peoples R China.
摘要：
High-performance luminescent gold(I) complexes have attracted considerable attention due to their potential applications in various fields, but their construction is a significantly challenging task. Herein, we designed and synthesized a series of novel dinuclear gold(I) complexes 1-4 based on 1,2-bis(diphenylphosphino)benzene and 1,4-bis(diphenylphosphino)benzene frameworks, where para-substitutions of benzene ring were employed for comparison and bulky t-butyl groups were introduced into carbazole ligands to assist flexibly regulating the aurophilicity. Among them, the structure of complex 1 was confirmed by single-crystal X-ray diffraction, and all the complexes exhibited typical aggregation-induced emission characteristics. Due to the construction of intramolecular aurophilicity and the formation of molecular clusters, noticeable enhancement of the luminescent efficiency was achieved for the core complex 1. Together with the introduction of flexible t-butyl groups, good responsiveness towards external mechanical force and solvent vapors were also realized. Moreover, the specific bioimaging ability of complex 1 towards cancer cells was demonstrated. Thus, this work presents the crucial capability of aurophilic manipulation in tuning the luminescence and smart behaviors of gold complexes, and it will open a new route to developing high-performance luminescent materials.
摘要：
Spinel cobalt oxide (Co3O4), consisting of tetrahedral Co2+ (CoTd) and octahedral Co3+ (CoOh), is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction (CER). Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost CER. Herein, combining density functional theory calculations and experiment results assisted with operando analysis, we found that the CoOh site acts as the main active site for CER in spinel Co3O4, which shows better Cl- adsorption and more moderate intermediate adsorption toward CER than CoTd site, and does not undergo redox transition under CER condition at applied potentials. Guided by above findings, the oxygen vacancies were further introduced into the Co3O4 to precisely manipulate the electronic configuration of CoOh to boost Cl- adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity significantly. Our work figures out the importance of geometric configuration dependent CER activity, shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level. (c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press
摘要：
CsPbBr(3) has received more and more attention in the field of optoelectronic devices due to its excellent stability. To address the cost and environmental concerns associated with the use of toxic methanol, water has been explored as a substitute solvent for CsBr in the preparation of CsPbBr(3) perovskite solar cells (PSCs). In this study, we utilized methanol as an anti-solvent of the CsBr/H(2)O solution to regulate the detrimental effects of water on the CsPbBr(3) film and control the crystallization process. From results of the experiment, it was found that methanol anti-solvent treatment greatly improved the crystallization of the CsPbBr(3) film, increased the grain size, and reduced the defect density. After the introduction of methanol anti-solvent treatment, the power conversion efficiency (PCE) increased from 6.09% to 7.91%, while the open-circuit voltage (V(oc)) increased from 1.18 V to 1.39 V. Furthermore, we incorporated 2-hydroxyethylurea into the CsPbBr(3) PSCs to improve the wettability of PbBr(2) towards the CsBr/H(2)O solution and ensure the formation of pure-phase CsPbBr(3) films. The introduction of 2-hydroxyethylurea resulted in an additional increase in V(oc) from 1.19 V to 1.42 V. The PCE further improved from 6.56% to 8.62% after methanol anti-solvent treatment. These results demonstrate that methanol treatment effectively addresses the low V(oc) issue observed in CsPbBr(3) PSCs prepared with water as a solvent. Importantly, this approach significantly reduces the reliance on methanol compared to conventional fabrication methods for CsPbBr(3) PSCs. Overall, this work presents a promising pathway for achieving high V(oc) and efficiency in CsPbBr(3) PSCs by utilizing water as a solvent.
作者机构：
[Zhao, Xia; Gu, Wenxin; Sun, Tengteng; Qin, Jingwen] Tianjin Normal Univ, Tianjin Key Lab Struct & Performance Funct Mol, Key Lab Inorgan Organ Hybrid Funct Mat Chem, Minist Educ,Coll Chem, Tianjin 300387, Peoples R China.;[Ye, Fei] Cent China Normal Univ, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.;[Lu, Kui] Tianjin Univ Sci & Technol, Coll Biotechnol, China Int Sci & Technol Cooperat Base Food Nutr Sa, Tianjin 300457, Peoples R China.
通讯机构：
[Zhao, X ] T;[Ye, F ] C;Tianjin Normal Univ, Tianjin Key Lab Struct & Performance Funct Mol, Key Lab Inorgan Organ Hybrid Funct Mat Chem, Minist Educ,Coll Chem, Tianjin 300387, Peoples R China.;Cent China Normal Univ, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.
摘要：
A copper-catalyzed thiocyanation of cycloketone oxime esters with ammonium thiocyanate has been developed for the first time. This innovative approach allows access to cyano and thiocyano bifunctionally substituted alkanes, which can be further transformed into their respective trifluoromethylthiol-substituted or difluoromethylthiol-substituted alkylnitriles, alkynyl sulfides, and phosphorothioate esters. The readily available nature of ammonium thiocyanate and the cost-effectiveness of the copper catalyst make this method a promising strategy for the synthesis of sulfur-containing alkylnitriles.
作者机构：
[Guan-Zhu Wang; Xue Wu] National Key Laboratory of Green Pesticide, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Center for Research and Development of Fine Chemicals Guizhou University, Guiyang, 550025, China;National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan, 430079, China;[Ge-Fei Hao] National Key Laboratory of Green Pesticide, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Center for Research and Development of Fine Chemicals Guizhou University, Guiyang, 550025, China<&wdkj&>National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan, 430079, China
通讯机构：
[Ge-Fei Hao] N;National Key Laboratory of Green Pesticide, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Center for Research and Development of Fine Chemicals Guizhou University, Guiyang, 550025, China<&wdkj&>National Key Laboratory of Green Pesticide, College of Chemistry, Central China Normal University, Wuhan, 430079, China
摘要：
Auxin is an important phytohormone that regulates a string of vital rapid responses, and its signaling perception mechanism has been one of the hot spots of research. It has been shown that the ABP1/TMKs module is involved in regulating extracellular auxin signaling, however, the role of ABP1 as an auxin receptor is highly controversial. Therefore, the mechanism of quintessential TMKs sense extracellular auxin remains unresolved. Recently, a study identified two new auxin-binding proteins, ABL1 and ABL2, which directly interact with TMKs to perceive apoplast auxin. This groundbreaking research unravels the mystery surrounding how plants perceive extracellular auxin signals.
摘要：
The contamination of drinking water by microbes is a critical health concern, underscoring the need for safe, reliable, and efficient methods to treat pathogenic microorganisms. While most sterilization materials are available in powder form, this presents safety risks and challenges in recycling. Herein, this study reports the preparation of an innovative copper oxide supported silver monolithic nanoarray mesh with abundant oxygen vacancies (Ag/CuO-V(O)) by laser ablation. The instantaneous high temperature caused by laser ablation preserves the material's original structure while generating oxygen vacancies on the CuO surface. The Ag/CuO-V(O) mesh demonstrated a remarkable ability to inactivate over 99% of Escherichia coli (E. Coli) within 20min. The oxygen vacancies in the Ag/CuO-V(O) enhance interactions between oxygen species and the Ag/CuO-V(O), leading to the accumulation of large amounts of reactive oxygen species (ROS). The generated ROS effectively disrupt both layers of the bacterial cell wall - the peptidoglycan and the phospholipid - as confirmed by Fourier Transform Infrared (FTIR) spectroscopy, culminating in cell death. This research presents a monolithic material capable of inactivating pathogenic microorganisms efficiently, offering a significant advancement in water sterilization technology.
摘要：
Water molecules are actively involved in many catalytic oxidation processes, which require the construction of highly active sites for their activation to accelerate the reaction rate, especially over non-noble metal catalysts. Herein, K species is embeded into the natural 2*2 channel of alpha-MnO2 by a hydrothermal coupled molten salt method, which would make these K species behave in an electron-rich state and provide more electrons for the activation of water molecules. Compared with surface K modification (namely, the electron-deficient K species), channel K confinement can lower the activation energy barrier of H2O dissociation on alpha-MnO2 to generate hydroxyl species with more nucleophilic oxygen atoms, contributing to the superior HCHO catalytic oxidation activity with a fourfold enhancement. The internal relationship among the confined channel, K species, and catalytic performance is systematically elucidated at the molecular level. This work offers a new ion confinement method and opens up new avenues to construct electron-rich metal sites with channel structures for the activation of water molecules.
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024年 ISSN：0002-7863
作者机构：
[Zhou, Yan; Luo, Zhen; Zhu, Chengzhou; Wu, Yu; Li, Jingshuai; Xi, Mengzhen; Gu, Wenling; Ling, Ling] State Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China;[Hu, Liuyong] Hubei Key Laboratory of Plasma Chemistry and Advanced Materials, Hubei Engineering Technology Research Center of Optoelectronic and New Energy Materials, Wuhan Institute of Technology, Wuhan 430205, P. R. China;[Wang, Canglong] Institute of Modern Physics, University of Chinese Academy of Sciences, Lanzhou 730000, P. R. China
摘要：
The development of potential-resolved electrochemiluminescence (ECL) systems with dual emitting signals holds great promise for accurate and reliable determination in complex samples. However, the practical application of such systems is hindered by the inevitable mutual interaction and mismatch between different luminophores or coreactants. In this work, for the first time, by precisely tuning the oxygen reduction performance of M-N-C single-atom catalysts (SACs), we present a dual potential-resolved luminol ECL system employing endogenous dissolved O(2) as a coreactant. Using advanced in situ monitoring and theoretical calculations, we elucidate the intricate mechanism involving the selective and efficient activation of dissolved O(2) through central metal species modulation. This modulation leads to the controlled generation of hydroxyl radical (·OH) and superoxide radical (O(2)(·-)), which subsequently trigger cathodic and anodic luminol ECL emission, respectively. The well-designed Cu-N-C SACs, with their moderate oxophilicity, enable the simultaneous generation of ·OH and O(2)(·-), thereby facilitating dual potential-resolved ECL. As a proof of concept, we employed the principal component analysis statistical method to differentiate antibiotics based on the output of the dual-potential ECL signals. This work establishes a new avenue for constructing a potential-resolved ECL platform based on a single luminophore and coreactant through precise regulation of active intermediates.
摘要：
Poly(ionic liquid)s (PILs) bearing high ionic densities are promising candidates for carbon dioxide (CO(2)) fixation. However, efficient and metal-free methods for boosting the catalytic efficiencies of PILs are still challenging. In this study, a novel family of poly(ionic liquid)-coated carbon nanotube nanoarchitectures (CNTs@PIL) were facilely prepared via a noncovalent and in-situ polymerization method. The effects of different carbon nanotubes (CNTs) and PILs on the structure, properties, and catalytic performance of the composite catalysts were systematically investigated. Characterizations and experimental results showed that hybridization of PIL with hydroxyl- or carboxyl-functionalized CNTs (CNT-OH, CNT-COOH) endows the composite catalyst with increased porosity, CO(2) capture capacity, swelling ability and diffusion rate with respect to individual PIL, and allows the CNTs@PIL to provide H-bond donors for the synergistic activation of epoxides at the interfacial layer. Benefiting from these merits, the optimal composite catalyst (CNT-OH@PIL) delivered a super catalytic efficiency in the cycloaddition of CO(2) to propylene oxide, which was over 4.5 times that of control PIL under metal- and co-catalyst free conditions. Additionally, CNT-OH@PIL showed high carbon dioxide/nitrogen (CO(2)/N(2)) adsorptive selectivity and could smoothly catalyze the cycloaddition reaction with a simulated flue gas (15% CO(2) and 85% N(2)). Furthermore, the CNT-OH@PIL exhibited broad substrate tolerance and could be readily recycled and efficiently reused at least 12 times. Hybridization of PIL with functionalized CNTs provides a feasible approach for boosting the catalytic performance of PIL-based solid catalysts for CO(2) fixation.
作者机构：
[Yi, Yun-Ying; Liu, Yu-Ting; Song, Ying-Chun; Wang, Ming-Xuan; Zhang, Wen-Xin; Wang, Zi-Yue; Zhu, Yan-Ping; Sun, Yuan-Yuan] Yantai Univ, Minist Educ, Collaborat Innovat Ctr Adv Drug Delivery Syst & Bi, Sch Pharm,Key Lab Mol Pharmacol & Drug Evaluat, Yantai 264005, Shandong, Peoples R China.;[Wu, An-Xin] 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;[Zhu, YP ] Y;Yantai Univ, Minist Educ, Collaborat Innovat Ctr Adv Drug Delivery Syst & Bi, Sch Pharm,Key Lab Mol Pharmacol & Drug Evaluat, Yantai 264005, Shandong, Peoples R China.;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
关键词：
Total synthesis;Oxidative cyclization;Natural products;Switchable synthesis;Luotonin alkaloids
摘要：
A total synthesis strategy was developed for the synthesis of luotonin A, B and their analogues using synergistic FeCl3/KI-catalyzed oxidative cyclization. This protocol utilizes cheap and widely available N-propargyl 2-methyl-quinazolinones and arylamines under mild conditions, and it has a wide substrate scope and high atom economy. Different natural products (luotonin A, B and derivatives) can be synthesized via a unique switchable approach. Further transformations from luotonin B to luotonin E and structural modification of natural products demonstrate the potential applications of this method. Moreover, camptothecin can also be modified with the reported protocol to afford the hydroxyl-substituted product.
期刊：
Sensors and Actuators B-Chemical,2024年406:135432 ISSN：0925-4005
通讯作者：
Feng, GQ
作者机构：
[Zheng, Zhoupeng; Feng, Guoqiang; Feng, GQ; Zhang, Jinzheng; Liu, Yijia; Gong, Shenyi] Cent China Normal Univ, Coll Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
通讯机构：
[Feng, GQ ] C;Cent China Normal Univ, Coll Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
关键词：
Dual -channel fluorescent probe;Viscosity;Peroxynitrite;Mitochondria;Diabetes;In vivo imaging
摘要：
Diabetes is a common metabolic disease worldwide, which often has serious complications and seriously threatens human health. Abnormal viscosity and peroxynitrite (ONOO-) concentration are closely related to diabetes. Herein, we report a fluorescent dual response probe AO, which can simultaneously detect the changes of viscosity and ONOO- in diabetes at dual fluorescence channels. AO sensitively responds to viscosity and ONOO- with significant emission signal changes at 710 nm and 645 nm, respectively. Moreover, AO selectively targets mitochondria and generates a new compound when detecting ONOO-, which can spontaneously target and light up another type of organelle (lipid droplets), thus showing spatially separated dual -channel fluorescence signals. More notably, AO was successfully used to simultaneously detect the viscosity and ONOO- variations in hyperglycemic cells, diabetes and its complications (using mice models) for the first time, which may lead to a better understanding of the physiological and pathological phenomena of diabetes.
期刊：
CHEMICAL SOCIETY REVIEWS,2024年53(1):137-162 ISSN：0306-0012
通讯作者：
Zhu, CZ;Lin, YH
作者机构：
[Xu, Weiqing; Zhu, Chengzhou; Wu, Yu; Zhu, CZ; Gu, Wenling] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Lin, YH; Du, Dan; Lin, Yuehe] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
通讯机构：
[Lin, YH ] W;[Zhu, CZ ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
摘要：
Natural metalloenzymes with astonishing reaction activity and specificity underpin essential life transformations. Nevertheless, enzymes only operate under mild conditions to keep sophisticated structures active, limiting their potential applications. Artificial metalloenzymes that recapitulate the catalytic activity of enzymes can not only circumvent the enzymatic fragility but also bring versatile functions into practice. Among them, metal-organic frameworks (MOFs) featuring diverse and site-isolated metal sites and supramolecular structures have emerged as promising candidates for metalloenzymes to move toward unparalleled properties and behaviour of enzymes. In this review, we systematically summarize the significant advances in MOF-based metalloenzyme mimics with a special emphasis on active pocket engineering at the atomic level, including primary catalytic sites and secondary coordination spheres. Then, the deep understanding of catalytic mechanisms and their advanced applications are discussed. Finally, a perspective on this emerging frontier research is provided to advance bioinspired catalysis. This review systematically summarizes the significant advances in MOF-based metalloenzyme mimics for bioinspired catalysis with a special emphasis on active pocket engineering at the atomic level.
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024年146(2):1410-1422 ISSN：0002-7863
通讯作者：
Xiao, Wen-Jing;Chen, JR
作者机构：
[Zhao, Ke; Qu, Wen-Yuan; Xiao, Wen-Jing; Chen, Jia-Rong; Mao, Zhi-Cheng; Zhang, Bin; Xiao, WJ; Li, Tian-Tian; Zhang, Zhihan; Chen, JR] Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;[Jiang, Min] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Hangzhou 310036, Peoples R China.;[Xiao, Wen-Jing; Chen, Jia-Rong; Xiao, WJ; Chen, JR] Wuhan Inst Photochem & Technol, Wuhan 430082, Hubei, Peoples R China.
通讯机构：
[Xiao, WJ; Chen, JR ] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;Wuhan Inst Photochem & Technol, Wuhan 430082, Hubei, Peoples R China.
摘要：
Alkene radical ions constitute an integral and unique class of reactive intermediates for the synthesis of valuable compounds because they have both unpaired spins and charge. However, relatively few synthetic applications of alkene radical anions have emerged due to a dearth of generally applicable and mild radical anion generation approaches. Precise control over the chemo- and stereoselectivity in alkene radical anion-mediated processes represents another long-standing challenge due to their high reactivity. To overcome these issues, here, we develop a new redox-neutral strategy that seamlessly merges photoredox and copper catalysis to enable the controlled generation of alkene radical anions and their orthogonal enantioselective cyanofunctionalization via distonic-like species. This new strategy enables highly regio-, chemo-, and enantioselective hydrocyanation, deuterocyanation, and cyanocarboxylation of alkenes without stoichiometric reductants or oxidants under visible light irradiation. This protocol provides a new blueprint for the exploration of the transformation potential of alkene radical anions.
摘要：
A visible‐light‐driven four‐component radical relay aminocarbonylation reaction of unactivated alkenes using 4CzIPN as an organic photocatalyst is developed, providing robust access to β‐fluoroalkyl amides with good yields and selectivity under metal‐free conditions. Importantly, this strategy also shows good compatibility with tertiary carbon radicals. Comprehensive Summary Catalytic four‐component radical carbonylation of unactivated alkenes has recently been recognized as a robust protocol for rapid construction of various structurally diverse carbonyl compounds. Given the significance of fluorine‐containing groups, this reaction class has been extensively applied to assembly of a variety of perfluoroalkyl carboxylic acid derivatives by transition metal catalysis. Herein, we report a visible‐light‐driven radical relay 1,2‐perfluoroalkylation aminocarbonylation of unactivated alkenes using CO gas as carbonyl source and 4CzIPN as organic photocatalyst. A wide range of alkenes and amines were well tolerated, providing the valuable β‐perfluoroalkylated amides with generally good yields and high chemoselectivity.
期刊：
CHEMISTRY-A EUROPEAN JOURNAL,2024年30(18):e202303742 ISSN：0947-6539
通讯作者：
Li, HB
作者机构：
[Chen, Chunxiu; Li, Guang; Xu, Weiwei; Cai, Meng; Li, Haibing; Ma, Cuiguang; Li, HB; Zhang, Haifan; Noruzi, Ehsan Bahojb; Qu, Haonan] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Li, Haibing; Li, HB] Guangxi Univ, State Key Lab Featured MetaMat & Life Cycle Safety, Nanning 530004, Peoples R China.;[Wang, Miao] Xiamen Univ, Coll Mat, Xiamen 361005, Peoples R China.;[Hou, Xu] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China.
通讯机构：
[Li, HB ] C;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Guangxi Univ, State Key Lab Featured MetaMat & Life Cycle Safety, Nanning 530004, Peoples R China.
摘要：
Excess fluoride ions in groundwater accumulate through the roots of crops, affecting photosynthesis and inhibiting their growth. Long-term bioaccumulation also threatens human health because it is poorly degradable and toxic. Currently, one of the biggest challenges is developing a unique material that can efficiently remove fluoride ions from the environment. The excellent properties of functionalized pillar[5]arene polymer-filled nanochannel membranes were explored to address this challenge. Constructing a multistage porous nanochannel membrane, consisting of microscale etched nanochannels and nanoscale pillar[5]arene cross-linked polymer voids. A fluoride removal rate of 0.0088 mmol & sdot; L-1 & sdot; min-1 was achieved. Notably, this rate surpassed the rates observed with other control ions by a factor of 6 to 8.8. Our research provides a new direction for developing water fluoride ion removal materials. Fluoride contamination of groundwater has become one of the most serious problems in the world. Currently, excessive absorption of fluoride can be toxic to humans and crops. To address the challenge, we explored the excellent properties of functionalized pillar[5]arene polymer framework. By constructing a multistage porous nanochannel membrane, the pillar[5]arene polymer-filled nanochannel membrane achieves a fluoride removal. image
作者机构：
[Zhu, Chengzhou; Gu, Wenling; Li, Jingshuai; Xi, Mengzhen] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Hu, Liuyong] Wuhan Inst Technol, Hubei Engn Technol Res Ctr Optoelect & New Energy, Hubei Key Lab Plasma Chem & Adv Mat, Wuhan 430205, Peoples R China.;[Sun, Hongcheng] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Key Lab Organosilicon Chem & Mat Technol, Minist Educ, Hangzhou 311121, Peoples R China.;[Gu, Wenling] Key Lab Opt Elect Sensing & Analyt Chem Life Sci, MOE, Qingdao 266042, Peoples R China.
通讯机构：
[Gu, WL ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;Key Lab Opt Elect Sensing & Analyt Chem Life Sci, MOE, Qingdao 266042, Peoples R China.
摘要：
Improving the sensitivity in electrochemiluminescence (ECL) detection systems necessitates the integration of robust ECL luminophores and efficient signal transduction. In this study, we report a novel ECL nanoprobe (Zr-MOF) that exhibits strong and stable emission by incorporating aggregation-induced emission ligands into Zr-based metal-organic frameworks (MOFs). Meanwhile, we designed a high-performance signal modulator through the implementation of a well-designed controlled release system with a self-on/off function. ZnS quantum dots (QDs) encapsulated within the cavities of aminated mesoporous silica nanoparticles (NH(2)-SiO(2)) serve as the ECL quenchers, while adenosine triphosphate (ATP) aptamers adsorbed on the surface of NH(2)-SiO(2) through electrostatic interaction act as "gatekeepers." Based on the target-triggered ECL resonance energy transfer between Zr-MOF and ZnS QDs, we establish a coreactant-free ECL aptasensor for the sensitive detection of ATP, achieving an impressive low detection limit of 0.033 nM. This study not only demonstrates the successful combination of ECL with controlled release strategies but also opens new avenues for developing highly efficient MOFs-based ECL systems.
期刊：
Sensors and Actuators B-Chemical,2024年405 ISSN：0925-4005
通讯作者：
Xu, Miao;Gu, WL;Ye, HR
作者机构：
[Xu, Weiqing; Chen, Yifeng; Zhu, Chengzhou; Xu, Miao; Sha, Meng; Zou, Chufan; Gu, Wenling; Chen, Guo] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Ye, Huarong; Ye, HR] China Resources & Wisco Gen Hosp, Wuhan 430080, Peoples R China.;[Zhu, Chengzhou] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Key Lab Organosilicon Chem & Mat Technol, Minist Educ, Hangzhou 311121, Peoples R China.;[Gu, Wenling] Hubei Univ, Sch Life Sci, State Key Lab Biocatalysis & Enzyme Engn, Wuhan 430062, Peoples R China.
通讯机构：
[Xu, M; Gu, WL ; Ye, HR ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;China Resources & Wisco Gen Hosp, Wuhan 430080, Peoples R China.;Hubei Univ, Sch Life Sci, State Key Lab Biocatalysis & Enzyme Engn, Wuhan 430062, Peoples R China.
摘要：
The fragility inherent in enzymes can be overcome by immobilizing them within nano-carriers, which offer designability and controllability and serve as a promising strategy for overcoming the inherent fragility of enzymes. While enzyme immobilization enhances enzyme stability and reusability, it can potentially hinder their bioactivity and catalytic efficiency. In this study, we present an enzyme-directed biomimetic mineralization approach for the in situ encapsulation of horseradish peroxidase (HRP) within hydrogen-bonded organic frameworks (HOFs) to obtain HOF@HRP nanocomposites. Remarkably, the HOF@HRP nanocomposites exhibit an ultrahigh protein content and demonstrate comparable catalytic activity to that of the free enzyme. Moreover, the HOFs act as protective shields, safeguarding the internal enzymes against various environmental disturbances. Leveraging the unique properties of HOF@HRP, we propose a dual-modal enzyme-linked immunosorbent assay for the sensitive detection of prostate-specific antigen in human serum. The resultant biosensor exhibits a good linear range, excellent sensitivity, and selectivity, showcasing its promising potential and clinical application in the field of diagnostic medicine.
作者机构：
[Lin, Jinying] Jilin Univ, Sch Stomatol, Dept Oral Implantol, Jilin Prov Key Lab Tooth Dev & Bone Remodeling, Changchun 130021, Peoples R China.;[Ding, Qihang] Korea Univ, Dept Chem, Seoul 02841, South Korea.;[Sun, Yao] 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：
[Sun, Y ] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
