作者机构：
[Lin, Fengcai; Li, Xiaoqing; Zhu, Jide; Zheng, Xiaoxiao; Xu, Yanlian; Chen, Jipeng; Xu, YL] Minjiang Univ, Coll Mat & Chem Engn, Fujian Engn Res Ctr New Chinese Lacquer Mat, Fuzhou 350108, Fujian, Peoples R China.;[Shen, Lijuan; Shen, LJ; Zhu, Jide; Zheng, Xiaoxiao; Chen, Xiaoping; Jiang, Lilong] Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China.;[Chen, Xiaoping] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Shen, Lijuan; Shen, LJ] Fujian Normal Univ, Coll Environm & Resource Sci, Coll Carbon Neutral Modern Ind, Fujian Key Lab Pollut Control & Resource Reuse, Fuzhou 350007, Fujian, Peoples R China.
通讯机构：
[Shen, LJ ] F;[Xu, YL ] M;Minjiang Univ, Coll Mat & Chem Engn, Fujian Engn Res Ctr New Chinese Lacquer Mat, Fuzhou 350108, Fujian, Peoples R China.;Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, Fuzhou 350002, Fujian, Peoples R China.;Fujian Normal Univ, Coll Environm & Resource Sci, Coll Carbon Neutral Modern Ind, Fujian Key Lab Pollut Control & Resource Reuse, Fuzhou 350007, Fujian, Peoples 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.
通讯机构：
[Peng, X ] C;[Shen, WJ ] W;Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430023, Peoples R China.
关键词：
Cu(II) reduction;Zero-valent iron;Boric acid;Oxygen adsorption;Electron transfer
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.
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.
摘要：
Viruses are ubiquitous in human life. Some viruses can be used as vectors of genetic engineering and specific pesticides. Other viruses trigger a variety of diseases in humans, animals and plants, resulting in high infection rates and mortality. Therefore, convenient, accurate and rapid detection of viruses is of great significance for the diagnosis and treatment of subsequent diseases. In contrast to traditional methods of detection, which rely on time-consuming and complex techniques such as polymerase chain reaction (PCR), fluorescent probes and imaging methods generate real-time results, with high specificity, and have been widely used in viral detection. In this review, the application of viral fluorescent probes in analyzing the molecular structure, detection and biological imaging is discussed. In particular, we catego-rized the probes based on their specificity for human and plant viruses, reviewing the latest findings and analyzing their limitations. The potential of fluorescent molecular probes in the treatment of viral dis-ease and environmental analysis, and their possible combinations with protein and immune technology are discussed.(c) 2023 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
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.
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.
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.
作者机构：
[Chen, Shuibing; Pan, Fong Cheng; Feng, Lingling; Evans, Todd; Pan, FC; Duan, Xiaohua; de Silva, Neranjan; Greenspun, Benjamin; Chandwani, Rohit] Weill Cornell Med, Dept Surg, 1300 York Ave, New York, NY 10065 USA.;[Chen, Shuibing; Evans, Todd; Duan, Xiaohua; Greenspun, Benjamin] Weill Cornell Med, Ctr Genom Hlth, 1300 York Ave, New York, NY 10065 USA.;[Zhang, Tuo] Weill Cornell Med, Genom Resources Core Facil, New York, NY 10065 USA.;[Feng, Lingling] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Wang, Xing; Moyer, Jenna; Elemento, Olivier; Martin, M. Laura] Weill Cornell Med, Caryl & Israel Englander Inst Precis Med, New York, NY USA.
通讯机构：
[Evans, T; Chen, SB; Chen, SB ; Pan, FC ] W;Weill Cornell Med, Dept Surg, 1300 York Ave, New York, NY 10065 USA.;Weill Cornell Med, Ctr Genom Hlth, 1300 York Ave, New York, NY 10065 USA.
关键词：
KRAS;SREBP2;cholesterol biosynthesis;colon cancer organoids;lung cancer organoids;orthotopic transplantation;pancreatic organoid;perhexiline maleate;targeted therapy
摘要：
KRAS mutations, mainly G12D and G12V, are found in more than 90% of pancreatic ductal adenocarcinoma (PDAC) cases. The success of drugs targeting KRAS(G12C) suggests the potential for drugs specifically targeting these alternative PDAC-associated KRAS mutations. Here, we report a high-throughput drug-screening platform using a series of isogenic murine pancreatic organoids that are wild type (WT) or contain common PDAC driver mutations, representing both classical and basal PDAC phenotypes. We screened over 6,000 compounds and identified perhexiline maleate, which can inhibit the growth and induce cell death of pancreatic organoids carrying the Kras(G12D) mutation both invitro and invivo and primary human PDAC organoids. scRNA-seq analysis suggests that the cholesterol synthesis pathway is upregulated specifically in the KRAS mutant organoids, including the key cholesterol synthesis regulator SREBP2. Perhexiline maleate decreases SREBP2 expression levels and reverses the KRAS mutant-induced upregulation of the cholesterol synthesis pathway.
作者机构：
[Hao, Ge-Fei; Li, Xiao-Hong; Gao, Yang-Yang] Guizhou Univ, Ctr Res & Dev Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang, Peoples R China.;[Li, Jing-Yi; Liu, Chun-Rong; Hao, Ge-Fei; Li, Meng-Zhao; Li, JY] Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan, Peoples R China.
通讯机构：
[Liu, CR; Li, JY] C;[Hao, GF ] G;Guizhou Univ, Ctr Res & Dev Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang, Peoples R China.;Cent China Normal Univ, Coll Chem, Natl Key Lab Green Pesticide, Wuhan, Peoples R China.
关键词：
wearable sensors;in-situ and continuous;monitoring;plant health information;precision agriculture
摘要：
Plant health is intricately linked to crop quality, food security and agricultural productivity. Obtaining accurate plant health information is of paramount importance in the realm of precision agriculture. Wearable sensors offer an exceptional avenue for investigating plant health status and fundamental plant science, as they enable real-time and continuous in-situ monitoring of physiological biomarkers. However, a comprehensive overview that integrates and critically assesses wearable plant sensors across various facets, including their fundamental elements, classification, design, sensing mechanism, fabrication, characterization and application, remains elusive. In this study, we provide a meticulous description and systematic synthesis of recent research progress in wearable sensor properties, technology and their application in monitoring plant health information. This work endeavours to serve as a guiding resource for the utilization of wearable plant sensors, empowering the advancement of plant health within the precision agriculture paradigm.
作者机构：
[Zhou, Yan; Zhu, Chengzhou; Li, Jingshuai; Xi, Mengzhen; 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.;[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.;[Lu, Bingzhang] Xi An Jiao Tong Univ, Sch Chem Engn & Technol, Xian 710049, Shaanxi, Peoples R China.;[Zhu, Chengzhou; Zhu, CZ] Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Key Lab Organosilicon Chem & Mat Technol, Minist Educ, Hangzhou 311121, Peoples R China.
通讯机构：
[Lu, BZ ] X;[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.;Xi An Jiao Tong Univ, Sch Chem Engn & Technol, Xian 710049, Shaanxi, Peoples R China.;Hangzhou Normal Univ, Coll Mat Chem & Chem Engn, Key Lab Organosilicon Chem & Mat Technol, Minist Educ, Hangzhou 311121, Peoples R China.
摘要：
For conventional potential-resolved ratiometric electrochemiluminescence (ECL) systems, the introduction of multiplex coreactants is imperative. However, the undesirable interactions between different coreactants inevitably affect analytical accuracy and sensitivity. Herein, through the coordination of aggregation-induced emission ligands with gadolinium cations, the self-luminescent metal-organic framework (Gd-MOF) is prepared and serves as a novel coreactant-free anodic ECL emitter. By the intercalation of [Ru(bpy)(2)dppz](2+) with light switch effect into DNA duplex, one high-efficiency cathodic ECL probe is obtained using K(2)S(2)O(8) as a coreactant. In the presence of acetamiprid, the strong affinity between the target and its aptamer induces the release of [Ru(bpy)(2)dppz](2+), resulting in a decreasing cathode signal and an increasing anode signal owing to the ECL resonance energy transfer from Gd-MOF to [Ru(bpy)(2)dppz](2+). In this way, an efficient dual-signal ECL aptasensor is constructed for the ratiometric analysis of acetamiprid, exhibiting a remarkably low detection limit of 0.033 pM. Strikingly, by using only one exogenous coreactant, the cross interference from multiple coreactants can be eliminated, thus improving the detection accuracy. The developed high-performance ECL sensing platform is successfully applied to monitor the residual level of acetamiprid in real samples, demonstrating its potential application in the field of food security.
作者机构：
[Shu, C; Xuan, Chenglong; Shu, Chao; Liu, Meng; Ouyang, Xinke] Cent China Normal Univ CNNU, Coll Chem,Engn Res Ctr Photoenergy Utilizat Pollut, CCNU UOttawa Joint Res Ctr,Natl Key Lab Green Pest, Key Lab Pesticide & Chem Biol,Minist Educ, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.;[Shu, C; Shu, Chao] Wuhan Inst Photochem & Technol, 7 North Bingang Rd, Wuhan 430083, Hubei, Peoples R China.
通讯机构：
[Shu, C ] C;Cent China Normal Univ CNNU, Coll Chem,Engn Res Ctr Photoenergy Utilizat Pollut, CCNU UOttawa Joint Res Ctr,Natl Key Lab Green Pest, Key Lab Pesticide & Chem Biol,Minist Educ, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.;Wuhan Inst Photochem & Technol, 7 North Bingang Rd, Wuhan 430083, Hubei, Peoples R China.
摘要：
The term "cyclic architectures" refers to a class of molecules that are highly valuable and play significant roles in organic compounds. Therefore, there is growing interest in researching the development of efficient and straightforward methods for constructing these complex structures. Photoinduced radical-polar crossover cyclization (RPCC) of bifunctional alkenes represents a class of reactions that are of great synthetic utility because they show high chemoselectivity, broad functional group tolerance and proceed under mild conditions to produce high-value cyclic products with precise alkene design. This mini-review summarizes the recent representative advances in the development of RPCC over the past two decades through different synthetic strategies in the reactions, highlighting their product diversity, selectivity and applicability, and the mechanistic rationale where possible. The intention is to provide readers with a comprehensive understanding of the current state-of-play in this field and contribute to future research efforts. Photoinduced radical-polar crossover cyclization (RPCC) of bifunctional alkenes is of high synthetic utility to produce cyclic products with precise alkene design. This review summarizes the recent representative advances in the field of RPC.
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.
作者机构：
[Yan, HY; Yan, Hongye; Zhou, Yu; Ding, Xilin; Liu, Jin; Lei, Mengdie; Chen, Hongxiang] Wuhan Univ Sci & Technol, Sch Chem & Chem Engn, Key Lab Hubei Prov Coal Convers & New Carbon Mat, Wuhan 430081, Peoples R China.;[Tang, Yinjun; Zhu, Chengzhou] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, 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.
通讯机构：
[Yan, HY ] W;Wuhan Univ Sci & Technol, Sch Chem & Chem Engn, Key Lab Hubei Prov Coal Convers & New Carbon Mat, Wuhan 430081, Peoples R China.
摘要：
The urgent need for sensitive and accurate assays to monitor acetylcholinesterase (AChE) activity and organophosphorus pesticides (OPs) arises from the imperative to safeguard human health and protect the ecosystem. Due to its cost-effectiveness, ease of operation, and rapid response, nanozyme-based colorimetry has been widely utilized in the determination of AChE activity and OPs. However, the rational design of nanozymes with high activity and specificity remains a great challenge. Herein, trace amount of Bi-doped core-shell Pd@Pt mesoporous nanospheres (Pd@PtBi(2)) have been successfully synthesized, exhibiting good peroxidase-like activity and specificity. With the incorporation of trace bismuth, there is a more than 4-fold enhancement in the peroxidase-like performance of Pd@PtBi(2) compared to that of Pd@Pt. Besides, no significant improvement of oxidase-like and catalase-like activities of Pd@PtBi(2) was found, which prevents interference from O(2) and undesirable consumption of substrate H(2)O(2). Based on the blocking impact of thiocholine, a colorimetric detection platform utilizing Pd@PtBi(2) was constructed to monitor AChE activity with sensitivity and selectivity. Given the inhibition of OPs on AChE activity, a biosensor was further developed by integrating Pd@PtBi(2) with AChE to detect OPs, capitalizing on the cascade amplification strategy. The OP biosensor achieved a detection limit as low as 0.06 ng mL(-1), exhibiting high sensitivity and anti-interference ability. This work is promising for the construction of nanozymes with high activity and specificity, as well as the development of nanozyme-based colorimetric biosensors.
期刊：
POLYMER ENGINEERING AND SCIENCE,2024年 ISSN：0032-3888
通讯作者：
Wu, QX
作者机构：
[Liu, Yunguo; Wu, Qiangxian; Ren, Mingtian] Cent China Normal Univ, Coll Chem, Green Polymer Lab, Wuhan, Peoples R China.;[Liu, Yunguo; Wu, Qiangxian; Ren, Mingtian] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan, Peoples R China.;[Koranteng, Ernest] Univ Educ, Dept Chem Educ, Lab Sustainable Polymers & Synth, Winneba, Ghana.;[Weng, Fangqing] Hubei Univ Educ, Coll Chem & Life Sci, Hubei Key Lab Purificat & Applicat Plant Anticanc, Wuhan, Peoples R China.;[Wu, Qiangxian; Wu, QX] Cent China Normal Univ, Coll Chem, Wuhan 430205, Peoples R China.
通讯机构：
[Wu, QX ] C;Cent China Normal Univ, Coll Chem, Wuhan 430205, Peoples R China.
关键词：
biomaterials;composites;corn starch;PBAT;surfaces and interfaces
摘要：
Compatibility mechanise. Abstract Starch is an environmentally friendly, renewable, green resource and an ideal alternative to polymers from petroleum resources. The preparation of high‐performance poly (butylene adipate‐co‐terephthalate) (PBAT)/corn starch composite materials is of significant importance for saving production costs and expanding the application fields of PBAT plastics. This study employed novel processing techniques such as melt blending and injection molding to fabricate PBAT/corn starch composite materials with polyurethane prepolymer (PCLPU) as a compatibilizer. The impact of varying polyurethane prepolymer concentrations on the composite material's structure, mechanical properties, morphology, thermal behavior, and water absorption was scrutinized. Mechanical performance testing showed that compared to the composite material without PCLPU (P90CS10), adding 5% PCLPU can increase the material's elongation at break from 350.2% to 359.0% and the tensile strength from 12.9 to 19.8 MPa. Scanning electron microscopy, thermogravimetric analysis, and water absorption results indicate that the composite material with the addition of the PCLPU compatibilizer has better compatibility, thermal stability, and water resistance than P90CS10. Additionally, the prepared composite material could be successfully blown into a thin film, further enriching the application of the composite material. Highlights A special interface structure was prepared to increase the compatibility of the poly (butylene adipate‐co‐terephthalate)/corn starch composite. Both the strength and the flexibility of the composite were successfully improved. The processing method through which modification was conducted in the melt was convenient, green, and effective. The prepared composite material has potential application value, and the processing method of the composite material is easy to transfer to industrial production.
摘要：
A mild strategy for the synthesis of boron‐handled pyrazoles through photocatalytic cascade radical cyclization of LBRs (Lewis base‐boryl radicals) with vinyldiazo reagents is described here. The reaction starts with the addition of LBRs at diazo site, followed by intramolecular radical cyclization to access a wide range of important boron‐handled pyrazoles in good to excellent yields. Control experiments, together with detailed mechanism studies well explain the observed reactivity. Abstract Vinyldiazo compounds are one of the most important synthons in the construction of a cyclic ring. Most photochemical transformations of vinyldiazo compounds are mainly focusing on utilization of their C═C bond site, while reactions taking place at terminal nitrogen atom are largely unexplored. Herein, a photocatalytic cascade radical cyclization of LBRs with vinyldiazo reagents through sequential B─N/C─N bond formation is described. The reaction starts with the addition of LBRs (Lewis base–boryl radicals) at diazo site, followed by intramolecular radical cyclization to access a wide range of important boron‐handled pyrazoles in good to excellent yields. Control experiments, together with detailed mechanism studies well explain the observed reactivity. Further studies demonstrate the utility of this approach for applications in pharmaceutical and agrochemical research.
摘要：
In an effort to make pesticide use safer, more efficient, and sustainable, micro-/nanocarriers are increasingly being utilized in agriculture to deliver pesticide-active agents, thereby reducing quantities and improving effectiveness. In the use of nanopesticides, the choice to further design and prepare pesticide stimulus-responsive nanocarriers based on changes in the plant growth environment (light, temperature, pH, enzymes, etc.) has received more and more attention from researchers. Based on this, this paper examines recent advancements in nanomaterials for the design of stimulus-responsive micro-/nanocarriers. It delves into the intricacies of preparation methods, material enhancements, in vivo/ex vivo controlled release, and application techniques for controlled release formulations. The aim is to provide a crucial reference for harnessing nanotechnology to pursue reduced pesticide use and increased efficiency.
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024年146(13):8991-9003 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.
摘要：
The development of efficient, bright, and stable narrowband light-emitting electrochemical cells (LECs) has remained a challenge. Here, intrinsically ionic multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters are reported as guest emitters for narrowband LECs, which are developed by attaching an imidazolium cation onto a typical MR-TADF emitter. In solution, the emitters show green-blue emission peaked at 486-497 nm with small full widths at half-maximum (FWHMs) at 24-26 nm. In doped films, they show narrowband green-blue emission with high luminescent efficiencies at approximate to 90%. LECs using an ionic exciplex host and the ionic MR-TADF guest emitters show green-blue emission peaked at 494-503 nm with small FWHMs at 31-34 nm, and afford high external quantum efficiencies (EQEs) up to 10% under constant-voltage driving. With ionic TADF small-molecule hosts, the narrowband LECs show high EQEs up to 13.0% under constant-voltage driving, which is the highest among all reported narrowband LECs, and afford peak brightness/EQE/half lifetime at 780 cd m-2/5.6%/62.2 h under constant-current driving. A long half-lifetime of approximate to 630 h has further been achieved at 136 cd m-2. The work demonstrates the great potential for the use of intrinsically ionic MR-TADF guest emitters and ionic TADF hosts to develop efficient, bright, and stable narrowband LECs. Narrowband light-emitting electrochemical cells (LECs) are fabricated with ionic multi-resonance thermally- activated delayed fluorescence (TADF) guest emitters, which show high external quantum efficiencies (EQEs) up to 13.0% under constant-voltage driving and peak brightness/EQE/half-lifetime at 780 cd m-2/5.6%/62.2 h under constant-current driving. A half-lifetime of approximate to 630 h is further achieved at 136 cd m-2. image
期刊：
Highlights in Chemical Science,2024年15(14):5061-5081 ISSN：2041-580X
通讯作者：
Luo, Zhu;Guo, YB
作者机构：
[Guo, YB; Qiu, Xiaofeng; Luo, Zhu; Wu, Yan; Guo, Yanbing; Zhang, Shuhong; Zhu, Yuhua; Hao, Quanguo] Cent China Normal Univ, Coll Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control &, Minist Educ, Wuhan 430082, Hubei, Peoples R China.;[Guo, YB; Luo, Zhu; Guo, Yanbing] Wuhan Inst Photochem & Technol, 7 North Bingang Rd, Wuhan 430082, Hubei, Peoples R China.;[Zhu, Yuhua] Wuhan Univ, Sch Civil Engn, Wuhan 430072, Peoples R China.
通讯机构：
[Guo, YB ; Luo, Z] C;Cent China Normal Univ, Coll Chem, Engn Res Ctr Photoenergy Utilizat Pollut Control &, Minist Educ, Wuhan 430082, Hubei, Peoples R China.;Wuhan Inst Photochem & Technol, 7 North Bingang Rd, Wuhan 430082, Hubei, Peoples R China.
摘要：
Graphdiyne (GDY)-based materials, owing to their unique structure and tunable electronic properties, exhibit great potential in the fields of catalysis, energy, environmental science, and beyond. In particular, GDY/metal oxide hybrid materials (GDY/MOs) have attracted extensive attention in energy and environmental catalysis. The interaction between GDY and metal oxides can increase the number of intrinsic active sites, facilitate charge transfer, and regulate the adsorption and desorption of intermediate species. In this review, we summarize the structure, synthesis, advanced characterization, small molecule activation mechanism and applications of GDY/MOs in energy conversion and environmental remediation. The intrinsic structure-activity relationship and corresponding reaction mechanism are highlighted. In particular, the activation mechanisms of reactant molecules (H2O, O2, N2, etc.) on GDY/MOs are systemically discussed. Finally, we outline some new perspectives of opportunities and challenges in developing GDY/MOs for efficient energy and environmental catalysis. This review summarizes the structure, synthesis, advanced characterization, structure-activity relationship, and mechanisms of graphdiyne/metal oxide hybrid materials in efficient energy and environmental catalysis.
期刊：
Proceedings of the National Academy of Sciences of the United States of America,2024年121(14):e2318391121 ISSN：0027-8424
作者机构：
[Ye, Yu-Yuan; Xiao, Ju; Wang, Xiao-Qiang; Li, Wen-Zhen; Wang, Zi-Xin] Interdisciplinary Institute of NMR and Molecular Sciences, Key Laboratory of Coal Conversion and New Carbon Materials of Hubei Province, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, China;[Liu, Ling-Ran; Sun, Yan] Key Laboratory for Special Functional Materials of Ministry of Education, School of Materials Science and Engineering, Collaborative Innovation Center of Nano Functional Materials and Applications, Henan University, Zhengzhou 450046, China;[Zhu, Mai-Yong; Liu, Ling-Ran] Research School of Polymeric Materials, School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, China;[Wang, Xin-Qiong] Department of Paediatrics, Ruijin Hospital, School of Medicine, Shanghai Jiao Tong University, Shanghai 200240, China;[Sun, Yao] Key Laboratory of Pesticides and Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China
摘要：
The exploitation of novel wound healing methods with real-time infection sensing and high spatiotemporal precision is highly important for human health. Pt-based metal-organic cycles/cages (MOCs) have been employed as multifunctional antibacterial agents due to their superior Pt-related therapeutic efficiency, various functional subunits and specific geometries. However, how to rationally apply these nanoscale MOCs on the macroscale with controllable therapeutic output is still challenging. Here, a centimeter-scale Pt MOC film was constructed via multistage assembly and subsequently coated on a N,N'-dimethylated dipyridinium thiazolo[5,4-d]thiazole (MPT)-stained silk fabric to form a smart wound dressing for bacterial sensing and wound healing. The MPT on silk fabric could be used to monitor wound infection in real-time through the bacteria-mediated reduction of MPT to its radical form via a color change. The MPT radical also exhibited an excellent photothermal effect under 660 nm light irradiation, which could not only be applied for photothermal therapy but also induce the disassembly of the Pt MOC film suprastructure. The highly ordered Pt MOC film suprastructure exhibited high biosafety, while it also showed improved antibacterial efficiency after thermally induced disassembly. In vitro and in vivo studies revealed that the combination of the Pt MOC film and MPT-stained silk can provide real-time information on wound infection for timely treatment through noninvasive techniques. This study paves the way for bacterial sensing and wound healing with centimeter-scale metal-organic materials.
