作者机构:
[Zhu, Chengzhou; Fang, Qie; Wei, Xiaoqian; Zhu, CZ; Ling, Ling] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol &, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.;[Asahi, Toru; Zhao, Yingji; Wei, Xiaoqian] Waseda Univ, Fac Sci & Engn, Tokyo 1698555, Japan.;[Yamauchi, Yusuke; Zhao, Yingji; Wei, Xiaoqian] Nagoya Univ, Grad Sch Engn, Dept Mat Proc Engn, Nagoya, Aichi 4648603, Japan.;[Song, Weiyu; Song, Shaojia] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China.;[Cai, Weiwei] China Univ Geosci, Fac Mat Sci & Chem, Energy Lab, Wuhan 430074, Peoples R China.
通讯机构:
[Yamauchi, Y ] N;[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.;Nagoya Univ, Grad Sch Engn, Dept Mat Proc Engn, Nagoya, Aichi 4648603, Japan.;Univ Queensland, Australian Inst Bioengn & Nanotechnol AIBN, Brisbane, Qld 4072, Australia.
关键词:
Mn single atoms;Pt nanoparticles;atomic pairs;oxygen reduction reactions;synergistic effects
摘要:
The intrinsic roadblocks for designing promising Pt-based oxygen reduction reaction (ORR) catalysts emanate from the strong scaling relationship and activity-stability-cost trade-offs. Here, a carbon-supported Pt nanoparticle and a Mn single atom (Pt(NP)-Mn(SA)/C) as in situ constructed Pt(NP)-Mn(SA) pairs are demonstrated to be an efficient catalyst to circumvent the above seesaws with only ∼4 wt % Pt loadings. Experimental and theoretical investigations suggest that Mn(SA) functions not only as the "assist" for Pt sites to cooperatively facilitate the dissociation of O(2) due to the strong electronic polarization, affording the dissociative pathway with reduced H(2)O(2) production, but also as an electronic structure "modulator" to downshift the d-band center of Pt sites, alleviating the overbinding of oxygen-containing intermediates. More importantly, Mn(SA) also serves as a "stabilizer" to endow Pt(NP)-Mn(SA)/C with excellent structural stability and low Fenton-like reactivity, resisting the fast demetalation of metal sites. As a result, Pt(NPs)-Mn(SA)/C shows promising ORR performance with a half-wave potential of 0.93 V vs reversible hydrogen electrode and a high mass activity of 1.77 A/mg(Pt) at 0.9 V in acid media, which is 19 times higher than that of commercial Pt/C and only declines by 5% after 80,000 potential cycles. Specifically, Pt(NPs)-Mn(SA)/C reaches a power density of 1214 mW/cm(2) at 2.87 A/cm(2) in an H(2)-O(2) fuel cell.
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.
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.
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.
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.
作者机构:
[Duan, Gui-Yun; Li, Hong-Shuang; Zhao, Jun; Tian, Kai-Qiang] Shandong First Med Univ & Shandong Acad Med Sci, Natl Key Lab Adv Drug Delivery & Release Syst, Sch Pharmaceut Sci, Jinan 250117, Peoples R China.;[Duan, Gui-Yun; Li, Hong-Shuang; Zhao, Jun; Tian, Kai-Qiang] Shandong First Med Univ & Shandong Acad Med Sci, Inst Mat Med, Jinan 250117, Peoples R China.;[Zhang, Shi-Jiao] Qingdao Univ, Pharm Intravenous Admixture Serv, Affiliated Taian City Cent Hosp, Tai An 271000, Peoples R China.;[Cui, Guo-Hao; Guo, R; Wang, Qiao-Ling; Guo, Rui] Cent China Normal Univ CCNU, Int Joint Res Ctr Intelligent Biosensing Technol &, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol,Minist Educ,Coll Ch, Wuhan 430079, Peoples R China.
通讯机构:
[Guo, R ] C;[Li, HS ] S;Shandong First Med Univ & Shandong Acad Med Sci, Natl Key Lab Adv Drug Delivery & Release Syst, Sch Pharmaceut Sci, Jinan 250117, Peoples R China.;Shandong First Med Univ & Shandong Acad Med Sci, Inst Mat Med, Jinan 250117, Peoples R China.;Cent China Normal Univ CCNU, Int Joint Res Ctr Intelligent Biosensing Technol &, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol,Minist Educ,Coll Ch, Wuhan 430079, Peoples R China.
摘要:
The regio- and diastereoselective alkene isomerization and hydrofunctionalization sequence enabled by transition-metal complexes allows rapid activation and assembly of the C-(sp(3))-H bond that is either adjacent or distal to the initial double bond, which has been a longstanding challenge in this field. Herein, we develop unusual rhodium-catalyzed isomerization of alkylidenecyclobutanes with subsequent hydroacylation reaction to provide multisubstituted cyclobutanes with continuous stereocenters. Note that this tandem process features a good regio- and diastereoselectivity profile. Isotopic labeling experiments support the "exo to endo" migration of the double bond to a coordinated cyclobutene that is responsible for the deuterium incorporation observed in the cyclobutane product.
摘要:
Porous nanosheet can enhance the adsorption performance and light-harvesting ability of the photocatalyst due to the enlarged surface area and improved multi-reflection of the incident light between nanosheets. In this work, porous TiO2 nanosheets (TiO2-NSs) assembly was obtained by transformation TiO2 nanocubes in NaOH solution via hydrothermal reaction and followed by acid wash and heat treatment. The effect of reaction time (t) -dependent on photocatalytic activity of the obtained TiO2-NSs (St sample) was systematically investigated. It was found that TiO2-NSs exhibits superior catalytic activity for X3B dye degradation and NO oxidation when compared to pristine TiO2 nanocubes (S0 sample). The optimized photoreactivity of TiO2-NSs improved 8.1 and 5.0 times for X3B degradation (S1.5 sample) and NO oxidation (S3.0 sample), respectively. The enhanced photoreactivity of TiO2-NSs assembly is ascribed to the combined effects of enlarged surface area and unique structure of nanosheets assembly which facilitates the absorption of incident light. Both hydroxyl radicals and superoxide radicals are important reactive oxygen species (ROSs) responsible for the degradation of organic dye and NO oxidation. The present study provides a novel way to prepare high efficient semiconductor photocatalyst for water treatment and air purification.
摘要:
Direct aminolysis of selenoester in aqueous media was investigated as a glycopeptide ligation strategy. This strategy allows the peptide and glycopeptide ligation to proceed smoothly (even with hindered amino acids) without the need of cysteine residue, N-terminal thiol auxiliary or coupling additive, and to afford the corresponding amide products in excellent yields. No epimerization was observed during ligation reations. In this work, the selenoester of unprotected glycopeptide was readily prepared, and the direct aminolysis of glycopeptide selenoester was successfully applied to synthesize MUC1 mucin sequence efficiently.
摘要:
Peptide-based probes play prominent roles in biomedical research due to their promising properties such as high biocompatibility, fast excretion, favorable pharmacokinetics as well as easy and robust preparation. Considering the translation of imaging probes into clinical applications, peptide-based probes remain to be the most desirable and optimal candidates. This review summarized the development of peptide-based probes with promising imaging modalities and highlighted the successful applications for in vivo biomedical imaging.
摘要:
A simple and convenient method for N-aminosulfonamide synthesis from the cross-coupling of aryldiazonium tetrafluoroborates and rongalite under metal-free, oxidant-free, and room-temperature conditions is reported. This method does not require an external amine source, with the aryldiazonium tetrafluoroborates participating as both an aryl radical and a potential amine source in the transformation. Mechanistic studies revealed that rongalite could act as a radical initiator, a sulfur dioxide surrogate and a reducing reagent simultaneously in this reaction.
作者机构:
[Liu, Yan; Lin, Xuan; Li, Kenli; Quan, Zhe] Hunan Univ, Coll Informat Sci & Engn, Changsha, Hunan, Peoples R China.;[Wang, Zhi-Jie] Sun Yat Sen Univ, Sch Data & Comp Sci, Guangzhou, Guangdong, Peoples R China.;[Wang, Zhi-Jie] Guangdong Key Lab Big Data Anal & Proc, Guangzhou, Guangdong, Peoples R China.;[Wang, Zhi-Jie] Natl Engn Lab Big Data Anal & Applicat, Beijing, Peoples R China.;[Wang, Fan] Cent China Normal Univ, Coll Chem, Wuhan, Hubei, Peoples R China.
会议名称:
IEEE International Conference on Bioinformatics and Biomedicine (BIBM) - Human Genomics
会议时间:
DEC 03-06, 2018
会议地点:
Madrid, SPAIN
会议主办单位:
[Quan, Zhe;Lin, Xuan;Liu, Yan;Li, Kenli] Hunan Univ, Coll Informat Sci & Engn, Changsha, Hunan, Peoples R China.^[Wang, Zhi-Jie] Sun Yat Sen Univ, Sch Data & Comp Sci, Guangzhou, Guangdong, Peoples R China.^[Wang, Zhi-Jie] Guangdong Key Lab Big Data Anal & Proc, Guangzhou, Guangdong, Peoples R China.^[Wang, Zhi-Jie] Natl Engn Lab Big Data Anal & Applicat, Beijing, Peoples R China.^[Wang, Fan] Cent China Normal Univ, Coll Chem, Wuhan, Hubei, Peoples R China.
会议论文集名称:
IEEE International Conference on Bioinformatics and Biomedicine-BIBM
关键词:
machine learning;drug discovery;neural networks;molecule data
摘要:
In recent years, researchers in the fields of bioinformatics and cheminformatics have attempted to utilize machine learning methods for molecule modeling, bioactivity prediction, chemical property prediction, biology analysis, etc. In this paper, we present a system that merges the merits of various techniques such as long short-term memory (LSTM) recurrent neural networks, and is designed for learning atoms and solving the classic problems such as single task classification in the field of drug discovery. We have implemented our approach and conducted extensive experiments based on several widely used datasets such as SIDER and Tox21. The experimental results consistently demonstrate the feasibility and superiority of our proposed approach.
作者:
Cao, Yu;Luo, Shiying;Zhang, Yuannian;Xie, Xuan;Mukerabigwi, Jean Felix;...
期刊:
Journal of Controlled Release,2017年259:E178-E178 ISSN:0168-3659
通讯作者:
Yu Cao
作者机构:
[Su, Ping; Xiao, Wang; Luo, Shiying; Zhang, Yuannian; Mukerabigwi, Jean Felix; Cao, Yu; Xie, Xuan; Huang, Xueying] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Yu Cao] K;Key Laboratory of Pesticide and Chemical Biology (Ministry of Education), College of Chemistry, Central China Normal University, Wuhan 430079, China
会议名称:
4th Symposium on Innovative Polymers for Controlled Delivery (SIPCD)
摘要:
Immunoassay is a common analytic method with great practicability. Recently, there is a growing interest in applying graphene to modern biosensor research due to its distinct physical and chemical properties, such as excellent conductivity, high surface area, ease of functionalization, and so on. In this review, we summarized the recent researches on the development of electrochemical immunoassays based on graphene. We focus on the different roles of graphene in constructing various electrochemical immunosensors and provide a perspective about this research field.