摘要：
The existing source cell-phone recognition method lacks the long-term feature characterization of the source device, resulting in an inaccurate representation of the source cell-phone related features, which leads to insufficient recognition accuracy. In this paper, we propose a source cell-phone recognition method based on spatio-temporal representation learning, which includes two main parts: extraction of sequential Gaussian mean matrix features and construction of a recognition model based on spatio-temporal representation learning. In the feature extraction part, based on the analysis of the time-series representation of recording source signals, we extract sequential Gaussian mean matrix with long-term and short-term representation ability by using the sensitivity of Gaussian mixture model to data distribution. In the model construction part, we design a structured spatio-temporal representation learning network C3D-BiLSTM to fully characterize the spatio-temporal information, combine 3D convolutional network and bidirectional long short-term memory network for short-term spectral information and long-time fluctuation information representation learning, and achieve accurate recognition of cell-phones by fusing spatio-temporal feature information of recording source signals. The method achieves an average accuracy of 99.03% for the closed-set recognition of 45 cell-phones under the CCNU_Mobile dataset and 98.18% in small sample size experiments, with recognition performance better than the existing state-of-the-art methods. The experimental results show that the method exhibits excellent recognition performance in multi-class cell-phones recognition. Our codes are available at https://github.com/CCNUZFW/STRLESCR-SGMM .
摘要：
Electronic portfolios are crucial means to evaluate the performance of students. However, the traditional student e-portfolio(SEP) system cannot meet the needs of guaranteeing students' information safety due to the system using centralized third-party storage. In addition, the SEP system involves multiple stakeholders and has an extreme volume of learning data, while the current access control model fails to satisfy the requirements of the SEP system. Blockchain technology provides a possible solution to the issues, while the massive data stored in the blockchain can cause congestion in the blockchain network. Therefore, we propose StuChain, an efficient blockchain-based SEP platform integrating a hybrid access control approach, to solve the above problems. Firstly, we design a hybrid access control model to manage and share student e-portfolio. Secondly, we propose to use blockchain technology to solve the security issue and design smart contracts to realize identity certification, recording, access control management, and sharing. Thirdly, we present an efficient storage approach, which achieves massive storage without threatening the system's efficiency. The student e-portfolio information is encrypted through the symmetric encryption scheme(AES-128), signed through the Edwards-curve digital signature algorithm (EdDSA), and recorded in the off-chain. We store the corresponding storage address and hash values in the blockchain. Finally, we conduct theoretical analysis and extensive experiments. Theoretical analysis demonstrates that our proposed approach outperforms other schemes. Experimental results show that our proposed StuChain can achieve secure and efficient storage, fine-grained access control, and our proposed system maintains high throughput.
期刊：
Science of The Total Environment,2024年908:167878 ISSN：0048-9697
通讯作者：
Hao, GF
作者机构：
[Zhao, Wei; Zhang, Xiao; Hao, Ge-Fei; Gao, Yang-Yang; Huang, Yuan-Qin; Kumar, Vinit] Guizhou Univ, Ctr Res & Dev Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang 550025, Peoples R China.;[Hao, Ge-Fei] Cent China Normal Univ, Natl Key Lab Green Pesticide, Wuhan 430079, Peoples R China.
通讯机构：
[Hao, GF ] G;Guizhou Univ, Ctr Res & Dev Fine Chem, Natl Key Lab Green Pesticide, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang 550025, Peoples R China.
摘要：
Pesticides are indispensable to maintain crop quality and food production worldwide, but their use also poses environmental risks. Pesticide risk assessment involves a series of complex, expensive and time-consuming toxicity tests. To improve the efficiency and accuracy for assessing the environmental impact of pesticides, numerous computational tools have been developed. However, there is a notable deficiency in critical analysis or a systematic summary of environmental risk assessment tools and their applicable contexts. Here, many of the current approaches and tools for assessing environmental risks posed by pesticides are reviewed, and the question of whether these tools are fit for use on complex multicomponent scenarios is discussed. We analyze the adaptations of these tools to aquatic and terrestrial ecosystems, followed by the provision of resources for predicting pesticide concentrations in environmental medias, including air, soil and water. The successful application of computational tools for risk assessment and interpretation of predicted results will also be discussed. This assessment serves as a valuable resource, enabling scientists to utilize suitable models to enhance the robustness of pesticides risk assessments.
关键词：
Antibiotic alternatives;Antibiotic resistance genes;Layer feces;Microbiome;Mobile genetic elements
摘要：
Although antibiotic alternatives are widely used in livestock and poultry breeding industry after in-feed antibiotics ban, their intervention effects on antibiotic resistance genes (ARGs) in these food animals' feces remain poorly understood. Here effects of fructooligosaccharide (FOS) and astragalus polysaccharide (APS), as typical antibiotic alternatives in China, on ARGs in layer feces were estimated by performing metagenomic sequencings and fluorescence quantitative PCR. Fructooligosaccharide significantly reduced sum abundance of ARGs and mobile genetic elements (MGEs) by increasing Lactobacillus clones and reducing Escherichia clones which had relatively higher abundances of ARG subtypes and MGE subtypes in layer feces. However, at least parts of core ARGs and MGEs categories were not reduced by FOS, such as aminoglycosides- and tetracyclines-resistant genes, Tn916, Integrase, and so on. MGEs and microbiome, especially Escherichia genus and Lactobacillus genus, were the key factors affecting ARGs' sum abundance. MGEs had a higher correlation coefficient with ARGs' sum abundance than Escherichia genus and Lactobacillus genus. These findings firstly reveal the defects of antibiotic alternatives in controlling bacterial resistance in livestock and poultry breeding after in-feed antibiotics ban, and more strategies are needed to control pollutions and risks of core ARGs and MGEs in food animals' feces under a special environment.
摘要：
Stochastic resonance and energy consumption are significant for information processing and transmission in the neural system. In this paper, we constructed an excitatory–inhibitory cortical neuronal network to investigate the response of the system to weak signals and the corresponding energy consumption. The findings indicate that the excitability of neurons modulates the performance of signal response. Furthermore, the performance of signal response exhibits a bell-shaped dependence on ion channel noise, which is a typical manifestation of the stochastic resonance phenomenon. Stochastic resonance also exists in the network with increasing noise at different excitatory coupling strengths and inhibitory coupling strengths. Furthermore, it is found that the neuronal system obtains optimal transmission of the weak signal at a lower energy consumption. It illustrates that there is a certain economy and efficiency in the signal transmission. At weak inhibitory coupling strength, an optimal excitatory coupling strength exists to allow the neuronal network to make the optimal transmission of the weak signal. However, the phenomenon of double resonant peaks occurs at strong inhibitory coupling strength, which is due to the balance of excitatory and inhibitory synaptic currents. Finally, we demonstrated the robustness of the results to network topology and initial conditions. The results of this paper may contribute to the understanding of signal transmission and its energy consumption in cortical networks.
摘要：
Graphene-based nanomaterials (GBNs) consist of a single or few layers of graphene sheets or modified graphene including pristine graphene, graphene nanosheets (GNS), graphene oxide (GO), reduced graphene oxide (rGO), as well as graphene modified with various functional groups or chemicals (e.g., hydroxyl, carboxyl, and polyethylene glycol), which are frequently used in industrial and biomedical applications owing to their exceptional physicochemical properties. Given the widespread production and extensive application of GBNs, they can be disseminated in a wide range of environmental mediums, such as air, water, food, and soil. GBNs can enter the human body through various routes such as inhalation, ingestion, dermal penetration, injection, and implantation in biomedical applications, and the majority of GBNs tend to accumulate in the respiratory system. GBNs inhaled and substantially deposited in the human respiratory tract may impair lung defenses and clearance, resulting in the formation of granulomas and pulmonary fibrosis. However, the specific toxicity of the respiratory system caused by different GBNs, their influencing factors, and the underlying mechanisms remain relatively scarce. This review summarizes recent advances in the exposure, metabolism, toxicity and potential mechanisms, current limitations, and future perspectives of various GBNs in the respiratory system.
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.
期刊：
Journal of Materials Chemistry C,2024年 ISSN：2050-7526
通讯作者：
Tang, YW;Shi, Y
作者机构：
[Chen, Mingyue; Tang, Yiwen; Ran, Hongbing; Wu, Tong; Tang, YW] Cent China Normal Univ, Coll Phys Sci & Technol, Wuhan 430079, Peoples R China.;[Chen, Junfeng; Shi, Y; Shi, Yun; Zheng, Jiaqian; Li, Xiang] Chinese Acad Sci, Shanghai Inst Ceram, Shanghai 201899, Peoples R China.;[Chen, Junfeng; Shi, Y; Shi, Yun] Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China.;[Wu, Haodi] Huazhong Univ Sci & Technol, WNLO, Wuhan 430074, Peoples R China.;[Wu, Haodi] Huazhong Univ Sci & Technol, Sch Opt & Elect Informat, Wuhan 430074, Peoples R China.
通讯机构：
[Shi, Y ; Tang, YW ] C;Cent China Normal Univ, Coll Phys Sci & Technol, Wuhan 430079, Peoples R China.;Chinese Acad Sci, Shanghai Inst Ceram, Shanghai 201899, Peoples R China.;Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China.
摘要：
Ternary copper halides, such as Cs3Cu2I5, as an emerging class of nontoxic alternatives to lead halide perovskites, have drawn extensive attention in the X-ray detection field due to their efficient self-trapped exciton emissions. However, the light yield far below the theoretical limit seriously hinders the high-resolution X-ray detection application of copper halide scintillators. Herein, Cs3Cu2I5:K+ scintillation films and single crystals with enhanced photoluminescence (PL) and radiation luminescence (RL) were first obtained by adjusting the doping concentration of K+ ions in the 0-8 at% range. The substitution of Cs+ by doping K+ compacted the adjacent [Cu2I5](3-) dimer groups, resulting in a stronger exciton-photon coupling strength. Therefore, Cs3Cu2I5:K+ single crystals exhibited a stronger RL emission under X-ray excitation, and their light output was about 49.6% higher than that of the pure Cs3Cu2I5, with an accelerated scintillation decay time (330 to 241 ns). Benefiting from these advantages, X-ray detectors based on hydrophobic polymethyl methacrylate (PMMA)-coated Cs3Cu2I5:K+ flexible films could deliver a higher X-ray imaging resolution of 11.7 lp mm(-1)@MTF = 0.2 in comparison with the commercial gadolinium oxysulfide (GOS)-based detectors (6.2 lp mm(-1)@MTF = 0.2). This work provides insights for the design of metal halides for use in low-cost and high-resolution flexible X-ray imaging systems.
摘要：
Long-chain fatty acyl-CoAs (LCACoAs) are intermediates in lipid metabolism that exert a wide range of cellular functions. However, our knowledge about the subcellular distribution and regulatory impacts of LCACoAs is limited by a lack of methods for detecting LCACoAs in living cells and tissues. Here, we report our development of LACSerHR, a genetically encoded fluorescent biosensor that enables precise measurement of subtle fluctuations in the levels of endogenous LCACoAs in vivo. LACSerHR significantly improve the fluorescent brightness and analyte affinity, in vitro and in vivo testing showcased LACSerHR's large dynamic range. We demonstrate LACSerHR's capacity for real-time evaluation of LCACoA levels in specific subcellular compartments, for example in response to disruption of ACSL enzyme function in HEK293T cells. Moreover, we show the application of LACSerHR for sensitive measurement of elevated LCACoA levels in the livers of mouse models for two common metabolic diseases (NAFLD and type 2 diabetes). Thus, our LACSerHR sensor is a powerful, broadly applicable tool for studying LCACoAs metabolism and disease.
摘要：
Aspect-based sentiment analysis (ABSA), which aims to analyze users’ sentiment towards the targeted aspect, has recently gained increasing attention due to its importance in supporting corresponding decision-makings in various tasks. Most existing ABSA studies primarily depend on only textual modality, but ignore the fact that in many cases the targeted aspect doesn’t appear in the sentence. Thus, multimodal ABSA is expected to alleviate this dilemma. However, most existing MABSA approaches still suffer from the following limitations: (1) ignoring the possible aspect-image irrelevant issue; (2) ignoring the coarse-grained interaction between the sentence and its associated image; (3) failing to simultaneously leverage multiple types of useful knowledge information. To address these issues, we propose an aspect-guided multi-view interactions and fusion network (AMIFN) for MABSA. Specifically, we utilize the multi-head attention mechanism to generate aspect-guided textual representation, which is used as the extended aspect semantic for guiding the subsequent aspect-related interactions. When exploring aspect-guided visual representation, we employ the image gate to dynamically filter potential noise introduced by the associated image to generate the final image representation. Meanwhile, the coarse-grained sentence-image interaction, which contains context and semantics information, and the syntactic dependencies, are leveraged for graph construction to obtain aspect-guided text-image interaction representations. Finally, the extracted multi-view interaction representations are integrated for sentiment classification. Extensive experimental results on three multimodal benchmark datasets demonstrate the superiority and rationality of AMIFN.
作者机构：
[Zhang, Ze; Cui, Jianqun; Hsu, Chingfang; Zhao, Zhuo] Cent China Normal Univ, Comp Sch, Wuhan 430079, Peoples R China.;[Au, Man Ho] Hong Kong Polytech Univ, Dept Comp, Hong Kong 25809, Peoples R China.;[Harn, Lein] Univ Missouri Kansas City, Dept Comp Sci Elect Engn, Kansas City, MO 64110 USA.;[Xia, Zhe] Wuhan Univ Technol, Dept Comp Sci, Wuhan 430079, Peoples R China.
通讯机构：
[Hsu, CF ] C;Cent China Normal Univ, Comp Sch, Wuhan 430079, Peoples R China.
关键词：
Internet of Drones;Lightweight;Mutual authentication;Physical unclonable functions;UAVs;ROR;AVISPA
摘要：
In recent years, the industry and research have cast great attention to the Internet of Drones (IoD), which is becoming progressively popular since it can bring a great convenience to various application scenarios, such as national map exploration, public safety monitoring and automated military applications. In these scenarios, Unmanned Aerial Vehicles (UAVs) (called drones) will be used to collect private information. Due to the fact that the private information are very sensitive, and drones working in public places easily suffer from physical capture or tampering attacks, the primary concern is that this information could be collected by adversaries or unauthorized users. In addition, as resource-constrained devices, drones are mostly equipped with small memory and have limited computing power. Therefore, how to ensure robust security as much as possible while achieving lightweight computing and communication costs has become an urgent problem to be solved in this field. In this paper, we propose A PUF-based Robust and Lightweight Authentication Protocol for Drone-Gateway and Drone-Drone Communication (PRLAP-IoD) to address these issues. Both formal security validation using conventional tools (ROR Model and AVISPA) and other informal security analysis clearly demonstrate that PRLAP-IoD can not only provide physical security, but also defend against a variety of known attacks. Finally, compared with the recent Authentication and Key Agreement (AKA) schemes, PRLAP-IoD can attain a delicate balance between computation cost and communication cost in IoD environment.
摘要：
High-resolution remote-sensing-image change detection is widely used in urban dynamic monitoring, geographic information updating, natural disaster monitoring, illegal building investigation, and land resource surveys. Common change-detection algorithms are mainly implemented in a fully supervised manner that relies on a large number of high-quality samples. Compared with a building change-detection dataset, a building semantic-segmentation dataset is easier to accumulate and obtain. Making full use of this semantic information in the design of a building change-detection network can effectively reduce the sample size required to train a change-detection model. In view of this, a semantic feature-guided Siamese change-detection framework is devised in this letter. The framework effectively exploits the prior information of building semantic features and uses the popular transformer structure to improve the change analysis module. The results of extensive experiments on two public datasets show that the framework is more accurate than the other state-of-the-art change detection algorithms and can effectively reduce the dependence of data on change detection samples in the model training process.
作者：
Zhao, Long;Yang, Mao-Lin;Chen, Hao-Ran;Ding, Ming -Wu
期刊：
Tetrahedron,2024年152 ISSN：0040-4020
通讯作者：
Ding, MW
作者机构：
[Ding, MW; Yang, Mao-Lin; Ding, Ming -Wu; Chen, Hao-Ran; Zhao, Long] Cent China Normal Univ, Natl Key Lab Green Pesticide, Hubei Int Sci & Technol Cooperat Base Pesticide &, Wuhan 430079, Peoples R China.
通讯机构：
[Ding, MW ] C;Cent China Normal Univ, Natl Key Lab Green Pesticide, Hubei Int Sci & Technol Cooperat Base Pesticide &, Wuhan 430079, Peoples R China.
摘要：
A new efficient synthesis of polysubstituted benzo[d]pyrido[1 ',2':1,2]imidazo[4,5-f][1,3]diazepines and pyrido[2 ',1':2,3]imidazo[1,5-c]quinazolin-7-ium salts via sequential Groebke-Blackburn-Bienaym & eacute;/Staudinger/aza-Wittig/carbodiimide-mediated annulation has been developed. The three-component Groebke-Blackburn-Bienaym & eacute; reactions of 2-azidobenzaldehydes 1, isocyanides 2, and 2-aminopyridines 3 produced the azide intermediates 4, which were treated sequentially with triphenylphosphine and isocyanates to give polysubstituted benzo[d]pyrido[1 ',2':1,2]imidazo[4,5-f][1,3]diazepines and pyrido[2 ',1':2,3]imidazo[1,5-c]quinazolin-7-ium chlorides in good yields.
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：
Abstract 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.
摘要：
An asymmetric cascade cyclization of enynamides and alpha-diazoketones to produce chiral bicyclic lactams bearing chiral all-carbon quaternary stereocenters is realized with up to 95% yield, 98% ee, and >19:1 dr. The combination of visible light photoactivation and the relay of gold and N-oxide catalysis in a cascade process enabled the facile generation and controlled assembly of two reactive intermediates, ketene and aza-o-quinone methide. Theoretical calculations revealed a stepwise [4 + 2] cycloaddition mechanism, with the stereochemistry controlled by the amide group of the catalyst. Remarkably, this study presents the first example of chiral N-oxides serving as catalysts for asymmetric ketene cycloaddition and illustrates how a cascade strategy could be a promising means to access significant chiral heterocyclic scaffolds.
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：
Physica A-Statistical Mechanics and its Applications,2024年637:129533 ISSN：0378-4371
通讯作者：
Liu, FY
作者机构：
[Yang, Chunbin; Liu, Feiyi; Deng, Weibing; Li, Wei; Chen, Xiangna; Liu, FY] Cent China Normal Univ, Key Lab Quark & Lepton Phys MOE, Wuhan 430079, Peoples R China.;[Liu, Feiyi; Deng, Weibing; Li, Wei; Liu, FY] Cent China Normal Univ, Inst Particle Phys, Wuhan 430079, Peoples R China.;[Liu, Feiyi; Papp, Gabor; Liu, FY] Eotv Lorand Univ, Inst Phys, 1-A Pazmany P Setany, H-1117 Budapest, Hungary.;[Chen, Shiyang] Baoshan Univ, Sch Engn & Technol, Baoshan 678000, Peoples R China.;[Shen, Jianmin] Max Planck Inst Math Sci, D-04103 Leipzig, Germany.
通讯机构：
[Liu, FY ] C;Cent China Normal Univ, Key Lab Quark & Lepton Phys MOE, Wuhan 430079, Peoples R China.;Cent China Normal Univ, Inst Particle Phys, Wuhan 430079, Peoples R China.;Eotv Lorand Univ, Inst Phys, 1-A Pazmany P Setany, H-1117 Budapest, Hungary.
摘要：
Machine learning techniques exhibit significant performance in discriminating different phases of matter and provide a new avenue for studying phase transitions. We investigate the phase transitions of three dimensional q -state Potts model on cubic lattice by using a transfer learning approach, Domain Adversarial Neural Network (DANN). With the unique neural network architecture, it could evaluate the high -temperature (disordered) and low -temperature (ordered) phases, and identify the first and second order phase transitions. Meanwhile, by training the DANN with a few labeled configurations, the critical points for q = 2, 3, 4 and 5 can be predicted with high accuracy, which are consistent with those of the Monte Carlo simulations. These findings would promote us to learn and explore the properties of phase transitions in high -dimensional systems.
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. A copper-catalyzed thiocyanation of cyclobutanone oxime esters by potassium ammonium thiocyanate was achieved for the first time. Subsequent derivatization of thiocyano substituted alkylnitriles led to various sulfur-containing alkylnitriles.
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.
