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Engineering hierarchical quaternary superstructure of an integrated MOF-derived electrode for boosting urea electrooxidation assisted water electrolysis

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Green Energy & Environment 2024年第4期9卷 695-701页

作者： Jianjun Tian Changsheng cao Yingchun He Muhammad Imran Khan xin-Tao Wu Qi-Long Zhu State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences(CAS)Fuzhou350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China University of Chinese Academy of Sciences Beijing100049China Research Institute of Sciences and Engineering(RISE) University of SharjahSharjah27272United Arab Emirates

Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical ***,a self-supported integrated electrode(NiCo-ZLDH/NF)with a unique hierarchical quaternary superstructure was fabricated through a self-sacrificing template strategy from the metal–organic framework(Co-ZIF-67)nanoplate arrays,which features an intriguing well-defined hierarchy when taking the unit cells of the NiCo-based layered double hydroxide(NiCo-LDH)as the primary structure,the ultrathin LDH nanoneedles as the secondary structure,the mesoscale hollow plates of the LDH nanoneedle arrays as the tertiary structure,and the macroscale three-dimensional frames of the plate arrays as the quaternary ***,the distinctive structure of NiCo-ZLDH/NF can not only accelerate both mass and charge transfer,but also expose plentiful accessible active sites with high intrinsic activity,endowing it with an excellent electrochemical performance for urea oxidation reaction(UOR).Specially,it only required the low potentials of 1.335,1.368 and 1.388 V to deliver the current densities of 10,100 and 200 mA cm^(-2),respectively,much superior to those for typical *** NiCo-ZLDH/NF as the bifunctional electrode for both anodic UOR and cathodic HER,an energy-saving electrolysis system was further explored which can greatly reduce the needed voltage of 213 mV to deliver the current density of 100 mA cm^(-2),as compared to the conventional water electrolysis system composed of *** work manifests that it is prospective to explore the hierarchically nanostructured electrodes and the innovative electrolytic technologies for high-efficiency electrocatalysis.

关键词： Hierarchical superstructures Metal–organic frameworks Layered double hydroxides Urea oxidation reaction Hydrogen evolution reaction

Effects of serum proteins on corrosion rates and product bioabsorbability of biodegradable metals

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Regenerative Biomaterials 2024年第1期3卷 132-148页

作者： Hongjie Zhang xin Li Zehua Qu Wanqian Zhang Qunsong Wang Dinglingge cao Yaoben Wang xin Wang Yang Wang Lin Yu Jiandong Ding State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

Corrodible metals are the newest kind of biodegradable materials and raise a new problem of the corrosion ***,the removal of the precipitated products has been unclear and even largely ignored in ***,we find that albumin,an abundant macromolecule in serum,enhances the solubility of corrosion products of iron in blood mimetic Hank’s solution *** is universal for other main biodegradable metals such as magnesium,zinc and polyester-coated *** also influences corrosion rates in diverse trends in Hank’s solution and normal *** on quantitative study theoretically and experimentally,both the effects on corrosion rates and soluble fractions are interpreted by a unified mechanism,and the key factor leading to different corrosion behaviors in corrosion media is the interference of albumin to the Ca/P passivation layer on the metal *** work has illustrated that the interactions between metals and media macromolecules should be taken into consideration in the design of the next-generation metal-based biodegradable medical devices in the formulism of precision *** improved Hank’s solution in the presence of albumin and with a higher content of initial calcium salt is suggested to access biodegradable metals potentially for cardiovascular medical devices,where the content of calcium salt is calculated after consideration of chelating of calcium ions by albumin,resulting in the physiological concentration of free calcium ions.

关键词： biodegradable metal macromolecule albumin corrosion bioabsorbability iron polylactide magnesium zinc

Slow magnetic relaxation behaviors and diamagnetic dilution studies of a carboxyl bridged dinuclear dysprosium(Ⅲ) complex

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Journal of Rare Earths 2024年第11期42卷 2088-2096页

作者： Wenting Liu Yibo Qiu Weiqin Xu Manli cao xin Deng Weiquan Lin School of Chemistry and Materials Science Guangdong University of Education School of Chemistry and Chemical Engineering/Institute of Clean Energy and Materials Guangzhou University

By using a rigid bulky carboxylic ligand a-cyanocinnamic acid（CCA）,a dinuclear dysprosium（Ⅲ） complex [Dy2（CCA）6（MeOH）4]（1） was *** crystal X-ray crystallography reveals that the two eight-coordinate dysprosium ions are bridged by four deprotonated carboxyl groups,forming a centrosymmetric paddle-wheel-1ike *** magnetic property measurements indicate that complex 1 displays field-induced slow magnetic *** temperature-dependent relaxation times can be fitted using Orbach and Raman processes with parameters of n=2.8（2）,C=27（8） s-1/K~n,τ0=5（2） × 10-10s and Ueff=40（3） *** studies on the diamagnetic YⅢ-diluted analogue[Dy0.206Y1.794（CCA）6（MeOH）4]（2） reveal its slow magnetic relaxation behavior without external dc field and the antiferromagnetic coupling between the DyⅢions in *** on the obtained relaxation times of 2lead to the parameters of n=4.5（3）,C=0.7（2） s-1/K~n,τ0=2.8（2） × 10-9s and Ueff=38（2） *** results suggest that slow magnetic relaxation originates from the single-ion relaxation of DyⅢ***,the diamagnetic dilution can suppress other fast relaxation pathways at low temperature,on account of the elimination of magnetic coupling and dipolar *** initio calculations were then performed on the single DyⅢion species {YDy} and indicate that the first excited Kramers doublets（KDs）lie at ca.76 cm-1,which is slightly higher than the experimental *** intramolecular magnetic interactions were also calculated and indicate a weak ferromagnetic dipole-diploe magnetic interaction and an antiferromagnetic exchange coupling.

关键词： Diamagnetic dilution Dilanthanide complexes Rare earths Single-molecule magnets

Evolutionary Neural Architecture Search and Its Applications in Healthcare

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Computer Modeling in Engineering & Sciences 2024年第4期139卷 143-185页

作者： xin Liu Jie Li Jianwei Zhao Bin cao Rongge Yan Zhihan Lyu School of Economics and Management Hebei University of TechnologyTianjin300401China School of Artificial Intelligence Hebei University of TechnologyTianjin300401China School of Electrical Engineering Hebei University of TechnologyTianjin300401China Department of Game Design Uppsala UniversityUppsalaS-75105Sweden

Most of the neural network architectures are based on human experience,which requires a long and tedious trial-and-error *** architecture search(NAS)attempts to detect effective architectures without human *** algorithms(EAs)for NAS can find better solutions than human-designed architectures by exploring a large search space for possible *** multiobjective EAs for NAS,optimal neural architectures that meet various performance criteria can be explored and discovered ***,hardware-accelerated NAS methods can improve the efficiency of the *** existing reviews have mainly focused on different strategies to complete NAS,a few studies have explored the use of EAs for *** this paper,we summarize and explore the use of EAs for NAS,as well as large-scale multiobjective optimization strategies and hardware-accelerated NAS *** performs well in healthcare applications,such as medical image analysis,classification of disease diagnosis,and health *** for NAS can automate the search process and optimize multiple objectives simultaneously in a given healthcare *** neural network has been successfully used in healthcare,but it lacks *** data is highly sensitive,and privacy leaks are frequently reported in the healthcare *** solve these problems,in healthcare,we propose an interpretable neuroevolution framework based on federated learning to address search efficiency and privacy ***,we also point out future research directions for evolutionary ***,for researchers who want to use EAs to optimize NNs in healthcare,we analyze the advantages and disadvantages of doing so to provide detailed guidance,and propose an interpretable privacy-preserving framework for healthcare applications.

关键词： Neural architecture search evolutionary computation large-scale multiobjective optimization distributed parallelism healthcare

Strongly Coupled Ag/Sn-SnO_(2)Nanosheets Toward CO_(2)Electroreduction to Pure HCOOH Solutions at Ampere‑Level Current

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Nano-Micro Letters 2024年第3期16卷 212-226页

作者： Min Zhang Aihui cao Yucui xiang Chaogang Ban Guang Han Junjie Ding Li‑Yong Gan Xiaoyuan Zhou College of Physics and Center of Quantum Materials and Devices Chongqing UniversityChongqing 401331People’s Republic of China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences(CAS)Fuzhou 350002People’s Republic of China College of Materials Science and Engineering Chongqing UniversityChongqing 400044People’s Republic of China Institute of New Energy Storage Materials and Equipment Chongqing 401135People’s Republic of China State Key Laboratory of Coal Mine Disaster Dynamics and Control Chongqing UniversityChongqing 400044People’s Republic of China

Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance ***,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible *** a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to ***,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 *** work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2).

关键词： Electrochemical CO_(2)reduction Coupled Ag/Sn-SnO_(2)nanosheets Electronic structure Porous solid electrolyte Pure

A comprehensive analysis of DAC-SDC FPGA low power object detection challenge

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Science China(Information Sciences) 2024年第8期67卷 300-320页

作者： Jingwei ZHANG Guoqing LI Meng ZHANG xinye cao Yu ZHANG xiang LI Ziyang CHEN Jun YANG School of Electronics Science and Engineering Southeast University

The lower power object detection challenge(LPODC) at the IEEE/ACM Design Automation Conference is a premier contest in low-power object detection and algorithm(software)-hardware co-design for edge artificial intelligence, which has been a success in the past five years. LPODC focused on designing and implementing novel algorithms on the edge platform for object detection in images taken from unmanned aerial vehicles(UAVs), which attracted hundreds of teams from dozens of countries to participate. Our team SEUer has been participating in this competition for three consecutive years from 2020 to 2022 and obtained sixth place respectively in 2020 and 2021. Recently, we achieved the championship in 2022. In this paper, we presented the LPODC for UAV object detection from 2018 to 2022, including the dataset, hardware platform,and evaluation method. In addition, we also introduced and discussed the details of methods proposed by each year's top three teams from 2018 to 2022 in terms of network, accuracy, quantization method, hardware performance, and total score. Additionally, we conducted an in-depth analysis of the selected entries and results, along with summarizing representative methodologies. This analysis serves as a valuable practical resource for researchers and engineers in deploying the UAV application on edge platforms and enhancing its feasibility and reliability. According to the analysis and discussion, it becomes evident that the adoption of a hardware-algorithm co-design approach is paramount in the context of tiny machine learning(TinyML).This approach surpasses the mere optimization of software and hardware as separate entities, proving to be essential for achieving optimal performance and efficiency in TinyML applications.

关键词： tiny machine learning object detection convolutional neural networks algorithm-hardware co-design low power field programmable gate array

Triggering triplet excitons of carbon nanodots through nanospace domain confinement for multicolor phosphorescence in aqueous solution

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Nano Research 2024年第7期17卷 6534-6543页

作者： Ya-Chuan Liang Qing cao Yuan Deng Yong Wang Kai-Kai Liu Chong-xin Shan School of Electronics and Information Zhengzhou University of Light IndustryZhengzhou 450002China Henan Key Laboratory of Diamond Optoelectronic Material and Devices Key Laboratory of Material PhysicsMinistry of EducationSchool of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450001China Academy for Quantum Science and Technology Zhengzhou University of Light IndustryZhengzhou 450002China Institute of Quantum Materials and Physics Henan Academy of SciencesZhengzhou 450046China

Easy non-radiative decay property of long-lived triplet excitons in aqueous solution obstructs their applications in aquatic *** reported phosphorescence phenomena in aqueous solution have excited researchers enormously but achieving full-color water-soluble phosphorescent carbon nanodots(CNDs)is still a challenging ***,full-color phosphorescence of water-soluble CNDs has been demonstrated by triggering their triplet excitons through nanospace domain confinement,and Förster energy resonance transfer is used for further tuning phosphorescence *** phosphorescence spans across most of the visible spectrum,ranging from 400 to 700 *** an aqueous solution,the CNDs exhibits blue,green,and red phosphorescence,lasting for approximately 6,10,and 7 s,***,the phosphorescence quantum yields are 11.85%,8.6%and 3.56%,making them readily discernible to the naked eyes and laying a solid foundation for practical ***,phosphorescence flexible optical display and bioimaging have been demonstrated by using the multicolor CNDs-based nanomaterials,showing distinct superiority for accuracy and complete display and imaging in complex emission background.

关键词： carbon nanodots triplet excitons multicolor aqueous solution

Detecting compromised email accounts via login behavior characterization

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Cybersecurity 2024年第1期7卷 16-36页

作者： Jianjun Zhao Can Yang Di Wu Yaqin cao Yuling Liu xiang Cui Qixu Liu Institute of Information Engineering Chinese Academy of SciencesBeijing100085China School of Cyber Security University of Chinese Academy of SciencesBeijing100049China China Cybersecurity Review Technology and Certification Center Beijing100013China Zhongguancun Laboratory Beijing100089China

The illegal use of compromised email accounts by adversaries can have severe consequences for enterprises and *** compromised email accounts is more challenging than in the social network field,where email accounts have only a few interaction events(sending and receiving).To address the issue of insufficient features,we propose a novel approach to detecting compromised accounts by combining time zone differences and alternate logins to identify abnormal *** on this approach,we propose a compromised email account detection framework that relies on widely available and less sensitive login logs and does not require *** framework characterizes login behaviors to identify logins that do not belong to the account owner and outputs a list of account-subnet pairs ranked by their likelihood of having abnormal login *** approach reduces the number of account-subnet pairs that need to be investigated and provides a reference for investigation *** evaluation demonstrates that our method can detect most email accounts that have been accessed by disclosed malicious IP addresses and outperforms similar ***,our framework has the capability to uncover undisclosed malicious IP addresses.

关键词： Compromised account detection Mixture model Login log analysis Attribution and forensic

Selective CO_(2)Electroreduction to Multi-Carbon Products on Organic-Functionalized CuO Nanoparticles by Local Micro-Environment Modulation

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Nano-Micro Letters 2024年第12期16卷 120-132页

作者： Shan Ren Xi cao Qikui Fan Zhimao Yang Fei Wang xin Wang Licheng Bai Jian Yang Materials Interfaces Center Shenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055GuangdongPeople’s Republic of China Key Laboratory of Functional Molecular Solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002AnhuiPeople’s Republic of China School of Physics Xi’an Jiaotong UniversityXi’an 710049ShaanxiPeople’s Republic of China College of Materials Science and Engineering Shenzhen UniversityShenzhen 518071GuangdongPeople’s Republic of China

Surface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO_(2)reduction reaction(CO_(2)RR)toward multi-carbon(C2+)products,primarily by suppressing the parasitic hydrogen evolution reaction and facilitating a localized CO_(2)/CO concentration at the *** upon this approach,we developed surface-functionalized catalysts with exceptional activity and selectivity for electrocatalytic CO_(2)RR to C_(2+)in a neutral *** CuO nanoparticles coated with hexaethynylbenzene organic molecules(HEB-CuO NPs),a remarkable C_(2+)Faradaic efficiency of nearly 90%was achieved at an unprecedented current density of 300 mA cm^(-2),and a high FE(>80%)was maintained at a wide range of current densities(100-600 mA cm^(-2))in neutral environments using a flow ***,in a membrane electrode assembly(MEA)electrolyzer,86.14%FEC2+was achieved at a partial current density of 387.6 mA cm^(-2)while maintaining continuous operation for over 50 h at a current density of 200 mA cm^(-2).In-situ spectroscopy studies and molecular dynamics simulations reveal that reducing the coverage of coordinated K⋅H2O water increased the probability of intermediate reactants(CO)interacting with the surface,thereby promoting efficient C-C coupling and enhancing the yield of C_(2+)*** advancement offers significant potential for optimizing local micro-environments for sustainable and highly efficient C_(2+)production.

关键词： CO_(2)electroreduction to C_(2+) Neutral electrolyte Organic-functionalized CuO nanoparticles Local micro-environment