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Electron and configuration engineering of atomic Cu and multioxidated Cu_(2+1)O centers via gasifiable reductant strategy for efficient oxygen reduction toward Zn-air battery

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Nano Research 2023年第2期16卷 2383-2391页

作者： Hongbin Li jia-jia zheng Mingfan Yang Jingui Duan State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China Laboratory of Theoretical and Computational Nanoscience National Center for Nanoscience and TechnologyChinese Academy of SciencesBeijing 100190China

Efforts in a large number of transition metal-carbon systems are devoted to the development of efficient catalysts for oxygen reduction reaction(ORR).However,unsatisfied O_(2)adsorption and slow reduction of OH*at the active centers hinder the further development of these *** here report a gasifiable reductant strategy,of which a new Cu-based metal organic framework(MOF:termed NTU-83)nanosheet was co-pyrolyzed with melamine to produce the N-coordinated atomic Cu and multi-oxidated Cu_(2+1)O active centers on the carbon foam with ultrathin *** engineered electrons and configuration of the active centers boost the catalyst(Cu/NC-1000)to show superior ORR activity(E_(1/2)=0.85 V),excellent stability,and methanol *** modeling calculation and controlled experiments reveal that the Cu_(2+1)O species play a crucial role in kinetically accelerated adsorption and activation of O_(2),while the N_(4)coordinated atomic Cu facilitates fast reduction of OH*.Such characteristics endow the Zn-air battery that containing Cu/NC-1000 as air cathode to show a high peak power density(138 mW·cm^(−2)),a high specific capacity of 763 mAh·gZn^(−1),and outstanding long-term cycle *** plausible mechanism and excellent performance show that gasifiable reductant strategy opens up a new route for regulation of the electronic of active sites but also provides a candidate for the practical application in energy conversion/storage devices.

关键词： metal organic framework nanosheet carbon foam atomic Cu Cu_(2+1)O nanosheet electron and configuration engineering

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Plasmonic nanostructures acting as a light-driven O_(2)-sensitive nitroreductase mimic for enhanced photochemical oxidation of para-aminothiophenol

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Nano Research 2023年第11期16卷 12697-12705页

作者： Xinshuang Gao jia-jia zheng Hanbo Li Rui Cai Xingfa Gao Xiaochun Wu CAS Key Laboratory of Standardization and Measurement for Nanotechnology National Center for Nanoscience and TechnologyBeijing 100190China Laboratory of Theoretical and Computational Nanoscience National Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Nanozymes,as a novel form of enzyme mimics,have garnered considerable *** overcoming the main disadvantages of their natural analogs,they still face challenges such as restricted mimic types and low substrate ***,we introduce a reactive ligand modification strategy to diversify enzyme mimic ***,we have utilized helical plasmonic nanorods(HPNRs)modified with para-nitrothiophenol(4-NTP)to create an oxygen-sensitive nitroreductase(NTR)with *** act as a light-adjustable source of nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate(NAD(P)H),providing photon-generated energetic electrons to adsorbed 4-NTP *** the presence of O_(2),the activated 4-NTP transfers the captured electron to the adsorbed O_(2),mimicking the electron transfer process in its natural *** enhanced O_(2)activation notably boosts the oxidative coupling of para-aminothiophenol(4-ATP).Density functional theory(DFT)calculations reveal that hot electrons injected into the lowest unoccupied molecular orbital(LUMO)energy level of 4-NTP can be transferred to that of molecular *** conclusion,our findings underline the potential of the reactive ligand modification strategy in developing new types of enzyme reactions,which opens up promising avenues for the enhancement and diversification of nanozyme functionalities.

关键词： plasmonic nanostructure nanozyme nitroreductase para-nitrothiolphenol hot electron injection para-aminothiolphenol

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Remote substituent effects on catalytic activity of metal-organic frameworks: a linker orbital energy model

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npj Computational Materials 2023年第1期9卷 1747-1755页

作者： Zhenzhen Wang Huan Meng Xuejiao J.Gao jia-jia zheng Xingfa Gao Laboratory of Theoretical and Computational Nanoscience National Center for Nanoscience and Technology of ChinaBeijingChina CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety National Center for Nanoscience and Technology of ChinaBeijingChina College of Chemistry and Chemical Engineering Jiangxi Normal UniversityNanchangChina

The Hammett equation is commonly used to theoretically depict the remote electronic effects of substituents on catalytic activitiesof metal nodes of metal-organic frameworks (MOFs). However, the application of the theory to MOF catalysts usually encountersproblems because it relies heavily on empirical parameters with unknown transferability. To develop an alternative predictiontheory, the linker orbital energy model has been proposed by density functional theory calculations. The model provides a simplemethod to approximately depict the remote electronic substituent effects on catalytic activities of metal nodes of MOFs, and itsgeneral applicability to MOFs is supported by extensively revisiting the structure-activity relationships reported in the *** model can be used to design catalytic activity of metal nodes of MOFs by engineering the electronic properties of linkers andsubstituents.

关键词： substituent catalytic orbital

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Growth of ZSM-5 crystals within hollow β-zeolite

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Chinese Chemical Letters 2011年第9期22卷 1103-1106页

作者： Qing Hu Zeng Xiang Bai jia Jun zheng jia Qi Chen Rui Feng Li Key Laboratory of Coal Science and Technology MOE Taiyuan University of Technology Taiyuan 030024 China

A zeolite composite composed of ZSM-5 and β-zeolites has been synthesized by a procedure of the nucleation and crystallization of ZSM-5 zeolite in the hollow β-zeolite. The property of β-zeolite crystals with aluminum-poor interior and aluminum-rich outer rim results in silicon extraction favorably in the aluminum-poor bulk rather than the aluminum-rich external surface. Subsequently, alkaline treatment offl-zeolite crystals during the second-step synthesis leads to a preferential dissolution of the aluminum-poor center and the formation of hollow β-zeolite crystals. ZSM-5 zeolite crystals are therefore embedded and grown within the hollow β-zeolite. The catalytic activities of Co-Hβ, Co-HZSM-5 and Co-HZSM-5/BEA are investigated during the reaction of methane catalytic reduction NO in the presence of O2.

关键词： ZSM-5 β-Zeolite Zeolite composite

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Distribution and drug resistance of pathogenic bacteria in emergency patients

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World Journal of Clinical Cases 2019年第20期7卷 3175-3184页

作者： Wei Huai Qing-Bian Ma jia-jia zheng Yang Zhao Qiang-Rong Zhai Emergency Department Third Clinical Medical CollegePeking UniversityBeijing 100191China Laboratory Department Third Clinical Medical CollegePeking UniversityBeijing 100191China

BACKGROUND Antibiotic resistance has become a global threat for human health,calling for rational use of *** To analyze the distribution and drug resistance of the bacteria,providing the prerequisite for use of antibiotics in emergency *** A total of 2048 emergency patients from 2013 to 2017 were *** clinical examination specimens were collected,followed by isolation of *** bacterial identification and drug susceptibility testing were carried *** A total of 3387 pathogens were *** top six pathogens were Acinetobacter baumannii(660 strains),Staphylococcus aureus(436 strains),Klebsiella pneumoniae(347 strains),Pseudomonas aeruginosa(338 strains),Escherichia coli(237 strains),and Candida albicans(207 strains).The isolation rates of these pathogens decreased year by year except Klebsiella pneumoniae,which increased from 7.1%to 12.1%.Acinetobacter baumannii is a widely-resistant strain,with multiple resistances to imipenem,ciprofloxacin,minocycline and *** Staphylococcus aureus had high resistance rates to levofloxacin,penicillin G,and *** the susceptibility of it to vancomycin and tigecycline were 100%.Klebsiella pneumoniae had high resistance rates to imipenem,cefoperazone/sulbactam,amikacin,and ciprofloxacin,with the lowest resistance rate to *** resistance rates of Pseudomonas aeruginosa to cefoperazone/sulbactam and imipenem were higher,with the resistance rate to amikacin below 10%.Besides,Escherichia coli had high resistance rates to ciprofloxacin and cefoperazone/sulbactam and low resistance rates to imipenem,amikacin,and *** The pathogenic bacteria isolated from the emergency patients were mainly Acinetobacter baumannii,Staphylococcus aureus,Klebsiella pneumoniae,Pseudomonas aeruginosa,Escherichia coli,and Candida *** detection rates of drugresistant bacteria were high,with different bacteria having multiple drug resistances to commonly

关键词： Distribution Drug resistance Bacteria Emergency department

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Boosting C_(2)H_(6)/C_(2)H_(4) separation via the precise electrostatic modulation of synthetic 1D channel at atomic level

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Nano Research 2024年第11期17卷 10083-10087页

作者： Salamanti Ainiwaner Hengcong Huang jia-jia zheng Fengting Li Xue-Tong Yang Yang-Yang Guo Fangli Yuan Ming-Shui Yao Yifan Gu College of Environmental Science and Engineering State Key Laboratory of Pollution Control and Resource Reuse Tongji University Shanghai 200092 China Laboratory of Theoretical and Computational Nanoscience National Center for Nanoscience and Technology Chinese Academy of Sciences Beijing 100190 China Skate Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China Chinese Academy of Sciences University of Chinese Academy of Sciences Beijing 100049 China

The regulation of gas sorption via simple pore modification is crucial to molecular recognition and chemical ***,a rational pore surface electrostatic modulation in synthetic one dimensioned(1-D)channel is demonstrated to boost ethane/ethylene(C_(2)H_(6)/C_(2)H_(4))selectivity for one-step extraction of C_(2)H_(4) from C_(2)H_(6)/C_(2)H_(4) *** the precise modulation of the surface charge arrangement with negatively charged moieties in the 1-D channel of a metal—organic framework(MOF),enhanced C_(2)H_(6)—host framework and decreased C_(2)H_(4)—host framework electrostatic interactions were obtained,which resulted in an obvious improvement in adsorption ***,the breakthrough separation performance rendered the obtained MOF an efficient adsorbent for C_(2)H_(4) purification from C_(2)H_(6)/C_(2)H_(4) *** combined detail theoretical studies prove that the gas sorption selectivity is remarkably sensitive to framework electrostatic change even in the case of pore surface modification at the atomic *** results are of fundamental importance to the design of porous materials for challenging separation tasks.

关键词： metal—organic framework ethane/ethylene separation ethane—selective MOF adsorption electrostatic modulation

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Enhanced carbon capture with motif-rich amino acid loaded defective robust metal-organic frameworks

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Nano Research 2024年第3期17卷 2004-2010页

作者： Qi-Ye Ju jia-jia zheng Li Xu Hai-Yan jiang Zi-Qian Xue Lu Bai Yang-Yang Guo Ming-Shui Yao Ting-Yu Zhu State Key Laboratory of Multi-phase Complex Systems CAS Key Laboratory of Green Process and EngineeringBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Laboratory of Theoretical and Computational Nanoscience National Center for Nanoscience and TechnologyChinese Academy of SciencesBeijing 100190China School of Rare Earths University of Science and Technology of ChinaHefei 230026China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China University of Chinese Academy of Sciences Chinese Academy of SciencesBeijing 100049China Institute for Integrated Cell-Material Sciences Kyoto UniversityInstitute for Advanced StudyKyoto UniversityYoshidaUshinomiya-choSakyokuKyoto 606-8501Japan

The use of metal-organic frameworks(MOFs)as solid adsorption materials for carbon capture is promising,but achieving efficient and reversible adsorption with a balance of capacity and selectivity for carbon dioxide(CO_(2))over N_(2) remains a *** take full advantage of the strong channel traffic and robustness of MOFs with relatively small pores,it is highly necessary to employ a defect-engineering strategy to construct a broader channel structure that can facilitate the loading of functional motif-rich amino acids(AAs).This strategy can greatly enhance the CO_(2) adsorption performance of *** this study,motif-rich amino acids are loaded into the defective and robust porous frameworks via combined defect-engineering and post-synthetic *** defective Zr/Hf-MOF-808s modified with AAs,especially for the 18 mol%4-nitroisophthalic acid,generated defective products allowing for the loading of L-serine(L-Ser).This modification resulted in a significant improvement in both the adsorption capacity(248%improvement at 298 K,100 kPa)and the selectivity of CO_(2)/N_(2) using the ideal adsorbed solution theory(IAST),with the selectivity increasing to 120.55 and 38.27 at 15 and 100 kPa,respectively,while maintaining good cycling *** functional theory(DFT)simulation,CO_(2) temperature-programmed desorption(CO_(2)-TPD),and in situ Fourier transform infrared spectroscopy(FTIR)were further employed to have a better understanding of the enhanced CO_(2) adsorption ***,unlike the AAs loaded pristine MOF-808s that showed the best CO_(2) adsorption capacity with the loading of short and small glycine(Gly),the broadened channel size in our work enables the loading of functional motif-rich L-serine,which brings more active binding sites,improving CO_(2) adsorption.

关键词： carbon capture and storage metal-organic framework(MOF) amino acids(AAs) defect-engineering motif-rich

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Undrained anisotropy and non-coaxial behavior of clayey soil under principal stress rotation

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2014年第4期15卷 241-254页

作者： jian ZHOU jia-jia YAN zheng-yi LIU Xiao-nan GONG Research Center of Coastal and Urban Geotechnical Engineering Zhejiang University Hangzhou 310058 China

In this study, a series of undrained tests were conducted on both intact and reconstituted clay using an automatic hollow cylinder apparatus. Monotonic shearing tests with fixed principal stress directions were carried out, pure and cyclic prin- cipal stress rotation tests were also performed. The non-coaxiality, defined as the non-coincidence of the principal plastic strain increment direction and the corresponding principal stress direction, of clayey soil was studied experimentally. The effects of the intermediate principal stress, shear stress level, and inherent anisotropy were highlighted. Clear non-coaxiality was observed during pure principal stress rotation, in both intact and reconstituted clay. The influence of the intermediate principal stress pa- rameter, shear stress level, and inherent anisotropy on the non-coaxial behavior of the clayey soil was found to be insignificant when compared with the sand. The non-coaxial behavior of the clayey soil depended more on the stress paths. Under undrained conditions, the contribution of elastic strain to the direction of the total principal strain increment cannot be ignored.

关键词： Non-coaxiality Clay Principal stress rotation Anisotropy

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Layer-by-layer assembled dual-ligand conductive MOF nano-films with modulated chemiresistive sensitivity and selectivity

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Nano Research 2021年第2期14卷 438-443页

作者： Ai-Qian Wu Wen-Qing Wang Hong-Bin Zhan Lin-An Cao Xiao-Liang Ye jia-jia zheng Pendyala Naresh Kumar Kashi Chiranjeevulu Wei-Hua Deng Guan-E Wang Ming-Shui Yao Gang Xu College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Institute for Integrated Cell-Material Sciences(WPI-iCeMS) Kyoto University Institute for Advanced StudyKyoto UniversityYoshida Ushinomiya-choSakyo-kuKyoto 606-8501Japan

In this paper,a dual-ligand design strategy is demonstrated to modulate the performance of the electronically conductive metalorganic frameworks(EC-MOFs)thin film with a spray layer-by-layer assembly *** thin film not only can be precisely prepared in nanometer scale(20-70 nm),but also shows the pin-hole-free smooth *** high quality nano-film of 2,3,6,7,10,11-hexaiminotriphenylene(HITP)doped Cu-HHTP enables the precise modulation of the chemiresistive sensitivity and *** improvement over 220%were realized for benzene ***3>as well as enhanced response and recovery *** addition,the selectivity of the EC-MOF thin film sensors toward other gases(***,methane,ethylbenzene,hydrogen,butanone,and acetone)***3 at room temperature is also discussed.

关键词： metal-organic frameworks electronic conductivity dual-ligand thin films gas sensors

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Passive activity enhances residual control ability in patients with complete spinal cord injury

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Neural Regeneration Research 2025年第8期20卷 2337-2347页

作者： Yanqing Xiao Mingming Gao Zejia He jia zheng Hongming Bai jia-Sheng Rao Guiyun Song Wei Song Xiaoguang Li Beijing Key Laboratory for Biomaterials and Neural Regeneration Beijing Advanced Innovation Center for Biomedical EngineeringSchool of Biological Science and Medical EngineeringBeihang UniversityBeijingChina Department of Rehabilitation Evaluation China Rehabilitation Research CenterBeijingChina Cardiac Center Beijing Children’s HospitalCapital Medical UniversityBeijingChina The State Key Laboratory of Virtual Reality Technology and Systems Beihang UniversityBeijingChina Department of Rehabilitation Engineering China Rehabilitation Science InstituteBeijingChina

Patients with complete spinal cord injury retain the potential for volitional muscle activity in muscles located below the spinal injury ***,because of prolonged inactivity,initial attempts to activate these muscles may not effectively engage any of the remaining neurons in the descending pathway.A previous study unexpectedly found that a brief clinical round of passive activity significantly increased volitional muscle activation,as measured by surface *** this study,we further explored the effect of passive activity on surface electromyographic signals during volitional control tasks among individuals with complete spinal cord *** patients with chronic complete thoracic spinal cord injury were *** electromyography data from eight major leg muscles were acquired and compared before and after the passive activity *** results indicated that the passive activity led to an increased number of activated volitional muscles and an increased frequency of *** the cumulative root mean square of surface electromyography amplitude for volitional control of movement showed a slight increase after passive activity,the difference was not statistically *** findings suggest that brief passive activity may enhance the ability to initiate volitional muscle activity during surface electromyography tasks and underscore the potential of passive activity for improving residual motor control among patients with motor complete spinal cord injury.

关键词： complete spinal cord injury cycle training epidural electrical stimulation motor training passive activity physiological state spinal cord circuit surface electromyography volitional control task

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