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Design of bifunctional single-atom catalysts NiSA/ZIF-300 for CO_(2) conversion by ligand regulation strategy

Nano Research 2024年第5期17卷 3827-3834页

作者： Wengang Fu Yapei Yun Hongting Sheng Xiaokang Liu Tao Ding shuxian Hu Tao Yao Binghui Ge Yuanxin du Didier Astruc Manzhou Zhu Department of Chemistry and Centre for Atomic Engineering of Advanced Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationCollege of Materials Science and EngineeringInstitutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefei 230601China Universitéde Bordeaux ISMUMR CNRS N°5255351 Cours de La Libération33405 Talence CedexFrance National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230026China Department of Physics University of Science and Technology BeijingBeijing 100083China Anhui Tongyuan Environment Energy Saving Co. LtdHefei 230041China

Carbon-supported noble-metal-free single-atom catalysts(SACs)have aroused widespread interest due to their green chemistry aspects and excellent ***,we propose a“ligand regulation strategy”and achieve the successful fabrication of bifunctional SAC/MOF(MOF=metal-organic framework)nanocomposite(abbreviated NiSA/ZIF-300;ZIF=ZIF-8)with exceptional catalytic performance and *** designed NiSA/ZIF-300 has a planar interfacial structure with the Ni atom,involving one S and three N atoms bonded to Ni(Ⅱ),fabricated by controllable pyrolysis of volatile Ni-S *** CO_(2) cycloaddition to styrene epoxide,NiSA/ZIF-300 exhibits ultrahigh activity(turnover number(TON)=1.18×105;turnover frequency(TOF)=9830 molSC·mol_(Ni)^(-1)·h^(-1);SC=styrene carbonate)and durability at 70℃ under 1 atm CO_(2) pressure,which is much superior to Ni complex/ZIF,NiNP/ZIF-300,and most reported *** study offers a simple method of bifunctional SAC/MOF nanocomposite fabrication and usage,and provides guidance for the precise design of additional original SACs with unique catalytic properties.

关键词： single atom catalyst bifunctional CO_(2)conversion cycloaddition

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Iron-nickel alloy particles with N-doped carbon “armor” as a highly selective and long-lasting catalyst for the synthesis of Nbenzylaniline molecules

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Nano Research 2024年第4期17卷 2308-2319页

作者： Gang Wang Longchao Sun Wanyi Liu Haijuan Zhan shuxian Bi College of Chemistry and Chemical Engineering Ningxia UniversityYinchuan 750021China

A scalable strategy for the convenient and rapid preparation of nitrogen-doped carbon-coated iron-based alloy catalysts was *** controlling the type and amount of metal salts in the precursor,various types of nitrogen-doped carbon-coated alloy catalysts can be prepared in a targeted ***_(2)Ni2@CN materials with small particle sizes and relatively homogeneous basic sites showed promising results in the N-alkylation reaction of benzyl alcohol with aniline(optimum yield:99%).It is worth noting that the catalyst can also be magnetically separated and recovered after the reaction,and its performance can be regenerated through simple ***,it was confirmed by kinetic experiments that the activation of C–H at the benzyl alcohol benzylic position is the rate-determining step(RDS).According to density flooding theory calculations,Fe_(2)Ni2@CN catalysts require less energy than other materials(Fe@CN and Ni@CN)for the RDS(dehydrogenation reaction)*** N-alkylation reactions are more easily carried out on Fe_(2)Ni2@CN catalysts,which may be the reason for the best catalytic activity of Fe-Ni alloy *** carbon-coated alloy materials will show great potential in more types of heterogeneous catalysis.

关键词： iron-nickel alloy catalyst N-alkylation reaction magnetic separation reaction path dehydrogenation reaction

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Agricultural Investment Project Decisions Based on an Interactive Preference Disaggregation Model Considering Inconsistency

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Computer Modeling in Engineering & Sciences 2024年第6期139卷 3125-3146页

作者： Xingli Wu Huchang Liao shuxian Sun Zhengjun Wan Business School Sichuan UniversityChengdu610064China National Institute of Measurement and Testing Technology Chengdu610021China

Agricultural investment project selection is a complex multi-criteria decision-making problem,as agricultural projects are easily influenced by various risk factors,and the evaluation information provided by decisionmakers usually involves uncertainty and *** literature primarily employed direct preference elicitation methods to address such issues,necessitating a great cognitive effort on the part of decision-makers during evaluation,specifically,determining the weights of *** this study,we propose an indirect preference elicitation method,known as a preference disaggregation method,to learn decision-maker preference models fromdecision *** enhance evaluation ease,decision-makers merely need to compare pairs of alternatives with which they are familiar,also known as reference *** linguistic preference relations are employed to account for the presence of incomplete and uncertain information in such pairwise *** address the inconsistency among a group of decision-makers,we develop a pair of 0-1mixed integer programming models that consider both the semantics of linguistic terms and the belief degrees of ***,we conduct a case study and comparative *** reveal the effectiveness of the proposed model in solving agricultural investment project selection problems with uncertain and inconsistent decision information.

关键词： Multiple criteria analysis preference disaggregation inconsistency probability linguistic preference relation investment project selection

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Developmental toxicity assessment of neonicotinoids and organophosphate esters with a human embryonic stem cell-and metabolism-based fast-screening model

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Journal of Environmental Sciences 2024年第3期137卷 370-381页

作者： shuxian Zhang Miaomiao Zhao Shichang Li Renjun Yang Nuoya Yin Francesco Faiola State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China College of Resources and Environment University of Chinese Academy of SciencesBeijing 100049China

In recent years,neonicotinoids(NEOs)and organophosphate esters(OPEs)have been widely used as substitutes for traditional pesticides and brominated fame-retardants,*** studies have shown that those compounds can be frequently detected in environmental and human samples,are able to penetrate the placental barrier,and are toxic to ***,it is reasonable to speculate that NEOs and OPEs may have potential adverse effects in humans,especially during *** employed a human embryonic stem cell differentiation-and liver S9 fraction metabolism-based fast screening model to assess the potential embryonic toxicity of those two types of *** show that four NEO and five OPE prototypes targeted mostly ectoderm specification,as neural ectoderm and neural crest genes were down-regulated,and surface ectoderm and placode markers *** liver S9 fraction's treatment could generally reduce the effects of the chemicals,except in a few specific instances,indicating the liver may detoxify NEOs and *** findings suggest that NEOs and OPEs interfere with human early embryonic development.

关键词： Neonicotinoids Organophosphate esters Human embryonic stem cells Fast screening model Developmental toxicity

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3D printing encouraging desired in-situ polypyrrole seed-polymerization for ultra-high energy density supercapacitors

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Journal of Energy Chemistry 2024年第8期95卷 117-125,I0004页

作者： Tiantian Zhou Shangwen Ling shuxian Sun Ruoxin Yuan Ziqin Wu Mengyuan Fu Hanna He Xiaolong Li Chuhong Zhang State Key Laboratory of Polymer Materials Engineering Polymer Research InstituteSichuan UniversityChengdu 610065SichuanChina

The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered ***(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world ***,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass *** preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer *** agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based *** work highlights a promising route to preparing high energy density energy storage modules for real-world applications.

关键词： 3D printing Seed-induced polymerization Supercapacitor Polypyrrole High energy density

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Development and Characterization of Novel FAP-Targeted Theranostic Pairs: A Bench-to-Bedside Study

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Research 2024年第3期2023卷 473-485页

作者： Wei Huang Yizhen Pang Qiufang Liu Chenyi Liang shuxian An Qianyun Wu You Zhang Gang Huang Haojun Chen Jianjun Liu Weijun Wei Department of Nuclear Medicine Institute of Clinical Nuclear MedicineRenj HospitalSchool of Medicine Shanghai Jiao Tong UniversityShanghai 200127China Department of Nuclear Medicine and Minnan PET Center Xiamen Cancer CenterXiamen Key Laboratory of Radiation OncologyThe First Affiliated Hospital of Xiamen UniversitySchool of MedicineXiamen UniversityXiamen 361003China Department of Nuclear Medicine Fudan University Shanghai Cancer CenterFudan UniversityShanghai 200032China

Fibroblast activation protein (FAP) is among the most popular targets in nuclear medicine imaging and cancer theranostics. Several small-molecule moieties (FAPI-04, FAPI-46, etc.) are used for developing FAP-targeted theranostic agents. Nonetheless, the circulation time of FAP inhibitors is relatively short, resulting in rapid clearance via kidneys, low tumor uptake, and associated unsatisfactory treatment efficacy. To address the existing drawbacks, we engineered 3 peptides named FD1, FD2, and FD3 with different circulation times through solid-phase peptide synthesis. All the 3 reported peptides bind to human and murine FAP with single-digit nanomolar affinity measured by surface plasmon resonance. The diagnostic and therapeutic potential of the agents labeled with 68Ga and 177Lu was assessed in several tumor models exhibiting different levels of FAP expression. While radiolabeled FD1 was rapidly excreted from kidneys, radiolabeled FD2/FD3 have significantly prolonged circulation, increased tumor uptake, and decreased kidney accumulation. Our findings indicated that [68Ga]Ga-DOTA-FD1 positron emission tomography (PET) effectively detected FAP dynamics, whereas [177Lu]Lu-DOTA-FD2 and [177Lu]Lu-DOTA-FD3 exhibited remarkable therapeutic efficacy in FAP-overexpressing tumor models, including pancreatic cancer cell models characterized by abundant stroma. Moreover, a pilot translational investigation demonstrated that [68Ga]Ga-DOTA-FD1 had the capability to identify both primary and metastatic tumors with precision and distinction. In summary, we developed [68Ga]Ga-DOTA-FD1 for same-day PET imaging of FAP dynamics and [177Lu]Lu-DOTA-FD2 and [177Lu]Lu-DOTA-FD3 for effective radioligand therapy of FAP-overexpressing tumors.

关键词： DOTA expressing labeled

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Bifunctional noble-metal-free cocatalyst coating enabling better coupling of photocatalytic CO_(2)reduction and H_(2)O oxidation on direct Z-scheme heterojunction

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Nano Research 2024年第6期17卷 5022-5030页

作者： Wei Zhao Weihao Mo Yan Zhang Lingxuan Hu Yiyi Zheng Zhulei Chen Xiangyue Niu Yuling Zhao Lichun Liu shuxian Zhong Song Bai Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials ScienceZhejiang Normal UniversityJinhua 321004China College of Biological Chemical Sciences and Engineering and Nanotechnology Research InstituteJiaxing UniversityJiaxing 314001China College of Geography and Environmental Sciences Zhejiang Normal UniversityJinhua 321004China College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310058China School of Biological and Chemical Engineering Panzhihua UniversityPanzhihua 617000China

Selective loading of spatially separated redox cocatalysts on direct Z-scheme heterojunctions holds great promise for advancing the efficiency of artificial photosynthesis,which however is limited to the photodeposition of noble metal cocatalysts and the fabrication of hollow double-shelled semiconductor ***,the co-exposure of discrete cocatalyst and semiconductor increases the product diversity when both the exposed sites of which participate in CO_(2)***,we present a facile and versatile protocol to overcome these limitations via surface coating of Z-scheme heterojunctions with bifunctional noble-metal-free *** Cu_(2)O/Fe_(2)O_(3)(CF)as a model heterojunction and layered Ni(OH)_(2)as a model cocatalyst,it is found that Ni(OH)_(2)lying on the surfaces of Cu_(2)O and Fe_(2)O_(3)separately co-catalyzes the CO_(2)reduction and H_(2)O *** experimental and theoretical investigation reveals that the Ni(OH)_(2)outer layer:(i)mitigates the charge recombination in CF and balances their transfer and consumption;(ii)reduces the rate-determining barriers for CO_(2)-to-CO and H_(2)O-to-O_(2)conversion,(iii)suppresses the side proton reduction occurring on CF,and(iv)protects the CF from component *** expected,the redox reactions stoichiometrically proceed,and significantly enhanced photocatalytic activity,selectivity,and stability in CO generation are achieved by the stacked Cu_(2)O/Fe_(2)O_(3)@Ni(OH)_(2)in contrast to *** study demonstrates the significance of the synergy between bifunctional cocatalysts and Z-scheme heterojunctions for improving the efficacy of overall redox reactions,opening a fresh avenue for the rational design of artificial photosynthetic systems.

关键词： Z-scheme heterojunction bifunctional cocatalyst CO_(2)reduction H_(2)O oxidation stoichiometric redox reaction

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Re-Os age for molybdenite from the Gangdese porphyry copper belt on Tibetan plateau: Implication for geody- namic setting and duration of the Cu mineralization

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Science China Earth Sciences 2004年第3期47卷 221-231页

作者： HOU Zengqian1, QU Xiaoming1, WANG shuxian2, du Andao2, GAO Yongfeng3 & HUANG Wei4 1. Institute of Mineral Resources, Chinese Academy of Geological Sciences, Beijing 100037, China 2. National Center of Geoanalysis, Chinese Academy of Geological Sciences, Beijing 100037, China 3. Shijiazhuang College of Economy, Shijiazhuang 056000, China 4. Xizang Bureau of Geology and Mineral Resources, Lhasa 850000, China Institute of Mineral Resources Chinese Academy of Geological Sci. Beijing 100037 China National Center of Geoanalysis Chinese Academy of Geological Sci. Beijing 100037 China Shijiazhuang College of Economy Shijiazhuang 056000 China Xizang Bureau of Geol./Mineral Rsrc. Lhasa 850000 China

The Gangdese porphyry copper belt consists of one large and five middle-small deposits in addition to dozens of ore-bearing porphyry bodies. The belt trends 350 km long along the EW-striking Gangdese batholith, and locally occurs as a string of beads extending about 50 km within the SN-trending rifting zones (grabens) on the Tibetan plateau. Monzonitic granite- porphyry and quartz monzonitic porphyry, as dominant host rocks, are shoshonitic and potassic calc-alkaline. Available dating data indicate that the ages of the shallow-level emplacement for these porphyries vary from 10 Ma to 18 Ma, which are identical to that of associated potassic calc-alkaline volcanic rocks (10—15 Ma) and mafic dykes (13—18 Ma). The timing and duration of Cu mineralization events are constrained by Re-Os ages for molybdenites from three porphyry copper deposits in the Gangdese porphyry copper belt. Five molybdenite samples from the Nanmu deposit yielded an 187Re-187Os isochron with a highly pre-cise age of (14.76?.22) Ma; six molybdenites from the Chongjiang deposit gave an isochron age of (14.04?.16) Ma. Re-Os model ages for two molybdenite samples from Lakang抏 deposit vary from 13.5 Ma to 13.6 Ma, which are basically identical to isochron ages mentioned above. All the thirteen samples from these three deposits yielded a linear array in the isochron diagram with a higher correlation coefficient of 0.99719 and an isochron age of (14.39?.22) Ma (1s error), suggesting an coeval event of the Cu mineralization and a shared source of ore materials for the Gangdese porphyry copper belt. Compared with the longer-lived felsic magmatic-hydrothermal system, the Cu mineralization is a relatively short event with duration of about 0.5 Ma, and usu-ally occurs in the later-stage of the complicate magmatic system. The emplacement age of the Gangdese porphyries indicates that they intruded after the rapid rising of the Gangdese Mountains at 21—23 Ma, and formed in a post-collision crustal ex-tension env

关键词： porphyry copper deposit, Re-Os age, Gangdese, Tibetan plateau.

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A Study on the Titles of Dianshizhai Pictorial

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Cultural and Religious Studies 2024年第4期12卷 234-236页

作者： GE shuxian ZHANG Pei Beijing Institute of Graphic Communication BeijingChina

With its unique title art,Dianshizhai Pictorial has become an important document for the study of the intersection of news communication and traditional Chinese culture in the Late Qing *** study explores the formation mechanism,artistic features,and social influence of the title,from historical allusion,report content,stylistic structure to the appearance of sound and *** this research,we hope to reveal the unique charm of the Dianshizhai Pictorial title and its important position in the history of journalism and communication,and to provide a new perspective for understanding the changes of Chinese traditional culture in the process of modernization.

关键词： Dianshizhai Pictorial title

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The First-in-Human Whole-Body Dynamic Pharmacokinetics Study of Aptamer

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Research 2024年第1期2023卷 119-130页

作者： Ding Ding Haitao Zhao Dali Wei Qinglai Yang Cai Yang Ruowen Wang Yumei Chen Lianghua Li shuxian An Qian Xia Gang Huang Jianjun Liu Zeyu Xiao Weihong Tan Institute of Molecular Medicine(IMM) Renji HospitalState Key Laboratory of Oncogenes and Related GenesShanghai Jiao Tong University School of Medicineand College of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Nuclear Medicine Renji HospitalSchool of MedicineShanghai Jiao Tong UniversityShanghai 200127China Center for Molecular Imaging Probes Cancer Research InstituteUniversity of South ChinaHengyangHunan 421001China The Key Laboratory of Zhejiang Province for Aptamers and Theranostics Zhejiang Cancer HospitalHangzhou Institute of Medicine(HIM)Chinese Academy of SciencesHangzhouZhejiang 310022China Molecular Science and Biomedicine Laboratory(MBL) State Key Laboratory of Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringHunan UniversityChangshaHunan 410082China Shanghai Key Laboratory of Molecular Imaging Shanghai University of Medicine and Health SciencesShanghai 201318China Department of Pharmacology and Chemical Biology Shanghai Jiao Tong University School of MedicineShanghai200127China

Serving as targeting ligands,aptamers have shown promise in precision ***,the lack of knowledge of the biosafety and metabolism patterns in the human body largely impeded aptamers’clinical *** bridge this gap,here we report the first-in-human pharmacokinetics study of protein tyrosine kinase 7 targeted SGC8 aptamer via in vivo PET tracking of gallium-68(^(68)Ga)radiolabeled *** specificity and binding affinity of a radiolabeled aptamer,named ^(68)Ga[Ga]-NOTA-SGC8,were maintained as proven in *** preclinical biosafety and biodistribution evaluation confirmed that aptamers have no biotoxicity,potential mutation risks,or genotoxicity at high dosage(40 mg/kg).Based on this result,a first-in-human clinical trial was approved and carried out to evaluate the circulation and metabolism profiles,as well as biosafety,of the radiolabeled SGC8 aptamer in the human *** advantage of the cutting-edge total-body PET,the aptamers’distribution pattern in the human body was acquired in a dynamic fashion.

关键词： metabolism dosage Whole

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