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Confinement of Fe atoms between MoS_(2) interlayers drives phase transition for improved reactivity in Fenton-like reactions

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Nano Research 2024年第3期17卷 1132-1139页

作者： Yibing Sun Yu Zhou Hongchao li chuan Wang Xuan Zhang Qian Ma Yingchun Cheng Jieshu Qian Bingcai Pan Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological EngineeringNanjing University of Science and TechnologyNanjing 210094China Key Laboratory of Flexible Electronics and Institute of Advanced Materials Jiangsu National Synergetic Innovation Center for Advanced MaterialsNanjing Tech UniversityNanjing 211816China Department of General Dentistry Affiliated Stomatological Hospital of Nanjing Medical UniversityJiangsu Province Key Laboratory of Oral DiseasesNanjing 210029China Research Center for Environmental Nanotechnology(ReCENT) State Key Laboratory of Pollution Control and Resources ReuseSchool of EnvironmentNanjing UniversityNanjing 210023China

Phase manipulation of MoS_(2) from thermodynamically stable 2H phase to the unstable but more reactive 1T phase represents a crucial strategy for improving the reactivity in many *** widely adopted wet chemistry approach uses intercalating entities especially alkali metal ions to achieve the phase transition;however,these entities are normally inert for the target ***,we describe the first use of iron atoms for the intercalation of 2H-MoS_(2) layers,driving the partial transition from 2H to 1T ***,in the peroxymonosulfate(PMS)-based Fenton-like reactions,the interlayered confinement of Fe atoms not only activates the inert basal plane,but also adds more reactive Fe sites for the formation of metal-PMS complex as primary reactive species for pollutant *** the degradation of a model pollutant carbamazepine(CBZ),the Fe-intercalated MoS_(2) exhibits a first order rate constant 13.3 times higher than 2H-MoS_(2).This strategy is a new direction for manipulating the phase composition and boosting the catalytic reactivity of MoS_(2)-based catalysts in various scenarios,including environmental remediation and energy applications.

关键词： confinement MoS_(2) Fe atoms Fenton-like reactions hydrogen evolution reaction

Robust tantalum tuned perovskite oxygen electrode for reversible protonic ceramic electrochemical cells

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Rare Metals 2024年第7期43卷 3055-3065页

作者： Yu-Shi Feng Yu Shen Fang Wang chuan Tian Qin-Yi Hu Qian Duan Jing-Wei li Di Bao School of Materials Science and Engineering Changchun University of Science and TechnologyChangchun 130022China Zhongshan Institute of Changchun University of Science and Technology Zhongshan528437China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of SciencesChangchun 130022China Key Laboratory of Preparation and Applications of Environmental Friendly Materials Ministry of EducationJilin Normal UniversityChangchun 130103China

Perovskite oxides with diverse composition and structure have exhibited grand advances in boosting the oxygen reduction and evolution reaction(ORR/OER),which are essential for the reversible protonic ceramic electrochemical cell(R-PCEC)toward the sustainable hydrogen production and ***,enhancement of their activity and stability remains ***,we develop the Ta-regulated BaCo_(0.7)Fe_(0.3)O_(3-δ)perovskite oxygen electrode(Ba(Co_(0.7)Fe_(0.3))_(1-x)Ta_xO_(3-δ))with abundant oxygen defects and achieve the simultaneous enhancement in the electrocatalytic activity and stability toward ORR and ***-fabricated R-PCEC with(Ba(Co_(0.7)Fe_(0.3))_(0.9)Ta_(0.1)O_(3-δ))(BCFT10)oxygen electrode performs high power density of 1.47 W·cm^(-2)at 650℃in fuel cell mode,and the current density is up to-2.11 A·cm^(-2)at 1.4 V at 650℃in electrolysis mode,as well as the good stability in both the fuel cell and electrolysis ***,the cell also demonstrates a stable cycling operation between fuel cell and electrolysis mode,suggesting a great potential of BCFT10 as oxygen electrode material for R-PCECs.

关键词： Reversible protonic ceramic electrochemical cells Perovskite oxide Oxygen electrode Ta element doping Oxygen defects

Nutrient enrichment driven by canopy rainfall redistribution:Mechanism,quantification,and pattern

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Science China Earth Sciences 2024年第5期67卷 1529-1544页

作者： chuan YUAN Xiaoping YUE Yafeng ZHANG Yu ZHANG Yanting HU Qiang TANG li GUO Shuai WANG Xingwu DUAN Wenhua XIANG Xiaohua WEI Xiaoyan li College of Forestry and Biotechnology Zhejiang A&F UniversityHangzhou 311300China Chongqing Jinfo Mountain Karst Ecosystem National Observation and Research Station School of Geographical SciencesSouthwest UniversityChongqing 400715China Shapotou Desert Research and Experiment Station Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesLanzhou 730000China School of Geographical Sciences Hebei Normal UniversityShijiazhuang 050024China Faculty of life Science and Technology Central South University of Forestry and TechnologyChangsha 410004China State Key Laboratory of Hydraulics and Mountain River Engineering College of Water Resource and HydropowerSichuan UniversityChengdu 610065China State Key Laboratory of Earth Surface Processes and Resource Ecology Faculty of Geographical ScienceBeijing Normal UniversityBeijing 100875China Yunnan Key Laboratory of Soil Erosion Prevention and Green Development Institute of International Rivers and Eco-securityYunnan UniversityKunming 650091China Department of Earth Environmental and Geographic SciencesUniversity of British Columbia(Okanagan)KelownaBritish Columbia V1V 1V7Canada

Vegetation canopies intercept and redistribute rainfall into throughfall and stemflow,which transfer substantial amounts of elements into the soil,influencing soil microbial community,plant survival,and plant community *** advancements in ecohydrological research,the implication of nutrient enrichment resulting from this redistribution of rainfall by canopies remains largely *** address this gap,we conducted a systematic review of 1020 papers published between 2000 and 2022,gathering data on nutrient concentration and enrichment for critical ions(including K^(+),Na^(+),Ca^(2+),Mg^(2+),NH_(4)^(+),Cl^(-),NO_(3)^(-)and SO_(4)^(2-))from the Web of Science and Chinese Knowledge Infrastructure *** aimed to synthesize the mechanisms,quantify the enrichments,and identify global patterns of nutrient enrichment in stemflow and throughfall across climate zones,and vegetation types and *** results of this study indicate that stemflow exhibits,on average,2.1times greater ion concentration(6.13 mg L^(-1))compared to *** particular,among the investigated ions,SO_(4)^(2-)(12.45and 6.32 mg L^(-1))for stemflow and throughfall,respectively,and Cl^(-)(9.21 and 4.81 mg L^(-1))exhibit the highest concentrations in both rainfall redistribution components,while K^(+)(13.7 and 5.8)and Mg^(2+)(5.6 and 2.8)have the highest enrichment *** climate zones,throughfall and stemflow show the lowest ion concentrations but the highest enrichment factors in extremely humid *** the temperature gradient,ion concentrations are the highest in cold climates with no clear patterns observed for enrichment factors with increasing *** addition,shrubs,conifers,mixed forests,and artificial ecosystems demonstrate enrichment factors 1.1 to 3.0 times greater than those of trees,broad-leaved plants,pure forests,and natural *** findings emphasize the need for increased attentions to artificial ecosystems,such as urban

关键词： Ecohydrology Rainfall redistribution Nutrients transport Enrichment characteristics Climate zones

A chiral fluorescent probe for molecular recognition of basic amino acids in solutions and cells

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Chinese Chemical Letters 2024年第10期35卷 390-395页

作者： chuan-Zhi Ni Ruo-Ming li Fang-Qi Zhang Qu-Ao-Wei li Yuan-Yuan Zhu Jie Zeng Shuang-Xi Gu School of Chemistry and Environmental Engineering School of Chemical Engineering & Pharmacy Pharmaceutical Research Institute Hubei Key Laboratory of Novel Reactor and Green Chemical Technology Wuhan Institute of Technology Nanjing Pusheng Biomedical Co. Ltd.

A novel and readily available binaphthyl-based fluorescent probe（S）-1 was designed and synthesized.（S）-1 can be used to not only chemoselectively discriminate 3 basic amino acids out of common amino acids, but also enantioselectively recognize histidine. Encouragingly, enantioselective imaging of histidine in cells was achieved for the first time by the probe（S）-1. These performances endowed it potential application in the chiral analysis of basic amino acids in asymmetric synthesis and cell imaging for diagnosis of diseases caused by racemization of histidine. Nuclear magnetic resonance（NMR） and mass spectrometry investigations suggested that different reaction extent of（S）-1 with L/D-histidine and different product structures generated the observed enantioselective fluorescent response. The molecular structures and thermodynamic stability of the complexes, formed from（S）-1 + Zn2+and enantiomers of histidine, were calculated by Gaussian 16 based on density functional theory（DFT） to validate the above action mechanism.

关键词： Basic amino acids Cell imaging Chemoselectivity Chiral recognition Enantioselectivity Fluorescent probe

Probing quantum causality with geometric asymmetry in spatial-temporal correlations

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Science China(Information Sciences) 2024年第9期67卷 294-305页

作者： Yu MENG Zheng-Hao liU Zhikuan ZHAO Peng YIN Yi-Tao WANG Wei liU Zhi-Peng li Yuan-Ze yang Zhao-An WANG Jin-Shi XU Shang YU Jian-Shun TANG chuan-Feng li Guang-Can GUO CAS Key Laboratory of Quantum Information University of Science and Technology of China CAS Center for Excellence in Quantum Information and Quantum Physics University of Science and Technology of China Department of Computer Science Eidgen?ssische Technische Hochschule Zürich Hefei National Laboratory Department of Physics Imperial College London Research Center for Quantum Sensing Zhejiang Lab

Causation promotes the understanding of correlation to an advanced stage by elucidating its underlying mechanism. Although statisticians have specified the possible causal relations among correlations,inferring causal structures is impossible from only the observed correlations in the classical world. Quantum correlations encapsulating the most defining aspects of quantum physics have taken a new turn for the causal inference problem — the two-point spatial and temporal quantum correlations with observationally discernible characteristics correspond exactly to the two most basic causal structures. However, a direct causal interpretation for quantum correlations has only been established in very limited cases. Here, we explore to what extent quantum correlations promote causal inference. Theoretically, we have found that the distinguishable causal regime of two-point Pauli correlations can be expanded from a single value to an asymmetric interval, and the causal structures determining the quantum correlations can be interpreted by a simple distance criterion. Experimentally, we have devised and implemented a versatile non-unital quantum channel in an optical architecture to directly observe such an asymmetric interval. The setup enabled quantum causal inference without any requirement of active intervention, which is impossible in the classical realm. Our work facilitates the identification of causal links among quantum variables and provides insight into characterizing causation and spatial-temporal correlation in quantum mechanics.

关键词： causality quantum information quantum channel channel-state duality non-unital channel

Axial enantiomers with donor-regulated TADF feature for multicolor circularly polarized electroluminescence

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Science China Chemistry 2024年第6期67卷 2039-2045页

作者： Chen-Hao Guo Wen-Long Zhao Ke-Ke Tan Wei-Chen Guo liheng Feng chuan-Feng Chen Meng li School of Chemistry and Chemical Engineering Shanxi UniversityTaiyuan030006China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences Beijing100049China

This study optimized the TADF feature of axial chiral enantiomers through precise donor engineering,and multicolor CP-TADFwas achieved in the axial chiral *** pairs of axial enantiomers with donor-regulated TADF feature,namely(R/S)-TPCBD,(R/S)-DPCBD,and(R/S)-DPACBD,were synthesized by introducing carbazole donors with different substituents onto biphenyl cyanide *** the electron-donating ability of donors increases,the emission of these axial enantiomers ranges from 455,476 to 552 nm,their singlet-triplet energy gaps(ΔE_(ST))gradually decrease from 0.30,0.22 to 0.02 e V,accompanied by an increasement in the transition rate(k_(RISC))of RISC process,and the k_(RISC)of DPACBD could reach up to 7.16×10^(5)s^(-1).These axial enantiomers also exhibit mirror-image CD and circularly polarized luminescence(CPL)***,OLEDs based on TPCBD,DPCBD,and DPACBD as emitter were then fabricated,which displayed blue,green,and orange electroluminescence with EQE_(max)of 13.0%,16.4%,and 25.0%,*** results also exhibited a phenomenon of device efficiency increasing with the enhancement of donor ***,the CP-OLEDs using(R/S)-TPCBD,(R/S)-DPCBD and(R/S)-DPACBD as emitters displayed intense CPEL signals with g_(EL)values of 3.4×10^(-3)/-4.1×10^(-3),3.2×10^(-3)/-3.1×10^(-3)and2.3×10^(-3)/-2.1×10^(-3),*** convenient molecular engineering of donor regulation in the same molecular skeleton,CP-TADF materials with multicolor CPEL and improved device performance could be conveniently achieved.

关键词： axial chirality thermally activated delayed fluorescence circularly polarized luminescence electroluminescence organic light-emitting diodes

Cryogenian and Ediacaran integrative stratigraphy,biotas,and paleogeographical evolution of the Qinghai-Tibetan Plateau and its surrounding areas

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Science China Earth Sciences 2024年第4期67卷 919-949页

作者： Lang SUN Malik Muhammad Saud Sajid KHAN chuan yang Zhixin SUN Bing PAN Shehryar AHMED Lanyun MIAO Weichen SUN Chunlin HU Xiaojuan SUN Cui LUO Bo CHEN Zongjun YIN Fangchen ZHAO Guoxiang li Maoyan ZHU State Key Laboratory of Palaeobiology and Stratigraphy Nanjing Institute of Geology and PalaeontologyChinese Academy of SciencesNanjing 210008China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China

The complex evolutionary history of the Qinghai-Tibetan Plateau and its surrounding areas,including the continental blocks(Indian,Lhasa,South Qiangtang,Tarim,Olongbuluk,Central Qilian,Alxa,North China,yangtze,Central Iran and Oman)and the orogenic belts between them,has long been the frontier in Earth science *** Cryogenian and Ediacaran strata are extensively distributed in these ***,relatively complete Cryogenian and Ediacaran successions have been discovered in Oman,Indian,yangtze,and Tarim blocks,while only the Ediacaran successions have been reported in Iran,the South Qiangtang,Central Qilian,Alxa,and North China *** on previous studies together with the integration of new materials and advancement obtained through the Second Tibetan Plateau Scientific Expedition and Research,this review aims to synthesize a correlative stratigraphic framework of the representative Cryogenian and Ediacaran sequences from the Qinghai-Tibetan Plateau and its surrounding ***,the Cryogenian and Ediacaran biotas and major geological events in these areas are comprehensively discussed in aspects of current research *** results indicate that,in general,Ediacaran fossils of each area exhibit distinct features in preservation and assemblage composition,but the typical late Ediacaran fossils Cloudina and Shaanxilithes have been reported from most of these *** addition to the two global Cryogenian glaciations,late Ediacaran glaciogenic deposits are extensively recorded in the areas within and around the northern QinghaiTibetan Plateau(including the North China,Alxa,Central Qilian,Olongbuluk,and Tarim blocks,and the North Qilian Accretionary Belt),as well as central and southern ***,further research is required to determine the age,distribution,and origin of these late Ediacaran glaciogenic ***,the middle Ediacaran DOUNCE/Shuram Excursion is widely documented in the Qinghai-Tibetan Plateau and its surroundi

关键词： Qinghai-Tibetan Plateau Cryogenian Ediacaran Stratigraphy Palaeogeography Biota Gondwana

High-Power Raman Soliton Generation at 1.7 μm in All-Fiber Polarization-Maintaining Erbium-Doped Amplifier

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Chinese Physics Letters 2024年第5期41卷 35-39页

作者：徐子鹏王萱姚传飞杨林京李平雪 Institute of Ultrashort Pulsed Laser and Application Beijing University of TechnologyBeijing 100124China

An all-fiber polarization maintaining high-power laser system operating at 1.7 μm based on the Ramaninduced soliton self-frequency shifting effect is demonstrated. The entirely fiberized system is built by erbiumdoped oscillator and two-stage amplifiers with polarization maintaining commercial silica fibers and devices, which can provide robust and stable soliton generation. High-power soliton laser with the average power of 0.28 W,the repetition rate of 42.7 MHz, and pulse duration of 515 fs is generated directly from the main *** experiment provides a feasible method for high-power all-fiber polarization maintaining femtosecond laser generation working at 1.7 μm.

关键词： polarization fiber amplifier

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网络语言二十年发展综述

湖南大学学报（社会科学版） 2014年第5期28卷 136-141页

作者：胡凌刘云杨传丽湖南大学外国语与国际教育学院湖南长沙410082

从1994年至今,中国网络语言经历了从无到有,从有到优的二十年发展过程。本文主要针对网民自创的并用于网络交际的语言,通过梳理这类语言二十年间的形式变化、观点交锋、理论认知和规范立法展现网络语言发展变化,并对网络语言的未来发展... 详细信息

从1994年至今,中国网络语言经历了从无到有,从有到优的二十年发展过程。本文主要针对网民自创的并用于网络交际的语言,通过梳理这类语言二十年间的形式变化、观点交锋、理论认知和规范立法展现网络语言发展变化,并对网络语言的未来发展作出展望。

关键词：网络语言形式变化观点交锋理论认知规范立法

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