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Azocalixarenes: a scaffold of universal excipients with high efficiency

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Science China Chemistry 2024年第5期67卷 1697-1706页

作者： Yu-Xin Yue Yi-Lin Lin Meng-Meng Chen Han-Wen Tian Rong Ma Ze-Han Wang Fang-Yuan Chen Yu-Chen Pan Dong-Sheng Guo College of Chemistry State Key Laboratory of Elemento-Organic ChemistryKey Laboratory of Functional Polymer Materials(Ministry of Education)Frontiers Science Center for New Organic MatterCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Nankai UniversityTianjin 300071China

Excipients are important components of pharmaceutical preparations that affect their quality, safety, and efficacy. Macrocyclic receptors are a family of supramolecular excipients with several advantages, including molecular-level protection, small sizes,fast kinetics of host-guest recognition, and modular construction. With the continuous advances in the medical field, personalized and precision medicine requires the development of excipients with low dosages, integrated modifying effects, universality,and controlled release. To meet these requirements, we have developed a new family of macrocyclic excipients based on calixarenes by integrating their covalent(broad chemical design space) and noncovalent(wide range of substrates) ***, azocalixarenes(Azo CAs) were designed, showing high binding affinities to a broad spectrum of active pharmaceutical ingredients(APIs), selectivity to interferents, and responsiveness to hypoxic microenvironments. Due to their highly efficient and controllable recognition, Azo CAs serve as low-dose excipients for 30 APIs. Molecular encapsulation by Azo CAs results in the integrated modification of the physicochemical properties of APIs, including solubility, stability, bioavailability,and biocompatibility. Moreover, Azo CAs can be reduced by azoreductases overexpressed in hypoxic microenvironments,leading to the controlled release of APIs. Collectively, Azo CA excipients have broad application prospects for a series of diseases such as enteritis, arthritis, stroke, cancer, bacterial infection and kidney injury, with diverse therapeutic modalities,including chemotherapy, photodynamic therapy, photothermal therapy, immunotherapy, boron neutron capture therapy, radiotherapy, fluorescence imaging, and their combinations.

关键词： supramolecular chemistry host-guest systems excipient calixarene molecular recognition

Engineering Shewanella-re duce d graphene oxide aerogel biohybrid to efficiently synthesize Au nanoparticles

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Journal of Materials Science & Technology 2024年第1期168卷 50-61页

作者： Baocai Zhang Shulin Shao Huan Yu Qijing Liu Sicheng Shi Qingyuan Wu Zijie Wu Yiyu Feng Yifei Wang Xi Sun Deguang Wu Feng Li Hao Song Frontier Science center for Synthetic Biology and Key Laboratory of Systems Bioengineering(Ministry of education) Tianjin UniversityTianjin 300072China Collaborative innovation center of Chemical Science and Engineering(Tianjin) School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Beijing advanced innovation center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China School of Materials Science and Engineering Tianjin UniversityTianjin 300350China College of Biological Engineering Tianjin Agricultural UniversityTianjin 300384China Department of Brewing Engineering Moutai InstituteLuban AveRenhuai 564507China

Biosynthesizing Au nanoparticles(AuNPs)from gold-bearing scraps provides a sustainable method to meet the urgent demand for ***,it remains challenging to efficiently biosynthesize AuNPs of which the diameter is less than 10 nm from a trace amount of Au^(3+)concentration at the level of tens ***,we constructed an exoelectrogenic cell(eCell)-conductive reduced-graphene-oxide aero-gel(rGA)biohybrid by assembling Shewanella sp.S1(SS1)as living biocatalyst and rGA as conductive ad-sorbent,in which Au^(3+)at trace concentrations would be enriched by the adsorption of rGA and reduced to AuNPs through the extracellular electron transfer(EET)of *** regulate the size of the synthe-sized AuNPs to 10 nm,the strain SS1 was engineered to enhance its EET,resulting in strain RS2(pYYD-P tac-ribADEHC&pHG13-P_(bad)-omcC in SS1).Strain RS2 was further assembled with rGA to construct the RS2-rGA biohybrid,which could synthesize AuNPs with the size of 7.62±2.82 nm from 60 ppm Au^(3+)*** eCell-rGA biohybrid integrated Au^(3+)adsorption and reduction,which enabled AuNPs biosyn-thesis from a trace amount of Au^(3+).Thus,the required Au^(3+)ions concentration was reduced by one or two orders of magnitude compared with conventional methods of AuNPs *** work devel-oped an AuNPs size regulation technology via engineering eCell’s EET with synthetic biology methods,providing a feasible approach to synthesize AuNPs with controllable size from trace level of gold ions.

关键词： Au nanoparticles Exoelectrogenic cell(e-Cell) Shewanella Synthesis biology Extracellular electron transfer Reduced graphene oxide aerogel

Microwave electrometry with Rydberg atoms in a vapor cell using microwave amplitude modulation

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Chinese Physics B 2024年第5期33卷 65-74页

作者：郝建海贾凤东崔越王昱寒周飞刘修彬张剑谢锋白金海尤建琦王宇钟志萍 School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China Institute of Nuclear and New Energy Technology Collaborative Innovation Center of Advanced Nuclear Energy TechnologyKey Laboratory of Advanced Reactor Engineering and Safety of Ministry of EducationTsinghua UniversityBeijing 100084China Science and Technology on Metrology and Calibration Laboratory Changcheng Institute of Metrology & MeasurementAviation Industry Corporation of ChinaBeijing 100095China CAS center for Excellence in Topological Quantum Computation University of Chinese Academy of SciencesBeijing 100190China

We have theoretically and experimentally studied the dispersive signal of the Rydberg atomic electromagneticallyinduced transparency(EIT)Autler–Townes(AT)splitting spectra obtained using amplitude modulation of the microwave(MW)electric *** addition to the two zero-crossing points interval△f_(zeros),the dispersion signal has two positive maxima with an interval defined as the shoulder interval△f_(sho),which is theoretically expected to be used to measure a much weaker MW electric *** relationship of the MW field strength E_(MW)and△f_(sho)is experimentally studied at the MW frequencies of 31.6 GHz and 9.2 GHz *** results show that△f_(sho)can be used to characterize the much weaker E_(MW)than that of△f_(zeros)and the traditional EIT–AT splitting interval△f_(m);the minimum E_(MW)measured by△f_(sho)is about 30 times smaller than that by△f_(m).As an example,the minimum E_(MW)at 9.2 GHz that can be characterized by△f_(sho)is 0.056 mV/cm,which is the minimum value characterized by the frequency interval using a vapor cell without adding any auxiliary *** proposed method can improve the weak limit and sensitivity of E_(MW)measured by the spectral frequency interval,which is important in the direct measurement of weak E_(MW).

关键词： quantum sensor Rydberg atoms electromagnetically induced transparency amplitude modulation

How the microenvironment dominated by the distance effect to regulate the FeN_(4)site ORR activity and selectivity?

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Nano Research 2024年第6期17卷 5735-5741页

作者： Peng Li Qingfeng Guo Jianrui Zhang Ruilin Chen Shujiang Ding Yaqiong Su School of Chemistry Engineering Research Center of Energy Storage Materials and Devices of Ministry of EducationNational Innovation Platform(Center)for Industry-Education Integration of Energy Storage TechnologyXi’an Jiaotong UniversityXi’an 710049China Huanghe Science and Technology College Zhengzhou 450063China General Research Institute of Engineering of Gotion High-Tech Hefei 230041China

The distance effect of the doped heteroatoms away from the catalytic centers has rarely been *** this work,we conducted density functional theory calculations to thoroughly investigate the influence of heteroatom(N,P,B,and S atoms)doping distance on the oxygen reduction reaction(ORR)activity of graphene-based FeN_(4)*** uncovered a Sabatier-like relationship between heteroatom doping distance and ORR activity of FeN_(4)*** nearest doping does not significantly improve and even block the ORR activity of FeN_(4)*** ORR activity is achieved when the heteroatoms are 4-5Å(N,P,and S atoms)or 6-7Å(B atoms)away from the Fe *** of electronic structure indicates that distance effect can modulate the local chemical environment of Fe atoms,thereby account for the changes in ORR activity along with the doping distance and doping *** study provides insights into the influence of heteroatom doping on the chemical environment of reaction active centers,and provides the theoretical guidance for controlling the doping distance of heteroatoms to achieve optimal catalytic activity and selectivity.

关键词： distance effect microenvironment heteroatom doping FeN_(4) Sabatier-like relationship structure-activity relationship

Human influence on the duration of extreme temperature events in Asia's hotspot regions

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Advances in Climate Change Research 2024年第2期15卷 312-326页

作者： Zi-Meng WANG Hong-Yun MA Wei LI Hai-Shan CHEN Collaborative innovation center on Forecast and Evaluation of Meteorological Disasters(CIC-FEMD)/Key Laboratory of Meteorological Disaster Ministry of Education(KLME)Nanjing University of Information Science and TechnologyNanjing 210044China

Observations and models indicate that human activities exert a considerable impact on the frequency and intensity of extreme temperature events,which are associated with global ***,changes in the duration of extreme temperature events and their association with human influence have not been considered in most ***,the possible relationship between the observed changes in the warm and cold spell duration(WSDI and CSDI)in hotspot regions during 1960-2014 and human influence was investigated based on the NCEP/NCAR reanalysis version 1 and Coupled Model Inter-comparison Project Phase 6(CMIP6)*** projection based on these attribution results was also *** optimal fingerprinting technique was used to compare observed changes in WSDI and CSDI to simulated changes averaged across eight CMIP6 *** show that anthropogenic(ANT)forcing contributed to the observed increase in WSDI in the three hotspot regions(West Asia,South Asia and Southeast Asia),with the majority of the changes being attributed to greenhouse gas ***,a generally weak ANT signal can be observed in the decreasing trend of CSDI and can be detected in South and Southeast *** influence of aerosol forcing remains undetected in either WSDI or CSDI,which differs from the results for frequency and intensity of extreme *** attribution results revealed that the constrained projection of WSDI is lower than the raw projection for 2015-2100 in West Asia and Southeast ***,no differences in future CSDI changes are found in Southeast Asia between the constrained and raw projections.

关键词： Extreme temperature events Duration Detection attribution Constraint projection Hotspot regions

Constructing high-capacity and flexible aqueous zinc-ion batteries with air-recharging capability using organic cathodes

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Chinese Chemical Letters 2024年第3期35卷 468-472页

作者： Xiaojuan Chen Haoqi Su Baozhu Yang Xiaocen Liu Xiuting Song Lixin Su Gui Yin Qi Liu Jiangsu Key Laboratory of advanced Catalytic Materials and Technology Advanced Catalysis Green Manufacturing Collaborative Innovation Center and School of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China State Key Laboratory of Coordination Chemistry Nanjing UniversityNanjing 210093China

Flexible aqueous zinc-ion batteries(AZIBs)with air-recharging capability are a promising self-powered system applied in future wearable *** is desired to develop high-capacity air-rechargeable ***,we developed a flexible AZIB with air-recharging capability based on trinitrohexaazatrinaphthylene(TNHATN)cathode and a ZnSO_(4)*** flexible Zn//TNHATN battery exhibits high volumetric energy density(21.36 mWh/cm^3)and excellent mechanical ***,the discharged flexible Zn//TNHATN battery can be chemical self-charged via the redox reaction between TNHATN cathode and O_(2)from the *** oxidation in air for 15 h,such flexible Zn//TNHATN battery can deliver a high specific capacity of 320 mAh/g at 0.5 A/g,displaying excellent air-recharging ***,this flexible Zn//TNHATN battery also works well in chemical or/and galvanostatic charging mixed modes,showing *** work provides a new insight for designing flexible aqueous self-powered systems.

关键词： Aqueous zinc-ion battery Trinitrohexaazatrinaphthylene Organic cathode materials Flexible air-rechargeable battery Self-powered system

C_(60) as a metal-free catalyst for lithium-oxygen batteries

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Nano Research 2024年第5期17卷 3982-3987页

作者： Xinxin Zhang Jiaming Tian Yu Wang Shaohua Guo Yafei Li Jiangsu Collaborative innovation Centre of Biomedical Functional Materials School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China College of Engineering and Applied Sciences Jiangsu Key Laboratory of Artificial Functional MaterialsNational Laboratory of Solid State MicrostructuresCollaborative Innovation Center of Advanced MicrostructuresFrontiers Science Center for Critical Earth Material CyclingNanjing UniversityNanjing 210023China

Carbon materials have shown significant potential as catalysts for lithium-oxygen batteries(LOBs).However,the intrinsic carbon sites are typically inert,necessitating extensive modifications and resulting in a limited density of active *** we present C_(60) as a metal-free cathode catalyst for LOBs,using density functional theory calculations and experimental *** lithiation reactions on the pristine carbon sites of C_(60) are energetically favorable due to its curvedπ-conjugation over the pentagon-hexagon *** kinetic analysis specifically reveals low energy barriers for Li_(2)O_(2) decomposition and Li diffusion on C_(60).Consequently,C_(60) exhibits significantly higher catalytic activity than typical carbon materials such as graphene and carbon *** electrochemical measurements validate the predictions,notably demonstrating that the intrinsic activity of C_(60) is comparable to that of noble metals.

关键词： lithium-oxygen batteries C_(60) density functional theory(DFT)calculations metal-free cathode

A Framework Based on the DAO and NFT in Blockchain for Electronic Document Sharing

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Computer Modeling in Engineering & Sciences 2024年第9期140卷 2373-2395页

作者： Lin Chen Jiaming Zhu Yuting Xu Huanqin Zheng Shen Su Cyberspace Institute of advanced Technology Guangzhou UniversityGuangzhou510006China Engineering Research center of lntegration and Application of Digital Learning Technology Ministry of EducationBeijing100816China

In the information age,electronic documents(e-documents)have become a popular alternative to paper documents due to their lower costs,higher dissemination rates,and ease of knowledge ***,digital copyright infringements occur frequently due to the ease of copying,which not only infringes on the rights of creators but also weakens their creative ***,it is crucial to establish an e-document sharing system that enforces copyright ***,the existing centralized system has outstanding vulnerabilities,and the plagiarism detection algorithm used cannot fully detect the context,semantics,style,and other factors of the *** watermark technology is only used as a means of infringement *** paper proposes a decentralized framework for e-document sharing based on decentralized autonomous organization(DAO)and non-fungible token(NFT)in *** use of blockchain as a distributed credit base resolves the vulnerabilities inherent in traditional centralized *** e-document evaluation and plagiarism detection mechanisms based on the DAO model effectively address challenges in comprehensive text information checks,thereby promoting the enhancement of e-document *** mechanism for protecting and circulating e-document copyrights using NFT technology ensures effective safeguarding of users’e-document copyrights and facilitates e-document ***,recognizing the security issues within the DAO governance mechanism,we introduce an innovative optimization *** experimentation,we validate the enhanced security of the optimized governance mechanism,reducing manipulation risks by up to 51%.Additionally,by utilizing evolutionary game analysis to deduce the equilibrium strategies of the framework,we discovered that adjusting the reward and penalty parameters of the incentive mechanism motivates creators to generate superior quality and unique e-documents,while evaluators are more likely to engage in

关键词： Electronic document sharing blockchain DAO NFT evolutionary game

Complementary multicolor electrochromic devices with excellent stability based on porous tin oxide nanosheet scaffold

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Nano Research 2024年第4期17卷 3035-3042页

作者： Chenchen Bian Jinhui Wang Huanhuan Liu Yin Yan Ping Zhang Weilong Yang Sensen Jia Xiaodan Guo Guofa Cai Key Laboratory for Special Functional Materials of Ministry of education National&Local Joint Engineering Research Center for High-Efficiency Display and Lighting TechnologySchool of Materials and Engineeringand Collaborative Innovation Center of Nano Functional Materials and ApplicationsHenan UniversityKaifeng 475004China

Electrochromic devices(ECDs)have been extensively investigated as promising candidates in broad cutting-edge applications,such as smart windows,electronic labels,adaptive camouflage,***,they have suffered from either inadequate color variations or poor cycling stability for a long ***,we developed a general strategy to boost the cyclic stability and enrich the color variations of ECDs by scrupulous design of the composition and nanostructure of electrodes,in which porous tin oxide(SnO_(2))nanosheets serve as the scaffold and typical metal oxides or conducting polymers as the active electrochromic *** electrochromic composite materials,including polyaniline(PANI)@SnO_(2),V2O5@SnO_(2),and WO_(3)@SnO_(2) heterostructured nanoarrays were prepared by the facile wet-chemical *** composite electrodes exhibit remarkable electrochromic performances,e.g.,superior cycling stability(more than 2000 cycles),rich color variations(more than 5 colors for PANI@SnO_(2)),and enlarged optical *** excellent performances account for the heterogenous porous nanoarrays,which not only facilitate the intercalation/extraction of ions but also relieve the stress generated during the electrochemical *** addition,diverse prototypes of complementary multicolor ECD with excellent cycling stability(over thousands of cycles)and rich color variations(8 colors)were realized for the first *** believe that our work put forward a general strategy for developing high-quality multicolor complementary electrochromic devices.

关键词： electrochromism tin oxide metal oxide cycling stability multicolor complementary device