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The first chiral cerium halide towards circularly-polarized luminescence in the UV region

Science China chemistry 2024年第6期67卷 1961-1968页

作者： Xinyi Niu Zhichao Zeng Zhaoyu Wang Haolin Lu Bing Sun Hao-Li Zhang Yongsheng Chen Yaping Du Guankui Long Tianjin Key lab.for Rare Earth Materials and Applications Renewable Energy Conversion and Storage CenterSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China Tianjin Key lab.for Rare Earth Materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China State Key lab.ratory of Applied Organic chemistry Key Laboratory of Special Function Materials and Structure Design(Ministry of Education)College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China The Centre of Nanoscale Science and Technology and State Key lab.ratory of Elemento-Organic chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China

Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting diodes.However,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely reported.To fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/S-MCC.The chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and CPL.The emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV region.Notably,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV CPL.Our work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral OIHMH.The RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.

关键词： chiral rare-earth halide ultraviolet circularly-polarized luminescence d-f transition rare-earth halide perovskite chiral perovskite

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Production of the C/TiO_(2)composite with a high-performance electrochemical property from titanium-rich sludge via in-situ C coating

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Journal of Environmental Sciences 2024年第3期137卷 131-143页

作者： Hualong Wu Yanxia Zhao Jiexi Wang Xiaoyan Li Kaimin Shih Xuguang Li Wei Liu School of Water Conservancy and Environment University of JinanJinan 250022China State Key lab.of Physical chemistry of Solid Surface Collaborative Innovation Center of Chemistry for Energy MaterialsCollege of MaterialsXiamen UniversityXiamen 361005China School of Metallurgy and Environment Central South UniversityChangsha 410083China Department of Civil Engineering The University of Hong KongPokfulamHong KongChina Institute of Environment and Ecology Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China

Resource recycling from waste-water and sludge is an important part of the 14th Five-Year Plan in China.The emerging titanium-based coagulants have drawn growing attentions due to their strong coagulation capability in water purification and value-added Ti-loaded sludge production.Management and recovery of the high value-added sludge into functional nanomaterials is highly significant for both sludge reduction and environmental remediation.The present study was carried out to investigate the recycle of the coagulated Ti-loaded sludge to produce functional C/TiO_(2)composites as the anode materials for lithium-ion batteries(LIBs).It is the first time that the application of the Ti-loaded wastewater sludge derived C/TiO_(2)was evaluated for LIBs.The experimental results showed that the carbon coating through in-situ carbonization of the sludge produced the C/TiO_(2)composites with a high specific surface area,stable structural integrity,and excellent electrochemical properties that would facilitate Li+diffusion in long-term LIBs usage.The C/TiO_(2)composites calcinated from the polytitanium sulfate-coagulated sludge at 800℃(N_(2))exhibited the best electrochemical performance during the cycling tests(601 m Ah/g at 100 m A/g after 200 cycles).The research work demonstrates the promising prospect of the recycle and value-added utilization of the Ti-loaded sludge in the production of high-performance C/TiO_(2)composites for energy storage applications.This study provides a new way for the management and reuse of Ti-loaded waste-sludge.

关键词： Sludge recovery Ti-loaded sludge In-situ coating Lithium-ion battery

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A novel Tb^(3+) and Eu^(3+) co-doped dual-emitting phosphate K_(3)SrBi(P_(2)O_(7))_(2) phosphor for application in FIR thermometers

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Journal of Rare Earths 2024年第3期42卷 455-463,I0001页

作者： Baochen Wang Shifeng Sun Zeqi Li Zongwang Li Weiwei Lin Chao Zeng Yan-gai Liu Ruiyu Mi School of Chemical and Environmental Engineering Anhui Polytechnic UniversityWuhu241000China State-Province Joint Engineering lab.ratory of Zeolite Membrane Materials Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationInstitute of Advanced MaterialsCollege of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang330022China Beijing Key lab.ratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of GeosciencesBeijing100083China

Rare earth co-doped phosphor for fluorescence intensity ratio(FIR) thermometer has gained increasing attention in recent years. Herein, the novel Tb^(3+)and Eu^(3+)co-doped K_(3)SrBi(P_(2)O_(7))_(2)(KSBP) phosphate phosphors were reported. The crystal structure of the title phosphor was determined using Rietveld refinement and proved to have a three-dimensional structure. The time-resolved spectroscopy reveals that there is almost no energy transfer between Tb^(3+)and Eu^(3+). More importantly, Tb^(3+)and Eu^(3+)emissions show different thermal quenching behaviors, which claims the potential of this material for application in optical thermometer. The FIR of the typical KSBP:0.02Tb^(3+),0.04Eu^(3+)sample demonstrates a polynomial relationship as a function of temperature and the absolute and relative sensitivity are0.025 K^(-1) and 0.59%/K, respectively. In general, our study reports a novel and potential KSBP:Tb^(3+),Eu^(3+)phosphate phosphor that is promising for use in high-sensitive FIR thermometers.

关键词： Phosphor Thermometer Fluorescence intensity ratio Thermal stability Rare earths

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Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn‑Based MXene/ MAX Hybrids

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Nano-Micro Letters 2024年第5期16卷 154-168页

作者： Xinyu Dai Zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui Li Yang Fu Baohua Jia Lei Zhang Wenhui Fang Jieshan Qiu Tianyi Ma Key lab.ratory for Green Synthesis and Preparative chemistry of Advanced Materials of Liaoning Province College of ChemistryInstitute of Clean Energy ChemistryLiaoning UniversityShenyang 110036People’s Republic of China State Key lab.ratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China School of chemistry and Chemical Engineering Anhui UniversityHefei 230601People’s Republic of China School of Chemical Engineering The University of AdelaideAdelaideSA 5005Australia State Key lab.ratory of High‑Efficiency Utilization of Coal and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaPeople’s Republic of China School of Science RMIT UniversityMelbourneVIC 3000Australia Guangdong Provincial Key lab.ratory of Advanced Energy Storage Materials School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China College of Chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalab.e green ammonia production.However,relevant out-lab.research is still in its infancy.Herein,a novel Sn-based MXene/MAX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC MAX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 reduction.Due to the synergistic effect of MXene/MAX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long durability.Noticeably,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed stock.The as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic analysis.This work is of significance for large-scale green ammonia production.

关键词： Green ammonia synthesis N2 electroreduction Renewable energy Sn MXene/MAX hybrid

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Heterointerface engineering of assembled CoP_(2) on N-modified carbon as efficient trifunctional electrocatalysts for Zn-Air batteries and overall water splitting

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Nano Research 2024年第5期17卷 3801-3809页

作者： Yan Chen Zhenrui Yang Juan Wang Yun Yang Xuedong He Yang Wang Jiadong Chen Yaqing Guo Xin Wang Shun Wang Huile Jin Wenzhou Key lab.of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Zhejiang Engineering Research Center for Electrochemical Energy Materials and Devices Institute of New Materials and Industrial TechnologiesWenzhou UniversityWenzhou 325035China School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingapore 637459Singapore

Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),respectively.In addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air batteries.The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and HER.Density functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of reactions.These electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster reactions.This study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.

关键词： two-dimensional(2D)carbon metal-organic framework cobalt phosphide zinc air battery water splitting

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The initial stages of Li_(2)O_(2) formation during oxygen reduction reaction in Li-O_(2) batteries:The significance of Li_(2)O_(2) in charge-transfer reactions within devices

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Journal of Energy chemistry 2024年第1期88卷 223-231,I0006页

作者： Daniela M.Josepetti Bianca P.Sousa Simone A.J.Rodrigues Renato G.Freitas Gustavo Doubek Advanced Energy Storage Division LABCenter for Innovation on New EnergiesSchool of Chemical EngineeringUniversity of CampinasAv Albert Einstein 50013083-852CampinasSPBrazil Institute of Physics&Department of chemistry Laboratory of Computational MaterialsFederal University of Mato Grosso78060-900CuiabáMTBrazil

Lithium-oxygen batteries are a promising technology because they can greatly surpass the energy density of lithium-ion batteries.However,this theoretical characteristic has not yet been converted into a real device with high cyclab.lity.Problems with air contamination,metallic lithium reactivity,and complex discharge and charge reactions are the main issues for this technology.A fast and reversible oxygen reduction reaction(ORR)is crucial for good performance of secondary batteries',but the partial knowledge of its mechanisms,especially when devices are concerned,hinders further development.From this perspective,the present work uses operando Raman experiments and electrochemical impedance spectroscopy(EIS)to assess the first stages of the discharge processes in porous carbon electrodes,following their changes cycle by cycle at initial operation.A growth kinetic formation of the discharge product signal(Li_(2)O_(2))was observed with operando Raman,indicating a first-order reaction and enabling an analysis by a microkinetic model.The solution mechanism in the evaluated system was ascribed for an equivalent circuit with three time constants.While the time constant for the anode interface reveals to remain relatively constant after the first discharge,its surface seemed to be more non-uniform.The model indicated that the reaction occurs at the Li_(2)O_(2) surface,decreasing the associated resistance during the initial discharge phase.Furthermore,the growth of Li_(2)O_(2) forms a hetero-phase between Li_(2)O_(2)/electrolyte,while creating a more compact and homogeneous on the Li_(2)O_(2)/cathode surface.The methodology here described thus offers a way of directly probing changes in surface chemistry evolution during cycling from a device through EIS analysis.

关键词： Li-O_(2)battery Operando Raman analysis Equivalent circuit modeling Time-constant distribution

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Spatial tumor biopsy with fluorescence PCR microneedle array

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The Innovation 2024年第1期5卷 26-32页

作者： Xiaoxuan Zhang Guopu Chen Yu Wang Yuanjin Zhao Department of Rheumatology and Immunology Nanjing Drum Tower HospitalSchool of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China Oujiang lab.ratory(Zhejiang lab.for Regenerative Medicine Vision and Brain Health)Wenzhou InstituteUniversity of Chinese Academy of SciencesWenzhou 325001China chemistry and Biomedicine Innovation Center Nanjing UniversityNanjing 210023China

Biopsy is the gold standard for tumor diagnosis,as this technology provides highly detailed and reliable information on tumorigenesis and progression.Resembling the discrete wettability of desert beetles,in this study,a fluorescence polymerase chain reaction(F-PCR)microneedle array(MNA)platform is developed for efficient spatial tumor biopsy.This MNA is fabricated by the coupled strategies of bottom-up self-assembly and top-down photolithography;it comprises a hydrophobic silica nanoparticle-assembled substrate and graphene aerogel-hydrogel hybrid microneedle peaks.Benefitting from the hydrophilicity and absorption capacity of its graphene hybrid microneedle peaks,MNA can easily penetrate tissue specimens and collect tumor nucleic acid biomarkers stereoscopically.In addition,because of the discrete wettability of the platform,both tissue fluids and PCR liquids can be easily removed from the substrate,and each microneedle peak is similar to an independent island for directly conducting F-PCR reactions for tumor marker discovery.Based on these advantages,the F-PCR-MNA platform is demonstrated to be ideal for detecting DNA biomarkers of lung carcinoma in standard solutions,mouse tissue samples,and clinical specimens,thus indicating its practical potential as an innovative tumor biopsy system.

关键词： needle biopsy diagnosis

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Advances in All-Solid-State Lithium-Sulfur Batteries for Commercialization

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Nano-Micro Letters 2024年第9期16卷 209-246页

作者： Birhanu Bayissa Gicha Lemma Teshome Tufa Njemuwa Nwaji Xiaojun Hu Jaebeom Lee Research Institute of Materials chemistry Chungnam National UniversityDaejeon 34134Republic of Korea Institute of Fundamental Technological Research Polish Academy of Sciences02‑106 WarsawPoland School of Life Sciences Shanghai University200444 ShanghaiPeople’s Republic of China Department of chemistry Chungnam National UniversityDaejeon 34134Republic of Korea

Solid-state batteries are commonly acknowledged as the forthcoming evolution in energy storage technologies.Recent development progress for these rechargeable batteries has notably accelerated their trajectory toward achieving commercial feasibility.In particular,all-solid-state lithium-sulfur batteries(ASSLSBs)that rely on lithium-sulfur reversible redox processes exhibit immense potential as an energy storage system,surpassing conventional lithium-ion batteries.This can be attributed predominantly to their exceptional energy density,extended operational lifespan,and heightened safety attributes.Despite these advantages,the adoption of ASSLSBs in the commercial sector has been sluggish.To expedite research and development in this particular area,this article provides a thorough review of the current state of ASSLSBs.We delve into an in-depth analysis of the rationale behind transitioning to ASSLSBs,explore the fundamental scientific principles involved,and provide a comprehensive evaluation of the main challenges faced by ASSLSBs.We suggest that future research in this field should prioritize plummeting the presence of inactive substances,adopting electrodes with optimum performance,minimizing interfacial resistance,and designing a scalab.e fabrication approach to facilitate the commercialization of ASSLSBs.

关键词： All-solid-state lithium-sulfur batteries Commercialization Enhancement strategies Solid-state electrolytes Sulfurbased cathodes

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Progress in MXene-based catalysts for oxygen evolution reaction

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Electron 2024年第1期2卷 48-67页

作者： Jieli Chen Xiaohong Gao Jing Li Zhenye Kang Juan Bai Tianjiao Wang Yuliang Yuan Chenghang You Yu Chen Bao Yu Xia Xinlong Tian School of marine Science and Engineering Hainan Provincial Key Lab of Fine ChemistrySchool of Chemistry and Chemical EngineeringHainan UniversityHaikouChina School of chemistry and Physics Queensland University of TechnologyBrisbaneQueenslandAustralia Key lab.ratory of Macromolecular Science of Shaanxi Province School of Materials Science and EngineeringShaanxi Normal UniversityXi'anChina School of chemistry and Chemical Engineering State Key Laboratory of Materials Processing and Die&Mould TechnologyKey Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education)Hubei Key Laboratory of Material Chemistry and Service FailureWuhan National Laboratory for OptoelectronicsHuazhong University of Science and Technology(HUST)WuhanChina

Electrochemical water splitting for hydrogen generation is considered one of the most promising strategies for reducing the use of fossil fuels and storing renewable electricity in hydrogen fuel.However,the anodic oxygen evolution process remains a bottleneck due to the remarkably high overpotential of about 300 mV to achieve a current density of 10 mA cm^(−2).The key to solving this dilemma is the development of highly efficient catalysts with minimized overpotential,long-term stability,and low cost.As a new 2D material,MXene has emerged as an intriguing material for future energy conversion technology due to its benefits,including superior conductivity,excellent hydrophilic properties,high surface area,versatile chemical composition,and ease of processing,which make it a potential constituent of the oxygen evolution catalyst layer.This review aims to summarize and discuss the recent development of oxygen evolution catalysts using MXene as a component,emphasizing the synthesis and synergistic effect of MXene-based composite catalysts.Based on the discussions summarized in this review,we also provide future research directions regarding electronic interaction,stability,and structural evolution of MXene-based oxygen evolution catalysts.We believe that a broader and deeper research in this area could accelerate the discovery of efficient catalysts for electrochemical oxygen evolution.

关键词： MXene-based catalysts oxygen evolution reaction water splitting

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Steric hindrance modulation of hexaazatribenzanthraquinone isomers for high-capacity and wide-temperature-range aqueous proton battery

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National Science Review 2024年第4期11卷 271-282页

作者： Mingsheng Yang Yuxin Hao Bei Wang Yan Wang Liping Zheng Rui Li Huige Ma Xinyu Wang Xiaoming Jing Hongwei Li Mengxiao Li Zhihui Wang Yujie Dai Guangcun Shan Mingjun Hu Jun Luo Jun Yang School of Materials Science and Engineering Beihang University Beijing Institute of Nanoenergy &Nanosystems Chinese Academy of Sciences Center on Nanoenergy Research School of Physical Science & TechnologyGuangxi University School of chemistry and Chemical Engineering Center on Nanoenergy Research Guangxi University School of Instrumentation Science and Opto-electronics Engineering Beihang University ShenSi lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of China

Organic materials with rich active sites are good candidates of high-capacity anodes in aqueous batteries,but commonly low utilization of active sites limits their capacity.Herein,two isomers,symmetric and asymmetric hexaazatribenzanthraquinone（s-HATBAQ and a-HATBAQ）,with rich active sites have been synthesized in a controllab.e manner.It has been revealed for the first time that a sulfuric acid catalyst can facilitate the stereoselective formation of s-HATBAQ.Attributed to the reduced steric hindrance in favor of proton insertion as well as the amorphous structure conducive to electrochemical dynamics,s-HATBAQ exhibits 1.5 times larger specific capacity than a-HATBAQ.Consequently,the electrode of s-HATBAQ with50% reduced graphene oxide（s-HATBAQ-50%rGO） delivers a record high specific capacity of405 mAh g-1in H2SO4electrolyte.Moreover,the assembled MnO2//s-HATBAQ-50%rGO aqueous proton full batteries show an exceptional cycling stability at 25℃ and can maintain ～92% capacity after1000 cycles at 0.5 A g-1at-80℃.This work demonstrates the controllab.e synthesis of isomers,showcases a wide-temperature-range prototype proton battery and highlights the significance of precise mole cular structure modulation in organic energy storage.

关键词： stereoisomers steric effect aqueous battery super cycling stability ultra-low temperature proton battery

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