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An effective'salt in dimethyl sulfoxide/water'electrolyte enables high-voltage supercapacitor operated at-50℃

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Journal of Energy chemistry 2024年第6期93卷 361-367,I0009页

作者： Yingbin Liu Chang Yu Xuedan Song Siyi Hou Shuqin Lan Jinhe Yu Yuanyang Xie Jieshan Qiu State Key lab.of Fine Chemicals Frontier Science Center for Smart MaterialsSchool of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina School of chemistry Frontier Science Center for Smart MaterialsLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina College of Chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in supercapacitors.However,challenges remain for low-salt aqueous electrolytes operating at high voltage and low temperature.Herein,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid electrolyte.Furthermore,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid electrolyte.When paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 V.This modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.

关键词： Dimethyl sulfoxide Co-solvent High voltage Low temperature Supercapacitors

A Review of Rechargeable Zinc-Air Batteries:Recent Progress and Future Perspectives

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Nano-Micro Letters 2024年第7期16卷 358-401页

作者： Ghazanfar Nazir Adeela Rehman Jong-Hoon Lee Choong-Hee Kim Jagadis Gautam Kwang Heo Sajjad Hussain Muhammad Ikram Abeer AAlObaid Seul-Yi Lee Soo-Jin Park Department of Nanotechnology and Advanced Materials Engineering Hybrid Materials Research Center(HMC)Sejong UniversitySeoul 05006Republic of Korea Department of Chemical and Biomolecular Engineering Yonsei University50 Yonsei-RoSeodaemun-GuSeoul 03722Republic of Korea Department of chemistry Inha UniversityIncheon 22212Republic of Korea Solar Cell Applications Research lab Department of PhysicsGovernment College University LahoreLahore 54000 PunjabPakistan Department of chemistry College of ScienceKing Saud UniversityP.O.Box 2455Riyadh 11451Saudi Arabia

Zinc-air batteries(ZABs)are gaining attention as an ideal option for various applications requiring high-capacity batteries,such as portable electronics,electric vehicles,and renewable energy storage.ZABs offer advantages such as low environmental impact,enhanced safety compared to Li-ion batteries,and cost-effectiveness due to the abundance of zinc.However,early research faced challenges due to parasitic reactions at the zinc anode and slow oxygen redox kinetics.Recent advancements in restructuring the anode,utilizing alternative electrolytes,and developing bifunctional oxygen catalysts have significantly improved ZABs.Scientists have achieved battery reversibility over thousands of cycles,introduced new electrolytes,and achieved energy efficiency records surpassing 70%.Despite these achievements,there are challenges related to lower power density,shorter lifespan,and air electrode corrosion leading to performance degradation.This review paper discusses different battery configurations,and reaction mechanisms for electrically and mechanically rechargeable ZABs,and proposes remedies to enhance overall battery performance.The paper also explores recent advancements,applications,and the future prospects of electrically/mechanically rechargeable ZABs.

关键词： Zinc-air batteries Energy storage Affordability Reversibility

Copper-induced formation of heterostructured Co_(3)O_(4)/CuO hollow nanospheres towards greatly enhanced lithium storage performance

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Chinese Chemical Letters 2024年第2期35卷 594-598页

作者： Junjun Zhang Huiying Lu Tianhao Yao Xin Ji Qingmiao Zhang Lingjie Meng Jianmin Feng Hongkang Wang College of Geography & Environment Xianyang Normal UniversityXianyang 712000China State Key lab.of Electrical Insulation and Power Equipment Center of Nanomaterials for Renewable Energy (CNRE)School of Electrical EngineeringXi'an Jiaotong UniversityXi'an 710049China School of chemistry Xi'an Key Laboratory of Sustainable Energy Material Chemistryand Instrumental Analysis CenterXi'an Jiaotong UniversityXi'an 710049China

We report a facile template-free fabrication of heterostructured Co_(3)O_(4)/CuO hollow nanospheres using pre-synthesized Co/Cu-glycerate as conformal precursor.The introduction of copper nitrate in the solvothermal reaction system of glycerol/isopropanol/cobalt nitrate readily induces the conversion from solid Co-glycerate to hollow Co/Cu-glycerate nanospheres,and the effect of the Co/Cu atomic ratio on the structure evolution of the metal glycerates as well as their corresponding oxides were investigated.When examined as anode materials for lithium-ion batteries,the well-defined Co_(3)O_(4)/CuO hollow nanospheres with Co/Cu molar ratio of 2.0 demonstrate excellent lithium storage performance,delivering a high reversible capacity of 930 mAh/g after 300 cycles at a current density of 0.5 A/g and a stable capacity of 650 mAh/g after 500 cycles even at a higher current density of 2.0 A/g,which are much better than their counterparts of bare CuO and Co_(3)O_(4).The enhanced lithium storage performance can be attributed to the synergistic effect of the CuO and Co_(3)O_(4)heterostructure with hollow spherical morphology,which greatly enhances the charge/electrolyte transfer and effectively buffers the volume changes upon lithiation/delithiation cycling.

关键词： Lithium-ion batteries Co/Cu-glycerate Hollow nanospheres Co_(3)O_(4)/CuO heterostructure Electrochemical properties

Enabling heterogeneous catalysis to achieve carbon neutrality: Directional catalytic conversion of CO_(2) into carboxylic acids

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Carbon Energy 2024年第3期6卷 1-35页

作者： Xiaofei Zhang Wenhuan Huang Le Yu Max García-Melchor Dingsheng Wang Linjie Zhi Huabin Zhang KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)ThuwalSaudi Arabia Key lab.ratory of Chemical Additives for China National Light Industry College of Chemistry and Chemical EngineeringShaanxi University of Science and TechnologyXi'anChina State Key lab.of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijingChina School of chemistry CRANN and AMBERResearch CentresTrinity College DublinCollege GreenDublinIreland Department of chemistry Tsinghua UniversityBeijingChina Advanced Chemical Engineering and Energy Materials Research Center China University of Petroleum(East China)QingdaoChina

The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elab.rate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.

关键词： carbon neutrality carboxylic acids CO_(2)conversion heterogeneous catalyst in situ technology

Polyphenol-mediated interfacial deposition strategy for supported manganese oxide catalysts with excellent pollutant degradation performance

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Chinese Chemical Letters 2024年第5期35卷 493-498页

作者： Dong Cheng Youyou Feng Bingxi Feng Ke Wang Guoxin Song Gen Wang Xiaoli Cheng Yonghui Deng Jing Wei The Key lab.ratory of Biomedical Information Engineering of Ministry of Education State Key Lab of Transducer TechnologySchool of Life Science and TechnologyXi’an Jiaotong UniversityXi’an 710049China School of Environmental and Municipal Engineering Xi’an University of Architecture and TechnologyXi’an 710055China Department of chemistry State Key Laboratory of Molecular Engineering of PolymersState Key Laboratory of Transducer TechnologyFudan UniversityShanghai 200433China Key lab.ratory of Functional Inorganic Material chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China

In persulfate-based advanced oxidation process(PS-AOPs),fixing nanosized metal oxide on processable substrates is highly desirable to avoid the aggregation and loss of nanocatalysts during the practical application.However,it is still challenging to develop a versatile strategy for the deposition of metal oxide nanocatalysts on various substrates with different physicochemical properties.Herein,polyphenols are utilized as a“molecular glue”and reductant to mediate the interfacial deposition of MnO_(2) nanocatalysts on different substrates.MnO_(2) nanocatalysts were in-situ grown on macroscope mineral substrates(e.g.,airstone)via an interfacial redox strategy between tannic acid(TA)and oxidized KMnO4,and then employed as a fixed catalyst of peroxymonosulfate(PMS)activation for treating pharmaceutical and personal care products(PPCPs)in water.The fixed MnO_(2) exhibited superior catalytic performance toward different PPCPS via a singlet oxygen(^(1)O_(2))-dominated nonradical oxidation pathway.PPCPs in the secondary effluent of wastewater treatment plants could be effectively removed by a fixed-bed column of the fixed MnO_(2) with long term stability.Redox cycle of Mn^(4+)/Mn^(3+)and surface hydroxyl group of the fixed MnO_(2) was proved to be responsible for the activation of PMS.This work provides a new avenue for developing fixed metal oxides for sustainable water treatment.

关键词： Redox strategy Manganese oxides Fixed catalyst Peroxymonosulfate PPCPs

Recycling of waste aluminum scraps to fabricate sulfidated zero-valent iron-aluminum particles for enhanced chromate removal

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Journal of Environmental Sciences 2024年第4期138卷 650-659页

作者： Yahui Zhang Liguo Zhang Jiajia Zeng Shuqun Xu Jianyu Pan Wenzhuo Huang Jianliang Sun Feng Jiang Guangdong Provincial Key lab.ratory of Chemical Pollution and Environmental Safety&MOE Key lab.ratory of Theoretical chemistry of Environment School of EnvironmentSouth China Normal UniversityGuangzhou 510006China Guangdong Provincial Key lab.of Environmental Pollution Control and Remediation Technology School of Environmental Science&EngineeringSun Yat-Sen UniversityGuangzhou 510275China

Massive waste aluminum scraps produced from the spent aluminum products have high electron capacity and can be recycled as an attractive alternative to materials based on zerovalent iron(Fe^(0))for the removal of oxidative contaminants from wastewater.This study thus proposed an approach to fabricate micron-sized sulfidated zero-valent iron-aluminum particles(S-Al^(0)@Fe^(0))with high reactivity,electron selectivity and capacity using recycled waste aluminum scraps.S-Al^(0)@Fe^(0)with a three-layer structure contained zero-valent aluminum(Al^(0))core,Fe^(0) middle layer and iron sulfide(FeS)shell.The rates of chromate(Cr(Ⅵ))removal by S-Al^(0)@Fe^(0)at pH 5.0-9.0 were 1.6-5.9 times greater than that by sulfidated zero-valent iron(S-Fe^(0)).The Cr(Ⅵ)removal capacity of S-Al^(0)@Fe^(0)was 8.2-,11.3-and 46.9-fold greater than those of S-Fe0,zero-valent iron-aluminum(Al^(0)-Fe^(0))and Fe^(0),respectively.The chemical cost of S-Al^(0)@Fe^(0) for the equivalent Cr(Ⅵ)removal was 78.5%lower than that of S-Fe^(0).Negligible release of soluble aluminum during the Cr(Ⅵ)removal was observed.The significant enhancement in the reactivity and capacity of S-Al^(0)@Fe^(0)was partially ascribed to the higher reactivity and electron density of the Al0core than Fe^(0).More importantly,S-Al^(0)@Fe^(0) served as an electric cell to harness the persistent and selective electron transfer from the Al^(0)-Fe^(0) core to Cr(Ⅵ)at the surface via coupling Fe^(0)-Fe^(2+)-Fe^(3+)redox cycles,resulting in a higher electron utilization efficiency.Therefore,S-Al^(0)@Fe^(0) fabricated using recycled waste aluminum scraps can be a cost-effective and environmentally-friendly alternative to S-Fe^(0) for the enhanced removal of oxidative contaminants in industrial wastewater.

关键词： Recycled waste aluminum scraps Oxidative contaminants Cr(Ⅵ)reduction Sulfidated Al^(0)@Fe^(0)particle Electron transfer

Asymmetric Two-Component Alkenyl Catellani Reaction for the Construction of C—N Axial Chirality

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Chinese Journal of chemistry 2024年第7期42卷 699-704页

作者： Chenggui Wu Ze-Shui Liu Yong Shang Chang Liu Shuang Deng Hong-Gang Cheng Hengjiang Cong Yinchun Jiao Qianghui Zhou Sauvage Center for Molecular Sciences Engineering Research Center of Organosilicon Compounds&Materials(Ministry of Education)Hubei Key Lab on Organic and Polymeric OptoElectronic MaterialsCollege of Chemistry and Molecular SciencesThe Institute for Advanced Studiesand TaiKang Center for Life and Medical SciencesWuhan UniversityWuhanHubei 430072China Key lab.ratory of Xin'an Medicine Ministry of EducationAnhui University of Chinese MedicineHefeiAnhui 230038China School of chemistry and Chemical Engineering Hunan University of Science and TechnologyXiangtanHunan 411201China

Herein,we report an asymmetric two-component alkenyl Catellani reaction for the construction of C—N axial chirality through a palladium/chiral norbornene cooperative catalysis and an axial-to-axial chirality transfer process.Various partially aromatic iodinated 2-pyridones,quinolones,coumarin and uracil substrates react with 2,6-disubstituted aryl bromides with a tethered amide group,to afford a wide variety of polycyclic C—N atropisomers(38 examples,up to 97%e.e.).The obtained C—N axial chirality originates from the preformed transient C—C axial chirality with high fidelity.The synthetic utility of this chemistry is demonstrated by facile prepa-ration of complex quinoline and pyridine based C—N atropisomers through a N-deprotection and aromatization sequence.In addi-tion,a remote axial-to-central diastereoinduction process dictated by C—N axial chirality is observed with excellent diastereocontrol.

关键词： Alkenyl Catellani reaction Asymmetric catalysis Atropisomerism Axial-to-axial chirality transfer Heterocycles

Copper(Ⅰ)-catalyzed interrupted click/radical relay:A four-component modular synthesis of triazole sulfones

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Chinese Chemical Letters 2024年第3期35卷 247-251页

作者： Pengfei Sun Fang Wei Chen-Ho Tung Zhenghu Xu Key lab.for Colloid and Interface chemistry of Education Ministry Shandong UniversityJi'nan 250100China State Key lab.ratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Functional Molecules of Zhejiang Province School of ScienceWestlake UniversityHangzhou 310024China Key lab.ratory of Organic chemistry in Jiangxi Province Institute of Organic ChemistryJiangxi Science&Technology Normal UniversityNanchang 330013China

A new,four component copper(Ⅰ)-catalyzed interrupted click/radical relay cascade has been developed.This unprecedented interrupted click reaction provides a rapid modular synthesis of triazole sulfones,important privileged heterocyclic pharmacophores which cannot be accessed by a traditional click reaction.Radical interception of cuprate-triazole,the key reaction intermediate formed in situ,is an important feature of this process.

关键词： Click reaction Triazole Sulfone Radical relay

Building Feedback-Regulation System Through Atomic Design for Highly Active SO_(2)Sensing

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Nano-Micro Letters 2024年第7期16卷 343-357页

作者： Xin Jia Panzhe Qiao Xiaowu Wang Muyu Yan Yang Chen Bao-Li An Pengfei Hu Bo Lu Jing Xu Zhenggang Xue Jiaqiang Xu NEST lab Department of ChemistryCollege of SciencesShanghai UniversityShanghai 200444People’s Republic of China Shanghai Synchrotron Radiation Facility Zhangjiang LabShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204People’s Republic of China School of chemistry and Materials Science University of Science and Technology of ChinaHefei 230026People’s Republic of China Key lab.ratory of Organic Compound Pollution Control Engineering(MOE) School of Environmental and Chemical EngineeringShanghai UniversityShanghai 200444People’s Republic of China Shanghai University Instrumental Analysis&Research Center of Shanghai UniversityShanghai 200444People’s Republic of China

Reasonably constructing an atomic interface is pronouncedly essential for surface-related gas-sensing reaction.Herein,we present an ingen-ious feedback-regulation system by changing the interactional mode between single Pt atoms and adjacent S species for high-efficiency SO_(2)sensing.We found that the single Pt sites on the MoS_(2)surface can induce easier volatiliza-tion of adjacent S species to activate the whole inert S plane.Reversely,the activated S species can provide a feedback role in tailoring the antibonding-orbital electronic occupancy state of Pt atoms,thus creating a combined system involving S vacancy-assisted single Pt sites(Pt-Vs)to synergistically improve the adsorption ability of SO_(2)gas molecules.Further-more,in situ Raman,ex situ X-ray photoelectron spectroscopy testing and density functional theory analysis demonstrate the intact feedback-regulation system can expand the electron transfer path from single Pt sites to whole Pt-MoS_(2)supports in SO_(2)gas atmosphere.Equipped with wireless-sensing modules,the final Pt1-MoS_(2)-def sensors array can further realize real-time monitoring of SO_(2)levels and cloud-data storage for plant growth.Such a fundamental understanding of the intrinsic link between atomic interface and sensing mechanism is thus expected to broaden the rational design of highly effective gas sensors.

关键词： Feedback-regulation system Atomic interface SO_(2)sensor Single-atom sensing mechanism Intelligent-sensing array