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Low-melting mixture solvents: extension of deep eutectic solvents and ionic liquids for broadening green solvents and green chemistry

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Green Chemical Engineering 2024年第04期 409-417页

作者： Yu Chen Zhiwu Yu MOE Key Laboratory of Bioorganic Phosphorous chemistry and Chemical Biology Department of ChemistryTsinghua University

Green solvents such as water and ionic liquids(ILs) are pillars of the great mansion of green chemistry and green processing. Initially proposed as a new family of ILs,deep eutectic solvents(DESs) have received fast development in the past two decades. In this contribution,DESs are reviewed critically and the concept is extended to lowmelting mixture solvents(Lo MMSs),which cover all kinds of materials including ionic compounds,molecular compounds,and metals. Six classes of Lo MMSs are proposed as the new classification system and examples are given. Finally,several thermodynamic issues concerning Lo MMSs are discussed. Two new concepts,robustness of Lo MMSs and high-entropy Lo MMSs,are proposed.

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Electric-field-controlled highly regioselective thiocyanation of N-containing heterocycles

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Science China chemistry 2024年第4期67卷 1263-1269页

作者： Ming Gong Qian Wu Jung Keun Kim Mengmeng Huang Yabo Li Yangjie Wu Jong Seung Kim Henan Key Laboratory of Chemical Biology and Organic chemistry Key Laboratory of Applied Chemistry of Henan UniversitiesCollege of ChemistryZhengzhou UniversityZhengzhou 450052China Department of chemistry Korea UniversitySeoul 02841Korea

Achieving highly regioselective synthesis in organic chemistry is challenging due to the uncontrollable orientation between reacting *** electric fields(EEFs)can influence the reactivity and selectivity of the substrate by causing directional ***,scalable and efficient techniques for using EEFs as“smart catalysts”have been lacking,hindering their *** this study,we present a novel method for modifying the regioselectivity of quinoxaline-2(1H)-ones by functionalizing their C7-position using the electric double layer(EDL)*** approach led to moderate to good yields of the corresponding C7-thiocyanation *** calculations and control experiments demonstrated that EEFs could reverse the regioselectivity of quinoxaline-2(1H)-ones,allowing the C7-thiocyanation to proceed via a radical reaction ***,the resulting 7-thiocyano-1-methylquinoxaline-2(1H)-ones exhibited promising AIE *** work showcases a promising strategy for achieving highly regioselective functionalization by aligning the electric field with the desired reaction/bond axis.

关键词： electric fields reaction-axis rule electric double layer C7-thiocyanation C-S bond formation

Lithium Sulfur Batteries:Insights from Solvation chemistry to Feasibility Designing Strategies for Practical Applications

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Energy & Environmental Materials 2024年第4期7卷 5-27页

作者： Jian Tan Longli Ma Yuan Wang Pengshu Yi Chuming Ye Zhan Fang Zhiheng Li Mingxin Ye Jianfeng Shen Institute of Special Materials and Technology Fudan University Department of Materials Science Fudan University Department of chemistry Fudan University

Rechargeable lithium-sulfur (Li-S) batteries,featuring high energy density,low cost,and environmental friendliness,have been dubbed as one of the most promising candidates to replace current commercial rechargeable Li-ion ***,their practical deployment has long been plagued by the infamous"shuttle effect"of soluble Li polysulfides (LiPSs) and the rampant growth of Li dendrites.

关键词： characterization tools design strategies Li–S batteries practical applications solvation chemistry

Emerging perovskite materials for supercapacitors:Structure,synthesis,modification,advanced characterization,theoretical calculation and electrochemical performance

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Journal of Energy chemistry 2024年第2期89卷 41-70,I0003页

作者： Yuehua Qian Qingqing Ruan Mengda Xue Lingyun Chen Department of Applied chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China

As a new generation electrode materials for energy storage,perovskites have attracted wide attention because of their unique crystal structure,reversible active sites,rich oxygen vacancies,and good *** this review,the design and engineering progress of perovskite materials for supercapacitors(SCs)in recent years is ***,the review will focus on four types of perovskites,perovskite oxides,halide perovskites,fluoride perovskites,and multi-perovskites,within the context of their intrinsic structure and corresponding electrochemical performance.A series of experimental variables,such as synthesis,crystal structure,and electrochemical reaction mechanism,will be carefully analyzed by combining various advanced characterization techniques and theoretical *** applications of these materials as electrodes are then featured for various ***,we look forward to the prospects and challenges of perovskite-type SCs electrodes,as well as the future research direction.

关键词： Perovskite Modification engineering Oxygen vacancy Theoretical calculation methodology Supercapacitor

Micro/nanoelectrode-based electrochemical methodology for single cell and organelle analysis

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Nano Research 2024年第1期17卷 196-206页

作者： Chuchu Xu De Yang Yuchan Wang Ruolin Liu Fan Wang Zhongqun Tian Keke Hu Department of chemistry College of Chemistry&Chemical EngineeringXiamen UniversityXiamen 361005China

Cells are the basic unit of *** analysis of single cells/organelles is essential for uncovering the molecular mechanisms of physiological and pathological processes that are difficult to elucidate on a larger *** paper provides an overview of the commonly used fabrication methods for micro/nanoelectrodes applied in the investigations of single cells/organelles as well as the corresponding electrochemical measurements over the last four years including extracellular measurement,combination of extra and intracellular measurement,intracellular reactive oxygen species and reactive nitrogen species(ROS/RNS)measurement,and isolated organelles measurement.

关键词： single cell/organelle micro/nanoelectrode electrochemical measurement chemical transmitters

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 *** 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 *** 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

Intracellular redox potential-driven live-cell synthesis of CdSe quantum dots in Staphylococcus aureus

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Science China chemistry 2024年第3期67卷 990-999页

作者： Cai-Qin Wu An-An Liu Xu Li Jia-Wei Tu Juan Kong Ling-Ling Yang Jian-Hong Jia Chuan Wang Bin Hu Zhi-Xiong Xie Dai-Wen Pang The Institute for Advanced Studies College of Chemistry and Molecular SciencesCollege of Life SciencesHubei Key Laboratory of Cell HomeostasisWuhan UniversityWuhan 430072China Research Center for Analytical Sciences College of ChemistryState Key Laboratory of Medicinal Chemical BiologyTianjin Key Laboratory of Biosensing and Molecular RecognitionFrontiers Science Center for New Organic MatterFrontiers Science Center for Cell Responsesand Haihe Laboratory of Sustainable Chemical TransformationsNankai UniversityTianjin 300071China

Biosynthesized semiconductor quantum dots(QDs) have bright fluorescence,adjustable particle sizes,and environmental friendliness,endowing them with convenience and potential for biological *** to the unclear mechanism of the cellular environment on the live-cell synthesis of QDs,it is still difficult to regulate their optical ***,the critical role of the intracellular redox environment in regulating the fluorescence properties of biosynthesized CdSe QDs in Staphylococcus aureus(***) has been *** glutathione peroxidase(GPx) activity directly affects the intracellular H_(2)O_(2) produced in the SeO_(3)^(2-) reduction,which further manipulates the glutathione redox cycle to determine the content of low-valence *** a result,the fluorescence intensity of the synthesized CdSe QDs increases by 60% in the GPx overexpressed *** cellular redox potential that is controlled by the GSH redox cycle provides the driving force for the reduction of SeO_(3)^(2-),facilitating the synthesis of CdSe QDs in *** *** proposed mechanism of the cellular redox state provides a new perspective for regulating the synthesis of semiconductor nanomaterials in live cells.

关键词： redox H_(2)O_(2) peroxidase quantum dot Staphylococcus aureus

Intramolecular Hydrogen Bond Improved Durability and Kinetics for Zinc‑Organic Batteries

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Nano-Micro Letters 2024年第3期16卷 138-148页

作者： Tianjiang Sun Jun Pan Weijia Zhang Xiaodi Jiang Min Cheng Zhengtai Zha Hong Jin Fan Zhanliang Tao Key Laboratory of Advanced Energy Materials chemistry(Ministry of Education) Renewable Energy Conversion and Storage CenterCollege of ChemistryNankai UniversityHaihe Laboratory of Sustainable Chemical TransformationsTianjin 300071People’s Republic of China School of Physical and Mathematical Sciences Nanyang Technological UniversitySingapore 637371Singapore Shanghai Key Laboratory of Special Artificial Microstructure Materials and Technology School of Physics Science and EngineeringTongji UniversityShanghai 200092People’s Republic of China

Organic compounds have the advantages of green sustainability and high designability,but their high solubility leads to poor durability of zinc-organic ***,a high-performance quinone-based polymer(H-PNADBQ)material is designed by introducing an intramolecular hydrogen bonding(HB)*** intramolecular HB(C=O⋯N-H)is formed in the reaction of 1,4-benzoquinone and 1,5-naphthalene diamine,which efficiently reduces the H-PNADBQ solubility and enhances its charge transfer in *** situ ultraviolet-visible analysis further reveals the insolubility of H-PNADBQ during the electrochemical cycles,enabling high durability at different current ***,the H-PNADBQ electrode with high loading(10 mg cm^(-2))performs a long cycling life at 125 mA g^(-1)(>290 cycles).The H-PNADBQ also shows high rate capability(137.1 mAh g^(−1)at 25 A g^(−1))due to significantly improved kinetics inducted by intramolecular *** work provides an efficient approach toward insoluble organic electrode materials.

关键词： Zn-organic batteries H-PNADBQ polymer Intramolecular hydrogen bond Reduced solubility Improvedπ-conjugated level

Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds

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Nano Research 2024年第1期17卷 228-234页

作者： Pengyao You Shaoqi Zhan Pengpeng Ruan Ruixuan Qin Shiguang Mo Yazhou Zhang Kunlong Liu Lansun Zheng Nanfeng Zheng State Key Laboratory for Physical chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Department of chemistry BMCUppsala UniversityBMC Box 576Uppsala S-75123Sweden Department of chemistry University of OxfordOxford OX13QZUK

The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired ***,the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites(e.g.,metal,support,and metal/support interface).Here we develop a structurally controllable catalyst system(Pd/SBA-15)to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model *** investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone ***,oxidized Pd species were catalytically highly active for acetophenone *** catalytic activity decreased with the decreased oxidation state of *** work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds,e.g.,nitrobenzene,N-benzylidene-benzylamine,and carbon dioxide.

关键词： oxidized Pd metal/oxide interface constant particle size Pd/SBA-15 acetophenone hydrogenation