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Quantitative lithium substitution of carboxyl hydrogens in polyacrylic acid binder enables robust SiO electrodes with durable lithium storage stability

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Journal of Energy chemistry 2024年第10期97卷 352-360,I0007页

作者： Weihua Wang Wenyi Li Siyi Jing Huiping Yang Huiqun Wang Ling Huang Yuxiang Mao Xikun Pang Yudai Huang Li Zhang state key laboratory of Physical chemistry of Solid Surfaces Department of Chemical and Biochemical EngineeringCollege of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy Materials(iChEM)Xiamen UniversityXiamen 361005FujianChina state key laboratory of chemistry and Utilization of Carbon-Based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830017XinjiangChina

The design of advanced binders plays a critical role in stabilizing the cycling performance of large-volume-effect silicon monoxide(SiO)*** the classic polyacrylic acid(PAA)binder,the self-association of-COOH groups in PAA leads to the formation of intramolecular and intermolecular hydrogen bonds,greatly weakening the bonding force of the binder to SiO ***,strengthening the binder-material interaction from the perspective of binder molecular regulation poses a significant ***,a modified PAA-Li_(x)(0.25≤x≤1)binder with prominent mechanical properties and adhesion strength is specifically synthesized for SiO anodes by quantitatively substituting the carboxylic hydrogen with *** appropriate lithium substitution(x=0.25)not only effectively increases the number of hydrogen bonds between the PAA binder and SiO surface owing to charge repulsion effect between ions,but also guarantees moderate entanglement between PAA-Li_x molecular chains through the ion-dipole *** such,the PAA-Li_(0.25)/SiO electrode exhibits exceptional mechanical properties and the lowest volume change,as well as the optimum cycling(1237.3 mA h g^(-1)after 100cycles at 0.1 C)and rate performance(1000.6 mA h g^(-1)at 1 C),significantly outperforming the electrode using pristine PAA *** work paves the way for quantitative regulation of binders at the molecular level.

关键词： Polyacrylic acid binder SiO anode Quantitative lithium substitution Charge repulsion effect Adhesion strength

Construction of metallo-complexes with 2,2′:6′,2″-terpyridine substituted triphenylamine in different modified positions and their photophysical properties

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Chinese Chemical Letters 2024年第7期35卷 301-305页

作者： Shengwen Guan Zhaotong Wei Ningxu Han Yude Wei Bin Xu Ming Wang Junjuan Shi state key laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China

The stable coordinated metallo-complexes based on 2,2′:6′,2″-terpyridine(tpy)and its derivatives have been widely researched for various wide-ranging applications in photoelectronics,catalysis,sensor,photoluminescence,and so ***,the most reported studies ignored the comprehensive comparison between structures modified by different positions and ***,we design a series of metallo-complexes which were assembled with tpy substituted triphenylamine(TPA)at different positions and metal ions and explored their photophysical *** the solution state,MLE_(2)based on the 5,5″-positions modification showed the highest PLQYs and PL *** the increase of solvent polarity,MLB2exhibit the largest *** the solid state,from MLA_(2)to MLE_(2),the emission colours are gradually red-shifted from yellow to *** findings in this work may pave a new way to design functional metallo-complexes,not just for PL properties.

关键词： Metallo-complexes 2,2′:6′,2″-terpyridine Triphenylamine Different modified positions Photophysical properties

Antimony doped CsPbI_(2)Br for high-stability all-inorganic perovskite solar cells

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Nano Research 2024年第3期17卷 1508-1515页

作者： Mengfei Zhu Lina Qin Yuren Xia Junchuan Liang Yaoda Wang Daocheng Hong Yuxi Tian Zuoxiu Tie Zhong Jin state key laboratory of Coordination chemistry Ministry of Education(MOE)Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Nanjing Tieming Energy Technology Co. Ltd.Nanjing 210093China Suzhou Tierui New Energy Technology Co. Ltd.Suzhou 215228China

All-inorganic perovskites,adopting cesium(Cs+)cation to completely replace the organic component of A-sites of hybrid organic–inorganic halide perovskites,have attracted much attention owing to the excellent thermal ***,all-inorganic iodine-based perovskites generally exhibit poor phase stability in ambient ***,we propose an efficient strategy to introduce antimony(Sb^(3+))into the crystalline lattices of CsPbI_(2)Br perovskite,which can effectively regulate the growth of perovskite crystals to obtain a more stable perovskite *** to the much smaller ionic radius and lower electronegativity of trivalent Sb^(3+)than those of Pb^(2+),the Sb^(3+)doping can decrease surface defects and suppress charge recombination,resulting in longer carrier lifetime and negligible *** a result,the all-inorganic perovskite solar cells(PSCs)based on 0.25%Sb^(3+)doped CsPbI_(2)Br light absorber and screen-printable nanocarbon counter electrode achieved a power conversion efficiency of 11.06%,which is 16%higher than that of the control devices without Sb^(3+)***,the Sb^(3+)doped all-inorganic PSCs also exhibited greatly improved endurance against heat and *** to the use of low-cost and easy-to-process nanocarbon counter electrodes,the manufacturing process of the all-inorganic PSCs is very convenient and highly repeatable,and the manufacturing cost can be greatly *** work offers a promising approach to constructing high-stability all-inorganic PSCs by introducing appropriate lattice doping.

关键词： all-inorganic perovskite solar cells Sb doped cesium lead halide perovskites foreign B-site ions hole-conductor-free phase stability improvement

High-rate lithium-ion battery performance of a ternary sea urchin-shaped CoNiO_(2)@NiP_(6)Mo_(18)/CNTs composites

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Journal of Energy chemistry 2024年第9期96卷 516-525页

作者： Li-ping Cui Shuang Sun Kai Yu Shu Zhang Mei-lin Wang Jia-jia Chen Bai-bin Zhou key laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina state key laboratory of Physical chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy MaterialsXiamen UniversityXiamen 361005FujianChina

Bimetallic oxides are attractive anode materials for lithium-ion batteries(LIBs)due to their large theoretical ***,the low conductivity,short cycle life,and poor rate capability are the bottlenecks for their further *** overcome above issues,the basket-like polymolybdate(NiP_(6)Mo_(18))and carbon nanotubes(CNTs)were uniformly embedded on the urchin-shaped CoNiO_(2)nanospheres to yield a ternary composites CoNiO_(2)@NiP_(6)Mo_(18)/CNTs via electrostatic *** multi-level morphology of urchin spinules accelerates the diffusion rate of Li^(+);CNT improves the conductivity and enhances cycle stability of the material;and heteropoly acid contributes more redox activity ***,CoNiO_(2)@NiP_(6)Mo_(18)/CNTs as an anode of LIBs exhibits a high initial capacity(1396.7 mA h g^(−1)at 0.1 A g^(−1)),long-term cycling stability(750.2 mA h g^(−1)after 300 cycles),and rate performance(450.3 mA h g^(−1)at 2 A g^(−1)),which are superior to reported metallic oxides anode of *** density functional theory(DFT)and kinetic mechanism suggest that CoNiO_(2)@NiP_(6)Mo_(18)/CNTs delivers an outstanding pseudocapacitance and rapid Li^(+)diffusion behaviors,which is due to the rich surface area of the urchin-like CoNiO_(2)with the uniform embeddedness of NiP_(6)Mo_(18)and *** study provides a new idea for optimizing the performance of bimetallic oxides and developing high-rate lithium-ion battery composites.

关键词： Bi-metal oxides Transition metal oxides Polyoxometalates Nanocomposite LIBs

Oxidative spirolactonisation for modular access of γ-spirolactones via a radical tandem annulation pathway

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Chinese Chemical Letters 2024年第10期35卷 249-252页

作者： Jindian Duan Xiaojuan Ding Pui Ying Choy Binyan Xu Luchao Li Hong Qin Zheng Fang Fuk Yee Kwong Kai Guo College of Biotechnology and Pharmaceutical Engineering State Key Laboratory of Materials-Oriented Chemical EngineeringNanjing Tech UniversityNanjing 211816China Department of chemistry and state key laboratory of Synthetic chemistry The Chinese University of Hong KongHong KongChina

An oxidative annulation of 2-arylidene-1,3-indanediones with Meldrum's acid has been developed for the divergent syntheses of spirolactones with a spirocenter located at theγ-position with respect to the carbonyl *** heteroannulation protocol tolerates various functional groups and delivers moderate-to-good product ***,the reaction outcomes are exclusively controlled by the reaction oxidant/*** annulation strategy can also be executed in the flow system with decent product *** experiments revealed that the reaction proceeds via a radical tandem annulation pathway.

关键词： Spirolactonisation y-Spirolactones 2-Arylidene-1,3-indanediones Meldrum's acid Divergentsynthesis

Alkali-resistant NO_(x) reduction over FeVO_(4)/TiO_(2)catalysts via regulating the electron transfer between Fe and V

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Chinese Chemical Letters 2024年第2期35卷 489-495页

作者： Yunang Dong Penglu Wang Xiangyu Liu Jiang Deng Aling Chen Lupeng Han Dengsong Zhang International Joint laboratory of Catalytic chemistry State Key Laboratory of Advanced Special SteelCollege of SciencesShanghai UniversityShanghai 200444China

The presence of alkali metals in exhaust gas from stationary resources causes a grand challenge for the practical application of selective catalytic reduction(SCR)of NO_(x) with NH_(3).Here,alkali-resistant NO_(x) reduction has been successfully implemented via tailoring the electron transfer over Fe and V species on FeVO_(4)/TiO_(2)*** strong interaction between Fe and V induced electron transfer from V to Fe and strengthened the adsorption and activation of NH_(3)and NO over active VO_(x) *** the presence of K_(2)O,the strong electron withdrawing effect of Fe offset the electron donating effect of K on the VO_(x) species,thus protecting the active species VO_(x) to maintain the NO_(x) reduction *** enhanced adsorption and activation of NH_(3) allowed SCR reaction to proceed via E-R mechanism even after K_(2)O *** work elucidated the electronic effects on the alkali metals resistance of traditional ferric vanadate SCR catalysts and provided a promising strategy to design SCR catalysts with superior alkali resistance.

关键词： Air pollution control NO_(X)reduction Selective catalytic reduction Alkali metals Electron transfer

Molecule aging induced by electron attacking

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Journal of Energy chemistry 2024年第6期93卷 519-525,I0013页

作者： Ping Song Yining Dong Xue Gong Mingbo Ruan Baoxin Ni Xuanhao Mei Kun Jiang Weilin Xu state key laboratory of Electroanalytical chemistry and Jilin Province key laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of Chin1Hefei 230026AnhuiChina Shanghai key laboratory of Molecular Catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed *** further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)*** IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water *** facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule *** exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C *** density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water *** results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.

关键词： Aging of molecules Electron attacking Full width at half maxima Hydrogen evolution reaction

Delving into the dissimilarities in electrochemical performance and underlying mechanisms for sodium and potassium ion storage in N-doped carbon-encapsulated metallic Cu_(2)Se nanocubes

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Journal of Energy chemistry 2024年第8期95卷 336-347,I0008页

作者： Xinyu Wang Yanan Xu Xiaofeng Liu Lei Tan Huaiqiang Gu Xin Du Dan Li College of chemistry Zhengzhou UniversityZhengzhou 450001HenanChina Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001HenanChina Institute of theoretical Physics Lanzhou UniversityLanzhou 730000GansuChina School of Nuclear Science and Technology Lanzhou UniversityLanzhou 730000GansuChina key laboratory of Advanced Energy Materials chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China state key laboratory of chemistry and Utilization of Carbon Based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830046XinjiangChina

The large volumetric variations experienced by metal selenides within conversion reaction result in inferior rate capability and cycling stability,ultimately hindering the achievement of superior electrochemical ***,metallic Cu_(2)Se encapsulated with N-doped carbon(Cu_(2)Se@NC)was prepared using Cu_(2)O nanocubes as templates through a combination of dopamine polymerization and hightemperature *** unique nanocubic structure and uniform N-doped carbon coating could shorten the ion transport distance,accelerate electron/charge diffusion,and suppress volume variation,ultimately ensuring Cu_(2)Se@NC with excellent electrochemical performance in sodium ion batteries(SIBs)and potassium ion batteries(PIBs).The composite exhibited excellent rate performance(187.7 mA h g^(-1)at 50 A g^(-1)in SIBs and 179.4 mA h g^(-1)at 5 A g^(-1)in PIBs)and cyclic stability(246,8 mA h g^(-1)at 10 A g^(-1)in SIBs over 2500 cycles).The reaction mechanism of intercalation combined with conversion in both SIBs and PIBs was disclosed by in situ X-ray diffraction(XRD)and ex situ transmission electron microscope(TEM).In particular,the final products in PIBs of K_(2)Se and K_(2)Se_(3)species were determined after discharging,which is different from that in SIBs with the final species of Na_(2)*** density functional theory calculation showed that carbon induces strong coupling and charge interactions with Cu_(2)Se,leading to the introduction of built-in electric field on heterojunction to improve electron ***,the theoretical calculations discovered that the underlying cause for the relatively superior rate capability in SIBs to that in PIBs is the agile Na~+diffusion with low energy barrier and moderate adsorption *** findings offer theoretical support for in-depth understanding of the performance differences of Cu-based materials in different ion storage systems.

关键词： Cu_(2)Se nanocubes DFT calculations Ion storage mechanism Potassium ion batteries Sodium ion batteries

Site-specific incorporation of reduction-controlled guest amino acids into proteins for cucurbituril recognition

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Chinese Chemical Letters 2024年第5期35卷 193-196页

作者： Zhen Dai Linzhi Tan Yeyu Su Kerui Zhao Yushun Tian Yu Liu Tao Liu College of chemistry State Key Laboratory of Elemento-Organic ChemistryNankai UniversityTianjin 300071China state key laboratory of Natural and Biomimetic Drugs Department of Molecular and Cellular PharmacologySchool of Pharmaceutical SciencesPeking UniversityBeijing 100191China

Protein recognition using host-guest recognition approach is of great interest but has been limited mainly to the protein N-terminal ***,we site-specific incorporated two novel non-canonical amino acids containing supramolecular guest motifs into protein via an expanded genetic *** Staudinger reduction reactions,the encoded unnatural residues on protein becoming activated and can be specifically recognized by cucurbit[7]uril(CB[7])and cucurbit[8]uril(CB[8]).We demonstrated that enzyme containing guest amino acid incorporated near the active site can be reversibly regulated by CB[7]recognition,and CB[8]recognition induces protein *** amino acids will make useful addition to the supramolecular toolbox for protein targeting using molecular recognition approaches.

关键词： Protein recognition Host-guest recognition Non-canonical amino acids Staudinger reduction Expanded genetic code