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Ionic solid-like conductor-assisted polymer electrolytes for solid-state lithium metal batteries

Science China Chemistry 2024年第12期67卷 4116-4124页

作者： Shuaishuai Yan Hao Liu Xiaoxia Chen Yang Lu Qingbin Cao Kai Liu State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Hefei Institute for Public Safety Research Tsinghua UniversityHefei 230601China Beijing Huairou Laboratory Beijing 101400China

Solid polymer electrolytes(SPEs)have attracted extensive attention by virtue of lightweight and flexible processability for solidstate lithium metal batteries(LMBs)with high energy density and intrinsic ***,the SPEs suffer from the trade-off effect between ionic conductivity and mechanical ***,we report an ionic solid-like conductor with high Li+conductivity and good thermal stability as the conductive phase of polymer electrolytes for advanced *** poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)as the polymer matrix,the ionic solid-like conductor can be regarded as a solid plasticizer due to its advantages of non-fluidity and *** increases the amorphous region and the dissociation degree of lithium salts in SPEs,while minimizing the loss of mechanical *** a result,the Li+conductivity of SPEs incorporating the ionic solid-like conductor is enhanced by four orders of magnitude compared to the blank PVDF-HFPbased *** optimized SPE membranes can be processed as thin as 50μm with a high Young's modulus of 16.8 MPa,therefore ensuring stable long-term cycling of solid-state *** Li/Li symmetric cells stably cycled for more than 750 h without short circuits,and the LiFePO_(4)/Li solid-state batteries demonstrate excellent electrochemical performance over 350cycles with a capacity retention of 82.5%.This work provides a new strategy for designing ionic solid-like conductors as solid plasticizers for high-performance polymer electrolytes.

关键词： ionic solid-like conductors polymer electrolytes solid plasticizers solid-state lithium metal batteries

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Novel side chain grafted poly (biphenyl pyridine-co-N-methyl piperidine) anion exchange membranes for fuel cells

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International Journal of Hydrogen Energy 2025年 140卷 141-152页

作者： Zhu, Hong Tuo, Shujing Wang, Fanghui State Key Laboratory of Chemical Resource Engineering Institute of Modern Catalysis Department of Organic Chemistry College of Chemistry Beijing University of Chemical Technology Beijing100029 China

To explore the application of highly conductive and chemically stable anion exchange membranes in anion exchange membrane fuel cells. Herein, a series of novel poly (biphenyl pyridine-co-N-methyl piperidine) (s-PBPP-n-TMA) membranes were synthesized via superacid-catalyzed polymerization. Pyridine units with good thermal stability were added to poly (biphenyl piperidine) with moderately hydrophobic backbones, enhancing the differences and spatial nanostructures between hydrophilic/hydrophobic regions, and constructing obvious microphase separation. Furthermore, flexible hydrophobic alkyl spacer chains with different lengths are grafted at the N of rigid pyridine and piperidine rings, and the formation of multiple cationic sites greatly improves conductivity (>95.63 mS/cm at 80 °C). Compared to membranes without grafted flexible side chain (s-PBPP-80), the addition of side chains inhibits the formation of pyridone and the nucleophilic attack of OH−, resulting in long-term chemical stability of s-PBPP-n-TMA membranes (the residual conductivities were higher than 81.08 % in 2 M NaOH at 80 °C for 1800 h). In terms of single-cell testing, the s-PBPP-6-TMA with the best comprehensive performance achieved a maximum power density of 656.10 mW/cm2 (H2/O2) at 80 °C. © 2025

关键词： Cationic polymerization

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Rocking-chair ammonium ion battery with high rate and long-cycle life

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Chinese chemical Letters 2024年第1期35卷 563-567页

作者： Tongkai Wang Xiaojuan Li Shunshun Zhao Hongxia Bu Chuanlin Li Na Li Xixi Zhang Xijin Xu School of Physics and Technology University of JinanJi'nan 250022China State Key Laboratory of Chemical Resource Engineering Beijing Key Laboratory of Electrochemical Process and Technology of MaterialsBeijing University of Chemical TechnologyBeijing 100029China College of Physics and Electronic Engineering Qilu Normal UniversityJi'nan 250200China

Aqueous rechargeable ammonium-ion batteries(AIBs)have drew considerable attention because of their capacity for high rates,low cost,and high ***,developing desired electrodes requiring stable structure in the aqueous fast ammoniation/de-ammoniation becomes ***,an ammonium ion full battery using Cu_(3)[Fe(CN)_(6)]_(2)(CuHCF)acting to be a cathode and barium vanadate(BVO)acting to be an anode is *** excellent electrochemical behavior of Prussian blue analogs and the perfectly matched lattice structure of NH_(4)^(+)is *** the open structure of vanadium compounds satisfies the fast ammoniation/de-ammoniation of NH4+is also *** a result of these synergistic effects,the BVO//CuHCF full cell retains 80.5 percent of its capacity following 1000 *** achievements provide new ideas for developing low-cost and long-life AIBs.

关键词： Copper hexacyanoferrate Vanadium-based compounds Aqueous ammonium ion batteries Long-term cyclability Ammonium ion storage mechanism

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Screening of transition metal oxides for electrocatalytic nitrate reduction to ammonia at large currents

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Nano Research 2024年第5期17卷 3902-3910页

作者： Qiongfei Wu Weijie Zhu Dongxu Ma Chao Liang Zhoucheng Wang Hanfeng Liang State Key Laboratory of Physical Chemistry of Solid Surfaces Tan Kah Kee Innovation LaboratoryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of Chemical Engineering Tianjin UniversityTianjin 300072China

Electrochemical nitrate reduction reaction(NO_(3)RR)towards ammonia,as an emerging and appealing technology alternative to the energy-intensive Haber-Bosch process and inefficient nitrogen reduction reaction,has recently aroused wide concern and ***,the current research of the NO_(3)RR towards ammonia lacks the overall performance comparison of various *** this,we here make a comparison of 12 common transition metal oxide catalysts for the NO_(3)RR under a high cathodic current density of 0.25 A·cm^(-2),wherein Co_(3)O_(4) catalyst displays the highest ammonia Faradaic efficiency(85.15%)and moderate activity(ca.-0.25 V *** hydrogen electrode).Other external factors,such as nitrate concentrations in the electrolyte and applied potential ranges,have also been specifically investigated for the NO_(3)RR.

关键词： nitrate reduction reaction ammonia production transition metal oxides Co_(3)O_(4)

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Innovative construction of macroporous–mesoporous structured spherical alumina and its hydrothermal stability

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Particuology 2024年第7期90卷 429-435页

作者： Yufan Mo Chunli Li Huiyu Li Wei Han He Wen Yinghong Han Chunxia Che Yongjun Feng State Key Laboratory of Chemical Resource Engineering Beijing Engineering Center for Hierarchical CatalystsCollege of ChemistryBeijing University of Chemical TechnologyBeijing100029China Lanzhou Petrochemical Research Center Petrochemical Research InstitutePetroChinaLanzhou730060China

The pore structure of spherical alumina supports is closely related to the dispersion of catalytically active components and the diffusion of *** excellent pore structure under strict reaction conditions is of utmost *** this work,sphericalγ-Al_(2)O_(3)support with a bimodal pore structure,composed of macropores and mesopores,was successfully synthesized using dodecane as the pore-forming agent through the oil–ammonia column-shaping *** morphology and internal pore structure of the alumina were found to be influenced by the amount of surfactant added and ultrasound treatment ***,when concentration of surfactant was 4‰and ultrasound voltage of 20 V was applied,the resultingγ-Al_(2)O_(3)-4‰-20 displayed a highly concentrated distribution of macropores with an average pore size of 100 nm,resulting in an impressive porosity of 69.21%.In contrast,the untreated sample ofγ-Al_(2)O_(3)-0-0 only exhibited a mesoporous distribution with a porosity of 54.03%.Moreover,after being subjected to a hydrothermal treatment in a high temperature(600°C)and high humidity(water vapor)environment for 120 h,theγ-Al_(2)O_(3)-4‰-20 sample maintained a high BET specific surface area of 170.9 m^(2)g^(−1)and mercury intrusion porosimetry specific surface area of 263.3 m^(2)g^(−1).

关键词： Spherical alumina supports Pore-forming agent Oil-ammonia column shaping method Hydrothermal treatment Hydrothermal stability

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Lithiophilic Cu-Li_(2)O matrix on a Cu Collector to Stabilize Lithium Deposition for Lithium Metal Batteries

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Energy & Environmental Materials 2022年第4期5卷 1270-1277页

作者： Zhe Gong Cheng Lian Pengfei Wang Kai Huang Kai Zhu Ke Ye Jun Yan Guiling Wang Dianxue Cao Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education College of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001China State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Lithium metal anode is the most ideal candidate for next-generation energy storage ***,the uncontrolled dendrite growth,infinite volume expansion,and undesired side reactions lead to serious safety issues and hinder their potential ***,a pre-lithiation strategy is proposed to construct a high-lithiophilic Cu-Li_(2)O matrix on commercial Cu *** in situ-generated Li_(2)O promises adequate nucleation sites and strengthens solid electrolyte interphase and lateral lithium ***,the existence of 3D matrix reduces the local current *** synergy effect of Li_(2)O and Cu suppresses the growth of lithium *** a result,Cu-Li_(2)O matrix reveals an enhanced lithium plating/stripping behavior with Coulombic efficiency of 98.46%after 270 *** symmetrical cell assembled by Li-plated electrodes displays a prolonged lifespan of 1400 *** work demonstrates a scalable and effective approach for modified current collectors toward stable Li metal anode.

关键词： Cu-Li_(2)O matrix current collectors Li metal anodes SEI film

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Hybrid data-driven and physics-based modeling for viscosity prediction of ionic liquids

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Green Energy & Environment 2024年第12期9卷 1878-1890页

作者： Jing Fan Zhengxing Dai Jian Cao Liwen Mu Xiaoyan Ji Xiaohua Lu State Key Laboratory of Materials-Oriented and Chemical Engineering Nanjing Tech UniversityNanjing211816China Energy Engineering Division of Energy ScienceLulea University of TechnologyLulea97187Sweden

Viscosity is one of the most important fundamental properties of ***,accurate acquisition of viscosity for ionic liquids(ILs)remains a critical *** this study,an approach integrating prior physical knowledge into the machine learning(ML)model was proposed to predict the viscosity *** method was based on 16 quantum chemical descriptors determined from the first principles calculations and used as the input of the ML models to represent the size,structure,and interactions of the *** strategies based on the residuals of the COSMO-RS model were created as the output of ML,where the strategy directly using experimental data was also studied for *** performance of six ML algorithms was compared in all strategies,and the CatBoost model was identified as the optimal *** strategies employing the relative deviations were superior to that using the absolute deviation,and the relative ratio revealed the systematic prediction error of the COSMO-RS *** CatBoost model based on the relative ratio achieved the highest prediction accuracy on the test set(R^(2)=0.9999,MAE=0.0325),reducing the average absolute relative deviation(AARD)in modeling from 52.45% to 1.54%.Features importance analysis indicated the average energy correction,solvation-free energy,and polarity moment were the key influencing the systematic deviation.

关键词： Viscosity Fundamental property Ionic liquids COSMO-RS Machine learning

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Acylfluorination of enynes via phosphine and silver catalysis

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Chinese chemical Letters 2024年第8期35卷 260-264页

作者： Yu Mao Yilin Liu Xiaochen Wang Shengyang Ni Yi Pan Yi Wang State Key Laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

This work describes intermolecular acylfluorination of gem-difluoroenynes using acyl fluorides as both acyl source and fluorine ***-substituted allenones or furans could be selectively achieved via phosphine and silve... 详细信息

关键词： Phosphine catalysis Silver catalysis Difunctionalization Allenone Furan Trifluoromethyl

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Regulating the"core-shell"microstructure of hard carbon through sodium hydroxide activation for achieving high-capacity SIBs anode

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材料科学技术（英文版） 2025年第6期209卷 161-170页

作者： Haihua Wang Huizhu Niu Kewei Shu Liyu Sun Yu Wang Yifan Du Yun Han Cunguo Yang Yong-Mook Kang Shaanxi University of Science and Technology School of Chemistry and Chemical EngineeringXuefu RoadWeiyang DistrictXi'an 710021China Xi'an Key Laboratory of Advanced Performance Materials and Polymers Shaanxi University of Science and TechnologyXi'an 710021China Shaanxi Key Laboratory of Chemical Additives for Industry Shaanxi University of Science and TechnologyXi'an 710021China Shaanxi University of Science and Technology School of Chemistry and Chemical EngineeringXuefu RoadWeiyang DistrictXi'an 710021China Xi'an North Huian Chemical Industry Co Yuxia TownHu Yi DistrictXi'an 710302China Shaanxi Key Laboratory of Chemical Additives for Industry Shaanxi University of Science and TechnologyXi'an 710021China Department of Materials Science and Engineering Korea University.Seoul 02841Republic of Korea

Pore structure engineering has been acknowledged as suitable approach to creating active sites and en-hancing ion transport capabilities of hard carbon ***,conventional porous carbon materials exhibit high BET and surface ***,the sodium storage mechanism predominantly occurs in the slope *** contradicts practical application requirements because the capacity of the plateau region is crucial for determining the actual capacity of *** our work,we prepared a novel"core-shell"carbon framework(CNA1200).Introducing closed pores and carboxyl groups into coal-based carbon materials to enhance its sodium storage *** closed pore structure dominates in the"core"structure,which is attributed to the timely removal of sodium hydroxide(NaOH)to prevent further for-mation of active carbon *** presence of closed pores is beneficial for increasing sodium ion storage in the low-voltage plateau *** the"shell"structure originates from coal tar pitch,it not only uniformly connects hard carbon particles together to improve cycling stability,but is also rich in carboxyl groups to enhance the reversible sodium storage performance in slope ***1200 has ex-cellent electrochemical performance,it exhibits a specific capacity of 335.2 mAh g-1 at a current density of 20 mA g-1 with ICE=51.53％.In addition,CNA1200 has outstanding cycling stability with a capac-ity retention of 91.8％even when cycling over 200 *** CNA1200 is used as anode paired with Na3V2(PO4)3 cathode,it demonstrates a capacity of 109.54 mAh g-1 at 0.1 C and capacity retention of 94.64％at 0.5 *** work provides valuable methods for regulating the structure of sodium-ion battery(SIBs)anode and enhances the potential for commercialization.

关键词： Hard carbon plateau region NaOH controlled etching-thermal annealing Closed pore structure Carboxyl groups Coal-based carbon materials

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Enhanced gas production and CO_(2) storage in hydrate-bearing sediments via pre-depressurization and rapid CO_(2) injection

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Chinese Journal of chemical engineering 2024年第3期67卷 126-134页

作者： Hongnan Chen Yifei Sun Bojian Cao Minglong Wang Ming Wang Jinrong Zhong Changyu Sun Guangjin Chen State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China School of Chemistry and Chemical Engineering Changsha University of Science&TechnologyChangsha 410114China

Carbon emission reduction and clean energy development are urgent demands for mankind in the coming *** an efficient CO_(2) storage method can significantly reduce CO_(2) emissions in the short *** this study,we attempted to construct sediment samples with different residual CH_(4) hydrate amounts and reservoir conditions,and then investigate the potentials of both CO_(2) storage and enhanced CH_(4) recovery in depleted gas hydrate deposits in the permafrost and ocean zones,*** results demonstrate that CO_(2) hydrate formation rate can be significantly improved due to the presence of residual hydrate seeds;However,excessive residual hydrates in turn lead to the decrease in CO_(2) storage *** by the T-P conditions of the reservoir,the storage amount of liquid CO_(2) can reach 8 times that of gaseous CO_(2),and CO_(2) stored in hydrate form reaches 2-4 ***,we noticed two other advantages of this *** is that CO_(2) injection can enhance CH_(4) recovery rate and increases CH_(4) recovery by 10%-20%.The second is that hydrate saturation in the reservoir can be restored to 20%-40%,which means that the solid volume of the reservoir avoids serious ***,this is crucial for protecting the goaf *** summary,this approach is greatly promising for high-efficient CO_(2) storage and safe exploitation of gas hydrate.

关键词： Hydrate Depressurization CO_(2) storage CH_(4) production Reservoir remediation

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