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Enlarged interlayer of separator coating enabling high-performance lithiumsulfur batteries

Frontiers of Chemical Science and Engineering 2024年第2期18卷 103-112页

作者： Yanqi Feng Hui Liu Xiaoting Liu Qiongqiong Lu School of materials&environment Engineering Chengdu Technological UniversityChengdu 611730China School of materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science and TechnologyXi’an 710021China Green catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Institute of materials Henan Key Laboratory of Advanced Conductor MaterialsHenan Academy of SciencesZhengzhou 450046China Leibniz Institute for Solid State and materials Research(IFW) Dresden e.V.Dresden 01069Germany

Lithiumsulfur batteries have been intensively studied due to their high theoretical energy density and abundant sulfur resources. However, their commercial application is hindered by the low redox kinetics and high sulfur losses. In principle, in the design of cathodes and separators, the adsorption toward lithium-polysulfides should be enhanced and the conversion of soluble high-order lithium-polysulfides should be catalyzed. Herein, a KV_(3)O_(8)·0.75H_(2)O separator is designed as an effective lithium-polysulfides mediator in lithiumsulfur batteries. The intercalated K+ would enlarge the interlayer spacing of vanadium oxides, preventing the collapse of the layer structure and improving the electrical/ion conductivity of the interface. Moreover, the KV_(3)O_(8)·0.75H_(2)O modified separator possess a prior adsorption and high redox kinetics toward lithium-polysulfides due to the enhanced diffusion kinetics, which guarantees the high-rate capability and efficient utilization of sulfur. As a result, lithiumsulfur batteries exhibit a high capacity of 1362 mAh·g^(-1) and a long lifespan with a low capacity loss of 0.073% per cycle. This work may provide an alternative way to establish a functional separator to balance the adsorption and conversion of polysulfides during the redox back and forth.

关键词： lithium kinetics adsorption

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Copper-catalyzed C(sp)-H aryl amination enables modular synthesis of quinolines and 2-quinolinones

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Science China Chemistry 2024年第2期67卷 595-603页

作者： Yang Gao Haixia Li Simin Yang Yanping Huo Qian Chen Xianwei Li Zhe Wang Xiao-Qiang Hu School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou510006China Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory Jieyang515200China Key Laboratory of catalysis and Energy materials Chemistry of Ministry of Education&Hubei Key Laboratory of catalysis and materials Science School of Chemistry and Materials ScienceSouth-Central University for NationalitiesWuhan430074China

Herein,we disclose a novel copper-catalyzed C(sp)-H aryl amination of terminal alkynes with anthranils,enabling the rapid generation of highly reactive secondary N-aryl ynamines for the modular synthesis of structurally diverse C2-substituted quinolines and *** in-situ formed carbonyl-ynamines are prone to tautomerize to carbonyl-ketenimines,which can efficiently react with a series of nucleophiles,including amines,alcohols,phenols,thiols,thiophenols,active-methylene compounds,and even water to produce various quinoline derivatives with the generation of H_(2)O as a sole and green *** method also unlocks a practical route to create various quinoline-fused heterocycles and can be successfully applied to the late-stage modification of complex molecules and the concise synthesis of bioactive *** studies reveal a coppercatalyzed inner-sphere nitrene transfer process by using anthranils as novel aryl nitrene precursors.

关键词： copper catalysis anthranils C(sp)-H aryl amination carbonyl-ketenimines quinolines

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Reducing the voltage loss of Y-series acceptor based organic solar cells via ternary/quaternary strategies

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Chinese Chemical Letters 2024年第2期35卷 70-86页

作者： Pengyu Zhang Zhiyang Zhang Heng Sun Jie Li Yi Chen Jiang Wang Chuanlang Zhan Key Laboratory of Advanced materials Chemistry and Devices (AMC&DLab) of the Department of Education of Inner Mongolia Autonomous Region Inner Mongolia Key Laboratory of Green CatalysisCollege of Chemistry and Environment ScienceInner Mongolia Normal UniversityHuhehot 010022China

In recent years, with the emergence of non-fullerene fused-ring acceptors, power conversion efficiencies (PCEs) of organic solar cells (OSCs) have exceeded 19%.However, compared to inorganic or perovskite photovoltaic cells, a higher voltage loss has become one of the key factors limiting further improvement in the PCEs of *** ternary/quaternary strategy has been identified as a feasible and effective way to obtain high-efficiency *** this review, a brief outline is given of the key roles that guest materials played in reducing voltage losses in solar cell devices and a brief look at the future material design and the design of ternary/quaternary systems.

关键词： Organic solar cell Ternary/quaternary strategy Open-circuit voltage Voltage loss Non-radiative recombination loss

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Small amount but big impact:Trace oxygen interstitially inserted PtCu alloys by microalloying for efficient oxygen reduction catalysis

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Nano Research 2024年第8期17卷 7001-7012页

作者： Qiheng Wang Zhiguo Chen Jingyan Zhang Jingjun Liu Beijing Key Laboratory of Electrochemical process and Technology for materials Beijing 100029China Beijing University of Chemical Technology Beijing 100029China

The introduction of small size non-metal elements(e.g.,oxygen)into solid solution alloys may be a promising strategy for fabricating efficient Pt-based catalysts with high activity and stability toward oxygen reduction reaction(ORR).Herein,oxygen interstitially inserted PtCu(O-PtCu)alloys are firstly designed by an oxygen-microalloying strategy,through ultraviolet(UV)irradiation-assisted galvanic replacement in an aqueous solution containing H_(2)PtCl_(6) and Cu_(2)O nanowires as sacrificial *** obtained O-PtCu alloys feature a typical face-centered cubic(FCC)structure with majority Pt,Cu atoms as building bricks and trace interstitial oxygen(1.65 wt.%)existed in the octahedral sites surrounding Cu atoms,leading to a short-range disordered *** alloy reaches a recorded half-wave potential of 0.96 V(*** hydrogen electrode(RHE))and mass activity of 0.48 A·mgPt^(−1),much higher than those of commercial Pt/*** the accelerated degradation test(ADT),the mass activity lost only 4.2%after 10k cycles,while the commercial Pt/C lost 66.7%under the same *** with pure Pt and undoped PtCu alloy,the remarkably improved performance can be attributed to the lattice distortion and energy band reconstruction caused by the interstitial oxygen atoms in form of Cu–O ***,the stable Cu–O bonds delay the possible place exchange between surface Pt atoms and surface-adsorbed oxygen species,thereby hindering Pt dissolution,providing a new paradigm to address Pt degradation ***,the introduction of interstitial oxygen into Pt-based alloys may be a facile and smart strategy for the development of advanced Pt-based alloys electrocatalysts.

关键词： oxygen-microalloying platinum alloys octahedral interstices oxygen reduction reaction

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Design and construction of size-controlled CoO/CS catalysts for Fischer–Tropsch synthesis

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Nano Research 2024年第4期17卷 2520-2527页

作者： Wei Sun Ting Kuang Guiyou Wei Yue Li Yaqin Liu Shuai Lyu Yuhua Zhang Jinlin Li Li Wang Key Laboratory of catalysis and Energy materials Chemistry of Ministry of Education&Hubei Key Laboratory of catalysis and materials Science South-Central Minzu UniversityWuhan 430074China Hubei Key Laboratory of Biomass Fibers and Eco-dyeing&Finishing College of Chemistry and Chemical EngineeringWuhan Textile UniversityWuhan 430200China

The use of supported Co-based catalysts is widespread in various catalytic reactions due to their unique *** structural sensitivity of these catalysts is closely linked to their particle size and crystal ***,comprehending the structure–activity relationship requires the development of well-defined Co-based ***,we employed a colloidal wet chemical process and a heterogeneous nucleation method to prepare well-defined Co-based catalysts supported by inert carbon *** nanospheres’surface possesses abundant functional groups that efficiently capture metal complexes and facilitate the nucleation and growth of CoO *** adjusting the Co source concentration,solvent molar ratio,and nucleation growth kinetics,we successfully prepared CoO/carbon sphere(CS)catalysts with different particle sizes and crystal *** influence of metallic face-centered cubic(fcc)-Co^(0) particle size in the range of 6.6–17.6 nm on the performance of Fischer–Tropsch synthesis(FTS)using well-defined CoO/CS catalysts has been *** result demonstrated that the turnover frequency(TOF)remained constant for CoO/CS catalysts with metallic fcc-Co^(0) particle size larger than 7.7 ***,both the selectivity and the activity changed for CoO/CS catalysts with smaller particles(ructure–activity relationship,leading to a better understanding of Co catalyzed Fischer–Tropsch synthesis.

关键词： Fischer–Tropsch synthesis(FTS) cobalt size effects phase effects carbon nanospheres

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Direct observation of oxygen vacancy formation and migration over ceria surface by in situ environmental transmission electron microscopy

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Journal of Rare Earths 2024年第4期42卷 676-682页

作者： Dawei Pang Wei Li Ningqiang Zhang Hong He Shengcheng Mao Yanhui Chen Liwei Cao Chong Li Ang Li Xiaodong Han Beijing Key Laboratory of Solid Microstructure and Properties Department of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Beijing Key Laboratory for Green catalysis and Separation The Faculty of Environment and LifeBeijing University of TechnologyBeijing10124China International Joint Research Laboratory for Quantum Functional materials of Henan School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou450001China

The extremely high structural tolerance of ceria to oxygen vacancies(Ov)has made it a desirable catalytic material for the hydrocarbon oxidation to chemicals and pharmaceuticals and the reduction of gaseous *** is proposed that the formation and diffusion of Ov originate from its outstanding reduction ***,the formation and diffusion process of Ov over the surface of ceria at the atomic level is still ***,the structural and valence evolution of CeO_(2)(111)surfaces in reductive,oxidative and vacuum environments from room temperature up to 700℃was studied with in situ aberration-corrected environmental transmission electron microscopy(ETEM)*** is found to form under a high vacuum at elevated temperatures;however,the surface can recover to the initial state through the adsorption of oxygen atoms in an oxygen-contained ***,in hydrogen environment,the step-CeO_(2)(111)surface is not stable at elevated temperatures;thus,the steps tend to be eliminated with increasing *** with first-principles density function calculations(DFT),it is proposed that O-terminated surfaces would develop in a hypoxic environment due to the dynamic diffusion of Ov from the outer surface to the ***,in a reductive environment,H2 facilitates the formation and diffusion of Ov while Ce-terminated surfaces *** results reveal dynamic atomic-scale interplay between the nanoceria surface and gas,thereby providing fundamental insights into the Ov-dependent reaction of nano-CeO_(2) during catalytic processes.

关键词： Ceria Direct observation In situ ETEM Oxygen vacancy Density function calculations Rareearths

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Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li Department of Chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State Key Laboratory of Surface Physics and Department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable ***,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as *** key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon *** mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion *** method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

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UiO-66-NH_(2)nanoparticles supported on layered double hydroxides as an excellent adsorbent for levofloxacin capture

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Particuology 2024年第9期92卷 155-165页

作者： Yan Li Heng Lin Qiaolan Yu Na Ma Wei Dai College of Geography and environmental Sciences Zhejiang Normal UniversityJinhua321004China Key Laboratory of the Ministry of Education for Advanced catalysis materials College of Chemistry and Materials ScienceZhejiang Normal UniversityJinhua321004China

The adsorption performances of individual adsorbent such as UiO-66-NH_(2)and MgAl-layered double hydroxides(MgAl-LDH)toward levofloxacin(LVX)is less satisfactory due to the disappointing uptake capacity and adsorption ***,a 3D flower-like composite adsorbent prepared via iterative hydrothermal synthesis method anchoring UiO-66-NH_(2)nanoparticles onto the MgAl-LDH *** to the synergistic effects of UiO-66-NH_(2),and MgAl-LDH,the MgAl-LDH@UiO-66-NH_(2)exhibits an outstanding adsorption performance toward ***,the maximum LVX uptake capacity over MgAl-LDH@UiO-66-NH_(2)reached 268 mg/g,which was higher than that of the individual adsorption materials UiO-66-NH_(2)(41 mg/g),MgAl-LDH(140 mg/g),and some adsorbents reported in previous *** rapid adsorption process can reach equilibrium within 20 min,which conformed well to the pseudo-second-order kinetics and the Langmuir isotherm *** thermodynamic result also indicated that the adsorption was spontaneous and exothermic,simultaneous coexisting physical and chemical adsorption ***,the MgAl-LDH@UiO-66-NH_(2)still maintained excellent adsorption capacity with a slightly decrease after fifth cycle,exhibiting a remarkable reuse and stable *** work provides a highly novel strategy to prepare recyclable composite adsorbent for the LVX capture from aqueous solution.

关键词： Layered double hydroxides UiO-66-NH_(2) LVX Adsorption

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A weakly-solvated ether-based electrolyte for fast-charging graphite anode

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Chinese Chemical Letters 2024年第8期35卷 526-532页

作者： Xiao Zhu Yanbing Mo Jiawei Chen Gaopan Liu Yonggang Wang Xiaoli Dong Department of Chemistry and Shanghai Key Laboratory of Molecular catalysis and Innovative materials Institute of New EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Fudan UniversityShanghai 200433China

Weakly-solvated electrolytes(WSEs)utilizing solvents with weak coordination ability offer advantages for low-potential graphite anode owing to their facile desolvation process and anions-derived inorganic-rich solid electrolyte interphase(SEI)***,these electrolytes face challenges in achieving a balance between the weak solvation affinity and high ionic conductivity,as well as between rigid inorganic-rich SEI and flexible SEI for long-term ***,we introduce 1,3-dioxolane(DOL)and lithium bis(trifluoromethanesulfonyl)-imide(LiTFSI)as functional additives into a WSE based on nonpolar cyclic ether(1,4-dioxane).The well-formulated WSE not only preserves the weakly solvated features and anion-dominated solvation sheath,but also utilizes DOL to contribute organic species for stabilizing the SEI *** from these merits,the optimized electrolyte enables graphite anode with excellent fast-charging performance(210 mAh/g at 5 C)and outstanding cycling stability(600 cycles with a capacity retention of 82.0%at room temperature and 400 cycles with a capacity retention of 80.4%at high temper-ature).Furthermore,the fabricated LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)||graphite full cells demonstrate stable operation for 140 cycles with high capacity retention of 80.3%.This work highlights the potential of tailoring solvation sheath and interphase properties in WSEs for advanced electrolyte design in graphite-based lithium-ion batteries.

关键词： Weakly-solvated solvent Bisalt ether-based electrolyte Graphite anode NCM||graphite battery Interfacial optimization

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Metal-organic frameworks on 3D interconnected macroporous sponge foams for large-scale water decontamination:A mini review

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Chinese Chemical Letters 2024年第5期35卷 77-84页

作者： Xiao-Hong Yi Chong-Chen Wang Beijing Key Laboratory of Functional materials for Building Structure and environment Remediation School of Environment and Energy EngineeringBeijing University of Civil Engineering and ArchitectureBeijing 100044China

Water pollution caused by global population growth,urban expansion and industrialization development is one of the urgent issues that need to be addressed in the 21st *** to now,it was challenging for metal-organic frameworks(MOFs)to be used in the actual water treatment due to that the powder MOFs suffered from difficult reuse,poor water stability and easy *** is an effective strategy to immobilize MOFs powder onto porous sponge foam carriers for accomplishing large flux,facile recycling,easy processing water treatment *** this review article,the fabrication approaches and applications of different MOFs/sponge composites were highlighted,in which the fluorescence detection of pollutants,adsorption and separation of pollutants,catalytic reduction and oxidation of pollutants were ***,the future challenges and opportunities of MOF/sponge for water treatment are proposed,aiming to provide in-depth guidance for the future design and manufacture of the immobilized MOFs onto sponge foams.

关键词： Metal-organic frameworks Sponge foam Water decontamination Adsorption catalysis

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