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Lithiophilic CoF_(2)@C hollow spheres towards spatial lithium deposition for stable lithium metal batteries

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Journal of Energy Chemistry 2024年第10期97卷 55-67,I0002页

作者： Jianxing Wang Shuhao Yao Runming Tao Xiaolang Liu Jiazhi Geng Chang Hong Huiying Li Guiyun Yu Haifeng Li Xiao-Guang Sun Jianlin Li Jiyuan Liang School of Optoelectronic Materials&technology jianghan UniversityWuhan 430056HubeiChina institute for Advanced Materials and Manufacturing University of TennesseeKnoxilTN 37996USA School of Chemistry&chemical Engineering Yancheng Institute of TechnologyYancheng 224051JiangsuChina chemical Sciences Division Oak Ridge National LaboratoryOak RidgeTN 37831USA Applied Materials Division Argonne National LaboratoryLemontIL 60439USA

Lithium metal(LM)is a promising anode for next-generation batteries due to its high theoretical capacity and low electrode ***,side reactions,volume change,and unwanted lithium dendrite growth seriously limit the practical application of ***,with the aid of a hard template approach,a novel lithiophilic CoF_(2)-carbon hollow sphere(CoF_(2)@C-HS)composite material is successfully prepared via a facile in-situ fluorination and etching *** lithiophilic CoF_(2) acts as nucleation sites to reduce nucleation overpotential as well as induces the spatial Li deposition and the formation of LiFrich solid electrolyte interphase(SEI),and the hollow carbon matrix can enhance the electrical conductivity and offer free space for LM *** simulations reveal that the synergistic effect of lithiophilic CoF_(2) and hollow carbon matrix homogenizes the electric field distribution and Li~+*** from these advantages,the CoF_(2)@C-HS-modified copper substrate electrode delivers an enhanced Coulombic efficiency(CE)of 93.7%for 280 cycles at 1 mA cm^(-2)and 1 mA h cm^(-2).The symmetrical cell using CoF_(2)@C-HS can stably cycle more than 1800 h with a low voltage hysteresis of 11 mV at a current density of 0.5 MA cm^(-2)and an areal capacity of 0.5 mA h cm^(-2).Moreover,the Li@CoF_(2)@C-HS composite anode enables more than 300 stable cycles at 1 C with a capacity retention of 95%in LiFePO_(4)-based full cell and 110 stable cycles at 1 C in LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)-based highvoltage full *** work might shed a new light on designing lithiophilic hosts to spatially confine LM deposition,realizing dendrite-free LM anodes and the practical applications of LM batteries.

关键词： Lithium metal anode Spatial deposition Stability Nanocomposite Lithiophilic CoF_(2)

Revealing the Multifunctional Electrocatalysis of Indium-Modulated Phthalocyanine for High-Performance Lithium-Sulfur Batteries

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Energy & Environmental Materials 2024年第1期7卷 1-8页

作者： Yang Guo Zhaoqing Jin Jianhao Lu Zilong Wang Zihao Song Anbang Wang Weikun Wang Yaqin Huang Beijing Key Laboratory of Electrochemical Process and technology for Materials Key Laboratory of Biomedical Materials of Natural MacromoleculesMinistry of EducationBeijing University of Chemical TechnologyBeijing 100029China Research institute of chemical Defense Beijing Key Laboratory of Advanced Chemical Energy Storage Technology and MaterialsBeijing 100191China

The sluggish kinetics of complicated multiphase conversions and the severe shuttling effect of lithium polysulfides(LiPSs)significantly hinder the applications of Li-S battery,which is one of the most promising candidates for the next-generation energy storage ***,a bifunctional electrocatalyst,indium phthalocyanine self-assembled with carbon nanotubes(InPc@CNT)composite material,is proposed to promote the conversion kinetics of both reduction and oxidation processes,demonstrating a bidirectional catalytic effect on both nucleation and dissolution of Li_(2)S *** theoretical calculation shows that the unique electronic configuration of InPc@CNT is conducive to trapping soluble polysulfides in the reduction process,as well as the modulation of electron transfer dynamics also endows the dissolution of Li_(2)S in the oxidation reaction,which will accelerate the effectiveness of catalytic conversion and facilitate sulfur ***,the InPc@CNT modified separator displays lower overpotential for polysulfide transformation,alleviating polarization of electrode during *** integrated spectroscopy analysis,HRTEM,and electrochemical study reveal that the InPc@CNT acts as an efficient multifunctional catalytic center to satisfy the requirements of accelerating charging and discharging ***,the Li-S battery with InPc@CNT-modified separator obtains a discharge-specific capacity of 1415 mAh g^(-1)at a high rate of 0.5 ***,the 2 Ah Li-S pouch cells deliver 315 Wh kg^(-1)and achieved 80%capacity retention after 50 cycles at 0.1 C with a high sulfur loading of 10 mg cm^(-2).Our study provides a practical method to introduce bifunctional electrocatalysts for boosting the electrochemical properties of Li-S batteries.

关键词： bidirectional catalyst indium phthalocyanine lithium-sulfur batteries pouch cells

Phosphine-Catalyzed [4+3] Annulation Reaction of Indole Derivatives with MBH Carbonates:A Facile Access to Indole-1,2-fused 1,4-Diazepinones and Azepines

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Chinese Journal of Chemistry 2024年第3期42卷 271-275页

作者： Yannan Zhu Haoran Jiang Yi-Ning Wang Faculty of Chemistry and chemical Engineering Yancheng Institute of TechnologyYanchengJiangsu224051 China

A phosphine-catalyzed [4+3] annulation between dinucleophilic indole derivatives and Morita−Baylis−Hillman (MBH) carbonates was discovered by using the N1 and N4′/C4′ nucleophilicities of the indole precursors,in which indoles act as four atom synthons. This protocol provides an efficient and facile access to indole-1,2-fused 1,4-diazepinones and azepines in good to high yields in one step,which illustrates potential synthetic utilities in drug discovery.

关键词： Phosphine catalysis [4+3]Annulation Indole derivatives Nitrogen heterocycles Organocatalysis

Biomass-based production of trimellitic and trimesic acids

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Green Energy & Environment 2024年第8期9卷 1267-1278页

作者： Lin Yuan Yancheng Hu Guangyi Li Fengan Han Aiqin Wang Yu Cong Tao Zhang Feng Wang Ning Li CAS Key Laboratory of Science and technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences University of Chinese Academy of Sciences 19 A Yuquan RoadShijingshan District School of chemical Engineering and technology China University of Mining and Technology State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of Sciences

The production of industrial chemicals with renewable biomass feedstock holds potential to aid the world in pursuing a carbon-neutral *** and trimesic acids are important commodity chemicals in industry that are prepared by the oxidation of petroleum-derived *** reduce the dependence on the limited oil source,we develop a potential sustainable alternative towards trimellitic and trimesic acids using biomass-based 2-methyl-2,4-pentandiol （MPD）,acrylate and crotonaldehyde as starting *** process for trimellitic acid includes dehydration/D-A reaction of MPD and acrylate,flow aromatization over Pd/C catalyst,hydrolysis and catalytic aerobic oxidation （60%overall yield）.The challenging regioselectivity issue of D-A reaction is tackled by a matched combination of temperature and deep eutectic solvent ChCl/*** can also participate in the reaction,followed by Pd/C-catalyzed decarbonylation/dehydrogenation and oxidation to provide trimesic acid in 54%overall *** cycle assessment implies that compared to conventional fossil process,our biomass-based routes present a potential in reducing carbon emissions.

关键词： Biomass Trimellitic acid Trimesic acid Deep eutectic solvent Dehydration/D-A reaction

Coordination-environment regulation of atomic Co-Mn dual-sites for efficient oxygen reduction reaction

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Nano Research 2024年第8期17卷 6841-6848页

作者： Caiting Sun Yarong Liu Zunhang Lv Rui Liu Changli Wang Liuhua Li Jinming Wang Yu Zhang Wenxiu Yang Bo Wang Key Laboratory of Cluster Science(Ministry of Education) Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsAdvanced Technology Research Institute(Jinan)Advanced Research Institute of Multidisciplinary ScienceSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing institute of technology Library Beijing Institute of TechnologyBeijing 100081China

Precisely designing atomic metal-nitrogen-carbon(M-N-C)catalysts with asymmetric diatomic configurations and studying their structure–activity relationships for oxygen reduction reaction(ORR)are important for zinc-air batteries(ZABs).Herein,a dualatomic-site catalyst(DASC)with CoN_(3)S-MnN_(2)S_(2) configuration was prepared for the cathodes of *** with Co-N-C(Mn-free)and CoMn-N-C(S-free doping),CoMn-N/S-C exhibits excellent half-wave potential(0.883 V)and turnover frequency(1.54 e·s^(−1)·site^(−1)),surpassing most of the reported state-of-the-art Pt-free ORR *** CoMn-N/S-C-based ZABs achieve extremely high specific capacity(959 mAh·g^(−1))and good stability(350 h@5 mA·cm^(−2)).Density functional theory(DFT)calculation shows that the introduction of Mn and S can break the electron configuration symmetry of the original Co 3d orbital,lower the dband center of the Co site,and optimize the desorption behavior of*OH intermediate,thereby increasing the ORR activity.

关键词： metal organic frameworks oxygen reduction reaction dual-atom catalyst coordination-environment regulation zinc-air batteries

Microfluidic preparation of surfactant-free ultrafine DAAF with tunable particle size for insensitive initiator explosives

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Defence technology（防务技术） 2024年第9期39卷 42-52页

作者： Bo Yang Rui Li Wei Cao Si-min He Jincan Zhu Qi Wu Heng Ding Jin Chen Weimiao Wang Zhiqiang Qiao Xiaodong Li Guangcheng Yang institute of chemical Materials China Academy of Engineering PhysicsMianyang 621900China Southwest University of Science and technology Mianyang 621010China School of chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China

High purity and ultrafine DAAF(u-DAAF)is an emerging insensitive charge in *** there are many ways to obtain u-DAAF,developing a preparation method with stable operation,accurate control,good quality consistency,equipment miniaturization,and minimum manpower is an inevitable requirement to adapt to the current social technology development *** reported is the microfluidic preparation of u-DAAF with tunable particle size by a passive swirling *** the guidance of recrystallization growth kinetics and mixing behavior of fluids in the swirling microreactor,the key parameters(liquid flow rate,explosive concentration and crystallization temperature)were screened and optimized through screening *** the condition that no surfactant is added and only experimental parameters are controlled,the particle size of recrystallized DAAF can be adjusted from 98 nm to 785 nm,and the corresponding specific surface area is 8.45 m^(2)·g^(-1)to 1.33 m^(2)·g^(-1).In addition,the preparation method has good batch stability,high yield(90.8%-92.6%)and high purity(99.0%-99.4%),indicating a high practical application *** explosion derived flyer initiation tests demonstrate that the u-DAAF shows an initiation sensitivity much lower than that of the raw DAAF,and comparable to that of the refined DAAF by conventional spraying crystallization *** study provides an efficient method to fabricate u-DAAF with narrow particle size distribution and high reproducibility as well as a theoretical reference for fabrication of other ultrafine explosives.

关键词： Microfluidic preparation Screening crystallization conditions Narrow particle size distribution Low initiation sensitivity Ultrafine DAAF

Recent advances in Pt catalysts and membrane electrode assemblies fabrication for proton exchange membrane fuel cells

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Rare Metals 2024年第9期43卷 4198-4221页

作者： Miao Ma Li-Xiao Shen Jing Liu Bin Xu Yun-Long Zhang Lei Zhao Zhen-Bo Wang School of Chemistry and chemical Engineering Harbin Institute of TechnologyHarbin 150001China College of Environmental and chemical Engineering Yanshan UniversityQinhuangdao 066004China Unipower Hydrogen technology(Jiangsu)Corporation Changzhou 213176China

Proton exchange membrane fuel cells(PEMFCs)have been identified as a highly promising means of achieving sustainable energy conversion.A crucial factor in enhancing the performance of PEMFCs for further potential energy applications is the advancement in the field of catalyst engineering that has led to remarkable performance enhancement in facilitating the oxygen reduction reaction(ORR).Subsequently,it is important to acknowledge that the techniques used in preparation of membrane electrode assemblies(MEAs),the vital constituents of PEMFCs,also possess direct and critical influence on exhibiting the full catalytic activity of meticulously crafted ***,a succinct summary of the most recent advancements in Pt catalysts for ORR was offered and their underly catalytic mechanism were ***,both laboratory-scale and industrial-scale MEA fabrication techniques of Pt catalysts were ***,a detailed analysis of the connections between materials,process,and performance in MEA fabrication was presented in order to facilitate the development of optimal catalyst layers.

关键词： Pt catalysts Oxygen reduction reaction Membrane electrode assemblies MEA fabrication techniques

Supramolecular Macrocycle Regulated Single-Atom MoS2@Co Catalysts for Enhanced Oxygen Evolution Reaction

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Energy & Environmental Materials 2024年第5期7卷 287-295页

作者： Shuai Cao Wenzhuo Wu Chaozhong Liu Leqian Song Qun Xu Huacheng Zhang Yanli Zhao School of chemical Engineering and technology Xi’an Jiaotong University Henan institute of Advanced technology Zhengzhou University Department of Materials Science and Engineering Zhengzhou University School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University

The development of active water oxidation catalysts for water splitting has stimulated considerable interest. Herein, the design and building of single atom Co sites using a supramolecular tailoring strategy are reported, that is,the introduction of pillar[4]arene[1]quinone （P4A1Q） permits mononuclear Co species stereoelectronically assembled on MoS2matrix to construct an atomically dispersed MoS2@Co catalyst with modulated local electronic structure, definite chemical environment and enhanced oxygen evolution reaction performance. Theoretical calculations indicate that immsobilized single-Co sites exhibit an optimized adsorption capability of oxygencontaining intermediates, endowing the catalyst an excellent electrocatalytic oxygen evolution reaction activity, with a low overpotential of 370 mV at10 mA cm-2and a small Tafel slope of 90 mV dec-1. The extendable potential of this strategy to other electrocatalysts such as MoS2@Ni and MoS2@Zn, and other applications such as the hydrogen evolution reaction was also demonstrated. This study affords new insights into the rational design of single metal atom systems with enhanced electrocatalytic performance.

关键词： electrocatalysis oxygen evolution reaction pillararenequinone single atoms transition-metal dichalcogenides

TiO_(2) nanofiber-supported copper nanoparticle catalysts for highly efficient methane conversion to C1 oxygenates under mild conditions

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Nano Research 2024年第5期17卷 3844-3852页

作者： Wencui Li Yu Ren Zean Xie Yipeng Wang Hang Zhang Dianxiang Peng Hengfang Shen Hongfei Shi Jiaxin Cai Peng Wang Tongxin Zhang Zhen Zhao State Key Laboratory of Heavy Oil Processing China University of Petroleum(Beijing)Beijing 102249China institute of Catalysis for Energy and Environment College of Chemistry&Chemical EngineeringShenyang Normal UniversityShenyang 110034China institute of Petrochemical technology Jilin Institute of Chemical TechnologyJilin 132022China

The selective oxidation of methane under mild conditions remains the“Holy Grail of Catalysis”.The key to activating methane and inhibiting over-oxidation of target oxygenates lies in designing active *** nanoparticles were loaded onto TiO_(2) nanofibers using the photo-deposition *** resulting catalysts were found to effectively convert methane into C1 oxygenated products under mild *** with previously reported catalysts,it delivers a superior performance of up to 2510.7 mmol·g_(Cu)^(-1)·h^(-1) productivity with a selectivity of around 100%at 80℃for 5 *** characterizations and density functional theory(DFT)calculations indicate that TiO_(2) in the mixed phase of anatase and rutile significantly increases the Cu^(+)/CuO ratio of the supported Cu species,and this ratio is linearly related to the formation rate of oxygen-containing *** CuI site promotes the generation of active O species from H_(2)O_(2) dissociation on Cu_(2)O(111).These active O species reduce the energy barrier for breaking the C-H bond of CH_(4),thus boosting the catalytic *** methane conversion mechanism was proposed as a methyl radical pathway to form CH_(3)OH and CH_(3)OOH,and then the generated CH_(3)OH is further oxidized to HOCH_(2)OOH.

关键词： TiO_(2)nanofiber copper nanoparticles photo-deposition method methane oxidation C1 oxygenates