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SSRN 2024年

作者： Tian, Du Chen, Weimin Shen, Yue Cao, Wenzhu Miao, Wenwen Lai, Zhenghan Chen, Hong Yang, Shanshan Wang, Liang Yu, Faquan Key Laboratory for Green Chemical Process Ministry of Education Hubei Key Laboratory for Novel Reactor and Green Chemistry Technology Hubei Three Gorges Laboratory Hubei Engineering Research Center for Advanced Fine Chemicals School of Chemical Engineering and Pharmacy Wuhan Institute of Technology Wuhan430205 China State Key Laboratory of Material Processing and Die and Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan430074 China Chongqing Institute of Green and Intelligent Technology Chinese Academy of Sciences Chongqing400714 China

Thin lithium metal anodes (LMAs) play a crucial role in realizing lithium metal batteries (LMBs) with high-energy-density. However, the commercial production of thin lithium anode continues to face challenges in manufacturing complexities, inadequate reversible capacity and unstable cyclability. Herein, we show a facile and effective strategy to produce ultra-thin LMAs with tunable thickness (10~50 μm), in which the Li-Ag alloy is in-situ formed and uniformly loaded on the cellulose-derived carbon supported reduced graphene oxide (CC-rGO). Density functional theory (DFT) calculations reveal that the Li-Ag alloy has strong adsorption energy and minimal energy barrier for Li diffusion, which can effectively meliorate Li transfer and homogeneous deposition. Due to the advantages of the synergistic effect of Li-Ag alloy modification, the elaborate-designed ultra-thin and 3D structure, the CC-rGO/LixAgy/Li anode facilitates the acceleration of Li-ion transport kinetics, reduce the nucleation barrier and offer adequate active sites, thereby improving the electrochemical characteristics. The CC-rGO/LixAgy/Li symmetric cell exhibits stably Li plating/stripping for 5000 h at 1 mA cm−2. When matched with LiFePO4 cathode, the full cell delivers remarkable cycling reversibility for 900 cycles at 3 C and the negative/positive capacity (N/P) ratio can be down to 1.18. More impressively, the pouch cell reveals an excellent flexibility with maintaining more than 80% capacity over 80 cycles at 0.3 C in folded states. This study provides a promising avenue to developing viable high-energy-density LMBs. © 2024, The Authors. All rights reserved.

关键词： Lithium alloys

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Chemical Disproportionation-Driven Li Metal-Free Prelithiation of Silicon Monoxide into Practical Anode Materials for Li-Ion Batteries

SSRN

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SSRN 2023年

作者： Gao, Zhe Chai, Fengtao Liu, Fan Liu, Jingbo Zhao, Chongchong Dong, Jiayu Huo, Feng Henan Key Laboratory of Engergy Storage Materials and Processes Zhengzhou Institute of Emerging Industrial Technology Zhengzhou450003 China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial Technology Henan University Zhengzhou450000 China Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China

Silicon monoxide (SiO) has been explored and confirmed as a promising anode material, which can improve the energy density of Li-ion batteries (LIBs) that are required for the advancement of electric vehicles. However, its poor initial coulombic efficiency (ICE) strictly limits its commercial application. Here, we propose that chemical disproportionation-driven Li metal-free prelithiation method to improve the ICE of SiO anode. Low cost and stable lithium compound using lithium hydroxide (LiOH) reacts with commercially available solid SiO particles at a relatively low temperature (800℃) to produce reversible lithium silicate and nano/micro-structured silicon surrounded by SiO (Si–SiO–LixSiOy multicomponents) in the molten state, while that can also be demonstrated by transmission electron microscopy or X-ray photoelectron spectroscopy. The SiO which prelithiation and disproportionation, or SiO without the coating of carbon sample (PD-SiO), has high ICE (82.5%)，high charging capacity (1419mAh g-1) and highly stable cycling performance (94.6% capacity retention rate after 200 cycles at 0.5 A g-1). With this work, we tend to offer a promising direction toward the practical industrialization of SiO anode material. © 2023, The Authors. All rights reserved.

关键词： Lithium compounds

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CoSe_(2)/MoS_(2) Heterostructures to Couple Polysulfide Adsorption and Catalysis in Lithium-Sulfur Batteries

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Chinese Journal of Chemistry 2021年第5期39卷 1138-1144页

作者： Zihan Shen Qingwen Zhou Huiling Yu Jiaming Tian Man Shi Chaoquan Hu Huigang Zhang Notional Laboratory of Solid State Microstructures College of Engineering and Applied SciencesInstitute of Materials Engineeringand Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjingJiangsu 210046China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Nanjing IPE Institute of Green Manufacturing Industry NanjingJiangsu 211100China

Lithium-sulfur batteries have been regarded as one of most promising next-generation energy storage devices because of their high energy density and low ***,polysulfide shuttling and slow kinetics hinder the practical *** fabricated hierarchically heterostructured CoSe_(2)/MoS_(2) nanoarrays on carbon clothes as the sulfur cathode *** resulting heterostructures facilitate electron conduction and improve electrolyte *** importantly,the composite heterostructures couple the strong poly-sulfide adsorption of CoSe_(2) and high catalytic activity of MoS_(2) to synergistically accelerate polysulfide conversion,demonstrating higher catalytic activity than their individual components.

关键词： Lithium-sulfur batteries Heterostructure Electrocatalyst CoSe_(2) MoS_(2)

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Light doping of tungsten into copper-platinum nanoalloys for boosting their electrocatalytic performance in methanol oxidation

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Nano Research Energy 2022年第2期1卷 194-200页

作者： Danye Liu Qing Zeng Chaoquan Hu Dong Chen Hui Liu Yongsheng Han Lin Xu Qingbo Zhang Jun Yang State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Nanjing IPE Institute of Green Manufacturing Industry Nanjing 211100China School of Chemistry and Materials Science Jiangsu Key Laboratory of New Power BatteriesJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjing 210023China Department of Bioengineering Rice UniversityHoustonTexas 77005USA

Coupling the bi-functional mechanism with compressive lattice strain might be an effective way to boost the electrocatalysis of platinum(Pt)-based nanoparticles for methanol oxidation reaction(MOR).This strategy weakens the chemisorption of poisoning CO-like intermediates generated during MOR on the active Pt sites by lowering their d-band *** this context,we herein report the synthesis of ternary copper-tungsten-platinum(CuWPt)nanoalloys with light doping of W element by simply co-reducing their precursors at elevated *** this ternary alloy system,the presence of only small amount of W element not only weakens the chemisorption of CO-like intermediates by lowering the Pt d-band center through compressive lattice strain,but also cleans the active Pt sites by“hydrogen spillover effect”,endowing the as-prepared CuWPt nanoalloys at an appropriate Cu/W/Pt ratio with good activity for *** specific,the ternary CuWPt alloy nanoparticles at a Cu/W/Pt molar ratio of 21/4/75 show a specific activity of 2.5 mA·cm^(−2)and a mass activity of 2.11 A·mg^(−1)with a better durability,outperforming those ternary CuWPt alloy nanoparticles at other Cu/W/Pt ratios,binary CuPt alloys and commercial Pt/C catalyst as well as a large number of reported Pt-based *** addition,a single direct methanol fuel cell(DMFC)assembled using ternary CuWPt nanoalloys as anodic catalysts shows a power density of 24.3 mW·cm^(−2)and an open-circle voltage of 0.6 V,also much higher than those of the single DMFC assembled from commercial Pt/C catalysts.

关键词： lattice strain d-band center electrocatalysis hydrogen spillover methanol oxidation reaction

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Effects of imidazolium-based ionic liquids on the isobaric vapor–liquid equilibria of methanol+dimethyl carbonate azeotropic systems

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Chinese Journal of Chemical engineering 2020年第3期28卷 766-776页

作者： Songsong Chen Li Dong Junping Zhang Weiguo Cheng Feng Huo Qian Su Wei Hua Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of Sciences.Beijing 100090China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China SINOPEC Beijing Yanshan CompanyBeijing 102500China Dalian National Laboratory for Clean Energy Dalian 116023China

The separation of methanol(MeOH)and dimethyl carbonate(DMC)is important but difficult due to the formation of an azeotropic *** this work,isobaric vapor–liquid equilibrium(VLE)data for the ternary systems containing different imidazolium–based ionic liquids(ILs),***+DMC+1-butyl-3-methy-limidazolium bis[(trifluoromethyl)sulfonyl]imide([Bmim][Tf2N]),MeOH+DMC+1-ethyl-3-methyl-imidazolium bis[(trifluoromethyl)sulfonyl]imide([Emim][Tf2N]),and MeOH+DMC+1-ethyl-3-methylimidazolium hexafluorophosphate([Emim][PF6])were measured at 101.3 *** mole fraction of IL was varied from0.05 to *** experimental data were correlated with the NRTL and Wilson equations,*** results show that imidazolium-based ILs were beneficial to improve the relative volatility of MeOH to DMC,and[Bmim][Tf2 N]showed a much more excellent performance on the activity coefficient of *** interaction energies of system components were calculated using Gaussian program,and the effects of cation and anion on the separation coefficient of the azeotropic system were discussed.

关键词： Vapor liquid equilibria Ionic liquid Azeotrope Separation Interaction energy

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Synthesis of Re-processable Polyurea Thermosets from CO2-Based Oligourea and Formaldehyde

ACS Sustainable Resource Management

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ACS Sustainable Resource Management 2024年第11期1卷 2502-2510页

作者： Wenhan Huang Hui Li Fengyu Zhao Haiyang Cheng State Key Laboratory of Electroanalytical Chemistry & Jilin Province Key Laboratory of Green Chemistry and Process Changchun Institute of Applied Chemistry Chinese Academy of Sciences No. 5625 Renmin Rd. Changchun 130022 China School of Applied Chemistry and Engineering University of Science and Technology of China No. 96 Jinzhai Rd. Hefei 230026 China

The synthesis of functional polymer materials from CO2, an abundant and cheap feedstock, is of great significance from the viewpoint of green and sustainable development. Using CO2as monomer to produce functional polymeric materials can reduce not only fossil consumption but also CO2emissions. Herein, we designed a re-processable polyurea thermoset from formaldehyde and CO2-based oligourea, which is an amino-terminated oligomer derived from CO2and 4,7,10-trioxa-1,13-tridecanediamine. The CO2-based oligourea reacted with formaldehyde to form polyurea hemiaminal networks (PHNs) with a hemiaminal structure and reversible hydrogen bonds. PHNs are of good mechanical properties due to their intermolecular hydrogen bonds and cross-linked structure. Moreover, the reversible non-covalent hydrogen bonds and hemiaminal structure in the chains enabled PHNs to be re-processable. The synthesized polyurea thermoset can be hot-molded, the tensile strength is about 20 MPa, and the elongation at break is about 20% of the original sample. In addition, the tensile strength and toughness can be nearly recovered after hot-reprocessed for 6 cycles. This is the first report of the re-processable thermosetting polyurea from CO2designed by hydrogen bonds and hemiaminal cross-linking structure.

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V2O3/VN Catalysts Decorated Free-Standing Multifunctional Interlayer for High-Performance Li-S Battery

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CHEMICAL engineering JOURNAL 2022年第0期441卷

作者： Zhao, Jie Zhao, Yuyan Yue, Wen-ce Li, Xue Gao, Ning Zhang, Yu-jiao Hu, Chao-quan [a]Nanjing IPE Institute of Green Manufacturing Industry Nanjing 211135 PR China [b]State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 PR China [c]Key Laboratory of Bio-inspired Materials and Interfacial Science Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 PR China [d]State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 PR China

The shuttle effect caused by soluble lithium polysulfides (LiPSs) hinders the practical application of lithium-sulfur batteries. The sluggish reaction kinetics of LiPSs results in rapid capacity decay. In this work, we constructed a free-standing multifunctional interlayer decorated with V2O3/VN catalysts to suppress the shuttle effect and boost the redox reaction kinetics. The introduction of VN with strong chemical adsorption improves the conductivity of V2O3, which is beneficial for the kinetics of conversion reaction. In addition, the micro/mesopores inside the structure not only facilitate ion diffusion but also buffer the volume change of the sulfur cathode during the cycling process. Benefiting from the synergistic effects, the fabricated cells exhibit a high specific capacity of 1419.5 mAh g(-1) at 0.1C. The cell with V2O3/VN/C exhibits a promising cycling performance over 1000 cycles with a decay rate of 0.037% per cycle at 1C. The synergistic effects of electrocatalysts and conductive carbon material provide inspiration on the development of high-performance Li-S batteries.

关键词： V2O3/VN nanowires Carbonized bacteria cellulose nanowires Interlayer Synergistic effect Lithium-sulfur batteries

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In-Depth Understanding of the key to Deactivation of Ts–1 in Epoxidation of Allyl Chloride to Epichlorohydrin

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SSRN 2023年

作者： Liu, Yueming Liu, Dongxu Wu, Huiying Fang, Nan Lin, Huanhao Jin, Yucheng He, Mingyuan a State Key Laboratory of Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China b Institute of Eco-Chongming Shanghai 202162 China

We present an intensive study of the deactivation mechanism of titanosilicates in epoxidation of allyl chloride to epichlorohydrin. Besides the generally accepted physical deactivation of titanosilicates caused by pore blocking, the product epichlorohydrin is the main reason for the deactivation of titanosilicates, in which the epoxy group undergoes a ring-opening reaction to form the poisoning species-bidentate ether species. Besides the acidity of titanosilicates and titanosilicates/H2O2, the effect of the properties of reactants and products on the formation of bidentate ether species was investigated. The reactant ALC is susceptible to ionization and the formation of new Brønsted acid, which accelerates the deactivation of titanosilicates. From the epoxide perspective, other groups in the vicinity of the epoxy group also have an effect on the formation of the bidentate ether species. In general, the formation of the bidentate ether species is promoted by the electron-donating groups and inhibited by the electron-absorbing groups. © 2023, The Authors. All rights reserved.

关键词： Ethers

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Investigation of the Adsorption Performance and Mechanism of Multi-Source Mineral Composite Calcination Materials on Heavy Metal Ions

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SSRN 2024年

作者： Yao, Yisong Feng, Yali Li, Haoran Liu, Mengyao Cui, Yufeng Xu, Chenglong Li, Yunhao Xue, Zhonghua Wang, Jianwei School of Civil and Resource Engineering University of Science and Technology Beijing Beijing100083 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China University of Chinese Academy of Sciences Beijing100049 China

To address the challenges of plume generation and the release of heavy metal ions caused by deep-sea mining operations, this study utilized multi-source minerals, including steel slag (SS), oceanic manganese nodules (OMN), attapulgite (AT), and sawdust (SD), to fabricate a multi-source mineral composite calcination material (MMCCM) through a sintering process. This MMCCM was then employed as an adsorbent in preliminary experiments exploring the adsorption of heavy metal ions. The results indicated that MMCCM had adsorption capacities of 46.99 (Cu2+), 40.49 (Co2+), and 38.65 mg/g (Ni2+). In a single-component system, the isotherm adsorption of Cu2+ adhered to both Langmuir and Freundlich models, adequately describing the adsorption behavior of Cu2+, while the Freundlich model was more applicable in competitive systems. The adsorption of Co2+ and Ni2+ consistently aligned with the Langmuir model across all systems. The adsorptive behavior of the three ions conformed to pseudo-second-order kinetics, with the adsorption dynamics indicating that chemical adsorption was the predominant mechanism and intraparticle diffusion was the principal rate-limiting step. Thermodynamic analyses of the adsorption process confirmed its spontaneous nature. Characterization techniques such as the Brunauer–Emmett–Teller (BET) method for surface area, thermogravimetric-differential thermal analysis (TG-DTG), scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy (SEM-EDS), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), and X-ray photoelectron spectroscopy (XPS) elucidated that surface physical adsorption, ion exchange, complexation with functional groups, electrostatic attraction, and co-precipitation, which were the predominant adsorption mechanisms for MMCCM. Evaluations of regenerability, economy, security, and suitability demonstrated that MMCCM is an eco-friendly adsorbent, which provides substantial experimental materials and data su

关键词： Adsorption

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Investigation of Hydraulic Behavior in a Gas-Agitated Disc and Doughnut Column for Solvent Extraction

SSRN

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SSRN 2024年

作者： Wang, Chi Xu, Dongbing Tan, Boren Chang, Chao Wang, Chenye Wang, Yong Xing, Peng Li, Huiquan Gui, Xiahui Yang, Jianguo State Key Laboratory of Coking Coal Resources Green Exploitation China University of Mining and Technology Xuzhou221116 China School of Chemical Engineering and Technology China University of Mining and Technology Xuzhou221116 China CAS Key Laboratory of Green Process and Engineering National Engineering Research Center of Green Recycling for Strategic Metal Resources Institute of Process Engineering Chinese Academy of Sciences Beijing100090 China University of Chinese Academy of Sciences Beijing100049 China Monash University Australia Nanjing IPE Institute of Green Manufacturing Industry China

The gas-agitated extraction column represents a novel extraction technology that employs gas to break-up droplets. Hydraulic characteristics, including droplet size (d32), dispersed-phase holdup (xd), and gas holdup (xg), are critical for design and scaling-up of extraction columns. These parameters were evaluated using a 30 mm disc-and-doughnut column (DDC) equipped with a gas-input unit. The water as dispersed-phase and tributyl phosphate (TBP)/kerosene as continuous-phase. The results show that when no gas is introduced, the countercurrent cannot be maintained, and reach flooding directly. Once gas is introduced, the flow state returns to normal. Results indicate that d32 diminishes with increasing gas-velocity, suggesting that gas can act as a substitute energy for droplet fragmentation. The xd initially decreases and then increases with greater gas-velocity, while increasing with the velocities of two-phases. xg only increases with gas-velocity. Empirical correlations for d32, xd, and xg are proposed with deviations of 11.59%, 15.85%, and 4.29%, respectively. © 2024, The Authors. All rights reserved.

关键词： Gases

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