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Construction of multifunctional lanthanum manganese mixed nanoparticles mediated by ionic liquids for selective aerobic oxidation of cyclohexane

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Rare Metals 2024年第5期43卷 2205-2221页

作者： Hao Li Rui-Rui Zhang Ke-Xin Li Shuang Wei Yu-Mei Liu Rui-Xia Liu 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 SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Selective oxidation of alkanes to produce highvalue chemicals is an essential strategy and means to realize efficient utilization of *** this work,a strategy of lanthanum manganese mixed metal oxides(LMMO)regulated via a facile ionic liquid(IL)-assisted hydrothermal method was proposed to construct the multifunctional catalysts,which exhibited excellent catalytic performance in the selective aerobic oxidation of *** 8.9%cyclohexane conversion with 90%KA oi(cyclohexanol and cyclohexanone)selectivity was achieved over the optimal LMMO catalyst under mild *** effects of anion type,carbon chain length and concentration of ILs on the structure and properties of catalysts were investigated through various characterizations,indicating the structure-directing and template effect of ILs on the multifunctional *** formation of self-assembled spherical nanoparticles followed the"dissolution-nucleation-proliferation"mechanism with the introduction of 1-butyl-3-methylimidazolium hydrogen sulfate,ascribing the synergistic effect between the microenvironment of ILs and the hydrothermal ***,the high reactive oxygen concentration redox capacity,and suitable basic sites of LMMO catalysts mediated by ILs enhance the activation of C-H bonds and molecular oxygen,simultaneously influencing the adsorption and desorption of the substrate.A comprehensive understanding of the high KA oil selectivity and radical reaction mechanism was elucidated based on in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and radical trapping *** recycling and regeneration experiments further illuminated that the removal of adsorbed cyclohexanone acting on the LMMO catalyst was the key to achieve high KA oil selectivity.

关键词： Ionic liquids Nanoparticle Multifunctional catalyst Cyclohexane oxidation

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Advanced 3D ordered electrodes for PEMFC applications: From structural features and fabrication methods to the controllable design of catalyst layers

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Green Energy & Environment 2024年第9期9卷 1336-1365页

作者： Kaili Wang Tingting Zhou Zhen Cao Zhimin Yuan Hongyan He Maohong Fan Zaiyong Jiang School of Chemistry&Chemical Engineering and Environmental Engineering Weifang UniversityWeifang261061China Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex SystemsCAS Key Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China College Engineering and Physical Sciences and School of Energy ResourcesUniversity of WyomingLaramieWY 82071USA

The catalyst layers(CLs) electrode is the key component of the membrane electrode assembly(MEA) in proton exchange membrane fuel cells(PEMFCs). Conventional electrodes for PEMFCs are composed of carbon-supported, ionomer, and Pt nanoparticles, all immersed together and sprayed with a micron-level thickness of CLs. They have a performance trade-off where increasing the Pt loading leads to higher performance of abundant triple-phase boundary areas but increases the electrode cost. Major challenges must be overcome before realizing its wide commercialization. Literature research revealed that it is impossible to achieve performance and durability targets with only high-performance catalysts, so the controllable design of CLs architecture in MEAs for PEMFCs must now be the top priority to meet industry goals. From this perspective, a 3D ordered electrode circumvents this issue with a support-free architecture and ultrathin thickness while reducing noble metal Pt loadings. Herein, we discuss the motivation in-depth and summarize the necessary CLs structural features for designing ultralow Pt loading electrodes. Critical issues that remain in progress for 3D ordered CLs must be studied and characterized. Furthermore, approaches for 3D ordered CLs architecture electrode development, involving material design, structure optimization, preparation technology, and characterization techniques, are summarized and are expected to be next-generation CLs for PEMFCs. Finally, the review concludes with perspectives on possible research directions of CL architecture to address the significant challenges in the future.

关键词： PEMFC 3D ordered electrode Structural features Preparation technology Ultralow Pt loading

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The infinite separation principle

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Green Energy & Environment 2023年第5期8卷 1229-1231页

作者： Suojiang Zhang 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 SciencesBeijing100190China

In this paper,we propose“The Infinite Separation Principle”.This principle contains two implications:firstly,even exhausting all separation approaches,including chemical techniques,it is impossible to achieve 100%pu... 详细信息

关键词： Separation Thermodynamics Purity Mixture

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Selective cyclohexane oxidation enhancement by electronic structures regulation of metal-poly(ionic liquid)s

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Green Chemical engineering 2024年第2期5卷 213-221页

作者： Ying Jin Shengxin Chen Ruirui Wang Yumei Liu Xinxin Li Yingwei Li Ruirui Zhang Ruixia Liu Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou450001China Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringInnovation Academy for Green ManufactureCASBeijing100190China

Poly(ionic liquids)(PILs)combined with the macromolecular structure and unique properties of ionic liquids show unlimited potential in *** this work,a series of metal-based PIL with different ionic ratios were prepared for the selective oxidation of *** analysis reveals that different degrees of ionization could adjust the Co-N sites of the catalysts efficiently,leading to significant changes in their electronic structure,which strongly relate to catalytic performance in oxidation.20.07%cyclohexane conversion and 13.06%cyclohexanone and cyclohexanol(KA oil)yield can be achieved by metal-based PILs that are better than other commercial *** with CoCl_(2),metal-based PILs perform well,with superior conversion and KA oil *** interestingly,the catalyst created in this study features a malleable Co-N site,which may potentially have an impact on how oxygen species adsorb and desorb from the ***,the catalyst studied in this work is used as molecular oxygen for the selective oxidation of cyclohexane to produce KA oil,and its application prospect is promising.

关键词： Metal-PILs Cyclohexane oxidation C-H activation Co-N sites

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Ionic liquid-trimetallic electrocatalytic system for C–O bond cleavage in lignin model compounds and lignin under ambient conditions

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Nano Research 2024年第4期17卷 2420-2428页

作者： Guangyong Liu Yumiao Lu JunFeng Lu Yanlei Wang Shijing Liang Hongyan He Lilong Jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhou 350002China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex SystemsBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial TechnologyZhengzhou 450000China

Electrocatalytic depolymerization of lignin into value-added chemicals offers a promising technique to make biorefining ***,we report a robust trimetallic PdNiBi electrocatalyst for reductive C–O bond cleavage of different lignin model dimers and oxidized lignin under mild *** reduction reaction proceeds with complete substrate conversion and excellent yields toward monomers of phenols(80%–99%)and acetophenones(75%–96%)in the presence of an ionic liquid electrolyte with operational *** experimental investigations together with density functional theory(DFT)calculations reveal that the outstanding performance of the catalyst results from the synergistic effect of the metal elements,which facilitates the easier formation of a key Cαradical intermediate and the facile desorption of the as-formed products at the *** results open up new opportunities for lignin valorization through the green electrocatalytic approach.

关键词： electrocatalytic depolymerization lignin Ionic liquids density functional theory(DFT)calculation

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Computational study of the effect of friction coefficients and particle shape on the repose angle and porosity of sinter piles

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Particuology 2025年第3期98卷 231-240页

作者： Meng Li Yaowei Yu Henrik Saxén Process and Systems Engineering Laboratory Faculty of Science and EngineeringÅbo Akademi University20500TurkuFinland State Key Laboratory of Advanced Special Steel Shanghai Key Laboratory of Advanced FerrometallurgySchool of Materials Science and EngineeringShanghai University200444ShanghaiChina

Shape has an undeniable impact on particle behaviour,and the shapes of naturally occurring granular matter are typically *** studies of irregularly shaped particles are challenging but necessary to gain a better understanding of the flow of particulate *** study focuses on the behaviour of irregular sinter particles and applies the discrete element method to examine the effects of static and rolling friction coefficients and particle shape on the angle of repose and porosity of sinter piles.A three-dimensional model of an irregular sinter particle reconstructed by close-range photogrammetry served as the template for generating multi-sphere particles with varying numbers of sub-spheres(1,3,7,22,and 135)and sphericity ranging from 1 to *** of particle piles were conducted for a range of values of the coefficients of static and rolling *** results indicate that the angle of repose increases with static friction and also increases with rolling friction coefficient when it is lower than the static *** angle of repose shows clear dependence on particle shape,particularly for lower rolling friction *** friction coefficients for particles of five different shapes were individually determined through bulk calibration,and irregularly shaped particles in DEM were found to require lower friction *** was marginally affected by the static and rolling friction coefficients for spherical particles,while non-spherical particles showed porosity increasing with the rolling friction *** relationship between particle sphericity and porosity was nonlinear:as sphericity decreases from 1.00 to 0.69,the porosity first decreases to a minimum and then *** findings confirmed that both friction and particle shape have a significant influence on the structure of sinter piles,with implications for material handling and processing in industrial applications.

关键词： Sinter Discrete element method Friction coefficients Particle shape Repose angle Porosity

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An improved EMMS model for turbulent flow in pipe and its solution

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Particuology 2023年第5期76卷 1-12页

作者： Lin Zhang Wen Lai Huang Jianhua Chen State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China

Based on the existing energy-minimization multi-scale(EMMS)model for turbulent flow in pipe,an improved version is proposed,in which not only a new radial velocity distribution is introduced but also the quantification of total dissipation over the cross-section of pipe is improved for the dominant mechanism of fully turbulent flow in *** four dynamic equality constraints and some other constraints are constructed but there are five parameters involved,leading to one free variable *** the compromise in competition between dominant mechanisms for laminar and fully turbulent flow in pipe respectively,the above four constructed dynamic equality constraints can be ***,the cases for turbulent flow in pipe with low,moderate and high Reynolds number are simulated by the improved EMMS *** numerical results show that the model can obtain reasonable results which agree well with the data computed by the direct numerical simulation and those obtained by *** illustrates that the improved EMMS model for turbulent flow in pipe is reasonable and the compromise in competition between dominant mechanisms is indeed a universal governing principle hidden in complex ***,one more EMMS model for a complex system is offered,pro-moting the further development of mesoscience.

关键词： Mesoscience EMMS Compromise in competition Dominant mechanism Turbulent flow in pipe

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A brief review of preparation and applications of monolithic aerogels in atmospheric environmental purification

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Journal of Environmental Sciences 2025年第3期149卷 209-220页

作者： Linfeng Nie Shuangde Li Mengjie Cao Ning Han Yunfa Chen 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 Key Laboratory of Science&Technology on Particle Materials Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Monolithic aerogels are promising candidates for use in atmospheric environmental purification due to their structural advantages,such as fine building block size together with high specific surface area,abundant pore structure,***,monolithic aerogels possess a unique monolithic macrostructure that sets them apart from aerogel powders and nanoparticles in practical environmental clean-up *** review delves into the available synthesis strategies and atmospheric environmental applications of monolithic aerogels,covering types of monolithic aerogels including SiO_(2),graphene,metal oxides and their combinations,along with their preparation *** particular,recent developments for VOC adsorption,CO_(2)capture,catalytic oxidation of VOCs and catalytic reduction of CO_(2)are ***,challenges and future opportunities for monolithic aerogels in the atmospheric environmental purification field are *** reviewprovides valuable insights for designing and utilizing monolithic aerogel-based functional materials.

关键词： Monolithic aerogel Environmental purification Catalysis Adsorption

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Boosting electrochemical reduction of CO_(2)to CO using molecule-regulated Ag nanoparticle in ionic liquids

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Green Energy & Environment 2025年第4期10卷 813-820页

作者： Fangfang Li Kuilin Peng Chongyang Jiang Shaojuan Zeng Xiangping Zhang Xiaoyan Ji Energy Engineering Division of Energy ScienceLuleåUniversity of TechnologyLuleå97187Sweden Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China College of Chemical Engineering and Environment China University of PetroleumBeijing102249China

Electrochemical reduction of CO_(2)is a promising approach to convert CO_(2)to high-valued chemicals and ***,developing efficient electrocatalysts featuring desirable activity and selectivity is still a big *** this work,a strategy of introducing functionalized molecules with desirable CO_(2)affinity to regulate Ag catalyst for promoting electrochemical reduction of CO_(2)was ***,3-mercapto-1,2,4-triazole was introduced onto the Ag nanoparticle(Ag-m-Triz)for the first time to achieve selectively converting CO_(2)to carbon monoxide(CO).This Ag-m-Triz exhibits excellent performance for CO_(2)reduction with a high CO Faradaic efficiency(FECO)of 99.2%and CO partial current density of 85.0 mA cm^(-2)at-2.3 V ***/Ag^(+) in H-cell when combined with the ionic liquid-based electrolyte,30 wt%1-butyl-3-methylimidazolium hexafluorophosphate([Bmim][PF6])-65 wt%acetonitrile(AcN)-5 wt%H2O,which is 2.5-fold higher than the current density in Ag-powder under the same *** studies confirm that the significantly improved performance of Ag-m-Triz originates from(i)the stronger adsorption ability of CO_(2)molecule and(ii)the weaker binding energy to form the COOH*intermediate on the surface of Ag-m-Triz compared with the Ag-powder catalyst,which boosts the conversion of CO_(2)to *** research provides a facile way to regulate electrocatalysts for efficient CO_(2)reduction by introducing functionalized molecules.

关键词： CO_(2)reduction CO Electrochemical Molecule-regulated Silver Ionic liquid

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A novel synthetic method of porous and nanoflower-like Al_(2)O_(3)/MoS_(2)catalyst for reduction of SO_(2)to elemental sulfur

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Nano Research 2023年第5期16卷 6076-6084页

作者： Yiqian Yang Jiayuan Yu Yu Chen Gang Wang Chunshan Li Erqiang Wang Zhijian Peng School of Engineering and Technology China University of GeosciencesBeijing 100083China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex SystemsBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China

MoS_(2)nanoflowers are favored for their potential in the production of elemental sulfur due to abundant surface area and good catalytic performance for reducing SO_(2).A novel synthetic strategy of porous Al_(2)O_(3)supported on the MoS_(2)with nanoflower structure was *** effects of preparation concentration,calcination atmosphere,Al_(2)O_(3)contents on the growth of catalysts with nanoflower structure were systematically studied via X-ray diffraction(XRD),scanning electron microscopy(SEM),X-ray photoelectron spectroscopy(XPS),transmission electron microscopy(TEM),Fourier transform infrared(FTIR)spectroscopy,Brunauer–Emmett–Teller(BET).The surface area was increased to 295.502 m^(2)/g and the amount of Lewis acid on the surface of the Al_(2)O_(3)/MoS_(2)catalyst was increased by adjusting the ratio of Al/*** porous and nanoflower structures of Al_(2)O_(3)/MoS_(2)catalysts promoted the sulfur selectivity without inhibiting the catalytic performance of MoS_(2).The conversion of SO_(2)and the selectivity of sulfur were 100%and 92%after 100 h life evaluation.

关键词： porous catalyst nanoflower reduction of SO_(2) sulfur production hydrogen

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