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Synthesis of spherical nano-ZSM-5 zeolite with intergranular mesoporous for alkylation of ethylbenzene with ethanol to produce m-diethylbenzene

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Chinese Journal of Chemical engineering 2024年第3期67卷 298-309页

作者： Siyue Wang Jinhong Li Qingxin Xu Shengjie Song Yu'ni Jiang Lidong Chen Xin Shi Weiguo Cheng Faculty of Chemistry and Chemical engineering Liaoning Normal UniversityDalian 110629China Beijing Key Laboratory of Ionic Liquids Clean process Key Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Catalytic synthesis of m-diethylbenzene(m-DEB)through alkylation of ethylbenzene(EB)may be a promising alternative route in comparison with traditional rectification of mixed DEB,for which the top priority is to develop efficient and stable heterogeneous ***,the spherical nano-ZSM-5 zeolite with abundant intergranular mesoporous is synthesized by the seed-mediated growth method for alkylation of EB with ethanol to produce *** results show that the spherical nano-ZSM-5 zeolite exhibits better stability and higher alkylation activity at a lower temperature than those of commercial micropore *** then,the spherical nano-ZSM-5 is further modified by La_(2)O_(3) through acid treatment followed by immersion *** acid treatment causes nano-ZSM-5 to exhibit the increased pore size but decreased the acid sites,and subsequent La_(2)O_(3) loading reintroduces the weak acid *** a result,the HNO_(3)-La_(2)O_(3)-modified catalyst exhibits a slight increase in EB conversion and DEB yield in comparison with unmodified one,and meanwhile,it still maintains high m-DEB *** catalyst after acid treatment achieves higher catalytic stability besides maintaining the high alkylation activity of EB with *** present study on the spherical nano-HZSM-5 zeolite and its modification catalyst with excellent alkylation ability provides new insights into the production of mDEB.

关键词： Zeolite Modification Alkylation reaction m-diethylbenzene Catalyst Fixed-bed

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A projected Newton algorithm based on chemically allowed interval for chemical equilibrium computations

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Frontiers of Chemical Science and engineering 2024年第3期18卷 25-37页

作者： Hongbin Lu Shaohui Tao Xiaoyan Sun Li Xia Shuguang Xiang institute of process Systems engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao266042China

The chemical equilibrium equations utilized in reactive transport modeling are complex and nonlinear,and are typically solved using the Newton-Raphson *** this algorithm is known for its quadratic convergence near the solution,it is less effective far from the solution,especially for ill-conditioned *** such cases,the algorithm may fail to converge or require excessive *** address these limitations,a projected Newton method is introduced to incorporate the concept of *** method constrains the Newton step by utilizing a chemically allowed interval that generates feasible descending ***,we utilize the positive continuous fraction method as a preconditioning technique,providing reliable initial values for solving the *** numerical results are compared with those derived using the regular Newton-Raphson method,the Newton-Raphson method based on chemically allowed interval updating rules,and the bounded variable least squares method in six different test *** numerical results highlight the robustness and efficacy of the proposed algorithm.

关键词： chemical equilibrium reactive transport modeling numerical methods projected Newton method

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Alternative technology for the recovery of butyl acetate with low concentration:high capacity adsorbent and high efficiency adsorption

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Green Chemical engineering 2024年第2期5卷 236-244页

作者： Chi Ma Lihong Zhao Zhengxin Mao Hao Su Qingfen Liu CAS Key Laboratory of Green process and engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical engineering University of Chinese Academy of SciencesBeijing100049China

Industrial pharmaceutical wastewater usually contains butyl acetate(BA)with a concentration of 1 wt%-7 wt%,and the traditional method for BA recovery is distillation with high energy *** method is developed to recover BA with low concentration for the high efficiency and low energy *** polar polyacrylate resins with macroporous structure of 233.1 nm and average particle size of about 526.5μm are successfully synthesized by suspension polymerization and used for the BA adsorption and *** maximum adsorption capacity reaches 171.1 mg g^(-1)with relative standard deviation(RSD)value of 0.2%,which is more than twice the results in the *** BA desorption rate is 97.0%at 100℃with RSD value of 0.4%,and the resins are beneficial to the reuse in the adsorption-desorption *** adsorption thermodynamics and kinetics are investigated,and the BA adsorption is a spontaneous and endothermic process with the increase of disorder *** process is mainly contributed by physical absorption and agree well with Freundlich model and pseudo-first-order adsorption kinetic *** adsorption method avoids boiling a large amount of wastewater and hopefully provides a novel alternative technology for the BA recovery.

关键词： Butyl acetate recovery Resin adsorption Desorption Thermodynamics Kinetics

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Pressurized environments directly influence friction and wear of dry steel contacts—Investigations in a novel high fluid pressure tribometer

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Friction 2024年第7期12卷 1599-1617页

作者： Paul REICHLE Jakob BARZ Georg UMLAUF Günter E.M.TOVAR institute of Interfacial process engineering and Plasma Technology(IGVP) University of StuttgartStuttgart 70569Germany Fraunhofer institute for Interfacial engineering and Biotechnology(IGB) Stuttgart 70569Germany

To reduce the usage of classical lubricants in deep drawing,a new tribological system based on volatile lubricants was ***,a volatile medium is injected under high pressure into the interstice between drawing tool and sheet *** on temperature and pressure,the temporary lubricant may exist in its gaseous or liquid *** this study,a novel high fluid pressure tribometer was designed to investigate the friction and wear of dry steel contacts under comparable conditions like in dry deep ***,a new ball-on-disc tribometer was designed and integrated into a high-pressure *** specifically investigate the effects of different environments(technical air,liquid and gaseous carbon dioxide,nitrogen,argon)at atmospheric and high pressure(0.1 MPa,6 MPa)on tribology,the specimens and all components were operating *** the experiments,the friction was measured *** show that the highest friction occurs in air and the lowest in carbon dioxide *** to the experiments,the wear of the specimens was assessed along with changes in surface chemistry related to tribochemical ***,the tribology of the dry sliding contacts is correlated to changes of the surface *** differences as well as similarities regarding the different fluid environments are *** the results show,the differences between the media used are most pronounced at elevated ***,this work gives clear indications on the suitability of volatile lubricants in dry friction or rather gas lubrication,especially for dry deep drawing.

关键词： dry friction and dry wear gas lubrication carbon dioxide tribo-layer dry metal forming

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Mn-modified nitrogen-doped Pt-based electrocatalyst for efficient oxygen reduction in aluminum-air batteries

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Nano Research 2024年第8期17卷 7126-7135页

作者： Li Gao Yang Song Xuebing Xu Chang Li Chaoquan Hu State Key Laboratory of Mesoscience and engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Zhongke Nanjing institute of Green Manufacturing Industry Nanjing 211135China

In this study,a Mn-modified Pt-based catalyst loaded on nitrogen-doped Ketjen black(Mn-Pt/NKB)is prepared using a simple ethylene glycol reduction *** size of Pt nanoparticles(NPs)is effectively controlled by doping with Mn and *** the smallest average particle size of 1.7 nm,Mn-Pt/NKB demonstrates half-wave potentials of 0.890 and 0.688 V in the alkaline and neutral electrolytes,respectively,which are superior to those of commercial platinum on activated carbon(Pt/C).When applied as an air cathode in aluminum-air battery,it exhibits ultra-high power densities of 190(alkaline)and 26.2 mW·cm^(−2)(neutral).Moreover,the voltage remains stable after 5 h of *** practical application performance of the Mn-Pt/NKB catalyst in an aluminum-air battery is better than that of commercial Pt/***,the oxygen reduction reaction(ORR)mechanism on surfaces with different particle sizes is analyzed using density functional *** cracking is the major pathway on the surface of the small particles with lower energy consumption of 0.5 eV,while water molecule cleavage is the major pathway on the surface of the large particles with higher energy consumption of 0.97 *** lower energy consumption of the oxygen cracking pathway further confirms the ORR mechanism for higher activity on small-sized *** study provides a direction for the rational design of Pt-based catalysts for ORR and sheds light on the commercial development of aluminum-air batteries.

关键词： oxygen reduction reaction precious metal catalysts aluminum-air battery density functional theory(DFT)calculations reaction pathway

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Long‐life lithium batteries enabled by a pseudo‐oversaturated electrolyte

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Carbon Energy 2024年第4期6卷 115-127页

作者： Youchun Yu Simeng Wang Juyan Zhang Weiwei Qian Nana Zhang Guangjie Shao Haiyan Bian Yuwen Liu Lan Zhang Hebei Key Laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdaoChina Beijing Key Laboratory of Ionic Liquids Clean process CAS Key Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijingChina Haike Group Research institute of Innovation&Technology DongyingChina Langfang Green Industrial Technology Center LangfangChina

The specific energy of Li metal batteries(LMBs)can be improved by using high‐voltage cathode materials;however,achieving long‐term stable cycling performance in the corresponding system is particularly challenging for the liquid ***,a novel pseudo‐oversaturated electrolyte(POSE)is prepared by introducing 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropyl ether(TTE)to adjust the coordination structure between diglyme(G2)and lithium bis(trifluoromethanesulfonyl)imide(LiTFSI).Surprisingly,although TTE shows little solubility to LiTFSI,the molar ratio between LiTFSI and G2 in the POSE can be increased to 1:1,which is much higher than that of the saturation state,1:*** and experimental results prove that TTE promotes closer contact of the G2 molecular with Li^(+)in the ***,it also participates in the formation of electrolyte/electrode *** electrolyte shows outstanding compatibility with both the Li metal anode and typical high‐voltage ***||Li symmetric cells show a long life of more than 2000 h at 1 mA cm^(−2),1 mAh cm^(−2).In the meantime,Li||LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)cell with the POSE shows a high reversible capacity of 134.8 mAh g^(−1 )after 900 cycles at 4.5 V,1 C *** concept of POSE can provide new insight into the Li^(+)solvation structure and in the design of advanced electrolytes for LMBs.

关键词： high voltage lithium metal batteries pseudo‐oversaturated electrolyte solid electrolyte interphases(SEI) solvation structure

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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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Synthesis of NaY zeolite from a submolten depolymerized perlite:Alkalinity effect and crystallization kinetics

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Chinese Journal of Chemical engineering 2024年第6期70卷 130-138页

作者： Yanli Qu Peng Dong Li Yang Yuanyuan Yue Haoliang Wang Jingcai Cheng Chao Yang CAS Key Laboratory of Green process and engineering State Key Laboratory of Petroleum Molecular&Process EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical engineering University of Chinese Academy of SciencesBeijing 100190China Qingyuan Innovation Laboratory Quanzhou 362801China National engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350108China

NaY zeolites are synthesized using submolten salt depolymerized natural perlite mineral as the main silica and alumina sources in a 0.94 L stirred *** of alkalinity ranging from 0.38 to 0.55(n(Na2O)/n(SiO_(2)))on the relative crystallinity,textural properties and crystallization kinetics were *** results show that alkalinity exerts a nonmonotonic influence on the relative crystallinity and textural properties,which exhibit a maximum at the alkalinity of *** nucleation kinetics are studied by fitting the experimental data of relative crystallinity with the Gualtieri *** is shown that the nucleation rate constant increases with increasing alkalinity,while the duration period of nucleation decreases with increasing *** n(Na2O)/n(SiO_(2))ratios ranging from 0.38 to 0.55,the as-synthesized NaY zeolites exhibit narrower crystal size distributions with the increase in *** growth rates determined from the variations of average crystal size with time are 51.09,157.50,46.17 and 24.75 nm·h^(-1),*** is found that the larger average crystal sizes at the alkalinity of 0.38 and 0.43 are attributed to the dominant role of crystal growth over ***,the combined action of prominent crystal growth and the longer duration periods of nucleation at the alkalinity of 0.38 and 0.43 results in broader crystal size *** findings demonstrate that control of the properties of NaY zeolite and the crystallization kinetics can be achieved by conducting the crystallization process in an appropriate range of alkalinity of the reaction mixture.

关键词： NaY zeolite Submolten salt depolymerized perlite Alkalinity Crystallization kinetics

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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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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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