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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

Role of methoxy and C_(α)-based substituents in electrochemical oxidation mechanisms and bond cleavage selectivity of β-O-4 lignin model compounds

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Green Energy & Environment 2024年第1期9卷 114-125页

作者： Yang Zhou Qiang Zeng Hongyan He Kejia Wu Fuqiao Liu Xuehui Li School of Chemistry and chemical Engineering The Guangdong Provincial Key Laboratory of Green Chemical Product TechnologyState Key Laboratory of Pulp and Paper EngineeringSouth China University of TechnologyGuangzhouGuangdong510640China cas Key Laboratory of Green process and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China

In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para-methoxy(on the aryl ring closing to Cα) and Cα-OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the Cα-Cβbond cleavage induced by electrochemical oxidations.

关键词： Lignin model compounds β-O-4 dimers Electrochemical oxidation Oxidation mechanisms Substituent effect

Insight into the role of ethylene glycol on thermodynamics and nucleation kinetics of dimethyl terephthalate in mixed solvent system

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Particuology 2024年第2期85卷 1-12页

作者： Yujin Zhang Chunyan Shi Jing Tang Li Liu Dongxia Yan Qing Zhou Xingmei Lu Songyan Jia College of chemical Engineering Shenyang University of Chemical TechnologyShenyang110142China Bejing Key Laboratoryoflonic Liquids Clean process CAS Key LaboratoryofGreen Process and EngineeringState Key Laboratoryof Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemistry and chemical Engineering Qingdao UniversityQingdao266071China Henan institute of Advanced Technology Zhengzhou UniversityZhengzhou450001China School of chemical Engineering University of Chinese Academy of SciencesBeijing100049China

Dissolution and nucleation are two essential processes for industrial *** paper in-vestigates the effect of ethylene glycol addition on the crystallization behavior of dimethyl terephthalate(DMT)in *** DMT solubility in mixed solvent system(methanol-ethylene glycol)was deter-mined by isothermal satiation approach,and the solubility was associated using seven *** model fitting results were consistent with the experimental *** on the results,the metastable zone width(MSZW)of DMT was detected by the polythermal approach;the modified Sangwal's theory was used to investigate the nucleation behavior,which can provide a new way of thought for better analysis of the crystallization *** results demonstrated that MSZW was associated with various elements,such as cooling rate,saturation temperature and mass fraction of ethylene *** addition of ethylene glycol slowed down the nucleation rate as shown by the broadening of *** derive the solid-liquid interface energy,the nucleation driving force,the critical nucleation size and the critical Gibbs free energy according to the classical nucleation *** is demonstrated that the nucleation driving force and the solid-liquid interface energy are dependent and jointly influence the MSZW.

关键词： Dissolution Nucleation Solubility Apparent thermodynamic parameters Metastable zone width Solid-liquid interface energy

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(Na_(2)O)/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(Na_(2)O)/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

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

Current collectors' effects on the electrochemical performance of LiNi0.6Co0.2Mn0.2O2 suspension electrodes for lithium slurry battery

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Green Energy & Environment 2024年第8期9卷 1306-1313页

作者： Linshan Peng Yufei Ren Zhaoqiang Yin Zhitong Wang Xiangkun Wu Lan Zhang cas Key Laboratory of Green process and Engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of Sciences School of chemical Engineering University of Chinese Academy of Sciences Hefei University institute of Mechanics Chinese Academy of Sciences Langfang Green Industrial Technology Center

Take after the advantages of lithium-ion battery（LIB） and redox flow battery（RFB）, semi-solid flow battery（SSFB） is a promising electrochemical energy storage device in renewable energy utilization. The flowable slurry electrode realizes decouple of energy and power density,while it also brings about new challenge to SSFBs, electron transport between active material and the out circuit. In this consideration, three types of current collectors（CCs） are applied to study the resistance and electrochemical performances of slurry cathodes within pouch cells for the first time. It proves that the electronic resistance（Re） between slurry electrode and the CC plays a decisive role in SSFB operation, and it is so large when Al foil is adopted that the cell cannot even work. Contact angle between Ketjen black（KB） slurry without active material（AM） and the CC is a preliminarily sign for the Re, the smaller the angle, the lower the resistance, and the better electrochemical performance of the cell.

关键词： Semi-solid flow battery Slurry electrode Current collector Electronic resistance Carbon coated Al

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

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

Zincophilic Ti_(3)C_(2)Cl_(2)MXene and anti-corrosive Cu NPs for synergistically regulated deposition of dendrite-free Zn metal anode

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Journal of Materials Science & Technology 2024年第2期169卷 137-147页

作者： Yunfei Shen Yi Liu Kaisheng Sun Tiantian Gu Gang Wang Yue Yang Jianxiang Pang Yang Zheng Xiaodong Yang Long Chen Key Laboratory for Green process of chemical Engineering of Xinjiang Bingtuan School of Chemistry and Chemical EngineeringShihezi UniversityShihezi 832003China institute for Chemistry Chemnitz University of TechnologyChemnitz 09107Germany cas Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Key Laboratory of Electronic Information Materials and DevicesCenter of Materials Science and Optoelectronics EngineeringXinjiang Technical Institute of Physics and Chemistry of CASUrumqi 830011China Key Laboratory of Ecophysics and Department of Physics College of ScienceShihezi UniversityShihezi 832003China

Dendrites growth,chemical corrosion,and hydrogen evolution reaction(HER)on zinc anodes are the main barriers for the development of aqueous zinc-ion batteries(AZIBs).Constructing interfacial protec-tive layer is an effective way to alleviate the side reactions on the ***,Cu/Ti_(3)C_(2)Cl_(2)MXene(CMX)with high zincophilic and hydrophobic property is prepared by the lewis molten salts etching method,and the CMX interface protection layer is constructed by a simple spin *** CMX coat-ing layer can provide abundant nucleation sites and uniformize the charge distribution through the zin-cophilic Ti_(3)C_(2)Cl_(2)MXene matrix,leading to homogenous Zn *** addition,the hydrophobic coat-ing contained anti-corrosive Cu nanoparticles can prevent the Zn anode from the electrolyte,beneficial for suppressing the chemical corrosion and ***,the stable and reversible Zn plating/stripping is achieved for the Zn anode coated by the CMX,which exhibits the lifespan of over 1400 h at 0.5 mA cm^(−2),and even can steadily run for 700 h with 65 mV at 10 mA cm^(−2).Furthermore,CMX@Zn shows a high coulombic efficiency of over 100%for 3800 cycles,which indicates that the CMX@Zn electrode has excellent stability and reversibility of Zn stripping/*** full batteries assembled with ZnCoMnO/C(ZCM)cathodes also exhibits higher capacity(450.6 mAh g^(−1)at 0.1 A g^(−1))and cycle stability(capacity retention of 70%after 1500 cycles).This work enhanced the lifespan of AZIBs and broaden the research of multifunctional coating layer to other secondary batteries based on metal anodes.

关键词： Zinc anode Spin coating Zincophilic MXene Anti-corrosive Cu NPs Multifunctional coating

Multistep Desolvation as a Fundamental Principle Governing Peptide Self-Assembly Through Liquid-Liquid Phase Separation

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CCS Chemistry 2024年第1期6卷 255-265页

作者： Chengqian Yuan Ruirui Xing Jie Cui Wei Fan Junbai Li Xuehai Yan State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190 School of chemical Engineering University of Chinese Academy of SciencesBeijing 100049 Analysis and Test Center Institute of ChemistryChinese Academy of SciencesBeijing 100190 Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Center for Mesoscience Institute of Process EngineeringChinese Academy of SciencesBeijing 100190

Biomolecular self-assembly based on peptides and proteins is a general phenomenon encountered in natural and synthetic ***–liquid phase separation(LLPS)is intimately involved in biomolecular self-assembly,yet the key factors at a molecular scale activating or modulating such a process remain largely ***,we discovered in our experiments that multistep desolvation is fundamental to the formation and evolution of peptide-rich droplets:The first step was partial desolvation of peptides to form peptide clusters,and the second step was selective desolvation of hydrophobic groups within clusters to trigger LLPS and the formation of peptiderich droplets,followed by complete desolvation of droplets,initiating the nucleation of peptide *** of the degree of desolvation at different stages was an effective strategy to control the self-assembly pathways and *** study sheds light on the molecular origin of LLPS-mediated self-assembly distinct from classical one-step self-assembly and paves the way for the precise control of supramolecular self-assembly.

关键词： peptide liquid-liquid phase separation multistep desolvation nanostructures self-assembly