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

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

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Process intensification for the synthesis and purification of battery-grade Li_(2)CO_(3)with microfluidics

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Particuology 2024年第7期90卷 106-117页

作者： Haodu Li Jie Zhang Lin Dai Le Du Jiqin Zhu The State Key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Battery-grade lithium carbonate(Li_(2)CO_(3))with a purity of higher than 99.5 wt%is of great importance as a high value-added lithium ***,influences of different reaction systems and process control on product purity remain ***,a membrane dispersion microreactor was used to enhance the mass transfer of preparation and purification processes in homogeneous and heterogeneous *** systems of Na_(2)CO_(3)–LiCl,NH_(4)HCO_(3)–LiCl,and NH_(3)·H_(2)O−CO_(2)−LiCl,CO_(2)purification based on carbonation and decomposition were *** Li_(2)CO_(3)purity was increased by the improvement of mixing *** carbonation time was reduced by 62.5%and 58.3%for the NH_(3)·H_(2)O−CO_(2)and CO_(2)purification systems,*** the two ammonia-based systems,Li_(2)CO_(3)particles with a purity of 99.7–99.8 wt%were one-step prepared with a size of 3–5μm,which also met the requirement of the battery-grade *** purity was further increased to 99.9 wt%by CO_(2)purification and LiHCO_(3)*** investigation could provide a feasible alternative for the controllable preparation of battery-grade Li_(2)CO_(3)in one or multiple steps.

关键词： Microfluidics Battery grade Li_(2)CO_(3) Process intensification High purity

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Microfluidic-oriented synthesis of enriched iridium nanodots/carbon architecture for robust electrocatalytic nitrogen fixation

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Green Energy & Environment 2024年第3期9卷 544-555页

作者： Hengyuan Liu Xingjiang Wu Yuhao Geng Xin Li Jianhong Xu The State Key laboratory of chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless ***,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic ***,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon *** to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption *** a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH ***,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) *** microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.

关键词： Iridium nanodots Carbon Microfluidic technology Efficient synthesis Electrocatalytic nitrogen fixation

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Steady-state multiscale CFD simulation of a circulating fluidized bed riser

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Particuology 2024年第10期93卷 54-64页

作者： Zhaojie Ke Yujie Tian Fei Li Bona Lu Wei Wang State Key laboratory of Mesoscience and engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of chemical engineering University of Chinese Academy of SciencesBeijing100049China

Compared to transient simulation,steady-state simulation of circulating fluidized bed risers is more efficient,but is also harder to perform due to the complex scale-dependency of dense gas-solid *** this work,steady-state computational fluid dynamics(CFD)simulation of a riser is performed using the steady energy-minimization multi-scale(EMMS)*** is found that the steady state corresponds to an extremely large scale of length and time,thus the grid size required in steady-state simulation is larger than that in transient *** time-averaged two-fluid model(TFM)coupled with the steady-state EMMS/1M drag model enables a good prediction of the S-shaped,axial solids distribution and the choking transition,whereas the two-phase turbulence and solids stress models are important in predicting the radially core-annular distribution of *** far as we know,this is the first time that one can predict the choking transition in a steady-state CFD *** improvement may need an EMMS modeling of the time-averaged solid stresses.

关键词： Fluidization Drag force Steady state Simulation Mesoscale

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Insights into the role of oxygen-containing functional groups on carbon surface in water–electricity generation

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Nano Research 2024年第7期17卷 6645-6653页

作者： Wan Xue Zongbin Zhao Honghui Bi Bolun Zhang Xuzhen Wang Jieshan Qiu State Key laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China State Key laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024China State Key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage ***,an asymmetric generator was assembled based on functionalized carbon nanotubes films to investigate the relative contribution from various oxygen functional groups on carbon surface to the water-electrical *** and calculations demonstrate that the electricity mainly originates from the water molecule adsorption by carboxyl groups and dissociation of functional groups on carbon surface,which leads to the formation of electrical double layers at *** device allows the electricity generation with a variety of water sources,such as deionized water,tap water,as well as *** particular,the generator based on carboxyl carbon nanotubes can induce a voltage of over 200 mV spontaneously in natural seawater with the power density of about 0.11 mW·g^(−1).High voltages can be achieved easily through the series-connection strategy to power electronic products such as a liquid crystal *** work reveals the dominant role of carboxyl groups in carbon-based water–electricity conversion and is expected to offer inspiration for the preparation of carbon materials with high electrical performance.

关键词： electricity generation water adsorption dissociation carboxyl groups carbon nanotubes

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Enhancing alkyne semi-hydrogenation through engineering metal-support interactions of Pd on oxides

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Nano Research 2024年第5期17卷 3707-3713页

作者： Yuefeng Wu Xiaotong Lu Pengfei Cui Wenyu Jia Jun Zhou Yuan Wang Hussain Zahid Yuxin Wu Muhammad Umer Rafique Xiong Yin Baoshan Li Leyu Wang Guolei Xiang State Key laboratory of chemical Resource engineering Beijing University of Chemical TechnologyBeijing 100029China CAS Key laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China College of chemical engineering Beijing University of Chemical TechnologyBeijing 100029China

Supported Pd catalysts show superior activities for olefin productions from alkynes through semi-hydrogenation reactions,but over-hydrogenation into alkanes highly decreases olefin *** phenylacetylene semi-hydrogenation as a model reaction,here we explore the optimization approaches toward better Pd catalysts for alkyne semi-hydrogenation through investigating support effect and metal-support *** results show that the states of Pd with supports can be tuned by varying oxide reducibility,loading ratios,and *** our system,0.06 wt.%Pd on rutile-TiO_(2) nanorods shows the highest activity owing to the synergistic effects of single-atoms and *** reducibility can change the filling degrees of Pd 4d orbitals through varying interfacial bonding strengths,which further affect catalytic activity and selectivity.

关键词： alkyne semi-hydrogenation support effect metal-support interaction Pd catalyst single-atom catalyst

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Controllable Ring-opening Polymerization ofδ-Valerolactone Catalyzed by Quinolinyl-Urea/MTBD Systems

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Chinese Journal of Polymer Science 2024年第8期42卷 1103-1110页

作者： Xin-Yu Liu Liang Zhu Su-Yun Jie Bo-Geng Li State Key laboratory of chemical engineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China

Due to their excellent biocompatibility and biodegradability,aliphatic polyesters are widely used in the biomedical,packaging and agricultural fields,which are usually accessed by the ring-opening polymerization(ROP)of lactones and the catalysts particularly play an important *** a series of quinolinyl-urea catalysts have been synthesized via the reaction between isocyanate and aminoquinoline with an amino group at different substitution positions and *** combination with 7-methyl-1,5,7-triazabicyclo[4,4,0]dec-5-ene(MTBD)as a cocatalyst and benzyl alcohol(BnOH)as an initiator,1-(3,5-bis(trifluoromethyl)phenyl)-3-(quinolin-3-yl)urea(3-QU)was observed to be most active for the ROP ofδ-valerolactone(δ-VL).The polymerization conditions were optimized by varying the type of organic base,catalyst concentration and reaction *** changing the ratio of[M]_0/[I],linear polyvalerolactones(PVLs)with different molecular weights and narrow molecular weight distribution were *** kinetic and chain extension experiments were carried out to prove the"living"/controllable *** the NMR experiments were used to support the proposal of possible mechanism.

关键词： Quinolinyl-urea Ring-opening polymerization PVL

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Progresses and Prospects of Asymmetrically Coordinated Single Atom Catalysts for Lithium-Sulfur Batteries

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Energy & Environmental Materials 2024年第4期7卷 48-63页

作者： Rong Zhou Shaonan Gu Meng Guo Shuzheng Xu Guowei Zhou Key laboratory of Fine chemicals in Universities of Shandong Jinan Engineering Laboratory for Multi-scale Functional Materials School of Chemistry and Chemical Engineering Qilu University of Technology(Shandong Academy of Sciences)

Lithium-sulfur batteries (LSBs) are widely regarded as promising next-generation batteries due to their high theoretical specific capacity and low material ***,the practical applications of LSBs are limited by the shuttle effect of lithium polysulfides (LiPSs),electronic insulation of charge and discharge products,and slow LiPSs conversion reaction kinetics.

关键词： asymmetrical coordination conversion catalysis Li-S batteries shuttle effect single atom catalysts

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3D coarse-grained DPM simulation of the MIP reaction-regeneration loop

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Particuology 2024年第6期89卷 57-66页

作者： Yanhao Ye Shuai Zhang Ji Xu Wei Ge State Key laboratory of Mesoscience and engineering(formerly State Key laboratory of Multiphase Complex Systems) Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of chemical engineering University of Chinese Academy of SciencesBeijing100049China

The reactor-regenerator loop is the core facility of the maximizing iso-paraffin(MIP)*** the discrete particle method(DPM)simulation can provide detailed information at the particle scale,it has been unable to simulate such a complex loop system due to limitations of coarse-grained(CG)models,computing software,and *** this study,a newly proposed soft-shell CG-DPM model with a CG ratio of up to 800 is used to simulate a 3.5 Mt/a industrial-scale MIP reactor-regenerator *** solid fraction distribution obtained is found to agree well with in-situ *** properties including the distribution of solid fraction,gas and solid velocity,standard derivation of solid fraction with time,temporal distribution of the flow field,and particle residence time distribution are measured in the simulation,which are meaningful to better design and operate such systems in the future.

关键词： Discrete particle method Coarse-grain Maximizing iso-paraffins Full-loop Reaction-regeneration system

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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

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