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Poisoning effect of polyvinyl chloride on the catalytic pyrolysis of mixed plastics over zeolites

Science China Chemistry 2024年第7期67卷 2265-2273页

作者： Jiangchun Yuan Wenjie Wang Weixiao Sun Zhirong Yang yueqiang cao Wenyao Chen Xiaohu Ge Gang Qian Xiang Feng Xuezhi Duan Xinggui Zhou Kevin M.Van Geem Jing Zhang State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Laboratory for Chemical Technology(LCT) Department of MaterialsTextiles and Chemical EngineeringFaculty of Engineering&ArchitectureGhent UniversityZwijnaarde B-9052Belgium State Key Lab of Heavy Oil Processing China University of PetroleumQingdao 266580China

Nowadays,the chemical recycling is applied for only 1%of total waste plastics,largely due to contaminants in plastic waste and difficulty in product control.As the major contaminant,polyvinyl chloride(PVC)often forms corrosive hydrogen chloride(HCl)during the chemical recycling,which may cause severe catalyst deactivation and equipment damage.However,the investigation on catalytic pyrolysis(the major route for plastics chemical recycling)of the PVC containing mixed plastics has been rarely reported.Here,catalytic co-pyrolysis of PVC and polyethylene(PE)was studied over an aromatization catalyst,Pt/ZSM-5,since the basic building block aromatics are desired products from plastics chemical recycling.The poisoning effect of PVC vapor on the catalyst stability was explored by collective efforts of thorough product analysis and catalyst characterization.It was found that the HCl evolving from PVC has an autocatalytic effect that promotes the scission of dehydrochlorinated PVC,resulting in the high yield of benzene and acetylene from PVC.On the other hand,the presence of PVC suppressed the aromatics formation from PE,largely due to the poisoning effect of PVC-derived HCl on the Pt/ZSM-5.The deactivation is irreversible as evidenced by the decreased zeolite crystallinity and the loss of strong acid sites that are key to the aromatization,possibly due to the removal of framework Al upon the interaction with HCl.The modification with octadecylphosphonic acid only slightly alleviated the PVC poisoning effect.The insights on the PVC poisoning of zeolite catalysts provided in this work may guide the process design of chemical recycling of PVC containing waste plastics.

关键词： polyvinyl chloride polyethylene zeolite aromatics deactivation

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Thermosphere joint observations by TM-1 constellations and Swarm-B during the April 2023 geomagnetic storm

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Earth and Planetary Physics 2024年第2期8卷 307-316页

作者： YongPing Li yueqiang Sun XianGuo Zhang JiangZhao Ai XiaoLiang Zheng Jia Li YuJie Wang BiBo Guo Feng Yan ShiLong Wei XinChun Tang YuanYuan cao National Space Science Center Chinese Academy of SciencesBeijing 100190China Beijing Key Laboratory of Space Environment Exploration Beijing 100190China Key Laboratory of Science and Technology on Space Environment Situational Awareness Chinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Shenzhen Aerospace Dongfanghong Satellite LtdShenzhen 518057China

The response of thermosphere density to geomagnetic storms is a complicated physical process.Multi-satellite joint observations at the same altitude but different local times(LTs)are important for understanding this process;however,until now such studies have hardly been done.In this report,we analyze in detail the thermosphere mass density response at 510 km during the April 23−24,2023 geomagnetic storm using data derived from the TM-1(TianMu-1)satellite constellation and Swarm-B satellites.The observations show that there were significant LT differences in the hemispheric asymmetry of the thermosphere mass density during the geomagnetic storm.Densities observed by satellite TM02 at nearly 11.3 and 23.3 LTs were larger in the northern hemisphere than in the southern.The TM04 dayside density observations appear to be almost symmetrical with respect to the equator,though southern hemisphere densities on the nightside were higher.Swarm-B data exhibit near-symmetry between the hemispheres.In addition,the mass density ratio results show that TM04 nightside observations,TM02 data,and Swarm-B data all clearly show stronger effects in the southern hemisphere,except for TM04 on the dayside,which suggest hemispheric near-symmetry.The South-North density enhancement differences in TM02 and TM04 on dayside can reach 130%,and Swarm-B data even achieve 180%difference.From the observations of all three satellites,large-scale traveling atmospheric disturbances(TADs)first appear at high latitudes and propagate to low latitudes,thereby disturbing the atmosphere above the equator and even into the opposite hemisphere.NRLMSISE00 model simulations were also performed on this geomagnetic storm.TADs are absent in the NRLMSISE00 simulations.The satellite data suggest that NRLMSISE00 significantly underestimates the magnitude of the density response of the thermosphere during geomagnetic storms,especially at high latitudes in both hemispheres.Therefore,use of the density simulation of NRLMSISE00 may lead to large errors in satellite dra

关键词： TM-1 constellation Swarm-B joint observations geomagnetic storm Local Times

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Mechanistic aspects of facet-dependent CH_(4)/C_(2+)selectivity over aχ-Fe_(5)C_(2)Fischer-Tropsch catalyst

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Green Energy & Environment 2022年第3期7卷 449-456页

作者： Thanh Hai Pham Junbo cao Nan Song yueqiang cao Bingxu Chen Gang Qian Xinggui Zhou De Chen Xuezhi Duan State Key Laboratory of Chemical Engineering East China University of Science and Technology130 Meilong RoadShanghai200237China Vietnam Institute for Tropical Technology and Environmental Protection 57A Truong Quoc DungHo Chi MinhViet Nam Department of Chemical Engineering Norwegian University of Science and TechnologyN-7491TrondheimNorway

Structure-performance relationship is a complex issue in iron-catalyzed Fischer-Tropsch synthesis,and it is not easy to elucidate it by experimental investigations.First-principle calculation is a powerful method for explaining experimental results and guiding catalyst design.In this study,we investigated the reaction mechanisms of CH_(4)formation and C-C coupling on fourχ-Fe_(5)C_(2)surfaces and established the kinetic equations to compare the rates of CH_(4)formation and C_(1)+C_(1)coupling reactions and determine the CH_(4)/C_(2+)selectivity.The results show that the geometry of theχ-Fe_(5)C_(2)surfaces has little effect on the formation rate of CH_(4);however,the C_(1)+C_(1)coupling reactions are significantly affected by the surface geometry.The C_(1)+C_(1)coupling reaction rates on the terraced-like(510)and(021)surfaces are much higher than those on the stepped-like(001)and(100)surfaces.Based on these results,we established a Brùnsted-Evans-Polanyi(BEP)relationship between the effective barrier difference for CH_(4)formation and C_(1)+C_(1)coupling(ΔE_(eff))and the adsorption energy of C+4H(ΔE_(C+4H))onχ-Fe_(5)C_(2)surfaces.ΔE_(C+4H)can be used as a descriptor for CH_(4)/C_(2+)selectivity on different surfaces ofχ-Fe_(5)C_(2).

关键词： selectivity catalyst coupling

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Enhanced recycling performance of bimetallic Ir-Re/SiO_(2) catalyst by amberlyst-15 for glycerol hydrogenolysis

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Chinese Journal of Chemical Engineering 2022年第5期35卷 171-181页

作者： Xin Ren Li Leng yueqiang cao Jing Zhang Xuezhi Duan Xueqing Gong Jinghong Zhou Xinggui Zhou State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Key Laboratory for Advanced Materials Centre for Computational Chemistry and Research Institute of Industrial CatalysisEast China University of Science and TechnologyShanghai 200237China

Recycling performance of heterogeneous catalysts is of crucial importance especially for a batch reaction system.In this work,we demonstrate a strategy for enhancing recycling performance of Ir-Re/SiO_(2) catalyst synergized with amberlyst-15 in glycerol hydrogenolysis to produce 1,3-propanediol.Comprehensive characterization results reveal that the Re sites in the Ir-Re/SiO_(2) catalyst undergo irreversible segregation and oxidation.These hinder the formation of active ReAOH species and thus contribute to a complete and irreversible deactivation.However,the introduction of amberlyst-15 into the reactant mixture can restrain the oxidation process of Re sites and favor the formation of ReAOH species,and thus significantly enhance the catalytic recycling performance.The results demonstrated here could guide the development of excellent bimetallic catalysts with the desirable recycling performances for the reaction.

关键词： Glycerol hydrogenolysis Ir-Re/SiO_(2)catalyst Deactivation mechanism Recycling performance Amberlyst-15 promoter

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Understanding the effects of electrode meso-macropore structure and solvent polarity on electric double layer capacitors based on a continuum model

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Chinese Journal of Chemical Engineering 2022年第10期50卷 423-434页

作者： Haotian Lu Jinghong Zhou yueqiang cao Tongxin Shang Guanghua Ye Quan-Hong Yang Xinggui Zhou State-Key Laboratory of Chemical Engineering East China University of Science of TechnologyShanghai 200237China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China Nanoyang Group State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China

The structures of electrode meso-macropore and the solvent polarity are the crucial factors dominating the performance of the electric double layer capacitors(EDLCs),but their impacts are usually tangled and difficult to decouple and quantitate.Here the effects of electrode meso-macropore structure and solvent polarity on the specific capacitance of an EDLC are quantitatively investigated using a steady-state continuum model.The simulation results indicate the specific capacitances are significantly affected by the meso-macropore surface structure.The specific capacitances significantly decrease for both convex surface structures but obviously increase for both concave surface structures,with the increase of curvature radius from 1 to 20 nm.As for solvents,the polar solvent with high saturated dielectric permittivity improves the capacitance performance.Moreover,the electrode meso-macropore structure is of more concern compared with solvent polarity when aiming at enhancing the specific capacitance.These results provide fundamentals for the rational design of porous electrodes and polar electrolytes for EDLCs.

关键词： Electric doublelayercapacitors Numerical simulation Meso-macropore Electrolytes Saturated dielectricpermittivity

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Mechanistic insights into the active intermediates of 2,6-diaminopyridine dinitration

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Chinese Journal of Chemical Engineering 2023年第4期56卷 160-168页

作者： Junao Zhu Zhirong Yang Yuanhan Chen Mingming Chen Zhen Liu yueqiang cao Jing Zhang Gang Qian Xinggui Zhou Xuezhi Duan State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Mechanistic understanding of the active intermediates of 2,6-diaminopyridine(DAP) dinitration in the concentrated nitric-sulfuric acid system is of crucial importance for the selectivity control of target product, i.e., 2,6-diamino-3,5-dinitropyridine(DADNP). The active intermediates determining the product selectivity are theoretically studied. The HSO_(4)^(-)-NO_(2)^(+) complex is proposed as the dominant active nitrating intermediate for the first time, which shows low energy barrier(i.e., 10.19 kcal·mol^(-1),1 kcal = 4.186 k J) for direct dinitration of DAP to DADNP. The formed water during the reaction results in not only the formation of less active SO_(4)^(2-)-NO_(2)^(+) complex, but also the occurance of DAP sulfonation(DAP-SO_(3)H intermediate)to facilitate the formation of mononitration byproduct. Meanwhile, the accompanied thermal effects cause the generation of undesirable pyridine-NHNO_(2) intermediate, which is difficult to be rearranged to yield DADNP, inhibiting the reaction and thus giving low DAP conversion. The insights reported here elucidates the importance of thermal effects elimination and water content control, confirmed experimentally in the batch-and micro-reaction systems.

关键词： 2,6-Diaminopyridine Nitration mechanism Active intermediates Thermal effects Negative water effects

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Dysfunction of synaptic endocytic trafficking in Parkinson's disease

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Neural Regeneration Research 2024年第12期19卷 2649-2660页

作者： Xin Yi Ng Mian cao Programme in Neuroscience and Behavioural Disorders Duke-NUS Medical SchoolSingaporeSingapore Department of Physiology National University of SingaporeSingaporeSingapore

Parkinson's disease is characterized by the selective degeneration of dopamine neurons in the nigrostriatal pathway and dopamine deficiency in the striatum.The precise reasons behind the specific degeneration of these dopamine neurons remain largely elusive.Genetic investigations have identified over 20 causative PARK genes and 90 genomic risk loci associated with both familial and sporadic Parkinson's disease.Notably,several of these genes are linked to the synaptic vesicle recycling process,particularly the clathrinmediated endocytosis pathway.This suggests that impaired synaptic vesicle recycling might represent an early feature of Parkinson's disease,followed by axonal degeneration and the eventual loss of dopamine cell bodies in the midbrain via a"dying back"mechanism.Recently,several new animal and cellular models with Parkinson's disease-linked mutations affecting the endocytic pathway have been created and extensively characterized.These models faithfully recapitulate certain Parkinson's disease-like features at the animal,circuit,and cellular levels,and exhibit defects in synaptic membrane trafficking,further supporting the findings from human genetics and clinical studies.In this review,we will first summarize the cellular and molecular findings from the models of two Parkinson's disease-linked clathrin uncoating proteins:auxilin(DNAJC6/PARK19)and synaptojanin 1(SYNJ1/PARK20).The mouse models carrying these two PARK gene mutations phenocopy each other with specific dopamine terminal pathology and display a potent synergistic effect.Subsequently,we will delve into the involvement of several clathrin-mediated endocytosis-related proteins(GAK,endophilin A1,SAC2/INPP5 F,synaptotagmin-11),identified as Parkinson's disease risk factors through genome-wide association studies,in Parkinson's disease pathogenesis.We will also explore the direct or indirect roles of some common Parkinson's disease-linked proteins(alpha-synuclein(PARK1/4),Parkin(PARK2),and LRRK2(PARK8))in synaptic endocytic trafficking.Additionall

关键词： autophagy auxilin/PARK19 clathrin-mediated endocytosis dopamine neurons neurodegeneration nigrostriatal pathway Parkinson's disease synaptic vesicle recycling synaptojanin1/PARK20

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Dynamic Setting Method of Assessment Indicators for Power Curves of Renewable Energy Sources Considering Scarcity of Reserve Resources

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Journal of Modern Power Systems and Clean Energy 2024年第1期12卷 101-114页

作者： Minghao cao Jilai Yu the Department of Electrical Engineering Harbin Institute of TechnologyHarbinChina

With the increasing proportion of renewable energy sources(RESs)in power grid,the reserve resource(RR)scarcity for correcting power deviation of RESs has become a potential issue.Consequently,the power curve of RES needs to be more rigorously assessed.The RR scarcity varies during different time periods,so the values of assessment indicators should be dynamically adjusted.The assessment indicators in this paper include two aspects,i.e.,deviation exemption ratio and penalty price.Firstly,this paper proposes a method for dynamically calculating the supply capacity and RR cost,primarily taking into account the operating status of thermal units,forecast information of RES,and load curve.Secondly,after clarifying the logical relationship between the degree of RR scarcity and the values of assessment indicators,this paper establishes a mapping function between them.Based on this mapping function,a dynamic setting method for assessment indicators is proposed.In the future,RES will generally be equipped with battery energy storage systems(BESSs).Reasonably utilizing BESSs to reduce the power deviation of RESs can increase the expected income of RESs.Therefore,this paper proposes a power curve optimization strategy for RESs considering self-owned BESSs.The case study demonstrates that the dynamic setting method of assessment indicators can increase the revenue of RESs while ensuring that the penalty fees paid by RESs to the grid are sufficient to cover the RR costs.Additionally,the power curve optimization strategy can help RESs further increase income and fully utilize BESSs to reduce power deviation.

关键词： Renewable energy battery energy storage system(BESS) power curve assessment reserve service parameter setting

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Zeros of Complete Symmetric Polynomials over Finite Fields

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Journal of Systems Science & Complexity 2024年第4期37卷 1772-1788页

作者： cao Wei School of Mathematics and Statistics Minnan Normal University

Wan and Zhang(2021) obtained a nontrivial lower bound for the number of zeros of complete symmetric polynomials over finite fields, and proposed a problem whether their bound can be improved. In this paper, the author improves Wan-Zhang's bound from three aspects. The proposed results are based on the estimates related to the number of certain permutations and the value sets of non-permutation polynomials associated to the complete symmetric polynomial. And the author believes that there are still possibilities to improve the bounds and hence Wan-Zhang's bound.

关键词： Complete symmetric polynomial finite field permutation polynomial value set

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Bioinspired Closed-loop CPG-based Control of a Robotic Manta for Autonomous Swimming

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Journal of Bionic Engineering 2024年第1期21卷 177-191页

作者： Yiwei Hao Yonghui cao Yingzhuo cao Xiong Mo Qiaogao Huang Lei Gong Guang Pan Yong cao School of Marine Science and Technology Northwestern Polytechnical UniversityXi'an 710072China Unmanned Vehicle Innovation Center Ningbo Institute of NPUNingbo 315103China Key Laboratory of Unmanned Underwater Vehicle Technology of Ministry of Industry and Information Technology Xi'an 710072China

Fish in nature exhibit a variety of swimming modes such as forward swimming,backward swimming,turning,pitching,etc.,enabling them to swim in complex scenes such as coral reefs.It is still difficult for a robotic fish to swim autonomously in a confined area as a real fish.Here,we develop an untethered robotic manta as an experimental platform,which consists of two flexible pectoral fins and a tail fin,with three infrared sensors installed on the front,left,and right sides of the head to sense the surrounding obstacles.To generate multiple swimming modes of the robotic manta and online switching of different modes,we design a closed-loop Central Pattern Generator(CPG)controller based on distance information and use a combination of phase difference and amplitude of the CPG model to achieve stable and rapid adjustment of yaw angle.To verify the autonomous swimming ability of the robotic manta in complex scenes,we design an experimental scenario with a concave obstacle.The experimental results show that the robotic manta can achieve forward swimming,backward swimming,in situ turning within the concave obstacle,and finally exit from the area safely while relying on the perception of external obstacles,which can provide insight into the autonomous exploration of complex scenes by the biomimetic robotic fish.Finally,the swimming ability of the robotic manta is verified by field tests.

关键词： Biomimetic robotic manta Central Pattern Generator Closed-loop control Backward swimming

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