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“Crystallinity Wave”-Driven Synthesis of Hollow Multi-Shell Covalent Organic Frameworks for Enhanced Supercapacitors

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Angewandte Chemie 2025年

作者： Yuanbo Sun Bin Zhao Ji Han Guangrui Chen Ruigang Sun Chengyue Yang Zhaohui Shi Bohan Liu Wenbin Tu Shanshan Li Benzheng Li Guiyuan Zhong Song Lin Zhang Wei Feng Dan Wang Buyuan Guan State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Qianjin Street 2699 Changchun 130012 P.R. China Key Lab of Groundwater Resources and Environment Ministry of Education Jilin University Changchun 130021 P.R. China International Center of Future Science Jilin University Qianjin Street 2699 Changchun 130012 P.R. China Center for Molecular Science and Engineering College of Science Northeastern University Shenyang 110819 P.R. China State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China Institute of Materials Research and Engineering (IMRE) Agency for Science Technology and Research (A*STAR) 2 Fusionopolis Way Singapore 138634 Singapore State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P.R. China University of Chinese Academy of Sciences Beijing 100049 P.R. China College of Chemistry and Environmental Engineering Shenzhen University Shenzhen 518060 P.R. China

Hollow multi-shell covalent organic frameworks (COFs) with abundant modular interfaces, high loading capacity, and various microenvironments are expected to hold great potential for chemical separation, heterogeneous catalysis, and energy storage/conversion. However, the synthetic methodology of COF hollow multi-shell nanoarchitectures has not been established. Herein, we demonstrate an ingenious “crystallinity wave”-induced regional difference ripening strategy to synthesize a series of hollow multi-shell COF particles with controllable shell numbers and shell thickness. The methodology relies on the isolation effect of the local crystalline COF thin layer inserted between the two layers of amorphous covalent organic polymer by the short-time Ostwald ripening, so that different regions of the particles exhibit distinct reaction stages before reaching chemical equilibrium in the subsequent dynamic imine exchange reaction, and then regions that tend to hydrolyze dissolve during the complete ripening process to form a hollow multi-shell structure. Remarkably, this strategy can be extended to prepare other hollow multi-shell COFs by altering monomers. As a proof-of-concept application, the obtained hollow multi-shell COFs are used as the electrode materials for supercapacitor. Benefiting from the short mass transfer path of the hollow multi-shell structure, ordered channels of the COF, and their high surface area, the as-prepared particles exhibit remarkably enhanced specific capacitance.

关键词： Covalent organic frameworks Hollow multi-shell structure Supercapacitor

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Carbonyl-Bridged Trifluoromethyl Pyridine Derivatives for Pest Control and Mechanistic Investigations

SSRN

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SSRN 2025年

作者： Sheng, Zhubo Deng, Jie Yuan, Qinglong Fu, Wen Xu, Zhiping Li, Xiaoyan Li, Zhong Shao, Xusheng Shanghai200237 China State Key Laboratory of Bioreactor Engineering East China University of Science and Technology Shanghai200237 China Shanghai Frontier Science Research Base of Optogenetic Techniques for Cell Metabolism School of Pharmacy East China University of Science and Technology Shanghai200237 China Engineering Research Center of Pharmaceutical Process Chemistry Ministry of Education School of Pharmacy East China University of Science and Technology Shanghai200237 China National Key Laboratory of Green Pesticide Guizhou University Guizhou Guiyang550025 China College of Humanities and Economic Management Yantai Institute of China Agricultural University Shandong Yantai264670 China

Trifluoromethyl pyridine (TFMP) motif is commonly discovered in structures of active pharmaceuticals. Flonicamid, characterized by the TFMP moiety, is well known as a prodrug in the knockdown of pests. The azobenzene-modified TFMP derivatives have been previously reported with excellent insecticidal activities. Herein, twenty-one TFMP derivatives were designed by the introduction of carbonyl-bridged aryl groups and synthesized via a one-step synthesis using Flonicamid as the starting material. The structure-activity relationships of these compounds were well analyzed and discussed. A molecular docking study and calcium ion concentration analysis indicated that compound FC13 could have interacted with the nicotinamidase enzyme, which further influenced the Ca2+ influx. © 2025, The Authors. All rights reserved.

关键词： Cyclization

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Degradable Ionic liquids as efficient catalysts for the glycolysis of PET

Degradable Ionic liquids as efficient catalysts for the glyc...

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中国化学会第七届全国热分析动力学与热动力学学术会议

作者： Yachan Liu Xingmei Lu Qing Zhou 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 Sciences Sino Danish College University of Chinese Academy of Sciences

As a thermoplastic polymer resin with excellent mechanical property and chemical stability,poly ethylene terephthalate（PET） is widely used in high-strength fibers,packaging,film and plastic bottles. The increasing comsumption of PET has caused serious environmental damage,which made PET recycling *** common recycling method is the glycolysis of PET into BHET monomer with effective catalysts.[3] In this work,a series of degradable ionic liquid catalysts were developed,which made the glycolysis process greener and environmentally *** conditions of temperature,time and catalyst dosage were *** the optimization condition,the conversion of PET and yield of BHET were 100% and 85%,***,this catalytic system is promising in industrial application of recycling of PET.

关键词： Polyethylene terephthalate glycolysis ionic liquid

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Background-free latent fingerprint imaging based on nanocrystals with long-lived luminescence and pH-guided recognition

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Nano Research 2018年第12期11卷 6167-6176页

作者： Zhiheng Li Qian Wang Yingqian Wang Qinqin Ma Jie Wang Zhihao Li Yingxue Li Xiaobo Lv Wei Wei Lang Chen Quan Yuan Key Laboratory of Analytical Chemistry for Biology and Medicine (Ministry of Education) College of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy ofSciencesBeijing 10090China School of Basic Medical Sciences Wuhan UniversityWuhan 430072China

Latent fingerprints (LFPs) are highly specific to individuals, and LFP imaging has played an important role in areas such as forensic investigation and law enforcement. Presently, LFP imaging still faces considerable problems, including background interference and destructive and complex operations. Herein, we have designed a background-free, nondestructive, and easy-to-perform method for LFP imaging based on pH-mediated recognition of LFPs by carboxyl group-functionalized Zn₂GeO₄:Mn (ZGO:Mn-COOH) persistent luminescence nanorods (PLNRs). By simply adjusting the pH of the ZGO:Mn-COOH colloid dispersion to a certain acidic range, the negatively charged ZGO:Mn-COOH readily binds to protonated fingerprint ridges via electrostatic attraction. The ZGO:Mn-COOH colloid dispersion can be stored in portable commercial spray bottles, and the LFPs have been easily detected in situ by simply dropping the colloid dispersion on the LFPs. Moreover, since the ZGO:Mn-COOH can remain luminescent after excitation ceases, background color and background fluorescence interference were efficiently removed by simply capturing the luminescent LFP images after the excitation ceased. The entire LFP imaging process can be easily conducted without any destructive or complex operations. Due to the great versatility of the developed method for LFP imaging, clear LFP images with well-resolved ridge patterns were obtained. The designed background-free, nondestructive, and easy-to-perform LFP imaging strategy has great potential for future applications, such as forensic investigations and law enforcement.

关键词： fingerprint persistent luminescence background interference nanoparticle imaging

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Production of Branched Alkanes by Upcycling of Waste Polyethylene over Controlled Acid Sites of SO4/ZrO2-Al2O3Catalyst

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Angewandte Chemie 2024年第6期137卷

作者： Wanying Han Longfei Lin Ziyu Cen Yubin Ke Qian Xu Junfa Zhu Xuelei Mei Zhanghui Xia Xinrui Zheng Yaqin Wang Yani Liu Mingyuan He Haihong Wu Buxing Han Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular & Process Engineering School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China Institute of Eco-Chongming 20 Cuiniao Road Chenjia Town Chongming District Shanghai 202162 China Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China School of Chemical Sciences University of Chinese Academy of Sciences Beijing 100049 China China Spallation Neutron Source Institute of High Energy Physics Chinese Academy of Science Dongguan 523000 China National Synchrotron Radiation Laboratory Department of Chemical Physics and Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes University of Science and Technology of China Hefei 230029 China

Branched alkanes, which enhance the octane number of gasoline, can be produced from waste polyethylene. However, achieving highly selective production of branched alkanes presents a significant challenge in the upcycling of waste polyethylene. Here, we report a one-pot process to convert polyethylene into gasoline-range hydrocarbons (C 4 –C 13 ) with yield of 73.3 % over SO 4 /ZrO 2 -Al 2 O 3 catalyst at 280 °C. The proportion of branched alkanes reaches 90.1 % within the C 4 –C 13 fraction. Incorporation of sulfate group endows the catalyst with strong Lewis acid sites and weak and moderate Brønsted acid sites. In situ X-ray absorption, in situ infrared spectroscopy, in situ small angle neutron scattering, and DFT calculations reveal that polyethylene activation occurs through the synergy between sulfate groups and strong Lewis acid sites (Zr sites). The weak and moderate Brønsted acid sites preferentially catalyze the isomerization and type A β-scission processes, which favors the formation of branched alkanes, while suppressing competing reactions that produce straight-chain alkanes.

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Experimental investigation of crossflow characteristics in multi-jets system at small nozzle-to-plate spacing

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排灌机械工程学报 2019年第2期37卷 142-147页

作者： ZHU Keqian SUN Tao YU Pingping LI Meixiang YUAN Ningyi DING Jianning Jiangsu Collaborative Innovation Center for Photovoltaic Science and Engineering Jiangsu Province Cultivation Base for State Key Laboratory of Photovoltaic Science and TechnologyJiangsu Key Laboratory of Green Process EquipmentChangzhou High Technology Research Key Laboratory of Mould Advanced ManufacturingSchool of Mechanical EngineeringChangzhou University Micro/Nano Science and Technology Center School of Mechanical EngineeringJiangsu University

To further extend knowledge about the detailed knowledge on the crossflow characteristics in a multi-jets system under a confined space,particle image velocimetry (PIV) was employed to investigate the flow structures together with the distributions of the mean velocity components for Reynolds numbers (Re) ranging from 6 213 to 13 418,nozzle-to-plate spacing (H/D) varying from 0. 20 to1. 25,respectively. Results show that the crossflow configuration is significantly different from those of large nozzle-to-plate spacing. In addition,a turning point H/D=0.50 is revealed in the profile of the normalized maximum radial velocity which is associated with the heat transfer distribution on the impingement plate.

关键词： crossflow multiple impinging jets small nozzle-to-plate spacing Reynolds numbers particle image velocimetry

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Integration of high-solid digestion and gasification to dispose horticultural waste and chicken manure

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Chinese Journal of Chemical engineering 2018年第5期26卷 1145-1151页

作者： Wangliang Li Changbo Lu Gaojun An Yuming Zhang Yen Wah Tong The Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China Beijing POL Research Institute Beijing 102300 China State Key Laboratory of Heavy Oil Processing China University of Petroleum (Belting) Beijing 102249 China NUS Environment Research Institute National University of Singapore Singapore 117411 Singapore

To realize full energy recovery from grass and chicken manure(CM), the integration of high-solid anaerobic digestion(HSAD) and gasification was investigated experimentally. The anaerobic biodegradability of grass can be enhanced through codigestion with CM. When the volatile solid(VS) ratio of CM to grass was 20:80, C/N ratio calculated to be 21.70, the cumulative biogas yield was the highest, 237 ml·(g VS)^(-1). The enhancement of biogas production was attributed to the buffering effects of ammonia and rich trace elements in CM. In semi-continuous systems, when the organic loading rate was 4.0 g VS·L^(-1)·d^(-1), the HSAD process was stable, with the average biogas yield 168 ml·(g VS)^(-1). More than 80% fractions of the digestates were volatile matters, which meant that the digestates can be used as feedstock for gasification to produce syngas. The VS ratio of grass to CM had significant overall energy generation through HSAD and gasification. Compared with gasification of digestate,cogasification with woodchips increased syngas yield and low heat value(LHV). Increasing of mass ratio of digestates to woodchips led to the decrease of LHV.

关键词： Codigestion High-solid Chicken manure Yard waste Gasification Energy recovery

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Corrigendum to < Selective hydrogenation of furfural to furfuryl alcohol over Pd/TiH 2 catalyst ><[Molecular Catalysis 508 (2021) 111599]>

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Molecular Catalysis 2022年 526卷

作者： Zhuangqing Wang Xinchao Wang Chao Zhang Masahiko Arai Leilei Zhou Fengyu Zhao State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun 130022 China School of Applied Chemistry and Engineering University of Science and Technology of China Hefei Anhui 230026 China Jilin Province Key Laboratory of Green Chemistry and Process Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun 130022 China

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Heterogeneous Hollow Multi-Shelled Structures with Amorphous-Crystalline Outer-Shells for Sequential Photoreduction of CO2

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Angewandte Chemie 2022年第49期134卷

作者： Dr. Yanze Wei Dr. Feifei You Dr. Decai Zhao Prof. Jiawei Wan Prof. Lin Gu Prof. Dan Wang State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100049 P. R. China

Constructing delicate nano-/microreactors with tandem active sites in hierarchical architectures is a promising strategy for designing photocatalysts to realize the challenging but attractive CO 2 reduction. Herein, hollow multi-shelled structure (HoMS) based microreactors with spatial ordered hetero-shells are fabricated, which achieve two-step CO 2 -to-CH 4 photoreduction. The multiple inner CeO 2 shells increase the number of active catalytic sites to ensure efficient first-step reaction for generating CO, along with enriching the local CO concentration. The second-step CO-to-CH 4 reaction is consequently induced by amorphous TiO 2 (A-TiO 2 ) composites on the adjacent outer-most shell, thus realizing the CO 2 -to-CH 4 conversion capability using one CeO 2 @CeO 2 /A-TiO 2 HoMS. In-depth explorations in the microreactors provide compositional, structural, and interfacial guidance for engineering HoMS-based microreactors with temporally–spatially ordered shells toward efficient tandem catalysis.

关键词： Amorphous Phase CO2 Photoreduction Hollow Multi-Shell Structures Nano-/Microreactor Tandem Catalysis

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Effects of microalgal (Tetradesmus obliquus MCX38) attachment on photobioreactor treatment efficiency of raw swine wastewater

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Bioresource technology 2024年 403卷 130866页

作者： Chengxiao Ma Wenying Qu Shih-Hsin Ho Junfeng Li Fadong Li Lijuan Yi College of Water Conservancy and Architecture Engineering Shihezi University Shihezi 832000 Xinjiang China. Electronic address: mcxshz@***. College of Water Conservancy and Architecture Engineering Shihezi University Shihezi 832000 Xinjiang China. Electronic address: quwenying@***. State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology Harbin 150090 Heilongjiang China. Electronic address: stephen6949@***. College of Water Conservancy and Architecture Engineering Shihezi University Shihezi 832000 Xinjiang China. Electronic address: ljfshz@***. College of Water Conservancy and Architecture Engineering Shihezi University Shihezi 832000 Xinjiang China Key Laboratory of Ecosystem Network Observation and Modeling Institute of Geographic Sciences and Natural Resources Research Chinese Academy of Sciences 100101 Beijing China College of Resources and Environment University of Chinese Academy of Sciences 100190 Beijing China. Electronic address: lifadong@***. Key Laboratory for Green Process of Chemical Engineering of Xinjiang Bingtuan School of Chemistry and Chemical Engineering Shihezi University Shihezi 832003 Xinjiang China. Electronic address: ylj_xx@***.

Attachment of microalgae on the inner surfaces of photobioreactors impacts the efficiency of swine wastewater treatment by reducing the light intensity, which has been overlooked in previous studies. This study investigated the relationship between microalgal attachment biomass and light intensity in photobioreactors, determined the optimal attachment time for effective pollutant removal, and clarified the mechanisms of microalgal attachment in swine wastewater. After 9 days of treatment, the attached biomass in the photobioreactor increased from 0 to 6.4 g/m, decreasing the light intensity from 2,000 to 936 lux. At the 24 h optimal attachment time, the concentrations of chemical oxygen demand, ammonia nitrogen, and total phosphorus decreased from 2725.1, 396.4, and 87.2 mg/L to 361.2, 4.9, and 0.8 mg/L, respectively. Polysaccharides in the extracellular polymeric substances released by microalgae play a significant role in facilitating microalgae attachment. Optimizing the microalgal attachment time within photobioreactors effectively mitigates pollutant concentrations in swine wastewater.

关键词： Cell adhesion Extracellular polymeric substances Microalgae Piggery wastewater Pollutant removal

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