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An efficient approach for the treatment of radioactive waste perfluoropolyether lubricants via a synergistic effect of thermal catalysis and immobilization

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Journal of Environmental Sciences 2024年第2期136卷 512-522页

作者： Xinhang Du Wenhua Tong Xinyu Zhou Jia Luo Yuqiu Liu Yabo Wang Panyu Li Yongkui Zhang Department of pharmaceutical&Biological engineering School of Chemical EngineeringSichuan UniversityChengdu 610065China

Perfluoropolyether(PFPE)lubricants are a kind of high-molecular polymer with many excellent properties.However,the use of PFPEs in the nuclear industry can lead to partial decomposition and carrying radionuclides,resulting in a large amount of radioactive waste PFPE lubricants annually.Moreover,radioactive waste PFPE lubricants are difficult to be effectively treated due to their high stability,the risk of possible leakage of radionuclides,and hypertoxic fluorine-containing by-products.In this study,without any precedent,a strategy of Mn O_(2)-catalyzed decomposition and Na_(2)CO_(3)-immobilized conversion was proposed for PFPE lubricant decomposition and fluorine immobilization simultaneously based on the Lewis acid-base and oxygen vacancies concept.A high fluorine conversion efficiency of 95.4%was achieved.Meanwhile,the mechanism of decomposition suggested that Mn O_(2)mainly provided Lewis acid sites and attacked the(basic)fluorine or oxygen atoms in PFPE molecules.The decomposition of PFPE chains was proceed down and volatile fluorine-containing gas was released by partial electron transfer,intramolecular disproportionation reaction,and unzipping fashion.Subsequently,gas by-products could be further oxidized and then immobilized into fluoride salts by carbonate solid absorbents.Overall,this study provides a simple,safe,and potentially practical strategy for the harmless conversion of refractory fluorinated organic wastes,especially perfluoropolymers.

关键词： Perfluoropolyether lubricants Catalyzed decomposition Fluorine-containing gas Immobilized conversion Fluoride

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Glutamicibacter nicotianae AT6:A new strain for the efficient biodegradation of tilmicosin

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Journal of Environmental Sciences 2024年第8期142卷 182-192页

作者： Huijuan Li Hao Zhou Liling Fan Long Meng Yanyun Zhao Lanmei Zhao Bo Wang college of chemical and Biological engineering Shandong University of Science and TechnologyQingdao 266590China college of Chemistry and chemical engineering Heze UniversityHeze 274015China college of Safety and Environmental engineering Shandong University of Science and TechnologyQingdao 266590China

The degradation of tilmicosin(TLM),a semi-synthetic 16-membered macrolide antibiotic,has been receiving increasing attention.Conventionally,there are three tilmicosin degradation methods,and among them microbial degradation is considered the best due to its high efficiency,eco-friendliness,and low cost.Coincidently,we found a new strain,Glutamicibacter nicotianae sp.AT6,capable of degrading high-concentration TLM at 100 mg/L with a 97%removal efficiency.The role of tryptone was as well investigated,and the results revealed that the loading of tryptone had a significant influence on TLM removals.The toxicity assessment indicated that strain AT6 could efficiently convert TLM into less-toxic substances.Based on the identified intermediates,the degradation of TLM by AT6 processing through two distinct pathways was then proposed.

关键词： Tilmicosin Glutamicibacter nicotianae Biodegradation Degradation pathway pharmaceutical wastewater

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Cascade equilibrium stage relaxation method by introducing equilibrium efficiency parameter

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Chinese Journal of chemical engineering 2024年第2期66卷 145-156页

作者： Xuepu Cao Shengkun Jia Xing Qian Yiqing Luo Xigang Yuan college of chemical and pharmaceutical Hebei University of Science&TechnologyShijiazhuang 050018China School of chemical engineering and Technology State Key Laboratory of Chemical EngineeringTianjin UniversityTianjin 300072China college of Information Science and Technology Beijing University of Chemical TechnologyBeijing 100029China

Optimizing multistage processes,such as distillation or absorption,is a complex mixed-integer nonlinear programming(MINLP)problem.Relaxing integer into continuous variables and solving the easier nonlinear programming(NLP)problem is an optimization idea for the multistage process.In this article,we propose a relaxation method based on the efficiency parameter.When the efficiency parameter is 1or 0,the proposed model is equivalent to the complete existence or inexistence of the equilibrium stage.And non-integer efficiency represents partial existence.A multi-component absorption case shows a natural penalty for non-integer efficiency,which can assist the efficiency parameter converging to 0 or 1.However,its penalty is weaker than the existing relaxation models,such as the bypass efficiency model.In a simple distillation case,we show that this property can weaken the nonconvexity of the optimization problem and increase the probability of obtaining better optimization results.

关键词： Mathematical modeling Absorption Distillation Optimization

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Regulation of solvation structure and the cooperation environment of potassium bonds for wider-temperature adaptive potassium storage

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Rare Metals 2024年第4期43卷 1610-1621页

作者： Bing-Bing Liu Yi-Hui Liu You-Bin Zhang Zhen-Guo Qi Guo-Hui Qin State Key Laboratory Base for Eco-chemical engineering College of Chemical EngineeringQingdao University of Science and Technology Shandong Synergetic Innovation Center of Ecological and chemical engineering

Antimony selenide（Sb2Se3） is one of the perspective candidates for potassium-ion batteries due to its advanced virtues stem including featured high capacity,fertile reserves and the relative narrow band gap.Despite the unique advantages,it is still plagued by the unstable interface compatibility and poor wider-temperature adaptability.The optimization of microstructure and the construction of inorganic-organic hybrids with a low desolvation barrier and rapid kinetics behaviors are efficient to address these issues.The Sb2Se3nanorods enclosed by the S-doped carbon layer（SC）,further crosslinked by the poly（N-isopropylacrylamide）(PM) film（PM@Sb2Se3@SC）,were artificially fabricated,and it displays the enrichment ion aggregated model as well as contacted ion pair state,the well-tailored cooperation environment of potassium bonds,assuring a homogeneous potassium deposition and an excellent widertemperature adaptability.The complicated experimental studies and theoretical calculations authenticate the synergistic effects of geometric conformation and compositional design for the tremendously enhanced potassium storage.Moreover,the full device over PM@Sb2Se3@SC anode and the potassium Prussian blue cathode manifests impressively durable cycling life and wider-temperature adaptability,verifying the glorious contribution from the finely manipulation in solvation structure and potassium bonds to enhancing the potassium storage behaviors.

关键词： Anode Sb 2 Se 3 rods Interface compatibility Inorganic–organic electrode Potassium ion battery

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Ternary-phase layered cathodes toward ultra-stable and highrate sodium ion storage

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Rare Metals 2024年第4期43卷 1589-1598页

作者： Wen-Ji Yin Pei-Dan Su Qi Lu Xiao-Qiong Li Ji-Ming Peng Teng-Fei Zhou Ge-Meng Liang Yu-Liang Cao Hong-Qiang Wang Qing-Yu Li Si-Jiang Hu Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal University Institutes of Physical Science and Information Technology Anhui University Department of Chemistry and pharmaceutical Sciences Guilin Normal College college of Chemistry and chemical engineering Huanggang Normal University School of chemical engineering and Advanced Materials The University of Adelaide engineering Research Center of Organosilicon Compounds and Materials of Ministry of Education College of Chemistry and Molecular SciencesWuhan University

With the shortage of lithium resources,sodiumion batteries（SIBs） are considered one of the most promising candidates for lithium-ion batteries.P2-type and O3-type layered oxides are one of the few cathodes that can access high energy density.However,they usually exhibit structural change,capacity decay,and slow Na ion kinetic.Herein,we present layered ternary-phase cathodes with P2,P3 and O3 phases by a lattice doping strategy,which is demonstrated by X-ray diffraction（XRD） refinement.Combining the characteristics of P2,P3 and O3 phases,the layered composites show performance improvement during long-term battery cycling.In particular,Na0.7Li0.1Co0.3-Fe0.3Mn0.3O2（NLCFM） delivers a reversible capacity of120.1 mAh·g-1at 0.1C(1.0C=175 mA·g-1) with a superior capacity retention of 72.5% after 1000 cycles at10.0C.This work offers insights into the development of advanced cathode materials for SIBs.

关键词： Sodium-ion battery Cathode material Layered oxides Lattice doping Mixed phase

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Recent progress on nanomaterial-based electrochemical dissolved oxygen sensors

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Chinese Journal of chemical engineering 2024年第4期68卷 103-119页

作者： Shaoqi Zhang Tao Liu Zhenyu Chu Wanqin Jin State Key Laboratory of Materials-Oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

Dissolved oxygen(DO)usually refers to the amount of oxygen dissolved in water.In the environment,medicine,and fermentation industries,the DO level needs to be accurate and capable of online monitoring to guide the precise control of water quality,clinical treatment,and microbial metabolism.Compared with other analytical methods,the electrochemical strategy is superior in its fast response,low cost,high sensitivity,and portable device.However,an electrochemical DO sensor faces a trade-off between sensitivity and long-term stability,which strongly limits its practical applications.To solve this problem,various advanced nanomaterials have been proposed to promote detection performance owing to their excellent electrocatalysis,conductivity,and chemical stability.Therefore,in this review,we focus on the recent progress of advanced nanomaterial-based electrochemical DO sensors.Through the comparison of the working principles on the main analysis techniques toward DO,the advantages of the electrochemical method are discussed.Emphasis is placed on recently developed nanomaterials that exhibit special characteristics,including nanostructures and preparation routes,to benefit DO determination.Specifically,we also introduce some interesting research on the configuration design of the electrode and device,which is rarely introduced.Then,the different requirements of the electrochemical DO sensors in different application fields are included to provide brief guidance on the selection of appropriate nanomaterials.Finally,the main challenges are evaluated to propose future development prospects and detection strategies for nanomaterial-based electrochemical sensors.

关键词： Nanomaterial Dissolved oxygen Electrochemical sensor Nanostructures Detection principles

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A thermodynamic view on the in-situ carbon dioxide reduction by biomass-derived hydrogen during calcium carbonate decomposition

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Chinese Journal of chemical engineering 2024年第4期68卷 231-240页

作者： Peng Jiang Hao Zhang Guanhan Zhao Lin Li Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu State Key Laboratory of Materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream processes.This study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen Plus.Following this,process optimization and energy integration were implemented to provide optimized operation conditions.Lastly,a life cycle assessment was carried out to assess the carbon footprint of the coupled process.Results reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous products.By optimizing systemic energy through heat integration,an energy efficiency of 86.30%was achieved.Additionally,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.

关键词： Biomass CaCO_(3)reductive calcination chemical looping Hydrogen production Carbon footprint Thermodynamics process

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Drug delivery with Mn-doped MoO2 for photothermalenhanced chemotherapy in fighting cancers

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Rare Metals 2024年第5期43卷 2230-2240页

作者： Ping Zhao Hai-Fa Zheng Ju Peng Xing-Long Li Fazal Raziq Xiao-Jun Liu Hao-Quan Yu Jin-Lu Tang Yi-Fan Kang Wen-Huan Huang School of Chemistry and chemical engineering Guangdong Pharmaceutical University KAUST Catalysis Center King Abdullah University of Science and Technology 23955-6900 Thuwal Key Laboratory of chemical Additives for China National Light Industry College of Chemistry and Chemical EngineeringShaanxi University of Science and Technology

Although chemotherapy has been intensively applied in cancer treatments,its inadequate therapeutic efficacy and severe side effects are still under constant concerns.Nanoplatforms used as anti-tumor drug delivery system （DDS） have attracted tremendous attentions owing to their various intriguing properties.Herein,Mn-doped Mo O2nanoparticles coated with Zr O2and capped with Bi2O3have been designed as a DDS,namely MMZB.MMZB possesses good magnetic properties,great photothermal conversion ability,sensitive tumor microenvironment （TME） responsiveness,and good biocompatibility in hemocompatibility in vitro.Thus,MMZB has been utilized to load the chemotherapeutic agent daunomycin（DNM）(MMZB@DNM) for chemo-photothermal combined therapy.MMZB@DNM demonstrates a more impressive anti-cancer effect than the individual photothermal or chemotherapy both in vitro and in vivo.Furthermore,the analysis of tumor specimen sections and serum levels after the treatment indicates negligible side effects for MMZB@DNM in vivo.This contribution provides a valuable concept in designing therapeutic agents for achieving significantly enhanced tumor treatments,which benefits from the synergistic combination of chemotherapy and photothermal therapy in one single nanoagent.

关键词： Mn-doped MoO 2 Bi 2 O 3 Nanocarrier Photothermal Chemotherapy

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FeNi Prussian blue analogues on highly graphitized carbon nanosheets as efficient glucose sensors

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Rare Metals 2024年第6期43卷 2730-2738页

作者： Jin-Hang Xue Qiu-Hong Sun Cheng Han Yuan-Dong Yang Shao-Jie Xu Qi-Peng Li Jin-Jie Qian college of Life and Environmental Science Wenzhou University college of Chemistry and Materials engineering Wenzhou University college of Chemistry and chemical engineering Zhaotong University

Meeting the continuous glucose monitoring requirements of individuals necessitates the research and development of sensors with high sensitivity and stability.In this study,a straightforward strategy was proposed for synthesizing ultra-thin oxygen-rich graphitized carbon nanosheets（denoted as GCS-O）.These nanosheets are obtained by calcining a topologically two-dimensional indium-based coordination polymer.Subsequently,the growth of FeNi Prussian blue analogue（PBA） on GCS-O effectively introduces active sites and increases the nitrogen content within the carbonaceous matrix.The resulting FeNi-PBA/GCS-O composite exhibits excellent glucose sensing performance with a broad linear range of 1 to 1300μmol·L-1.Meanwhile,it also achieves a high sensitivity of 2496 μA·mmol-1·L·cm-2,a limit of detection of 100nmol·L-1（S/N=3）,and commendable long-term durability.The relatively simple synthesis process,exceptional sensitivity,and satisfactory electrochemical sensing performance of FeNi-PBA/GCS-O open up new directions for biosensor applications.

关键词： Coordination polymer Carbon nanosheet Prussian blue analogue Surface reconstruction Glucose oxidation

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Iron-nickel alloy particles with N-doped carbon “armor” as a highly selective and long-lasting catalyst for the synthesis of Nbenzylaniline molecules

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Nano Research 2024年第4期17卷 2308-2319页

作者： Gang Wang Longchao Sun Wanyi Liu Haijuan Zhan Shuxian Bi college of Chemistry and chemical engineering Ningxia UniversityYinchuan 750021China

A scalable strategy for the convenient and rapid preparation of nitrogen-doped carbon-coated iron-based alloy catalysts was developed.By controlling the type and amount of metal salts in the precursor,various types of nitrogen-doped carbon-coated alloy catalysts can be prepared in a targeted manner.Fe_(2)Ni2@CN materials with small particle sizes and relatively homogeneous basic sites showed promising results in the N-alkylation reaction of benzyl alcohol with aniline(optimum yield:99%).It is worth noting that the catalyst can also be magnetically separated and recovered after the reaction,and its performance can be regenerated through simple calcination.Furthermore,it was confirmed by kinetic experiments that the activation of C–H at the benzyl alcohol benzylic position is the rate-determining step(RDS).According to density flooding theory calculations,Fe_(2)Ni2@CN catalysts require less energy than other materials(Fe@CN and Ni@CN)for the RDS(dehydrogenation reaction)process.Therefore N-alkylation reactions are more easily carried out on Fe_(2)Ni2@CN catalysts,which may be the reason for the best catalytic activity of Fe-Ni alloy materials.These carbon-coated alloy materials will show great potential in more types of heterogeneous catalysis.

关键词： iron-nickel alloy catalyst N-alkylation reaction magnetic separation reaction path dehydrogenation reaction

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