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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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Tribological performance of various metal-doped carbon dots as water-based lubricant additives and their potential application as additives of poly(ethylene glycol)

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Friction 2022年第5期10卷 688-705页

作者： Weiwei TANG Xuejun ZHU Yufeng LI school of biological and chemical engineering Panzhihua UniversityPanzhihua 617000China

Advances in nano-lubricant additives are vital to the pursuit of energy efficiency and sustainable development.Carbon dots(CDs)have been widely investigated in the domain of lubricant additives owing to their extraordinary tribological properties,in particular,their friction-reducing and anti-wear properties.Metal-doped CDs are a new type of CDs,and their friction-reducing and anti-wear properties are attracting increasing attention.Therefore,a series of CDs doped with various divalent metal ions have been successfully synthesized via one-pot pyrolysis.The tribological properties of the synthesized CDs as water-based lubricant additives are in the following order:Zn-CDs>Cu-CDs>>Mg-CDs>Fe-CDs>U-CDs.Specifically,adding 1.0 wt%of Zn-CDs into water-based lubricant results in 62.5%friction and 81.8%wear reduction.Meanwhile,the load-carrying capacity of the water-based lubricant increases from 120 N to at least 500 N.Zn-CDs as an additive have long service life.Additionally,anion-tuned Zn-CDs fabricated via anion exchange exhibit promise as lubricant additives for poly(ethylene glycol).Based on the results of wear scar surface analyses,it is discovered that tribochemical films,primarily composed of iron oxides,nitrides,metal carbonates,zinc oxides,zinc carbonates,organic compounds,and embedded carbon cores,formed on the rubbing surfaces with a thickness of approximately 270 nm when Zn-CDs are used as additives.This film combined with the“ball-bearing”and third-particle effects of Zn-CDs contributed to excellent lubrication performance.

关键词： metal-doped carbon dots(CDs) water-based lubricant additives tribological performance lubrication mechanism

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Simultaneous purification of minor components in natural products using twin-column recycling chromatography with a step solvent gradient

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Chinese Journal of chemical engineering 2024年第5期69卷 212-219页

作者： Jin, Guangxia Wu, Yuxue Wei, Feng school of biological and chemical engineering NingboTech University Ningbo 315100 China

The isolation of minor components from complex natural product matrices presents a significant challenge in the field of purification science due to their low concentrations and the presence of structurally similar compounds. This study introduces an optimized twin-column recycling chromatography method for the efficient and simultaneous purification of these elusive constituents. By introducing water at a small flowing rate between the twin columns, a step solvent gradient is created, by which the leading edge of concentration band would migrate at a slower rate than the trailing edge as it flowing from the upstream to downstream column. Hence, the band broadening is counterbalanced, resulting in an enrichment effect for those minor components in separation process. Herein, two target substances, which showed similar peak position in high performance liquid chromatography (HPLC) and did not exceed 1.8% in crude paclitaxel were selected as target compounds for separation. By using the twin-column recycling chromatography with a step solvent gradient, a successful purification was achieved in getting the two with the purity almost 100%. We suggest this method is suitable for the separation of most components in natural produces, which shows higher precision and recovery rate compared with the common lab-operated separation ways for natural products (thin-layer chromatography and prep-HPLC). © 2024 The chemical Industry and engineering Society of China, and chemical Industry Press Co., Ltd

关键词： Recycling

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Fabrication and characterization of hierarchical porous Ni2+doped hydroxyapatite microspheres and their enhanced protein adsorption capacity

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Chinese Journal of chemical engineering 2022年第5期35卷 238-247页

作者： Yaling Li Hao Ai Liangzhi Qiao Yinghong Wang Kaifeng Du Department of Pharmaceutical&biological engineering School of Chemical EngineeringSichuan UniversityChengdu 610065China

Hydroxyapatite(HAP)is a common bio-adsorbent,which performance depends heavily upon its morphology and microporous structure.In this study,a novel synthesis strategy was proposed for hierarchical porous HAP microspheres by a simple"one-pot"hydrothermal reaction.In the strategy,L-glutamic acid serves as soft template to modulate the morphology and inner crystalline of HAP.To evaluate the application potential,doping Ni^(2+) on hierarchical porous HAP microspheres gives metal chelated affinity adsorbents.The prepared adsorbents show a perfect spherical shape,particles size of 96.6μm,relatively specific surface area of 48.5 m^(2)·g^(-1) and hierarchical pores(mesopores:4 nm and macropores:53 nm).By the adsorption evaluation,it reveals that the Ni^(2+)-HAP adsorbents have high adsorption capacities of275.11 and 97.55 m^(2)·g^(-1) for hemoglobin and bovine serum albumin,respectively,which is comparable to other similar adsorbent.Therefore,this work provides a promising method for high-efficiency hydroxyapatite microspheres for proteins purification.

关键词： Hierarchical porous hydroxyapatite microspheres Templates Metal doping Proteins adsorption

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Anode-less all-solid-state batteries:recent advances and future outlook

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Materials Futures 2023年第1期2卷 122-131页

作者： Nohjoon Lee Jihoon Oh Jang Wook Choi School of Chemical and Biological Engineering Seoul National UniversitySeoul 08826Republic of Korea

While all-solid-state batteries have built global consensus with regard to their impact in safety and energy density,their anode-less versions have attracted appreciable attention because of the possibility of further lowering the cell volume and cost.This perspective article summarizes recent research trends in anode-less all-solid-state batteries(ALASSBs)based on different types of solid electrolytes and anticipates future directions these batteries may take.We particularly aim to motivate researchers in the field to challenge remaining issues in ALASSBs by employing advanced materials and cell designs.

关键词： all-solid-state batteries anode-free anode-less interface stability lithium dendrite

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Extraction of lithium from the simulated pyrometallurgical slag of spent lithium-ion batteries by binary eutectic molten carbonates

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International Journal of Minerals,Metallurgy and Materials 2022年第9期29卷 1715-1721页

作者： Hui Dang Zhidong Chang Hualei Zhou Sihang Ma Min Li Jialing Xiang Department of Chemistry and chemical engineering School of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China

The effective and low-temperature extraction of lithium from the pyrometallurgical slag of spent lithium-ion batteries(LIBs)remains a great challenge.Herein,potassium carbonate/sodium carbonate(K_(2)CO_(3)/Na_(2)CO_(3)),which could form a eutectic molten salt system at 720℃,was used as a roasting agent to extract lithium from pyrometallurgical slag.Lithium was successfully extracted from the slag by K_(2)CO_(3)/Na_(2)CO_(3) roasting followed by water leaching.Theoretical calculation results indicate that the lengths of Li-O bonds increase after K^(+)/Na^(+)adsorption,resulting in the easy release of Li^(+)from the LiAlSi_(2)O_(6) lattice after roasting with K_(2)CO_(3)/Na_(2)CO_(3).Thermogravimetry-differential scanning calorimetry results indicate that the eutectic phenomenon of K_(2)CO_(3) and Na_(2)CO_(3) could be observed at 720℃ and that the reaction of the slag and eutectic molten salts occurs at temperatures above 720℃.X-ray diffraction results suggest that Li^(+)in the slag is exchanged by K^(+)in K_(2)CO_(3) with the concurrent formation of KAlSiO_(4),while Na_(2)CO_(3) mainly functions as a fluxing agent.The lithium extraction efficiency can reach 93.87%under the optimal conditions of a roasting temperature of 740℃,roasting time of 30 min,leaching temperature of 50℃,leaching time of 40 min,and water/roasted sample mass ratio of 10:1.This work provides a new system for extracting lithium from the pyrometallurgical slag of spent LIBs.

关键词： spent lithium-ion battery lithium recovery silicate structure low roasting temperature binary eutectic carbonates roasting

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On the determination of particle impact breakage in selection function

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Particuology 2022年第6期20卷 117-132页

作者： Li Ge Wang Ruihuan Ge Xizhong Chen Process Systems Enterprise HammersmithLondonUK Department of chemical and biological engineering University of SheffieldUK Process and chemical engineering School of EngineeringUniversity College CorkIreland

This paper presents a thorough study of particle impact breakage in selection function with a unified breakage criterion.The impact mode and breakage pattern for particulate materials are classified based on a significant review of well-established impact testers.It was found that the lack of a unified breakage criterion to determine the breakage probability disables a direct comparison of particle breakage propensity from different impact loading testers.The literature breakage models to describe the breakage probability are reviewed where the advantage and drawback of these models are scrutinized.The sourced literature breakage models are compared with the zeolite breakage datasets in a unified breakage criterion to evaluate the model performance.A novel computational modelling workflow for a milling process is proposed to provide a guidance in implementing the digital twin in milling process prediction.The breakage probability models,i.***.the selection functions are comprehensively assessed in population balance model to examine the model serviceability.The model simplicity and fidelity in the model assessment are specifically discussed and the value of digital twin in substantially reducing the experimental trials is highlighted.

关键词： Impact breakage Breakage criteria Breakage model assessment Selection function Population balance model Digital twin

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Rapid quantification of acid value in frying oil using iron tetraphenylporphyrin fluorescent sensor coupled with density functional theory and multivariate analysis

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Food Quality and Safety 2022年第4期6卷 534-544页

作者：顾海洋董艺凝吕日琴黄星奕陈全胜 Department of biological and chemical engineering Yangzhou Polytechnic CollegeYangzhouChina school of Bio and Food engineering Chuzhou UniversityChuzhouChina school of Food and biological engineering Jiangsu UniversityZhenjiangChina

A metalloporphyrin-based fluorescent sensor was developed to determine the acid value in frying oil.The electronic and structural performances of iron tetraphenylporphyrin(FeTPP)were theoretically investigated using time-dependent density functional theory and density functional theory at the B3LYP/LANL2DZ level.The quantified FeTPP-based fluorescent sensor results revealed its excellent performance in discriminating different analytes.In the present work,the acid value of palm olein was determined after every single frying cycle.A total of 10 frying cycles were conducted each day for 10 consecutive days.The FeTPP-based fluorescent sensor was used to quantify the acid value,and the results were compared with the chemical data obtained by conventional titration method.The synchronous fluorescence spectrum for each sample was recorded.Parallel factor analysis was used to decompose the three-dimensional spectrum data.Then,the support vector regression(SVR),partial least squares,and back-propagation artificial neural network methods were applied to build the regression models.After the comparison of the constructed models,the SVR models exhibited the highest correlation coefficients among all models,with 0.9748 and 0.9276 for the training and test sets,respectively.The findings suggested the potential of FeTPP-based fluorescent sensor in rapid monitoring of frying oil quality and perhaps also in other foods with higher oil contents.

关键词： Synchronous fluorescence spectrum fluorescent sensor oil quality density functional theory parallel factor analysis

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Dynamic response surface methodology using Lasso regression for organic pharmaceutical synthesis

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Frontiers of chemical Science and engineering 2022年第2期16卷 221-236页

作者： Yachao Dong Christos Georgakis Jacob Santos-Marques Jian Du Institute of chemical Process Systems engineering School of Chemical EngineeringDalian University of TechnologyDalian 116024China Department of chemical and biological engineering and Systems Research Institute Tufts UniversityMedfordMA 02155USA

To study the dynamic behavior of a process,time-resolved data are collected at different time instants during each of a series of experiments,which are usually designed with the design of experiments or the design of dynamic experiments methodologies.For utilizing such time-resolved data to model the dynamic behavior,dynamic response surface methodology(DRSM),a datadriven modeling method,has been proposed.Two approaches can be adopted in the estimation of the model parameters:stepwise regression,used in several of previous publications,and Lasso regression,which is newly incorporated in this paper for the estimation of DRSM models.Here,we show that both approaches yield similarly accurate models,while the computational time of Lasso is on average two magnitude smaller.Two case studies are performed to show the advantages of the proposed method.In the first case study,where the concentrations of different species are modeled directly,DRSM method provides more accurate models compared to the models in the literature.The second case study,where the reaction extents are modeled instead of the species concentrations,illustrates the versatility of the DRSM methodology.Therefore,DRSM with Lasso regression can provide faster and more accurate datadriven models for a variety of organic synthesis datasets.

关键词： data-driven modeling pharmaceutical organic synthesis Lasso regression dynamic response surface methodology

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Atomically dispersed dual-metal-site PGM-free electrocatalysts for oxygen reduction reaction:Opportunities and challenges

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SusMat 2022年第5期2卷 569-590页

作者： Xiaoxuan Yang Cameron Priest Yang Hou Gang Wu College of chemical and biological engineering Zhejiang UniversityHangzhouChina Department of chemical and biological engineering University at BuffaloThe State University of New YorkBuffaloNew YorkUSA Institute of Zhejiang University-Quzhou QuzhouChina school of biological and chemical engineering NingboTech UniversityNingboChina

Atomically dispersed and nitrogen coordinated single metal site(MNx,M=Fe,Co,or Mn)moieties embedded in partially graphitized carbon(denoted as M–N–C)are recognized as the most promising platinum group metal-free catalysts for the oxygen reduction reaction(ORR)in proton exchange membrane fuel cells.However,simply regulating their coordination environments and local structures of single metal sites cannot fundamentally change active site structure,which leads to insufficient activity and stability.A second transition metal can be incorporated to design dual-metal sites,offering a new opportunity to modulate the electronic and geometric structures of M–N–C catalysts.Therefore,exploring optimal atomically dispersed dual-metal-site is essential to designing new active sites with enhanced ORR activity,and stability,especially breaking the activity-stability trade-off.This review provides a comprehensive analysis of the advances in developing atomically dispersed dual-metal site catalysts for the ORR,including innovative synthesis methods,primary structural configurations,and the mechanisms to promote catalytic performance.We aim to elucidate the crucial structure–property correlation,emphasizing the inherent electronic and geometric effects of dual metal sites.Finally,we discuss the current challenges of dual-metal site catalysts concerning rational design,precise synthesis,and high-fidelity structural characterization.

关键词： dual metal sites electrocatalysis fuel cells oxygen reduction PGM-free catalyst

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