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Multifunctional AlPO_(4)reconstructed LiMn_(2)O_(4)surface for electrochemical lithium extraction from brine

Journal of Energy Chemistry 2024年第2期89卷 410-421,I0010页

作者： Jun Gu Linlin Chen Xiaowei Li Guiling Luo Linjing Fan yanhong chao Haiyan Ji Wenshuai Zhu School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina College of Science State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing 102249China School of the Environment and Safety Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina

LiMn_(2)O_(4)(LMO)electrochemical lithium-ion pump has gained widespread attention due to its green,high efficiency,and low energy consumption in selectively extracting lithium from brine.However,collapse of crystal structure and loss of lithium extraction capacity caused by Mn dissolution loss limits its industrialized application.Hence,a multifunctional coating was developed by depositing amorphous AlPO_(4)on the surface of LMO using sol-gel method.The characterization and electrochemical performance test provided insights into the mechanism of Li^(+)embedment and de-embedment and revealed that multifunctional AlPO_(4)can reconstruct the physical and chemical state of LMO surface to improve the interface hydrophilicity,promote the transport of Li^(+),strengthen cycle stability.Remarkably,after 20 cycles,the capacity retention rate of 0.5AP-LMO reached 93.6%with only 0.147%Mn dissolution loss.The average Li^(+)release capacity of 0.5AP-LMO//Ag system in simulated brine is 28.77 mg/(g h),which is 90.4%higher than LMO.Encouragingly,even in the more complex Zabuye real brine,0.5AP-LMO//Ag can still maintain excellent lithium extraction performance.These results indicate that the 0.5AP-LMO//Ag lithium-ion pump shows promising potential as a Li^(+)selective extraction system.

关键词： LiMn_(2)O_(4) Multifunctional AlPO_(4)coating Li^(+)embedment and de-embedment mechanism Stability Hydrophilicity Various solution

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Few-layered hexagonal boron nitride nanosheets stabilized Pt NPs for oxidation promoted adsorptive desulfurization of fuel oil

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Green Energy & Environment 2024年第3期9卷 495-506页

作者： Peiwen Wu Xin Song Linlin Chen Lianwen He Yingcheng Wu Duanjian Tao Jing He Chang Deng Linjie Lu yanhong chao Mingqing Hua Wenshuai Zhu School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang212013China College of Chemical Engineering and Environment State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China College of Chemistry and Chemical Engineering Jiangxi Normal UniversityNanchang330022China College of Science State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China

A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.

关键词： Desulfurization Adsorption Catalytic oxidation Active adsorbent Dibenzothiophene

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Engineering Dual Oxygen Simultaneously Modified Boron Nitride for Boosting Adsorptive Desulfurization of Fuel

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Engineering 2022年第7期8卷 86-93页

作者： Jing Luo Yanchen Wei yanhong chao chao Wang Hongping Li Jun Xiong Mingqing Hua Huaming Li Wenshuai Zhu School of Chemistry and Chemical Engineering&Institute for Energy Research Jiangsu UniversityZhenjiang 212013China State Key Laboratory of Heavy Oil Processing College of Chemical Engineering and EnvironmentChina University of Petroleum(Beijing)Beijing 102249China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China School of Pharmacy Jiangsu UniversityZhenjiang 212013China

Oxygen atoms usually co-exist in the lattice of hexagonal boron nitride(h-BN). The understanding of interactions between the oxygen atoms and the adsorbate, however, is still ambiguous on improving adsorptive desulfurization performance. Herein, simultaneously oxygen atom-scale interior substitution and edge hydroxylation in BN structure were constructed via a polymer-based synthetic strategy.Experimental results indicated that the dual oxygen modified BN(BN–2O) exhibited an impressively increased adsorptive capacity about 12% higher than that of the edge hydroxylated BN(BN–OH) fabricated via a traditional method. The dibenzothiophene(DBT) was investigated to undergo multimolecular layer type coverage on the BN–2O uneven surface via π–π interaction, which was enhanced by the increased oxygen doping at the edges of BN–2O. The density functional theory calculations also unveiled that the oxygen atoms confined in BN interior structure could polarize the adsorbate, thereby resulting in a dipole interaction between the adsorbate and BN–2O. This effect endowed BN–2O with the ability to selectively adsorb DBT from the aromatic-rich fuel, thereafter leading to an impressive prospect for the adsorptive desulfurization performance of the fuel. The adsorptive result was in good accordance with Freundlich and pseudo-second-order adsorption kinetics model results. Therefore, the designing of a polymer-based strategy could be also extended to other heteroatom doping systems to enhance adsorptive performance.

关键词： Polymer-based synthetic strategy Interior substitution BN Oxygen doping Adsorptive desulfurization

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Engineering 3D-printed aqueous colloidal ceramic slurry for direct ink writing

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Green Chemical Engineering 2023年第1期4卷 73-80页

作者： Jie Zhu Jiangtao Yu Yingcheng Wu yanhong chao Peiwen Wu Linjie Lu Linlin Chen Jing He Wenshuai Zhu School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang212013China State Key Laboratory of Heavy Oil Processing China University of Petroleum-BeijingBeijing102249China School of the Environment and Safety Engineering Jiangsu UniversityZhenjiang212013China Key Laboratory of Water Pollution Treatment and Resource Reuse of Hainan Province College of Chemistry and Chemical EngineeringHainan Normal UniversityHaikou571158China

The construction of rapid prototyping for structured ceramics has a promoting effect on potential applications.In this work,engineering slurry with different formulations were used to develop aqueous colloidal ceramic slurry for direct ink writing(DIW).Optimized slurry of Formulation 5 possessed good printing effect for DIW with stable mechanical properties.Related characteristics,including shrinkage,compressive strength,rheological behavior,and chemical property,were also examined.DIW ceramics prepared from optimized slurry can be preliminarily applied to adsorption of Rhodamine B and chlortetracycline,and possessed the advantages of easy separation and operation compared with powder adsorbents.This work provides a strategy for the design of 3D-printed kaolin ceramic slurry,and also extends to potential application in adsorption.

关键词： 3D printing Direct ink writing Ceramic slurry Kaolin Adsorption

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Sustainable preparation of graphene-analogue boron nitride by ball-milling for adsorption of organic pollutants

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Chinese Journal of Chemical Engineering 2022年第2期35卷 73-81页

作者： Haofeng Wu yanhong chao Yan Jin Duanjian Tao Xiaowei Li Jing Luo Guohua Xia Linhua Zhu Wenshuai Zhu School of Pharmacy Jiangsu UniversityZhenjiang 212013China College of Chemistry and Chemical Engineering Jiangxi Normal UniversityNanchang 330022China School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China Key Laboratory of Tropical Medicinal Plant Chemistry of Education Hainan Normal UniversityHaikou 571158China

The method of fabricating low-cost adsorbents with high activity and durability via a convenient and ecofriendly procedure is of great importance to wastewater treatment. Herein, a high-efficient mechanical exfoliation strategy was proposed to facilely prepare few-layered graphene-analogue boron nitride(BN) via a one-step non-organic solvent assisted wet ball mill procedure. Ball-milling treatment increased the specific surface area of BN 3.5-fold by reducing the thickness to ~3 layers with 45 min. The exfoliated BN exhibited strikingly improved sorption performance to organic contaminants with around 124% and 116% increased removal efficiency respectively for oxytetracycline(OTC) and Rhodamine B(RhB) as compared to the bulk BN. Batches sorption experiments showed that the sorption processes were thermodynamic endothermic, and well fitted to pseudo-second-order kinetic model and Freundlich isotherm equation. The π-π stacking interaction, hydrophobic effect and electrostatic interaction were proposed as the dominated sorption mechanism. In addition, no significant decline in adsorptive removal ability for the sorbent after 5 times recycling. The results indicate that the ball-milling exfoliation is a fast, green,sustainable and promising strategy for synthesis of highly potent BN based two-dimensional layered adsorbents.

关键词： Boron nitride Ball mill Exfoliation Adsorption Water treatment

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Electrochemical lithium ions pump for lithium recovery from brine by using a surface stability Al_(2)O_(3)–ZrO_(2 )coated LiMn_(2)O_(4) electrode

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Journal of Energy Chemistry 2022年第6期31卷 244-252,I0007页

作者： Guiling Luo Lin Zhu Xiaowei Li Guolang Zhou Jing Sun Linlin Chen yanhong chao Lei Jiang Wenshuai Zhu School of the Environment and Safety Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina College of Chemistry and Chemical Engineering Hainan Normal UniversityHaikou 571158HainanChina School of Pharmacy Jiangsu UniversityZhenjiang 212013JiangsuChina Jiangsu Topfine New Materials Technology Co.Ltd. Zhenjiang 212009JiangsuChina

The rapid commercialization of lithium–ion batteries has caused significant expansion of the lithium demand.Electrochemical lithium ions pump is a promising technology because of its good selectivity and friendly environment.Herein,an Al_(2)O_(3)–ZrO_(2) film coating of the LiMn_(2)O_(4)(AlZr–LMO) electrode is prepared and operated for recovery of Li^(+)from brine.The Li^(+) maximum extraction capacity of AlZr–LMO reached 49.92 mg/g in one cycle.Compared with the solely LMO electrode,the AlZr–LMO demonstrated evident electrochemical stability and cycle life towards the Li^(+)recovery system.After 30 successive cycles,the extraction capacity for Li^(+)increased from 29.21%to 57.67%.The high cycle capacity of the material could be attributed to its low polarization,high active sites,and good chemical stability of the electrode surface owing to the synergy function of Al_(2)O_(3)–ZrO_(2)in the charging-discharging process.A dynamic model parameter identification method was performed to evaluate the active site of AlZr–LMO.This work may provide a way to design the AlZr–LMO electrode and develop a good method for the recovery of lithium from brine.

关键词： Al_(2)O_(3)-ZrO_(2)coated LiMn_(2)O_(4) Lithium Electrochemical extraction Cycling stability

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Construction of truncated-octahedral LiMn2O4 for battery-like electrochemical lithium recovery from brine

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Green Energy & Environment 2023年第4期8卷 1081-1090页

作者： Guolang Zhou Linlin Chen Xiaowei Li Guiling Luo Zhendong Yu Jingzhou Yin Lei Fan yanhong chao Lei Jiang Wenshuai Zhu School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang212013JiangsuChina School of Pharmacy Jiangsu UniversityZhenjiang212013JiangsuChina School of Chemistry and Chemical Engineering Huaiyin Normal UniversityHuai'an223001JiangsuChina School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou225002JiangsuChina Jiangsu Topfine New Materials Science&Technology Co. Ltd.Zhenjiang212013JiangsuChina

The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn_(2)O_(4)-based electrochemical lithium recovery system is one of the strongest candidates for commercial application due to its high inserted capacity and low energy consumption. However, the surface orientation of LiMn_(2)O_(4)that facilitates Li diffusion happens to be prone to manganese dissolution making it a great challenge to obtain high lithium inserted capacity and long life simultaneously. Herein, we address this problem by designing a truncated octahedral LiMn_(2)O_(4)(Tr-oh LMO) in which the dominant(111) facets minimize Mn dissolution while a small portion of(100) facets facilitate the Li diffusion. Thus, this Tr-oh LMO-based electrochemical lithium recovery system shows excellent Li recovery performance with high inserted capacity(20.25 mg g^(-1)per cycle) in simulated brine. In addition, the dissolution rate of manganese per 30 cycles is only 0.44% and the capacity maintained 85% of the initial after 30 cycles. These promising findings accelerate the practical application of LiMn_(2)O_(4)in electrochemical lithium recovery.

关键词： LiMn_(2)O_(4) Crystal facets Electrochemistry Lithium recovery Brine

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Construction of porous disc-like lithium manganate for rapid and selective electrochemical lithium extraction from brine

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Chinese Journal of Chemical Engineering 2023年第2期54卷 316-322页

作者： Guolang Zhou Xiaowei Li Linlin Chen Guiling Luo Jun Gu Jie Zhu Jiangtao Yu Jingzhou Yin yanhong chao Wenshuai Zhu School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China College of Chemical Engineering and Environment State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing 102249China School of Pharmacy Jiangsu UniversityZhenjiang 212013China School of Chemistry and Chemical Engineering Huaiyin Normal UniversityHuai'an 223001China

In order to satisfy the growing global demand for lithium, selective extraction of lithium from brine has attracted extensive attention. LiMn_(2)O_(4)-based electrochemical lithium recovery system is one of the best choices for commercial applications because of its high selectivity and low energy consumption.However, the low ion diffusion coefficient of lithium manganate limits the further development of electrochemical lithium recovery system. In this work, a novel porous disc-like LiMn_(2)O_(4) was successfully synthesized for the first time via two-step annealing manganese(Ⅱ) precursors. The as-prepared LiMn_(2)O_(4) exhibits porous disc-like morphology, excellent crystallinity, high Li^(+)diffusion coefficient(average 7.6×10^(-9)cm^(2)·s^(-1)), high cycle stability(after 30 uninterrupted extraction and release cycles, the crystal structure hardly changed) and superior rate capacity(93.5% retention from 10-120 mA·g^(-1)). The porous structure and disc-like morphology further promote the contact between lithium ions and electrode materials. Therefore, the assembled electrochemical lithium extraction device with LiMn_(2)O_(4) as positive electrode and silver as negative electrode can realize the rapid and selective extraction of lithium in simulated brine(adsorption capacity of lithium can reach 4.85 mg·g^(-1) in 1 h). The mechanism of disc-like LiMn_(2)O_(4) in electrochemical lithium extraction was proposed based on the analysis of electrochemical characterization and quasi in situ XRD. This novel structure may further promote the practical application of electrochemical lithium extraction from brine.

关键词： LiMn_(2)O_(4) Desalination Diffusion coefficient Electrochemistry Brine Selectivity

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Progress in electrochemical lithium ion pumping for lithium recovery

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Journal of Energy Chemistry 2021年第8期30卷 431-445,I0009页

作者： Guolang Zhou Linlin Chen yanhong chao Xiaowei Li Guiling Luo Wenshuai Zhu School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China School of Pharmacy Jiangsu UniversityZhenjiang 212013China Jiangsu Topfine New Materials Science&Technology Co. Ltd.Zhenjiang 212013China

Accelerating the development of lithium resources has attracted a great deal of attention with the explosive growth of new energy vehicles.As a new technology,electrochemical lithium ion pumping(ELIP)is featured by environment-friendly,low energy consumption and high efficiency.This review summarizes the research progress in ELIP,and focuses on the evaluation methods,electrode materials and electrochemical systems of ELIP.It can be concluded that ELIP is expected to achieve an industrial application and has a promising prospect.In addition,challenges and perspective of electrochemical lithium extraction are also highlighted.

关键词： Electrochemistry Lithium ion pumping Recovery Seawater/brine

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D-A共轭聚合强化光电性能及光催化CO_(2)转化

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化工进展 2024年第1期43卷 292-301页

作者：于笑笑巢艳红刘海燕朱文帅刘植昌中国石油大学(北京)理学院北京102249 中国石油大学(北京)化学工程与环境学院北京102249 江苏大学化学化工学院江苏镇江212013

2,6-二溴蒽醌(2,6-dibromoanthraquinone,AQ)分别与三(4-乙炔苯基)胺(tris(4-ethynylphenyl)amine,TEA)和1,3,5-三乙炔基苯(1,3,5-triethynylbenzene,TEB),通过Sonogashira偶联反应制备得到两种蒽醌功能化的给体-受体(D-A)共轭聚合物催化剂(AQ-TEA和AQ-TEB)。采用FTIR、XPS、XRD和TEM对其化学结构和形貌进行了表征。通过固体紫外/可见漫反射光谱、稳态荧光光谱、时间分辨荧光光谱和电化学表征探究了两种催化材料的光学和电学性能。结果表明,三(4-乙炔苯基)胺与2,6-二溴蒽醌构筑的AQ-TEA表现出更强的可见光吸收和电荷转移性能。研究了两种光催化剂在H2O环境下光还原CO_(2)的催化性能。特别是AQ-TEA表现出更好的光催化性能,其CO的生成速率为392μmol/(g·h),是AQ-TEB的1.8倍。基于实验和理论计算的结果,推测共轭聚合物中强的分子内电荷转移(intramolecular charge transfer,ICT)可促进其光吸收、光电转换和光催化效率的提升。本研究为设计和制备高效的光催化活性共轭聚合物催化剂提供了新的思路。

关键词：聚合物催化剂光化学二氧化碳

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