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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 *** 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

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

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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 ***,collapse of crystal structure and loss of lithium extraction capacity caused by Mn dissolution loss limits its industrialized ***,a multifunctional coating was developed by depositing amorphous AlPO_(4)on the surface of LMO using sol-gel *** 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 ***,after 20 cycles,the capacity retention rate of 0.5AP-LMO reached 93.6%with only 0.147%Mn dissolution *** 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 ***,even in the more complex Zabuye real brine,0.5AP-LMO//Ag can still maintain excellent lithium extraction *** 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

One-step selective separation and efficient recovery of valuable metals from spent lithium batteries by phosphoric acid-based deep eutectic solvent

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Green Chemical Engineering 2024年第3期5卷 390-398页

作者： Yuning Zhang Peng Cui Guiling Luo Linlin Chen Xiaowei Li yanhong chao Wenshuai Zhu School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang212013China College of Science State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China College of Chemical Engineering and Environment State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China

With more and more lithium-ion batteries(LIBs)being put into production and application,precious metals such as lithium and cobalt are scarce,so it is imminent to recover various strategic metal resources from spent ***,the complex and difficult problem of separating and recovering metals from leaching solutions has been an urgent question that needs to be *** this work,a phosphoric acid-based deep eutectic solvent(DES)was developed for extracting metals from spent LIBs and one-step selectively separating and efficiently recovering transition *** prepared DES shows excellent extraction performance for Li(100%)and Co(92.8%)at 100°*** addition,the extraction system can effectively separate and precipitate Co through its own components,avoiding the introduction of new precipitants and the destruction of the original composition structure of *** also contributes to the good cycle stability of the extraction system with excellent extraction performance for Li(94.3%)and Co(80.8%)after 5 *** work proposes a green method for one-step selectively separating and recovering valuable metals from spent LIBs.

关键词： Spent lithium-ion batteries Phosphoric acid-based deep eutectic solvent One-step separation Regenerate

3D-printing of integrated spheres as a superior support of phosphotungstic acid for deep oxidative desulfurization of fuel

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Journal of Energy Chemistry 2020年第6期29卷 91-97,I0004页

作者： Jie Zhu Peiwen Wu Linlin Chen Jing He Yingcheng Wu chao Wang yanhong chao Linjie Lu Minqiang He Wenshuai Zhu Huaming Li School of Chemistry and Chemical Engineering Institute for Energy ResearchJiangsu UniversityZhenjiang 212013JiangsuChina Zhenjiang Sandi New Materials Co. Ltd.Zhenjiang 212013JiangsuChina School of the Environment and Safety Engineering Institute of Environmental Health and Ecological SecurityJiangsu UniversityZhenjiang 212013JiangsuChina

Construction of catalysts with integral structure for oxidative reaction process is an essential promotion to catalysts in industrial *** this work,a 3D printing method was employed to prepare 3D printed spheres(3D-PSs),followed by carbonization to form 3D carbon spheres(3D-CSs).Then,a 3D-CSs supported phosphotungstic acid(HPW/3D-CSs)was prepared for deep oxidative *** with traditional powder catalysts,the as-prepared catalyst is easy to be operated and separated from oil *** supported catalyst possesses excellent catalytic performance and the removal of DBT,4-MDBT and 4,6-DMDBT in fuel oil,reaching^100%of sulfur *** effects of various experimental parameters on desulfurization efficiency were considered to optimize reaction ***,the catalyst shows excellent thermal and chemical stability,with no obvious decrease in desulfurization activity after 5 ***–MS analysis indicates DBT sulfone was the solely oxidized product of DBT.

关键词： 3D printing Integrated spheres Supported catalyst Oxidative desulfurization

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

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 *** lithium ions pump is a promising technology because of its good selectivity and friendly ***,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 *** Li^(+) maximum extraction capacity of AlZr–LMO reached 49.92 mg/g in one *** with the solely LMO electrode,the AlZr–LMO demonstrated evident electrochemical stability and cycle life towards the Li^(+)recovery *** 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–*** 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

Hexagonal boron nitride:A metal-free catalyst for deep oxidative desulfurization of fuel oils

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Green Energy & Environment 2020年第2期5卷 166-172页

作者： Peiwen Wu Linjie Lu Jing He Linlin Chen yanhong chao Minqiang He Fengxia Zhu Xiaozhong Chu Huaming Li Wenshuai Zhu School of Chemistry and Chemical Engineering Insitute for Energy ResearchJiangsu UniversityZhenjiang212013China School of the Environment and Safety Engineering Jiangsu University212013China School of Chemistry and Chemical Engineering Huaiyin Normal UniversityHuaian223300China

Oxidative desulfurization(ODS)has been proved to be an efficient strategy for the production of clean fuel *** metal-based materials have been employed as excellent ODS catalysts,but being hindered by their high-cost and potential secondary *** this work,we employed graphene analogous hexagonal boron nitride(h-BN)as a metal-free catalyst for ODS with hydrogen peroxide(H2O2)as the *** h-BN catalyst was characterized and proved to be a few-layered structure with relatively high specific surface *** h-BN catalyst showed a 99.4%of sulfur removal in fuel oil under the optimized reaction ***,the h-BN can be recycled for 8 times without significant decrease in the catalytic *** mechanism analysis found that it is the boron radicals in h-BN activated H2O2 to generate·OH species,which can readily oxidize sulfides to corresponding sulfones for *** work would provide another choice in choosing metal-free catalysts for ODS.

关键词： Boron nitride Metal-free Oxidation Deep desulfurization Fuel oils

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 ***, 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

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