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Highly dispersed Pd nanoparticles in situ reduced and stabilized by nitrogen-alkali lignin-doped phenolic nanospheres and their application in vanillin hydrodeoxygenation

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FRONTIERS OF CHEMICAL SCIENCE AND ENGINEERING 2024年第11期18卷 127-127页

作者： Gu, Xue Qin, yu Wei, Jiahui yuan, Bing yu, fengli Xin, Liantao Xie, Congxia yu, Shitao Qingdao Univ Sci & Technol Coll Chem & Mol Engn Coll Chem Engn State Key Lab Base Ecochem Engn Qingdao 266042 Peoples R China

Herein, we introduced a nitrogen-alkali lignin-doped phenolic resin (N@AL(n)PR) to produce palladium nanoparticles through an in situ reduction of palladium in an aqueous phase, without the need for additional reagents or a reducing atmosphere. The phenolic resin nanospheres and the resulting palladium nanoparticles were extensively characterized. Alkali lignin created a highly conducive environment for nitrogen incorporation, dispersion, reduction, and stabilization of palladium, leading to a distinct catalytic performance of palladium nanoparticles in vanillin hydrodeoxygenation. Under specific conditions of 1 mmol of vanillin, 40 mg of catalyst, 1 MPa H-2, 90 degrees C, and 3 h, the optimized Pd/N@AL(30)PR catalyst exhibited a nearly complete conversion of vanillin, 98.9% selectivity toward p-creosol, and good stability for multiple reuses. Consequently, an environmentally friendly lignin-based catalyst was developed and used for the efficient hydrodeoxygenation conversion of lignin-based platform compounds.

关键词： alkali lignin phenolic nanosphere palladium nanoparticles hydrodeoxygenation vanillin

Mild and Highly Selective Preparation of Alkylate Gasoline Promoted by Using Polyetheramine-Based Acidic Ionic Liquid

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China Petroleum Processing & Petrochemical Technology 2020年第2期22卷 64-70页

作者： Gao Xu yu fengli Wang Zhiping Xie Congxia State Key Laboratory Base of Eco-chemical Engineering College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao266042 College of Chemical Engineering Qingdao University of Science and TechnologyQingdao266042

A polyetheramine(PEA)-based Br?nsted-acidic ionic liquid(IL)was firstly prepared and used to promote the alkylation of isobutane with isobutene catalyzed by trifluoromethanesulfonic acid(TfOH).PEA-IL not only can resolve the persistent problem of poor solubility of the volatile and refractory reactants,but also can satisfactorily exhibit the separation of the catalyst from product oil for *** PEA-IL/TfOH catalytic system with an adjustable acidity ensures a high alkylate *** the conditions covering a VIL/VTfOH ratio of 10:3,a temperature of 25°C,and a reaction time of 25 min,the C8-product selectivity reaches 86.63%.The PEA-IL/TfOH catalyst can be reused 13 times without a decrease in the catalytic *** many operating cycles,the hydrophobic PEA-IL can be easily regenerated by simply adding *** study provides a green,economic,and highly efficient method for producing high-octane alkylate gasoline.

关键词： alkylation alkylate gasoline trifluoromethanesulfonic acid polyetheramine-based ionic liquid isobutene

Baeyer-Villiger Oxidation of Cyclic Ketones Catalyzed by Amino Acid Ionic Liquids

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Chemical Research in Chinese Universities 2020年第5期36卷 865-869页

作者： yu fengli CHI yujie GAO Chong CHEN Ruirui XIE Congxia yu Shitao State Key Laboratory Base of Eco-chemical Engineehng College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042P.R.China College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042P.R.China

A series of amino-acid-based ionic liquids was synthesized via one-step protonation of the corresponding L-amiiio acid by utilizing an array of proton *** catalytic activity of the amino-acid-based ionic liquids for the Baeyer-Villiger oxidation of cyclic ketones was investigated using cyclopentanone as a model ***-based ionic liquid[ProH]CF3SO3 was shown to exliibit thebest catalytic *** reaction condition was optimized to give the following reagent ratio of h(cyclopentanone):n(catalyst):w(H2O2)=1:0.06:4,60℃and 6 *** the optimum conditions,the conversion of cyclopentanone was 96.57%and the selectivity forδ-valerolactone was 73.01%.The catalytic activity was shown to be constant after 4 cycles.A simple treatment was allowed for the recover and the reuse of[ProH]*** successful utilization of[ProH]CF3SO3 to catalyze a host of cyclic ketones via Baeyer-Villiger oxidation clearly demonstrated the capacity of[ProH]CF3S03 to tolerate variation in the substrate.

关键词： Amino acid ionic liquid Baeyer-Villiger oxidation Cyclic ketone Lactone

Three-in-one LaNiO_(3) functionalized separator boosting electrochemical stability and redox kinetics for high-performance Li-S battery

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Journal of Energy Chemistry 2023年第7期82卷 581-591,I0013页

作者： Weiyu Wang Mingxiu Hou Fangqian Han Di yu Jie Liu Qian Zhang fengli yu Lei Wang Maoshuai He State Key Laboratory Base of Eco-chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Chemistry and Molecular Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Weifang Key Laboratory of Green Processing of Separator for Chemical Power Sources School of Chemistry and EngineeringWeifang Vocational CollegeWeifang 261108ShandongChina Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina

The lithium-sulfur(Li-S)battery,as one of the energy storage devices,has been in the limelight due to its high theoretical energy ***,the poor redox kinetics and the"shuttle effect"of polysulfides severely restrict the use of Li-S batteries in practical ***,a novel bimetallic LaNiO_(3) functional material with high electrical conductivity and catalytic property is prepared to act as a high-efficiency polysulfide shuttling *** three LaNiO_(3) samples with different physical/chemical characteristics are obtained by controlling the calcination *** conjunction with the high electrical conductivity and excellent catalytic properties of the as-prepared materials,the appropriate chemisorption toward polysulfides offers great potential to enhance electrochemical stability for highperformance Li-S ***,the Li-S cell with the separator modified by such functional material gives a specific capacity of 658 mA h g^(-1) after 500 cycles at a high current density of 2 *** with high sulfur loading of 6.05 mg cm^(-2),the Li-S battery still exhibits an areal specific capacity of 2.81 m A h cm^(-2)after 150 *** work paves a new avenue for the rational design of materials for separator modification in high-performance Li-S batteries.

关键词： Li-S battery Functional separator Catalytic property Electrochemical stability Redox kinetics

Synthesis and property of imidazolium oxidative-thermoregulated ionic liquids

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Chinese Science Bulletin 2014年第34期59卷 4705-4711页

作者： fengli yu Chunyu Liu Congxia Xie Bing yuan Tongan Bu Shitao yu State Key Laboratory Base of Eco-chemical Engineering College of Chemistry and Molecular Engineering Qingdao University of Science and Technology College of Chemical Engineering Qingdao University of Science and Technology

A series of novel imidazolium oxidative-thermoregulated bifunctional ionic liquids(ILs) have been synthesized by introducing the thermoregulated structural unit into imidazolium cation and using heteropolyanion as the anion of ILs. The structures of these new type of taskspecific ionic liquids(TSILs) are characterized by FT-IR and1 H NMR. The thermostability of ILs is analyzed by thermogravimetry. The thermoregulated properties of ILs in aqueous and organic solvents are mainly *** ILs have the corresponding cloud points(CPs) in aqueous. The effects of IL concentration, polymerization degree, inorganic additives and organic additives on the CP are studied. IL/DMF/n-heptane or n-octane biphasic system has the corresponding critical solution temperature(CST),and has the feature of ‘‘homogeneous at high temperature,heterogeneous at low temperature''. The effects of IL dosage and polymerization degree on the CST are ***/DMF/n-octane thermoregulated biphasic system has been successfully applied for catalytic oxidative desulfurization of model fuels. This study opens up a new way for catalytic oxidation to achieve an integration of homogeneous catalysis and heterogeneous separation.

关键词：催化氧化脱硫离子液体温控咪唑合成杂多阴离子财产结构单元

有机-无机型杂多酸相转移催化氧化脱硫性能研究

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化学学报 2014年第1期72卷 105-113页

作者：于凤丽王睿山东大学环境科学与工程学院济南250100

合成了四种有机-无机型杂多酸催化剂,包括[π-C5H5NC16H33]3[PW4O16],[π-C5H5NC16H33]3[PMo4O16],[π-C5H5NC12H25]3[PW4O16]和[π-C5H5NC12H25]3[PMo4O16].以有机硫的正辛烷溶液为模拟油品,H2O2为氧化剂,乙腈为萃取剂,在两相体系中,考察了上述四种催化剂对模拟油品中二苯并噻吩(DBT)氧化脱硫的催化活性.结果表明,[π-C5H5NC16H33]3[PW4O16]具有最佳的催化活性.采用[π-C5H5NC16H33]3[PW4O16]进行后续研究发现,反应完毕,[π-C5H5NC16H33]3[PW4O16]以沉淀的形式析出,可以重复利用且脱硫效果很好.研究表明,上述有机-无机型杂多酸属于相转移催化剂,氧化脱硫反应体系属于反应控制相转移催化体系.在相同实验条件下,由于电子云密度和空间位阻效应共同的作用,DBT、噻吩(TH)、苯并噻吩(BT)和4,6-二甲基二苯并噻吩(4,6-DMDBT)脱硫由易到难的顺序为DBT>4,6-DMDBT>BT>TH,并分别通过GC-MS分析确定它们的氧化产物.将[π-C5H5NC16H33]3[PW4O16]进一步应用于柴油氧化脱硫,其中硫含量由355 mg/kg(mg/kg等同于ppmw)降至26 mg/kg,去除率达92.7%.利用上述四种有机-无机型杂多酸作催化剂,研究DBT氧化反应过程动力学,确定DBT的表观反应级数均为一级,表观活化能为47.9~55.4kJ/mol.

关键词：有机硫氧化脱硫有机-无机型杂多酸相转移催化剂

氨基醇杂多酸类离子液体催化环酮的Baeyer-Villiger氧化反应

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高等学校化学学报 2020年第5期41卷 1101-1107页

作者：高崇于凤丽解从霞于世涛青岛科技大学化学与分子工程学院生态化工国家重点实验室培育基地青岛266042 青岛科技大学化工学院青岛266042

合成了一系列氨基醇杂多酸类离子液体,并将其用于催化环酮的Baeyer-Villiger氧化反应.以2-庚基环戊酮为模板底物,H2O2为氧化剂,探究了此类氨基醇杂多酸类离子液体的催化活性,筛选出催化活性最高的催化剂为[Pro-ps]H2PW12O40,最佳反应条... 详细信息

合成了一系列氨基醇杂多酸类离子液体,并将其用于催化环酮的Baeyer-Villiger氧化反应.以2-庚基环戊酮为模板底物,H2O2为氧化剂,探究了此类氨基醇杂多酸类离子液体的催化活性,筛选出催化活性最高的催化剂为[Pro-ps]H2PW12O40,最佳反应条件:n(2-庚基环戊酮)∶n(催化剂)∶n(H2O2)=1∶0.03∶4,反应温度40℃,反应时间8 h,无溶剂.在最佳条件下,2-庚基环戊酮的转化率为98.19%,产物δ-十二内酯的选择性可达82.84%.水相中的离子液体[Pro-ps]H2PW12O40经干燥后可以重复使用.经过5次循环使用后催化活性未见明显下降.[Pro-ps]H 2PW12O40还可用于催化其它多种环酮的Baeyer-Villiger氧化反应,结果表明,该催化剂具有良好的重复使用性和底物普适性.

关键词：氨基醇离子液体杂多酸 Baeyer-Villiger氧化环酮内酯

钒钼杂多酸盐相转移催化环戊烯氧化制备戊二醛

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有机化学 2023年第4期43卷 1444-1451页

作者：张旭征于凤丽袁冰解从霞于世涛青岛科技大学化工学院生态化工国家重点实验室培育基地青岛266042 青岛科技大学化学分子与工程学院青岛266042

设计合成了一系列含高价态钼、钒等金属的杂多酸类相转移催化剂,用于催化环戊烯(CPE)氧化制备戊二醛的反应,筛选出催化活性最优的咪唑基钼钒酸盐催化剂[C_(4)H_(9)N_(2)C_(3)H_(3)(CH_(3))]_(5)VMo_(7)O_(26),并对溶剂种类、H_(2)O_(2)... 详细信息

设计合成了一系列含高价态钼、钒等金属的杂多酸类相转移催化剂,用于催化环戊烯(CPE)氧化制备戊二醛的反应,筛选出催化活性最优的咪唑基钼钒酸盐催化剂[C_(4)H_(9)N_(2)C_(3)H_(3)(CH_(3))]_(5)VMo_(7)O_(26),并对溶剂种类、H_(2)O_(2)用量、催化剂用量、反应温度、时间等进行了条件优化.在优化的反应条件[V(乙酸乙酯)∶V(水)=4∶1,n(Cat.)∶n(H_(2)O_(2))∶n(CPE)=1∶170∶41.6,50℃,6 h]下,得到了88.7%的环戊烯转化率和62.1%的戊二醛选择性,并且催化剂在经过7次循环使用后仍能保持较高的催化活性.

关键词：过氧化氢环戊烯戊二醛相转移催化杂多酸离子液体

四聚型季铵类多金属氧酸盐相转移催化甲苯氧化合成苯甲醛

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高等学校化学学报 2024年第7期45卷 57-67页

作者：钱澍于凤丽顾雪袁冰解从霞于世涛青岛科技大学化学与分子工程学院生态化工国家重点实验室培育基地青岛266042 青岛科技大学化工学院青岛266042

甲苯氧化制备苯甲醛在工业应用中通常涉及有毒试剂或产生多种难以分离的副产物.本文采用乙二胺、环氧氯丙烷和N,N-二甲基丁基叔胺等作为初始原料,合成了四聚型季铵盐氯化物,然后与Keggin型钨钒磷杂多酸发生阴离子交换反应,制备了一系列... 详细信息

甲苯氧化制备苯甲醛在工业应用中通常涉及有毒试剂或产生多种难以分离的副产物.本文采用乙二胺、环氧氯丙烷和N,N-二甲基丁基叔胺等作为初始原料,合成了四聚型季铵盐氯化物,然后与Keggin型钨钒磷杂多酸发生阴离子交换反应,制备了一系列四聚型季胺类多金属氧酸盐;并通过在乙腈中使用H_(2)O_(2)(质量分数30%)将甲苯氧化为苯甲醛作为模型反应,评价了这些新型的多金属氧酸盐的催化性能.四核阳离子的引入不仅可以调节杂多阴离子的氧化还原性质,还可以使催化剂具有密集的协同催化活性位点.另外,优选出的催化剂具有良好的两亲性相转移催化能力,不仅显著提高了反应速率,而且实现了催化剂的简便回收和重复使用.在经过7次重复使用后,催化剂的性能几乎没有下降,并且实现了可接受的甲苯转化率(40%)和苯甲醛选择性(75%).本研究开发了一条与工业相关的碳氢化合物催化氧化的环境友好型工艺,为实际工业应用奠定了一定的理论基础.

关键词：甲苯氧化苯甲醛季铵盐两亲性相转移催化剂多金属氧酸盐