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Self-separation ionic liquid catalyst for the highly effective conversion of H_(2)S by α,β-unsaturated carboxylate esters under mild conditions

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Green Energy & Environment 2024年第9期9卷 1440-1448页

作者： Wenjie Xiong Xiaomin Zhang xingbang hu Youting Wu Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China The Institute of Green Chemistry and Engineering School of Chemistry and Chemical EngineeringNanjing UniversitySuzhouJiangsu215163China

The deep-processing utility of pure hydrogen sulfide (H_(2)S) is a significant direction in natural gas chemical ***,a brand-new strategy of H_(2)S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids (ILs) as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third *** can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H_(2)S to a,β-unsaturated carboxylate ***,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were ***,the proposed interaction mechanism of H_(2)S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical *** approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically ***-efficiency reaction activity can still be maintained after ten cycles of the ***,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and *** is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H_(2)S utilization,which will guide its application on an industrial scale.

关键词： Ionic liquid Cascade reaction Self-separation H_(2)S conversion Catalysis

A novel proton-gradient-transfer acid complexes as an efficient and reusable catalyst for fatty acid esterification

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Green Energy & Environment 2022年第1期7卷 137-144页

作者： Xiaomin Zhang Wenjie Xiong Zengyu Yin Yongle Chen Youting Wu xingbang hu Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China Yuxiu Postdoctoral Institute Nanjing UniversityNanjing210023China

In this work,a series of novel proton-gradient-transfer acid complexes(PGTACs)were *** physicochemical properties,including thermal stability,melting point,and Hammett acidity,were *** effects of catalyst loading,reaction temperature,and substrate expansion on the catalytic performance were systematically *** is found that the combination of bidentate N-heterocycle and H;SO;(1:2 M ratio)could form simultaneously N–H covalent bond and N…H hydrogen bond,which makes the PGTACs excellent catalysts integrate the advantages of strong acids(high catalytic activity)and ionic liquids(phase separation)in the esterification ***,these PGTACs can be reused by convenient phase separation without obvious diminution of catalytic *** is concluded that these PGTACs are potential alternative candidates for esterification reaction in the process of industrial catalysis.

关键词： Proton-gradient-transfer Hydrogen bond Catalysis Esterification Self-separation

Efficient conversion of H_(2)S into mercaptan alcohol by tertiary-amine functionalized ionic liquids

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Chinese Journal of Chemical Engineering 2022年第10期50卷 197-204页

作者： Wenjie Xiong Mingzhen Shi Yan Lu Xiaomin Zhang xingbang hu Zhuoheng Tu Youting Wu Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Institute of Green Chemistry and Engineering Nanjing UniversitySuzhou 215163China

The resource utilization of hydrogen sulfide(H_(2)S)is of great significance in natural gas chemical *** herein have developed a novel method mediated in tertiary amine-functionalized ionic liquids(ILs)to convert H_(2)S into mercaptan alcohols with *** effect of ILs,substra te scope,and regeneration experiments have been *** is found that the conversion of 3-methyl-2-buten-1-ol by H_(2)S can reach 52%with a 50%(mol)catalyst loading of bis(2-dimethylaminoethyl)ether methoxyacetate within 12 hat 90℃.The reaction mechanism was speculated based on theoretical ***,a plausible reaction-separation-integrated strategy was further *** work reveals an effective insight into the capture and catalytic conversion of H_(2)S to high valuable mercaptan alcohol,which makes the utilization method of H_(2)S resource universal and has the potentiality for industrial application.

关键词： Ionic liquids Reaction Catalysis Hydrogen sulfide DFT calculation

Facilitated transport separation of CO_(2) and H_(2)S by supported liquid membrane based on task-specific protic ionic liquids

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Green Chemical Engineering 2022年第3期3卷 259-266页

作者： Lingling Peng Mingzhen Shi Xiaomin Zhang Wenjie Xiong xingbang hu Zhuoheng Tu Youting Wu Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China Yuxiu Postdoctoral Institute Nanjing UniversityNanjing210023China

Selective separation of CO_(2) and H_(2)S from CH_(4) is of importance to the natural gas upgrading because of its cor-rosivity. As is well known, amine group can recognize reversibly CO_(2) and H_(2)S with a moderate interaction. Withthis in mind, this work prepared a series of amine-functionalized supported-protic-ionic-liquid membranes(SPILMs) for the selective separation of CO_(2) and H_(2)S from CH_(4) . For comparison, aprotic ionic liquid membranewas also prepared for natural gas sweetening. The effect of temperature and transmembrane pressure differenceon the permeability of single gas and ideal selectivity of CO_(2)/CH_(4) and H_(2)S/CO_(2) were studied. Facilitated transportmechanism was studied by NMR spectra. The permeability of CO_(2) in primary amine functionalized [DMPDAH][Tf_(2)N]-based membrane decreases with the increasing transmembrane pressure, indicating a typical feature offacilitated transport membrane. The permeability of CO_(2) and the ideal selective of CO_(2)/CH_(4) are as high as 2000 barrers and 53.2 at 313.2 K in [DMPDAH][Tf_(2)N] membrane, significantly higher than those in conventional ILsmembrane. It is anticipated that these amine-functionalized SPILMs can provide alternative insight for the se-lective separation of CO_(2) and H_(2)S from CH_(4) .

关键词： Ionic liquids Carbon dioxide Membrane separation Facilitated transport Natural gas sweentening

Effect of Neutral Axial Ligand on Iron (Ⅳ)-Oxo Porphyrin:A Theoretical Study

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Effect of Neutral Axial Ligand on Iron (Ⅳ)-Oxo Porphyrin:A ...

第十届全国计算(机)化学学术会议

作者： Yong Sun,xingbang hu,Haoran Li Department of Chemistry,Zhejiang University,Hangzhou 310027

Density functional theory calculations reveal that the ground state for iron(Ⅳ)-oxo porphyrin under study is triplet,with a spin density that is almost completely localized within the iron(Ⅳ)-oxo subunit. The main influence of the axial ligand on the iron(Ⅳ)-oxo is 3-fold:(i) the bound axial ligand weakens the Fe=O bond,which may favor the oxygen transfer in the oxidation process;(ii) the addition of axial ligand enlarges the energy gap between the two different spin states;(iii) the ground state of iron(Ⅳ)-oxo porphyrin with axial ligand has a spin density distribution of approximately 50/50 between the iron and oxygen atoms. Additionally,the more negative the N atom is,the more negative the O and Fe atoms of the iron(Ⅳ)-oxo porphyrin *** is also worth noting that the bound imidazoles make the Fe=O bond even longer than pyridines *** same trend can also be found for the effect on the energy gap between different spin states. However,for the same species of axial ligand,the influence on the iron(Ⅳ)-oxo porphyrin does not change a lot due to different substitute groups,unless there is a steric group inhibiting the *** instance, 2-methylpyridine has a less significant effect on the iron(Ⅳ)-oxo porphyrin than the other three pyridines do.

关键词： Axial-ligand effect Iron-Oxo porphyrin DFT

来源： cnki会议评论

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高速弓网系统载流磨损稳态

辽宁工程技术大学学报（自然科学版） 2013年第11期32卷 1513-1516页

作者：胡兴邦张建飞辽宁工程技术大学电气与控制工程学院辽宁葫芦岛125105

为考察弓网系统在高速大电流条件下的载流磨损现象,利用高速滑动电接触试验机开展浸金属碳滑板与铜导线的对磨实验,对不同速度、不同接触压力和接触电流下滑板的载流磨损行为进行研究.研究结果表明:在载流条件下,随着速度的增加,滑板与... 详细信息

为考察弓网系统在高速大电流条件下的载流磨损现象,利用高速滑动电接触试验机开展浸金属碳滑板与铜导线的对磨实验,对不同速度、不同接触压力和接触电流下滑板的载流磨损行为进行研究.研究结果表明:在载流条件下,随着速度的增加,滑板与导线的离线率增加,离线电弧和摩擦热也增加,而滑板的磨耗量却呈下降趋势.利用SSX-550型扫描电子显微镜对滑板的磨损形貌进行扫描分析,发现滑板表面呈现出特有的磨损形态,随着速度的增加,滑板表面形态相对比较光滑,磨损较少,这是一种稳定的磨损状态.滑板表面在高速运行时形成的稳定的载流磨损形态可以减小弓网系统的磨耗,有助于弓网系统的稳定运行.

关键词：弓网系统电接触载流磨损速度接触压力电流密度磨损量稳定态

MDEA-二元羧酸离子液体溶液吸收/解吸SO2性能

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化工学报 2014年第2期65卷 599-604页

作者：施丽娜陈茂兵黄宽胡兴邦吴有庭南京大学化学化工学院、分离工程研究中心江苏南京 210093

设计合成了三类N-甲基二乙醇胺(MDEA)-二元羧酸离子液体水溶液,研究了它们的物理性质和SO2吸收容量。结果表明:MDEA/有机酸的摩尔比及阴离子种类是影响吸收容量的主要原因。碱酸摩尔比越高,离子液体吸收能力越强,解吸能力越差且解吸时... 详细信息

设计合成了三类N-甲基二乙醇胺(MDEA)-二元羧酸离子液体水溶液,研究了它们的物理性质和SO2吸收容量。结果表明:MDEA/有机酸的摩尔比及阴离子种类是影响吸收容量的主要原因。碱酸摩尔比越高,离子液体吸收能力越强,解吸能力越差且解吸时间也越长。此外,不同阴离子的离子液体溶液吸收SO2的容量有如下关系:MDEA-丁二酸>MDEA-戊二酸>MDEA-苹果酸。对于MDEA-戊二酸和MDEA-苹果酸离子液体溶液,最具工业化应用前景的碱酸摩尔比分别为1.2:1和1.4:1。

关键词：离子液体脱硫吸收解吸二元羧酸

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环氧氯丙烷与离子液体的交联过程研究

化工学报 2020年第11期71卷 4971-4980页

作者：涂卓恒史名珍张效敏吴有庭胡兴邦南京大学化学化工学院江苏南京210023

鉴于目前离子液体交联反应所用交联剂存在的高成本、难制备的问题,提出以廉价易得的环氧氯丙烷交联二胺质子型离子液体制备离子液体凝胶的设想。基于此,通过监测反应体系动力学信息证明了反应的可能性,同时研究了与酸中和顺序、反应温... 详细信息

鉴于目前离子液体交联反应所用交联剂存在的高成本、难制备的问题,提出以廉价易得的环氧氯丙烷交联二胺质子型离子液体制备离子液体凝胶的设想。基于此,通过监测反应体系动力学信息证明了反应的可能性,同时研究了与酸中和顺序、反应温度、交联比例对环氧基团和氯基团转化率的影响。探究了环氧氯丙烷-二胺交联体系的凝胶转变性能以及可能的反应机理。并且初步测试了交联产物的CO2分离性能。

关键词：离子液体交联动力学膜碳捕集

基于X-12-ARIMA方法的武汉市空气污染指数波动分析

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环境污染与防治 2016年第2期38卷 19-22,28页

作者：俞艳胡兴帮任苏蕊童艳武汉理工大学资源与环境工程学院湖北武汉430070 华东师范大学地理科学学院上海201100

空气污染指数(API)用于表征区域空气污染程度和质量状况,其变动存在长期趋势、季节效应及随机扰动效应等特征。为探索API的波动规律,以武汉市2001—2012年API为例,进行X-12-ARIMA季节调整方法下的API演变趋势及内在规律探究。结果表明:... 详细信息

空气污染指数(API)用于表征区域空气污染程度和质量状况,其变动存在长期趋势、季节效应及随机扰动效应等特征。为探索API的波动规律,以武汉市2001—2012年API为例,进行X-12-ARIMA季节调整方法下的API演变趋势及内在规律探究。结果表明:在研究期内,武汉市API的变化受趋势成分的影响作用为85.2%;API月度及季节性变化显著;冬、春季节空气质量较差且变化不规则。最后,依据研究结果为武汉市空气环境质量的改善提出了建议。

关键词： X-12-ARIMA模型空气污染指数武汉市