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Synergistic and Antisynergistic Intracrystalline Diffusional Influences on Mixture Separations in Fixed-Bed Adsorbers

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Precision Chemistry 2023年第2期1卷 83-93页

作者： rajamani krishna Van’t Hoff Institute for Molecular Sciences University of Amsterdam Science Park9041098

Separations of mixtures in fixed-bed adsorbers are influenced by factors such as(1)selectivity of adsorption,Sads,(2)diffusional time constants,Đi/rc 2,and(3)diffusion selectivity,Đ1/Đ*** synergistic separations,intracrystalline diffusion of guest molecules serves to enhance the selectivities dictated by thermodynamics of mixture *** antisynergistic separations,intracrystalline diffusion serves to reverse the hierarchy of selectivities dictated by adsorption *** both scenarios,the productivities of the desired product in fixed-bed operations are crucially dependent on diffusional time constants,Đi/rc 2;these need to be sufficiently low in order for diffusional influences to be ***,the ratioĐ1/Đ2 should be large enough for manifestation of synergistic or antisynergistic *** synergistic and antisynergistic separations have two common,distinguishing ***,for transient uptake within crystals,the more mobile component attains supraequilibrium loadings during the initial stages of the *** overshoots,signifying uphill diffusion,are engendered by the cross-coefficientsΓij(i≠j)of thermodynamic correction ***,the component molar loadings,plotted in composition space,follow serpentine equilibration *** cross-coefficients are neglected,no overshoots in the loadings of the more mobile component are experienced,and the component loadings follow monotonous equilibration *** important takeaway message is that the modeling of mixture separations in fixed-bed adsorbers requires the use of the Maxwell−Stefan equations describing mixture diffusion employing chemical potential gradients as driving forces.

关键词： kinetic separations transient uptake microporous crystalline adsorbents Maxwell−Stefan equations thermodynamic coupling uphill diffusion transient breakthrough fixed-bed adsorber

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Commensurate stacking within confined ultramicropores boosting acetylene storage capacity and separation efficiency

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Nano Research 2023年第5期16卷 7742-7748页

作者： Zhenghui Huang Kungang Chai Chengjun Kang rajamani krishna Zhaoqiang Zhang Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology School of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore 117585Singapore Van’t Hoff Institute for Molecular Sciences University of AmsterdamPark 904Amsterdam 1098 XHThe Netherlands

Developing advanced porous materials possessing both a high storage capacity and selectivity for acetylene(C_(2)H_(2))remains challenging but a sought-after *** we show a strategy involving synergic combination of spatial confinement and commensurate stacking for enhanced C_(2)H_(2)storage and capture via maximizing the host–guest and guest–guest *** ultramicroporous metal-organic frameworks(MOFs),MIL-160 and MOF-303 are elaborately constructed to exhibit ultrahigh C_(2)H_(2)uptakes of 235 and 195 cm^(3)·g^(−1),respectively,due to the confinement effect of the suitable pore sizes and periodically dispersed molecular recognition ***,C_(2)H_(2)capacity of MIL-160 sets a new benchmark for C_(2)H_(2)*** exceptional separation performances of two materials for C_(2)H_(2)over both CO_(2)and ethylene(C_(2)H_(4)),which is rarely observed,outperform most of the benchmark materials for C_(2)H_(2)*** scrutinized the origins of ultrahigh C_(2)H_(2)loading in the confined channels via theoretical *** superior separation efficiency for C_(2)H_(2)/CO_(2)and C_(2)H_(2)/C_(2)H_(4)mixtures with unprecedented C_(2)H_(2)trapping capacity(>200 L·kg^(−1))was further demonstrated by dynamic breakthrough experiments.

关键词： adsorption and separation acetylene storage commensurate stacking gas cluster metal-organic frameworks

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Ultrafine tuning of the pore size in zeolite A for efficient propyne removal from propylene

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Chinese Journal of Chemical Engineering 2021年第9期34卷 217-221页

作者： Chaohui He rajamani krishna Yang Chen Jiangfeng Yang Jinping Li Libo Li College of Chemistry and Chemical Engineering Shanxi Key Laboratory of Gas Energy Efficient and Clean UtilizationTaiyuan University of TechnologyTaiyuan 030024China Van’t Hoff Institute for Molecular Sciences University of AmsterdamScience Park 9041098 XH Amsterdamthe Netherlands Key Laboratory of Coal Science and Technology Taiyuan University of TechnologyTaiyuan 030024China

The removal of trace propyne(C_(3)H_(4))from propyne/propylene(C_(3)H_(4)/C_(3)H_(6))mixtures is a technical and challenging task during the production of polymer-grade propylene in view of their very similar size and physical *** some progress has been made,it is still very challenging to use some highly stable and commercially available porous materials via an energy-efficient adsorptive separation ***,we report the ultrafine tuning of the pore apertures in type-A zeolites for the highly efficient removal of trace amounts of C_(3)H_(4)from C_(3)H_(4)/C_(3)H_(6)*** resulting ion-exchanged zeolite 5 A exhibits a large C_(3)H_(4)adsorption capacity(2.3 mmol g^(-1)under 10^(-4)MPa)and high C_(3)H_(4)/C_(3)H_(6)selectivity at room temperature,which were mainly attributed to the ultrafine-tuned pore size that selectively blocks C_(3)H_(6)molecules,while maintaining the stro ng adsorption of C_(3)H_(4)at low pressure *** purity of C_(3)H_(6)(>99.9999%)can be directly obtained on this material under ambient conditions,as demonstrated by the experimental breakthrough curves obtained for both 1/99 and 0.1/99.9(V V)C_(3)H_(4)/C_(3)H_(6) mixtures.

关键词： Type-A zeolite Ion-exchange Pore tuning Propyne/propylene separation Breakthrough experiments

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Th-MOF showing six-fold imide-sealed pockets for middle-sizeseparation of propane from natural gas

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Nano Research 2023年第2期16卷 3287-3293页

作者： Li Wang Wenhui Zhang Jie Ding Lele Gong rajamani krishna Youyuan Ran Lan Chen Feng Luo Jiangxi Province Key Laboratory of Synthetic Chemistry School of ChemistryBiology and Material ScienceEast China University of TechnologyNanchang 330013China Van’t Hoff Institute for Molecular Sciences University of AmsterdamScience Park 9041098 XH AmsterdamThe Netherlands

Separation of propane from natural gas is of great importance to ***,in light of size-based separation,there still lacks effective method to directly separate propane from natural gas,due to the comparable physical properties for these light alkanes(C1–C4)and the middle size of *** this work,we found that a new Th-metal-organic framework(MOF)could be an ideal solution for this *** Th-MOF takes UiO-66-type structure,but with the pocket sealed by six-fold imide groups;this not only precisely reduces the size of pocket to exactly match propane,but also enhances the host–guest interactions through multiple(C)H(^(δ+))∙∙∙(^(δ−))O(C)*** a result,highly selective adsorption of propane over methane,ethane,and butane was observed,implying unique middle-size *** actual separation was confirmed by breakthrough experiments of simulated natural gas,confirming its superior application in direct separation of propane from natural *** separation mechanism,as unveiled by both theoretical calculation and comparative experiments,is due to the six-fold imide-sealed pocket that could effectively distinguish propane from other light alkanes through both size effect and host–guest interactions.

关键词： Th-metal-organic framework(MOF) intermediate-size-separation natural gas selectivity

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Efficient capture of C_(2)H_(2)from CO_(2)and C_(n)H_(4)by a novel fluorinated anion pillared MOF with flexible molecular sieving effect

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Nano Research 2023年第2期16卷 3536-3541页

作者： Lingyao Wang Nuo Xu Yongqi Hu Wanqi Sun rajamani krishna Jiahao Li Yunjia Jiang Simon Duttwyler Yuanbin Zhang Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Life SciencesZhejiang Normal UniversityJinhua 321004China Van’t Hoff Institute for Molecular Sciences University of AmsterdamScience Park 904Amsterdam 1098 XHthe Netherlands Department of Chemistry Zhejiang UniversityHangzhou 310027China

The efficient separation of acetylene(C_(2)H_(2))from carbon dioxide(CO_(2))and CnH_(4)(n=1 and 2)to manufacture high purity C_(2)H_(2)and recover other light hydrocarbons is technologically important,while posing significant ***,we reported a new TiF62−anion(TIFSIX)pillared metal-organic framework(MOF)ZNU-5(ZNU=Zhejiang Normal University)with ultramicropores for highly selective C_(2)H_(2)capture with low adsorption heat through gate opening based molecular sieving ***-5 takes up a large amount of C_(2)H_(2)(128.6 cm^(3)/g)at 1.0 bar and 298 K but excludes CO_(2),CH_(4),and C_(2)H_(4).Such high capacity has never been realized in MOFs with molecular *** breakthrough experiments further confirmed the highly selective C_(2)H_(2)separation performance from multi-component gas mixtures.3.3,2.8,and 2.2 mmol/g of C_(2)H_(2)is captured at ZNU-5 from equimolar C_(2)H_(2)/CO_(2),C_(2)H_(2)/CO_(2)/CH_(4),and C_(2)H_(2)/CO_(2)/CH_(4)/C_(2)H_(4)mixtures,***,2.6,2.0,and 1.5 mmol/g of>98%purity C_(2)H_(2)can be recycled from the desorption *** high working capacity,low adsorption heat,as well as good recyclability,ZNU-5 is promising for C_(2)H_(2)purification.

关键词： metal-organic frameworks(MOFs) C_(2)H_(2)/CO_(2)separation acetylene recovery molecular sieving flexible MOFs

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Direct Ethylene Purification from Cracking Gas via a Metal–Organic Framework Through Pore Geometry Fitting

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Engineering 2024年第10期41卷 84-92页

作者： Yang Chen Zhenduo Wu Longlong Fan rajamani krishna Hongliang Huang Yi Wang Qizhao Xiong Jinping Li Libo Li College of Chemical Engineering and Technology Taiyuan University of TechnologyTaiyuan 030024China City University of Hong Kong(Dongguan) Dongguan 523000China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China Van’t Hoff Institute for Molecular Sciences University of AmsterdamAmsterdam 1098 XHNetherlands State Key Laboratory of Separation Membranes and Membrane Processes Tiangong UniversityTianjin 300387China Center for Neutron Scattering City University of Hong Kong Shenzhen Research InstituteShenzhen 518057China

The direct one-step separation of polymer-grade C_(2)H_(4) from complex light hydrocarbon mixtures has high industrial significance but is very ***,an ethylene-adsorption-weakening strategy is applied for precise regulation of the pore geometry of four tailor-made metal–organic frameworks(MOFs)with pillar-layered structures,dubbed TYUT-10/11/12/*** on its pore geometry design and functional group regulation,TYUT-12 exhibits exceptional selective adsorption selectivity toward C_(3)H_(8),C_(3)H_(6),C_(2)H_(6),C_(2)H_(2),and CO_(2) over C_(2)H_(4);its C_(2)H_(6)/C_(2)H_(4) adsorption selectivity reaches 4.56,surpassing the record value of 4.4 by Fe_(2)(O_(2))(dobdc)(dobdc^(4-)=2,5-dioxido-1,4-benzenedicarboxylate).The weak p–p stacking binding affinity toward C_(2)H_(4) in TYUT-12 is clearly demonstrated through a combination of neutron powder diffraction measurements and theoretical *** experiments demonstrate that C_(2)H_(4) can be directly obtained from binary,ternary,quaternary,and six-component light hydrocarbon mixtures with over 99.95%purity.

关键词： Metal-organic frameworks Pore regulation Adsorptive separation One-step purification C_(2)H_(4)purification

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Robust metal–organic framework with multiple traps for trace Xe/Kr separation

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Science Bulletin 2021年第11期66卷 1073-1079,M0003页

作者： Huiping Zhang Yaling Fan rajamani krishna Xuefeng Feng Li Wang Feng Luo School of Biology Chemistry and Material ScienceEast China University of TechnologyNanchang 344000China Van’t Hoff Institute for Molecular Sciences University of Amsterdam1098 XH Amsterdamthe Netherlands

Direct separation of Xe and Kr from air or used nuclear fuel(UNF)off-gas by means of porous adsorbents is of industrial importance but is a very challenging *** this work,we show a robust metal-organic framework(MOF),namely ECUT-60,which renders not only high chemical stability,but also unique structure with multiple *** leads to the ultrahigh Xe adsorption capacity,exceeding most reported porous ***,this MOF also enables high selectivity of Xe over Kr,CO2,O2,and N2,leading to the high-performance separation for trace quantitites of Xe/Kr from a simulated UNF reprocessing *** separation capability has been demonstrated by using dynamic breakthrough experiments,giving the record Xe uptake up to 70.4 mmol/kg and the production of 19.7 mmol/kg pure ***,ECUT-60 has promising potential in direct production of Xe from UNF off-gas or *** separation mechanism,as unveiled by theoretical calculation,is attributed to the multiple traps in ECUT-60 that affords rigid restrict for Xe atom via van der Waals force.

关键词： Xe/Kr separation MOFs UNF off-gas Multiple traps

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A[Th_(8)Co_(8)]Nanocage-Based Metal–Organic Framework with Extremely Narrow Window but Flexible Nature Enabling Dual-Sieving Effect for Both Isotope and Isomer Separation

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CCS Chemistry 2022年第3期4卷 1016-1027页

作者： Mengjia Yin rajamani krishna Wenjing Wang Daqiang Yuan Yaling Fan Xuefeng Feng Li Wang Feng Luo School of Chemistry Biology and Materials ScienceEast China University of TechnologyNanchang 330013 Van’t Hoff Institute for Molecular Sciences University of Amsterdam1098 XH Amsterdam State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002

The synthesis of nanoporous materials that display a combination of molecular sieving(MS)and quantum sieving(QS)effects is still a challenging *** this work,we have demonstrated the synthesis of a nanocaged metal–organic framework(MOF),ECUT-8,that has a dual-sieving ***-8 afforded H_(2)/D_(2) isotope separation due to its extremely narrow window size(3.0Å),resulting in ***,the framework flexibility of ECUT-8 was exploited for the separation of butane and hexane isomers due to its MS *** desirable features of ECUT-8 include high thermal,water,and chemical stability,making it suitable for practical ***,these results open up an avenue to design the effects of coexistence of multiple sieving in one material.

关键词： metal-organic framework molecular sieving effect quantum sieving effect gate-opening multiple sieving effects isotope separation isomer separation thorium-based cage

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利用ZIF-7材料的开门效应分离N2O和CO2混合气体的研究

利用ZIF-7材料的开门效应分离N2O和CO2混合气体的研究

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中国化学会第十二届全国量子化学会议

作者：陈德利王宁伟王芳芳谢建武钟依均朱伟东 rajamani krishna J.KarlJohnson 浙江师范大学物理化学研究所先进催化材料教育部重点实验室 Van’t hoff Institute for Molecular Science University of AmsterdamScience Park 9041098 XH AmsterdamThe Netherlands Department of Chemical and Petroleum Engineering University of Pittsburgh

N2O和CO2气体具有非常类似的物理性质,包括分子大小、四极距大小等,至今未有合适的材料能对其进行有效的分离。而这两种气体都是工业上己二酸和硝酸生产过程中的尾气。N2O的直接排放会对环境带来危害,它不但是一种重要的温室气体,更对...

N2O和CO2气体具有非常类似的物理性质,包括分子大小、四极距大小等,至今未有合适的材料能对其进行有效的分离。而这两种气体都是工业上己二酸和硝酸生产过程中的尾气。N2O的直接排放会对环境带来危害,它不但是一种重要的温室气体,更对臭氧层有破坏作用,因此对该气体的分离和捕获近年来越来越受到重视。本文中我们采用理论与实验结合的方法发现多孔材料ZIF-7（zeolite imidazolate framework）可用于对N2O/CO2混合气体进行有选择性的分离,并对其内在机理进行了详细的研究。两种气体的吸附等温线实验结果表明ZIF-7材料均具有开门效应,有趣的是,对应于N2O的开门压力（35千帕）要小于CO2的开门压力（50千帕）。我们采用了含色散校正的密度泛函理论（vd W-DF2）分别对两种气体分子在ZIF-7材料孔道的吸附位置和吸附强度进行了详细的计算,扫描得到了势能面。计算结果表明在孔道的最窄处N2O的吸附强度大于CO2,同时计算结果表明随着气体的吸附孔道会相应的增大,验证了ZIF-7材料的柔韧性和实验上表现出来的开门效应。我们对该混合气体还进行了穿透柱实验,结果证实了我们的想法,即该材料可用于对N2O/CO2混合气体进行有效分离,为工业上对N2O气体进行物理分离和提纯提供了很好的思路,具有重要的科学意义。

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通过孔隙几何拟合设计的金属有机框架从裂解气中直接提纯乙烯（英文）

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Engineering 2024年第10期 84-92页

作者： Yang Chen Zhenduo Wu Longlong Fan rajamani krishna Hongliang Huang Yi Wang Qizhao Xiong Jinping Li Libo Li College of Chemical Engineering and Technology Taiyuan University of Technology City University of Hong Kong (Dongguan) Center for Neutron Scattering City University of Hong Kong Shenzhen Research Institute Institute of High Energy Physics Chinese Academy of Sciences Van't Hoff Institute for Molecular Sciences University of Amsterdam State Key Laboratory of Separation Membranes and Membrane Processes Tiangong University

The direct one-step separation of polymer-grade C2H4from complex light hydrocarbon mixtures has high industrial significance but is very ***,an ethylene-adsorption-weakening strategy is applied for precise regulation of the pore geometry of four tailor-made metal-organic frameworks（MOFs） with pillar-layered structures,dubbed TYUT-10/11/12/*** on its pore geometry design and functional group regulation,TYUT-12 exhibits exceptional selective adsorption selectivity toward C3H8,C3H6,C2H6, C2H2,and CO2over C2H4;its C2H6/C2H4adsorption selectivity reaches 4.56,surpassing the record value of 4.4 by Fe2（O2）(dobdc)(dobdc4-=2,5-dioxido-1,4-benzenedicarboxylate).The weak π-π stacking binding affinity toward C2H4in TYUT-12 is clearly demonstrated through a combination of neutron powder diffraction measurements and theoretical *** experiments demonstrate that C2H4can be directly obtained from binary,ternary,quaternary,and six-component light hydrocarbon mixtures with over 99.95% purity.

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