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Boosting kinetic separation of ethylene and ethane on microporous materials via crystal size control

Chinese Journal of Chemical Engineering 2024年第1期65卷 85-91页

作者： Yixuan Ma Cong Yu Lifeng Yang Rimin You Yawen Bo Qihan Gong Huabin Xing xili cui Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310012China Fundamental Science&Advanced Technology Lab PetroChina Petrochemical Research InstituteChina National Petroleum CorporationBeijing 102200China ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang UniversityHangzhou 311200China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Hangzhou 310027China

The adsorptive separation of C_(2)H_(4)and C_(2)H_(6),as an alternative to distillation units consuming high energy,is a promising yet challenging research.The great similarity in the molecular size of C_(2)H_(4)and C_(2)H_(6)brings challenges to the regulation of adsorbents to realize efficient dynamic separation.Herein,we reported the enhancement of the kinetic separation of C_(2)H_(4)/C_(2)H_(6)by controlling the crystal size of ZnAtzPO_(4)(Atz=3-amino-1,2,4-triazole)to amplify the diffusion difference of C_(2)H_(4)and C_(2)H_(6).Through adjusting the synthesis temperature,reactant concentration,and ligands/metal ions molar ratio,ZnAtzPO4 crystals with different sizes were obtained.Both single-component kinetic adsorption tests and binary-component dynamic breakthrough experiments confirmed the enhancement of the dynamic separation of C_(2)H_(4)/C_(2)H_(6)with the increase in the crystal size of ZnAtzPO_(4).The separation selectivity of C_(2)H_(4)/C_(2)H_(6)increased from 1.3 to 98.5 with the increase in the crystal size of ZnAtzPO_(4).This work demonstrated the role of morphology and size control of adsorbent crystals in the improvement of the C_(2)H_(4)/C_(2)H_(6)kinetic separation performance.

关键词： Adsorption Adsorbent Ethylene Binary mixture Crystal size control Kinetic separation

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Porous framework materials for energy&environment relevant applications:A systematic review

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Green Energy & Environment 2024年第2期9卷 217-310页

作者： Yutao Liu Liyu Chen Lifeng Yang Tianhao Lan Hui Wang Chenghong Hu Xue Han Qixing Liu Jianfa Chen Zeming Feng xili cui Qianrong Fang Hailong Wang Libo Li Yingwei Li Huabin Xing Sihai Yang Dan Zhao Jinping Li College of Chemical Engineering and Technology Shanxi Key Laboratory of Gas Energy Efficient and Clean UtilizationTaiyuan University of TechnologyTaiyuan030024China School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou510640China Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China Department of Chemistry The University of ManchesterManchesterM139PLUK Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore 117585Singapore ZJU-Hangzhou Global Scientific and Technological Innovation Center Hangzhou311215China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin UniversityChangchun130012China Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of ChemistryUniversity of Science and Technology BeijingBeijing100083China

Carbon peaking and carbon neutralization trigger a technical revolution in energy&environment related fields.Development of new technologies for green energy production and storage,industrial energy saving and efficiency reinforcement,carbon capture,and pollutant gas treatment is in highly imperious demand.The emerging porous framework materials such as metal–organic frameworks(MOFs),covalent organic frameworks(COFs)and hydrogen-bonded organic frameworks(HOFs),owing to the permanent porosity,tremendous specific surface area,designable structure and customizable functionality,have shown great potential in major energy-consuming industrial processes,including sustainable energy gas catalytic conversion,energy-efficient industrial gas separation and storage.Herein,this manuscript presents a systematic review of porous framework materials for global and comprehensive energy&environment related applications,from a macroscopic and application perspective.

关键词： Porous framework materials Catalysis Separation Gas storage Carbon neutrality

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Efficient acetylene/carbon dioxide separation with excellent dynamic capacity and low regeneration energy by anion-pillared hybrid materials

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Frontiers of Chemical Science and Engineering 2022年第11期16卷 1616-1622页

作者： Yijian Li Jianbo Hu Jiyu cui Qingju Wang Huabin Xing xili cui Zhejiang Key Laboratory of Smart Biomaterials Key Laboratory of Biomass Chemical Engineering of Ministry of EducationCollege of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China ZJU-Hangzhou Global Scientific and Technological Innovation Center Hangzhou 311215China

Adsorptive separation of acetylene/carbon dioxide mixtures by porous materials is an important and challenging task due to their similar sizes and physical properties.Here,remarkable acetylene/carbon dioxide separation featuring a high dynamic breakthrough capacity for acetylene(4.3 mmol·g^(–1))as well as an ultralow acetylene regeneration energy(29.5 kJ·mol^(–1))was achieved with the novel TiF_(6)^(2–)-pillared material ZU-100(TIFSIX-bpy-Ni).Construction of a pore structure with abundant TiF_(6)^(2–)anion sites and pores with appropriate sizes enabled formation of acetylene clusters through hydrogen bonds and intermolecular interactions,which afforded a high acetylene capacity(8.3 mmol·g^(–1))and high acetylene/carbon dioxide uptake ratio(1.9)at 298 K and 1 bar.Moreover,the NbO_(5)^(2–)anion-pillared material ZU-61 investigated for separation of acetylene/carbon dioxide.In addition,breakthrough experiments were also conducted to further confirm the excellent dynamic acetylene/carbon dioxide separation performance of ZU-100.

关键词： acetylene carbon dioxide separation dynamic capacity anion-pillared hybrid material

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Efficient separation of C_(4) olefins using tantalum pentafluor oxide anion-pillared hybrid microporous material

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Chinese Journal of Chemical Engineering 2022年第2期35卷 49-54页

作者： Bin Gao Zhaoqiang Zhang Jianbo Hu Jiyu cui Liyuan Chen xili cui Huabin Xing Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Hangzhou Global Scientific and Technological Innovation Center Zhejiang UniversityHangzhou 311215China

With the increasing demand for synthetic rubber,the purification of 1,3-butadiene(C_(4)H_(6))is of great industrial significance.Herein,the successful removal of n-butene(n-C_(4)H_(8))and iso-butene(iso-C_(4)H_(8))from 1,3-butadiene(C_(4)H_(6))was realized by synthesizing a novel TaOF_(5)^(2-) anion-pillared ultramicroporous material TaOFFIVE-3-Ni(also referred to as ZU-96,TaOFFIVE=TaOF_(5)^(2-),3=pyrazine).Single-component adsorption isotherms show that TaOFFIVE-3-Ni can achieve the exclusion of n-C_(4)H_(8) and iso-C_(4)H_(8) in the low pressure region(0–30 kPa),and uptake C_(4)H_(6) with a high capacity of 92.78 cm^(3)·cm^(-3)(298 K and 100 kPa).The uptake ratio of C_(4)H_(6)/iso-C_(4)H_(8) on TaOFFIVE-3-Ni was 20.83(298 K and 100 kPa),which was the highest among the state-of-the-art adsorbents reported so far.With the rotation of anion and pyrazine ring,the pore size changes continuously,which makes smaller-size C_(4)H_(6) enter the channel while larger-size n-C_(4)H_(8) and iso-C_(4)H_(8) are completely blocked.The excellent breakthrough performance of TaOFFIVE-3-Ni shows great potential in industrial separation of C4 olefins.The specific adsorption binding sites within ZU-96 was further revealed through the modeling calculation.

关键词： Adsorptive separation C4 olefin 13-Butadiene Anion-pillared hybrid microporous material

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Efficient Splitting of Trans-/Cis-Olefins Using an Anion-Pillared Ultramicroporous Metal-Organic Framework with Guest-Adaptive Pore Channels

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Engineering 2022年第4期8卷 80-86页

作者： Zhaoqiang Zhang xili cui Xiaoming Jiang Qi Ding Jiyu cui Yuanbin Zhang Youssef Belmabkhout Karim Adil Mohamed Eddaoudi Huabin Xing Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Advanced Membranes and Porous Materials Center King Abdullah University of Science and TechnologyThuwal 23955Saudi Arabia

Trans-/cis-olefin isomers play a vital role in the petrochemical industry.The paucity of energy-efficient technologies for their splitting is mainly due to the similarities of their physicochemical properties.Herein,two new tailor-made anion-pillared ultramicroporous metal–organic frameworks(MOFs),ZU-36-Ni and ZU-36-Fe(GeFSIX-3-Ni and GeFSIX-3-Fe)are reported for the first time for the efficient trans-/cis-2-butene(trans-/cis-C_(4)H_(8))mixture splitting by enhanced molecular exclusion.Notably,ZU-36-Ni unexpectedly exhibited smart guest-adaptive pore channels for trapping trans-C_(4)H_(8)with a remarkable adsorption capacity(2.45 mmol∙g^(−1))while effectively rejecting cis-C_(4)H_(8)with a high purity of 99.99%.The dispersion-corrected density functional theory(DFT-D)calculation suggested that the guest-adaptive behavior of ZU-36-Ni in response to trans-C_(4)H_(8)is derived from the organic linker rotation and the optimal pore dimensions,which not only improve the favorable adsorption/diffusion of trans-C_(4)H_(8)with optimal host–guest interactions,but also enhance the size-exclusion of cis-C_(4)H_(8).This work opens a new avenue for pore engineering in advanced smart or adaptive porous materials for specific applications involving guest molecular recognition.

关键词： Adsorption and separation Trans-/cis-butene Ultramicroporous metal-organic frameworks Pore engineering Guest-adaptive

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羧酸端基Y型全氟聚醚的氟谱解析及结构表征

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化工学报 2024年第4期75卷 1718-1723页

作者：张文惠唐茹意崔希利邢华斌浙江大学化学工程与工业生物工程学院浙江杭州310027 浙江大学杭州国际科创中心浙江杭州311200

全氟聚醚及其衍生物(PFPEs)是一类高附加值的含氟聚合物,特异的理化性质使其具有较好的商业前景。目前国内相关产品严重依赖进口,对PFPEs的研究比较缺乏,尤其对Y型PFPEs的研究非常少,亟需加强对相关领域的开发和研究。核磁共振氟谱(^(19... 详细信息

全氟聚醚及其衍生物(PFPEs)是一类高附加值的含氟聚合物,特异的理化性质使其具有较好的商业前景。目前国内相关产品严重依赖进口,对PFPEs的研究比较缺乏,尤其对Y型PFPEs的研究非常少,亟需加强对相关领域的开发和研究。核磁共振氟谱(^(19)F NMR)是解析PFPEs结构的重要技术,但由于技术封锁、制备困难等原因,有关Y型PFPE羧酸(PFPE-CA)的^(19)F NMR谱图解析尚不完善。本研究采用合适的制样条件,得到了清晰的Y型PFPE-CA的^(19)F NMR谱图,并对主链和端基中不同化学环境的F原子化学位移进行归属。对谱峰进行积分可计算活性混合物的组成以及样品的数均分子量。该分析方法准确、快捷,可为Y型PFPEs的生产及分离技术的突破提供研究基础。

关键词：全氟聚醚羧酸 Y型结构解析聚合物电子材料

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Remarkable separation of C 5 olefins in anion-pillared hybrid porous materials

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Nano Research 2021年第2期14卷 541-545页

作者： Ying Yu Lifeng Yang Bin Tan Jianbo Hu Qingju Wang xili cui Huabin Xing Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China Ningxia Coal Industry Co. LtdCHN EnergyShizuishan 753200China

C5 olefin separation is of great importance and challenge in industry with the increasing demand for synthetic rubber.However,the related study is limited due to the complex compositions and the similar boiling points.Here,we for the first time employ two anionpillared hybrid porous materials(ZU-62 and TIFSIX-2-Cu-i)towards the challenging separation of C5 olefin mixtures(trans-2-pentene,1-pentene and isoprene).These two adsorbents not only exhibit the unprecedented separation performance,but also show excellent recycle performance.Owing to the favorable electrostatic environment within a suitable confined space,TIFSIX-2-Cu-i is able to distinguish the three C5 olefins(frans-2-pentene,1-pentene and isoprene)with a high uptake of trans-2-pentene(3.1mmgol·g^(-1))ZU-62(also termed as NbOFFIVE-2-Cu-i)with contracted aperture size shows exclusion effect to the relatively large molecule of isoprene at low pressure range(0-6 kPa),contributing to the excellent separation selectivity of 1-pentene/isoprene(300).The excellent separation performance of ZU-62 and TIFSIX-2-Cu-i is verified by the breakthrough experiment.And interestingly,the regeneration tests show that C5 olefins can be easily desorbed from ZU-62,TIFSIX-2-Cu-i under 298 K.Moreover,the detailed adsorption behavior is further revealed by simulation studies.

关键词： C5 olefin separation metal-organic frameworks adsorption

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二氧化碳直接空气捕集材料与技术研究进展

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化工进展 2022年第3期41卷 1152-1162页

作者：宋珂琛崔希利邢华斌浙江大学化学工程与生物工程学院浙江杭州310027 浙江大学杭州国际科创中心浙江杭州311200

直接空气捕集(DAC)等新兴负碳排放技术是实现“双碳”目标的托底技术保障,近年来受到广泛关注。本文简要分析了直接空气碳捕集技术的特性,归纳总结了胺功能化无机材料和聚合物、金属氢氧化物和碳酸盐、多孔材料等痕量二氧化碳捕集性能,... 详细信息

直接空气捕集(DAC)等新兴负碳排放技术是实现“双碳”目标的托底技术保障,近年来受到广泛关注。本文简要分析了直接空气碳捕集技术的特性,归纳总结了胺功能化无机材料和聚合物、金属氢氧化物和碳酸盐、多孔材料等痕量二氧化碳捕集性能,初步分析了负载方式、载体结构等与吸附容量和动力学的关系。浅析了该领域发展面临的问题和机遇,从能耗和性能方面对捕集材料和技术的研发提出以下建议:相较于物理吸附材料,胺功能化材料和固体碱等化学吸附材料具有更好的应用前景;在工艺开发领域,可以借鉴其他低浓度气体深度脱除工艺的经验;另一方面,可以结合不同工艺优势,设计多种工艺耦合的流程;最后,在严峻的环境问题下,必须加快材料研发的步伐,未来的研究重点应集中在材料的设计和低能耗再生方式的开发上。

关键词：二氧化碳直接空气捕集物理吸附化学吸附

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金属有机框架材料分离低碳烃的研究进展

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化工学报 2018年第6期69卷 2339-2352页

作者：崔希利邢华斌浙江大学化学工程与生物工程学院生物质化工教育部重点实验室浙江杭州310027

烯烃、烷烃和炔烃等结构相似物的高效分离是石油化学工业可持续发展的关键过程之一。低碳烃化合物结构和性质相近,仅在碳数和不饱和度存在微小差异,传统低温精馏过程选择性低、能耗高。金属有机框架材料/多孔配位聚合物(MOF/PCP)的结构... 详细信息

烯烃、烷烃和炔烃等结构相似物的高效分离是石油化学工业可持续发展的关键过程之一。低碳烃化合物结构和性质相近,仅在碳数和不饱和度存在微小差异,传统低温精馏过程选择性低、能耗高。金属有机框架材料/多孔配位聚合物(MOF/PCP)的结构多样性及可设计性使其可以精确识别相似物分子间的微小差异,在低碳烃分离领域取得重要进展。综述了金属有机框架材料在碳二/碳三的烯烃、炔烃和烷烃分离体系中取得的最新进展以及分离机理,探讨了金属有机框架材料在低碳烃吸附分离研究中存在的问题和发展方向。

关键词：低碳烃吸附分离烯烃烷烃炔烃金属有机框架材料

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阴离子功能化超交联离子多孔聚合物的构建及生物活性物质高效分离

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Science China Materials 2022年第4期65卷 1068-1075页

作者：锁显黄玉琦李侦糠潘罕骞崔希利邢华斌 Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China

多孔离子聚合物由于其独特的分子识别能力在高效分离中表现出巨大的潜力,但制备阴离子功能化离子聚合物用于结构高度相似生物活性物质分离仍然具有挑战.本文通过苄基咪唑离子液体与交联剂发生简易的Friedel-Crafts烷基化反应,报道了一... 详细信息

多孔离子聚合物由于其独特的分子识别能力在高效分离中表现出巨大的潜力,但制备阴离子功能化离子聚合物用于结构高度相似生物活性物质分离仍然具有挑战.本文通过苄基咪唑离子液体与交联剂发生简易的Friedel-Crafts烷基化反应,报道了一类具有强碱羧酸阴离子功能化、管状形貌和高热稳定性的超交联离子多孔聚合物(HIPs).实现了对结构高度相似的生物活性化合物的高容量(生育酚同系物:103.6 mg g^(−1))和高选择性(S_(βγ/α),4.26;S_(δ/α),3.19)吸附分离,其性能优于商业吸附剂、不含离子液体的超交联聚合物和含常规离子液体的HIPs.本研究展示了功能化吸附剂新的合成策略和合理的分子设计,为实现高效分离提供了新的机会.

关键词： anion-functionalization hypercrosslink porous ionic polymers adsorption tocopherol homologues phenolic compounds

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