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Methyl functionalization of trimesic acid in copper-based metal-organic framework for ammonia colorimetric sensing at high relative humidity

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Chinese Chemical Letters 2024年第6期35卷 211-215页

作者： Yuxin Wang Zhengxuan Song Yutao liu Yang Chen Jinping li libo li Jia Yao College of Chemical Engineering and Technology Shanxi Key Laboratory of Gas Energy Efficient and Clean UtilizationTaiyuan University of TechnologyTaiyuan 030024China Department of Gastroenterology Shanxi Bethune HospitalShanxi Academy of Medical SciencesTongji Shanxi HospitalThird Hospital of Shanxi Medical UniversityTaiyuan 030024China

Exhaled ammonia(NH_(3))can be used as a crucial biomarker of kidney and liver ***,the high humidity in the detection conditions remains a challenge for accurate detection by gas ***,a copper-based metal-organic framework(CH_(3)-Cu-BTC)with methyl(CH_(3)^(-))functionalization of trimesic acid was synthesized for NH_(3) colorimetric *** CH_(3)-Cu-BTC exhibited a strong response for 5 ppm NH_(3) with high selectivity under high relative humidity(75%RH).Density functional theory(DFT)simulations indicated that the NH_(3) molecules interacted more strongly with CH_(3)-Cu-BTC than H_(2)O molecules did,and the corresponding color switching was attributed to the lone-pair electron in NH_(3) changing the coordination environment of Cu^(2+)ions,leading to an obviously visible color switching response from ruby green to *** on the tailor-made pore chemistry,the precise detection of trace amounts of NH_(3) in exhaled air was realized through functionalized MOF *** strategy used in this study not only offers a new pathway for the rapid detection of low concentration NH_(3) under humid conditions,but also shows a method for early respiration diagnosis of kidney and liver diseases.

关键词： Metal-organic framework Ammonia sensing Naked-eye color switching High humidity Respiration diagnosis

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 *** 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 *** 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 ***,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

Penalization schemes for BSDEs and reflected BSDEs with generalized driver

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Probability, Uncertainty and Quantitative Risk 2024年第3期9卷 301-338页

作者： libo li Ruyi liu Marek Rutkowski School of Mathematics and Statistics University of New South WalesSydneyNSW 2052Australia School of Mathematics and Statistics University of SydneySydneyNSW 2006Australia Faculty of Mathematics and Information Science Warsaw University of Technology00-661 WarszawaPoland

The paper is directly motivated by the pricing of vulnerable European and American options in a general hazard process setup and a related study of the corresponding pre-default backward stochastic differential equations(BSDE)and pre-default reflected backward stochastic differential equations(RBSDE).The goal of this work is ***,we aim to establish the well-posedness results and comparison theorems for a generalized BSDE and a reflected generalized BSDE with a continuous and nondecreasing driver ***,we study penalization schemes for a generalized BSDE and a reflected generalized BSDE in which we penalize against the driver in order to obtain in the limit either a constrained optimal stopping problem or a constrained Dynkin game in which the set of minimizer's admissible exercise times is constrained to the right support of the measure generated by A.

关键词： Generalized BSDEs Reflected generalized BSDEs Penalization scheme Constrained optimal stopping Constrained Dynkin game

基于多氮唑配体制备金属有机框架用于乙炔吸附分离

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科学通报 2024年第16期69卷 2278-2287页

作者：王恺华陈杨王毅陈久弘李晋平李立博太原理工大学化学工程与技术学院太原030024 气体能源高效清洁利用山西省重点实验室太原030024

电石法制备的乙炔(C_(2)H_(2))中会混入氮气、氧气和二氧化碳等杂质组分,为获得高纯度乙炔,相应的纯化分离研究十分必要.金属有机框架(metal organic framework,MOF)材料是一种具有超高孔隙率和易于功能化的多孔材料.基于特殊的孔腔特点... 详细信息

电石法制备的乙炔(C_(2)H_(2))中会混入氮气、氧气和二氧化碳等杂质组分,为获得高纯度乙炔,相应的纯化分离研究十分必要.金属有机框架(metal organic framework,MOF)材料是一种具有超高孔隙率和易于功能化的多孔材料.基于特殊的孔腔特点,该类材料在气体吸附分离领域展现出优异的性能.本研究以一水合乙酸铜和5-(4-吡啶基)-1H-四唑为原料,制备了一种新的MOF材料——Cu(Hptz),命名为TYUT-15.该材料基于特殊的方形孔腔结构和多氮吸附位点触发了孔中乙炔分子间的偶极矩协同吸附,在主客体的共同作用下极大地提高了乙炔的吸附容量.采用单晶X射线衍射、同步热重分析、单组分气体吸附及混合气体穿透测试等对样品的结构及气体吸附分离性能进行了表征.分离实验表明,该材料可以从C_(2)H_(2)/CO_(2)/N_(2)/O_(2)四组分混合气体中直接捕集C_(2)H_(2).

关键词：乙炔二氧化碳金属有机框架混合气体分离

多级孔MOF的制备及其吸附分离应用研究进展

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化工进展 2024年第4期43卷 1882-1896页

作者：杨东晓熊启钊王毅陈杨李立博李晋平太原理工大学化学工程与技术学院山西太原030024 气体能源高效清洁利用山西省重点实验室山西太原030024

金属有机框架材料(MOF)因其具有高比表面积、丰富孔隙率、孔径可调的优点,受诸多学者关注,被认为是用于吸附分离的理想吸附剂。但是在实际应用中,大部分微孔MOF材料在吸附过程中的内在传质速率严重受限,而且构建多级孔的方法一般不具有... 详细信息

金属有机框架材料(MOF)因其具有高比表面积、丰富孔隙率、孔径可调的优点,受诸多学者关注,被认为是用于吸附分离的理想吸附剂。但是在实际应用中,大部分微孔MOF材料在吸附过程中的内在传质速率严重受限,而且构建多级孔的方法一般不具有普遍性。本文介绍了调节剂策略、模板策略、后处理策略等构建多级孔MOF的方法,制备了兼具介孔、大孔的多级孔材料,并结合应用场景评价各方法的优缺点,以获得在相对温和条件下构建孔径可调的多级孔MOF的普适性策略。针对多级孔MOF材料在气体吸附分离领域的应用问题,着重剖析了构建多级孔MOF对CO_(2)气体吸附提升的案例,发现多级孔的构建增加了孔径,提高了MOF的比表面积,提供了额外的孔通道,使气体分子的吸附容量和传质速率得到提升,表明多级孔MOF在气体吸附分离方面有优异的性能。最后讨论了多级孔MOF合成和应用存在的问题,并对多级孔MOF面临的合成过程绿色可重复等挑战进行了展望。

关键词： MOF材料多级孔气体吸附分离传质速率

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CO_2/CH_4 and CH_4/N_2 separation on isomeric metal organic frameworks

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Chinese Journal of Chemical Engineering 2016年第12期24卷 1687-1694页

作者： Xiaoqing Wang libo li Jiangfeng Yang Jinping li Research Institute of special Chemicals Taiyuan University of Technology Taiyuan 030024 China

Two isomeric metal-organic frameworks(MOFs) with 2-dimensional(2D) and 3-dimensional(3D) topologies both comprised of Cu(Ⅱ) and OTf(OTf = trifluoromethanesulfonate) ions were synthesized and *** CO_2,CH_4 and N_2 adsorption properties of the two isomeric MOFs were investigated from 263 K to 298 K at0.1 *** results showed that the 2D MOF exhibited a higher selectivity for CO_2 from CO_2/CH_4 and CH_4from CH_4/N_2 compared to the 3D MOF,even though it possessed a lower surface area and pore *** higher adsorption heats of gases on the 2D MOF inferred the strong adsorption potential energy in the layered *** separation experiments using CO_2/CH_4 and CH_4/N_2 mixtures on the two MOFs proved that the2 D MOF had a longer elution time than the 3D MOF as well as better separation abilities.

关键词： Metal–organic frameworks Isomeric frameworks Adsorption Separation

Water’s motions in x–y and z directions of 2D nanochannels:Entirely different but tightly coupled

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Nano Research 2023年第5期16卷 6298-6307页

作者： Shouwei liao Qia Ke Yanying Wei libo li Guangdong Provincial Key Lab of Green Chemical Product Technology School of Chemistry&Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhou 510640China

Two-dimensional(2D)material-based membrane separation has attracted increasing attention due to its promising performance compared with traditional ***,in-depth understanding of water transportation behavior in such confined nanochannels is still lacking,which hinders the development of 2D nanosheets ***,we investigated water confined in graphene or MoS_(2)nanochannels by molecular dynamics(MD)simulations and found water’s diffusivity always varied linearly with their mean square displacement along z direction(Δz^(2))when system variables(e.g.,water molecules’number,channel height,nonbonded interaction parameter,harmonic potential constraining water’s z-coordinate)*** linear correlation applies to different water models and different force fields(FFs)of channel walls(e.g.,different Lennard–Jones parameters or even flexible FF),no matter whether water molecules form 3-,2-,or quasi-2-layer structure in the *** indicates,though water molecules’motion along z direction(z-fluctuation,confined within 1 nm)and that in xy plane(xydiffusion)are entirely different,they are tightly coupled:Violent z-fluctuation would produce more transient void to facilitate xydiffusion,which is to the sharp contrary of bulk water,where motions in x,y,z directions are symmetric,but *** work could help design high performance 2D nanochannels and discover more novel principles in nano-fluidics and membrane separation fields.

关键词： graphene membranes nanochannel nanofluidics water diffusion

Selective adsorption of propene over propane on li-decorated poly(triazine imide)

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Green Energy & Environment 2022年第2期7卷 307-313页

作者： Yong Wang Xiaoxia Jia libo li Jiangfeng Yang Jinping li College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan030024China Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization Taiyuan University of TechnologyTaiyuan030024China College of Chemistry and Chemical Engineering Taiyuan University of TechnologyTaiyuan030024China

Solid adsorbents that simultaneously have high selectivity and uptake capacity are highly promising as alternatives to conventional cryogenic distillation of propene/propane(C_(3)H_(6)/C_(3)H_(8)) *** unsaturated metal sites(CUS) plays a vital role in selective adsorption of olefins over *** poly(triazine imide)(PTI) nanosheets can reach rapid gas adsorption equilibrium,due to its large surface-tovolume *** this work,combining the advantages of the CUS and the PTI nanosheets,li CUSs were introduced into the PTI nanosheets for C_(3)H_(6)/C_(3)H_(8) *** functional theory(DFT) calculations demonstrated the thermodynamic feasibility of incorporating li CUSs into the PTI *** highly exposed li CUSs were predicted to have a higher adsorption affinity toward C_(3)H_(6) than C_(3)H_(8).Using the DFTderived force field parameters,we further performed grand canonical Monte Carlo(GCMC) simulations to investigate C_(3)H_(6)/C_(3)H_(8) adsorption on the li–PTI complexes slit pore model with different pore widths(H).We found that the li–PTI complexes display considerable C_(3)H_(6)/C_(3)H_(8) selectivity(4.2–7.9) under relevant ***,the li–PTI complexes slit pore have large C_(3)H_(6) working capacities(1.5–4.0 mmol g-1),superior to those calculated for the most of adsorbent materials that have been *** li–PTI complexes with slit pore architecture show potential as C_(3)H_(6)/C_(3)H_(8) separation materials.

关键词： materials adsorption complexes

Nitrogen rejection from low quality natural gas by pressure swing adsorption experiments and simulation using dynamic adsorption isotherms

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Chinese Journal of Chemical Engineering 2022年第2期35卷 120-129页

作者： Xinran Zhang Hua Shang Jiangfeng Yang libo li Jinping li Research Institute of Special Chemicals College of Chemistry and Chemical EngineeringTaiyuan University of TechnologyTaiyuan 030024China Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization Taiyuan 030024China

In order to remove N_(2) from low quality natural gas,a mathematical model has been established by Aspen adsorption,using the CH_(4)-selective sorbent silicalite-1 *** dynamic adsorption isotherm was first simulated by breakthrough simulation of a CH_(4)/N_(2) mixture at different adsorption pressures and feed flow rates based on breakthrough *** resulting simulated CH_(4) dynamic adsorption amounts were very close to the experimental data at three different adsorption pressures(100,200,and 300 kPa).Moreover,a single-bed,three-step pressure swing adsorption(PSA)experiment was performed,and the results were in good agreement with the simulated data,further corroborating the accuracy of the gas dynamic adsorption isotherm obtained by the simulation ***,based on the simulated dynamic adsorption isotherm of CH_(4) and N_(2),a four-bed,eight-step PSA process has been designed,which enriched 75%(vol)CH_(4) and 80%(vol)CH_(4) to 95%(vol)and 99%(vol),and provided 99%(vol)recovery.

关键词： Natural gas Silicalite-1 Simulation Dynamic adsorption Pressure swing adsorption process