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Photo-switchable Cu^(+)sites in metal-organic frameworks for adsorptive desulfurization

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Nano Research 2023年第2期16卷 3333-3338页

作者： Yu-Yang Gu Guoliang Liu shi-chao qi Chen Gu Tao Yang Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Material(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

Photo-switchable metal-organic frameworks(PMOFs)as energy-saving adsorbents for tailorable guest capture show admirable potentials for various applications like adsorptive ***,the regulation behavior of most reported PMOFs is based on weak physical interaction,and it is highly desired to introduce specific active sites to satisfy the demand of higher adsorption capacity and ***,for the first time,we prepared the PMOFs,azobenzene-functionalized HKUST-1(HK-Azo),simultaneously decorated with Cu_(2)O active sites that possess strong interaction with guest *** toπ-complexation interaction of Cu^(+)with aromatic sulfur compounds,the obtained HK-Azo shows obviously higher adsorption capacity on benzothiophene compared with *** ultraviolet(UV)and visible irradiation,azobenzene moieties in the PMOFs can transform their configuration freely and *** trans/cis isomerization of azobenzene causes exposure/shelter of Cu_(2)O active sites,leading to controllable benzothiophene *** HK-Azo exhibits the change of benzothiophene uptake up to 29.7%upon trans and cis isomerization,which is obviously higher than HKUST-1 with negligible *** work may inspire the development of new adsorption process regulated by light for adsorptive desulfurization that is impossible to realize by conventional PMOFs.

关键词： Cu+active sites metal-organic frameworks photo-switchable property azobenzene adsorptive desulfurization

Photo-Responsive Carbon Capture over Metalloporphyrin-C_(60) Metal-Organic Frameworks via Charge-Transfer

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Research 2024年第3期2023卷 233-241页

作者： shi-chao qi Zhen Sun Zhi-Hui Yang Yun-Jie Zhao Jia-Xin Li Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China.

Great efforts have been devoted to the study of photo-responsive adsorption,but its current methodology largely depends on the well-defined photochromic units and their photo-driven molecular ***,a methodology to fabricate nondeforming photo-responsive sorbents is successfully *** C_(60)-fullerene doping in metalloporphyrin metal-organic frameworks(PCN-M,M=Fe,Co,or Ni)and intensively interacting with the metalloporphyrin sites,effective charge-transfer can be achieved over the metalloporphyrin-C_(60) architectures once excited by the light at 350 to 780 *** electron density distribution and the resultant adsorption activity are thus changed by excited states,which are also stable enough to meet the timescale of microscopic adsorption *** charge-transfer over Co(II)-porphyrin-C_(60) is proved to be more efficient than the Fe(II)-and Ni(II)-porphyrin-C_(60) sites,as well as than all the metalloporphyrin sites,so the CO_(2) adsorption capacity(CAC;at 0°C and 1 bar)over the C_(60)-doped PCN-Co can be largely improved from 2.05 mmol g^(−1) in the darkness to 2.69 mmol g−1 with light,increased by 31%,in contrast to photo-irresponsive CAC over all C_(60)-undoped PCN-M sorbents and only the photo-loss CAC over C_(60).

关键词： porphyrin adsorption excited

Implementing an“Impracticable”Copolymerization to Fabricate a Desired Polymer Precursor for N-doped Porous Carbons

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Engineering 2022年第9期16卷 154-161页

作者： shi-chao qi Xiao-Jie Lu Yin-Cong Lou Rui Zhou Ding-Ming Xue Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Material(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

It is common that a proof-of-concept of a desired reaction,which might generate materials with new functions or application potential,is eventually proved impracticable or commercially *** efforts have been made but wasted in searching for unknown reaction conditions in solvent environments because it was believed that the activity of reactants can be enhanced to facilitate reactions by dissolving them in ***,an abnormal case was discovered in this study.A desired copolymerization reaction between 1,3,5-tris(chloromethyl)-2,4,6-trimethylbenzene and melamine was confirmed to be impracticable under various solvent conditions;however,it was successfully implemented using a solvent-free *** first-principle calculations and molecular dynamics simulations,two decisive factors that the reaction in solvents cannot possess,namely the reaction equilibrium being pushed by the timely release of by-products and the confined thermal motions of the activated monomer molecules in the solid phase,were demonstrated to make the copolymerization successful in the solvent-free *** to the high aromaticity and azacyclo-content,the as-synthetic copolymer exhibited good application potential as a precursor to fabricate N-doped porous carbons with satisfactory carbon yields,ideal N contents,desired textural properties,and competitive CO_(2)capture abilities compared to other representative counterparts reported recently.

关键词： Solvent-free method Solvent effect Copolymerization N-doped porous carbon

An antiempirical strategy:sacrificing aromatic moieties in the polymer precursor for improving the properties of the derived N-doped porous carbons

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Green Chemical Engineering 2020年第1期1卷 70-76页

作者： shi-chao qi Ding-Ming Xue Guo-Xing Yu Rong-Rong Zhu Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Material(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing211816China

With the carbonization at an elevated temperature,high aromaticity of a precursor for porous carbons was traditionally thought to be crucial for the resultant perfect textural properties and ideal application performances of the porous ***,many efforts have been done to search or to artificially prepare the polymer precursors with higher aromaticity to generate more satisfying porous ***,an antiempirical case was found in this *** copolymerization between 1,3,5-tris(chloromethyl)-2,4,6-trimethylbenzene(TCM)and cyclohexane-1,4-diamine was successfully implemented to get a polymer code-named NUT-40,in which half of the ring structures are nonaromatic,while N-doped porous carbons(NDPCs)with better textural properties(e.g.,SBET=1363 m^(2)g^(-1)for NDPC-600)and competitive CO_(2)capture abilities(e.g.,CO_(2)capacity=4.3 mmol g^(-1)at 25℃and 1 bar for NDPC-600)were generated from the NUT-40,compared with the NDPC counterparts derived from the NUT-4 in a previous study(e.g.,SBET=958 m^(2)g^(-1)and CO_(2)capacity=3.8 mmol g^(-1)at 25℃and 1 bar for NDPC-600),in which TCM and ursol were employed as the monomers instead,and thus the ring structures in the NUT-4 was fully *** first-principle and molecular dynamics simulations,it was demonstrated that the embryo pore structure in the NUT-40 molecule can be more easily maintained during the carbonization than that of the NUT-4,which finally improves the surface area and porosity of the NUT-40 generated NDPCs.

关键词： Copolymer Aromaticity Pyrolysis Carbon capture N-doped porous carbon

Atomically dispersed calcium as solid strong base catalyst with high activity and stability

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Green Energy & Environment 2024年第10期9卷 1619-1626页

作者： Xiang-Bin Shao Zhi-Wei Xing Si-Yu Liu Ke-Xin Miao shi-chao qi Song-Song Peng Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech University30 South Puzhu RoadNanjing211816China

Solid strong base catalysts are highly attractive for diverse reactions owing to their advantages of neglectable corrosion,facile separation,and environmental ***,their widespread applications are impeded by basic components aggregation and low *** this work,we fabricate single calcium atoms on graphene(denoted as Ca1/G)by use of a redox strategy for the first time,producing solid strong base catalyst with high activity and *** precursor Ca(NO_(3))_(2)is first reduced to CaO at 400℃ by the support graphene,forming CaO/G with conventional basic sites,and the subsequent reduction at 850℃results in the generation of Ca1/G with atomically dispersed *** characterizations reveal that Ca single atoms are anchored on graphene in tetra-coordination(Ca-C_(2)-N_(2))where N is in situ doped from Ca(NO_(3))_(2).The atomically dispersed Ca,along with their anchoring on the support,endow Ca1/G with high activity and stability toward the transesterification reaction of ethylene carbonate with *** turnover frequency value reaches 128.0 h^(-1)on Ca1/G,which is much higher than the traditional counterpart CaO/G and various reported solid strong bases(2.9-46.2 h^(-1)).Moreover,the activity of Ca1/G is well maintained during 5 cycles,while 60%of activity is lost for the conventional analogue CaO/G due to the leaching of Ca.

关键词： Solid strong base Single Ca atoms Heterogeneous catalysts Transesterification Reaction

Graphene-anchored sodium single atoms:A highly active and stable catalyst for transesterification reaction

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Nano Research 2024年第6期17卷 4979-4985页

作者： Song-Song Peng Yao Nian Xing-Ru Song Xiang-Bin Shao Chen Gu Zhi-Wei Xing shi-chao qi Peng Tan You Han Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech University30 South Puzhu RoadNanjing 211816China School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Solid strong base catalysts have received considerable attention in various organic reactions due to their facile separation,neglectable corrosion,and environmental *** great progress has been made in the preparation of solid strong base catalysts,it is still challenging to avoid basic sites aggregation on support and active sites loss in reaction ***,we report a tandem redox strategy to prepare Na single atoms on graphene,producing a new kind of solid strong base catalyst(Na1/G).The base precursor NaNO_(3)was first reduced to Na2O by graphene(400℃)and successively to single atoms Na anchored on the graphene vacancies(800℃).Owing to the atomically dispersed of basicity,the resultant catalyst presents high activity toward the transesterification of methanol and ethylene carbonate to synthesize dimethyl carbonate(turnover frequency(TOF)value:125.7 h^(−1)),which is much better than the conventional counterpart Na2O/G and various reported solid strong bases(TOF:1.0-90.1 h^(−1)).Furthermore,thanks to the basicity anchored on graphene,the Na1/G catalyst shows excellent durability during *** work may provide a new direction for the development of solid strong base catalysts.

关键词： solid strong base catalyst basic sites redox graphene single Na atoms

Breathing Metal-Organic Polyhedra Controlled by Light for Carbon Dioxide Capture and Liberation

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CCS Chemistry 2021年第6期3卷 1659-1668页

作者： Yao Jiang Peng Tan shi-chao qi Chen Gu Song-Song Peng Fan Wu Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816

Metal-organic polyhedra(MOPs)have emerged as versatile platforms for artificial models of biological systems due to their discrete structure and modular ***,the design and fabrication of MOPs with special functionality for mimicking biological processes are *** by the breathing mechanism of lungs,we developed a new type of MOP(a breathing MOP,denoted as NUT-101)by directly using azobenzene units as the pillars of the polyhedra to coordinate with Zr-based metal *** addition to considerable thermal and chemical stability,the obtained MOP exhibits photocontrollable breathing *** irradiation with visible or UV light,the configuration of azobenzene units transforms,leading to reversible expansion or contraction of the cages and,correspondingly,capture or liberation of CO_(2)*** a breathing behavior of NUT-101 is further confirmed by density functional theory(DFT)*** system might establish an avenue for the construction of new materials with particular functionality that mimic biological processes.

关键词： metal-organic polyhedra breathing photoresponsive systems adsorbents carbon dioxide capture

Ce-Doped Smart Adsorbentswith Photoresponsive Molecular Switches for Selective Adsorption and Efficient Desorption

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Engineering 2020年第5期6卷 569-576页

作者： Peng Tan Yao Jiang shi-chao qi Xia-Jun Gao Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced MaterialsCollege of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

Achieving efficient adsorption and desorption processes by controllably tuning the properties of adsorbents at different technical stages is extremely ***,it is difficult for traditional adsorbents to reach the target because of their fixed active ***,we report on the fabrication of a smart adsorbent,which was achieved by introducing photoresponsive azobenzene derivatives with cis/trans isomers to Ce-doped mesoporous *** photoresponsive groups serve as “molecular switches”by sheltering and exposing active sites,leading to efficient adsorption and *** is also doped to provide additional active sites in order to enhance the adsorption *** results show that the cis isomers effectively shelter the active sites,leading to the selective adsorption of methylene blue(MB)over brilliant blue(BB),while the trans isomers completely expose the active sites,resulting in the convenient release of the *** selective adsorption and efficient desorption can be realized controllably by these smart adsorbents through ***,the performance of the obtained materials is well maintained after five cycles.

关键词： Azobenzene Ce-doped mesoporous silica Molecular switches Selective adsorption Efficient desorption

Smart adsorbents for CO2 capture:Making strong adsorption sites respond to visible light

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Science China Materials 2021年第2期64卷 383-392页

作者： qiu-Rong Wu Peng Tan Chen Gu Rui Zhou shi-chao qi Xiao-qin Liu Yao Jiang Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced MaterialsCollege of Chemical EngineeringNanjing Tech UniversityNanjing211816China

Due to the good controllability and high energy efficiency in adsorption processes,photoresponsive adsorbents are intriguing for CO2 ***,most reported photoresponsive adsorbents are designed based on weak adsorption sites,regulating CO2 adsorption through structural change or steric *** addition,ultraviolet(UV)light is commonly involved in the regulation of adsorption *** we report for the first time the smart adsorbents for CO2 capture,which makes strong adsorption sites respond to visible(Vis)*** adsorbents were fabricated by introducing primary amine and Dispersed Red 1(DR1,a kind of push-pull azobenzene that responds to Vis light rapidly)units to mesoporous silica,which act as strong adsorption sites and triggers,*** primary amine sites make the adsorbents highly selective in the adsorption of CO2 over *** light irradiation,azobenzene is in the form of trans configuration,which leads to decreased electrostatic potential of primary amines and subsequently,exposure of active sites and liberal adsorption of *** Vis-light irradiation,cis isomers are formed,which results in increased electrostatic potential of primary amines and subsequently shelter of active *** on such strong adsorption sites,the alteration of CO2 adsorption capacity can reach 40%for the adsorbent with and without Vis-light ***,the trans/cis isomerization of DR1 units can be triggered reversibly by Vis *** present smart system endows adsorbents with selective adsorption capacity and avoids the employment of UV light,which is unlikely to be achieved by conventional photoresponsive adsorbents.

关键词： CO2 adsorption strong adsorption sites selective adsorption push-pull azobenzene visible light response