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Special issue on “Green chemical process and intensification”

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Frontiers of Chemical Science and Engineering 2022年第11期16卷 1533-1535页

作者： You Han Xiang Ma lin-bing sun Jianhong Xu School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China Key Laboratory for Advanced Materials and Institute of Fine Chemicals School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Material(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China The State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

In order to better unite and lead young chemical engineering scholars,the Chemical Industry and Engineering Society of China will establish Youth Working *** the time of the establishment of Youth Working Committee,we were invited as guest editors to organize the special issue of Frontiers of Chemical Science and Engineering on green chemical process and intensification,aiming to inspire the innovative ideas and build an energetic and academic communication platform for young scholars.

关键词： intensification process chemical

Fabrication of bimetallic Cu–Zn adsorbents with high dispersion by using confined space for gas adsorptive separation

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Frontiers of Chemical Science and Engineering 2022年第11期16卷 1623-1631页

作者： Yu-Chao Wang Tian-Tian Li Li Huang 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

The number of active components and their dispersion degree are two key factors affecting the performance of ***,we report a simple but efficient strategy for dispersing active components by using a confined space,which is formed by mesoporous silica walls and templates in the as-prepared SBA-15(AS).Such a confined space does not exist in the conventional support,calcined SBA-15,which does not contain a *** Cu and Zn precursors were introduced to the confined space in the AS and were converted to CuO and ZnO during calcination,during which the template was also *** results show that up to 5 mmol·g^(–1) of CuO and ZnO can be well dispersed;however,severe aggregation of both oxides takes place in the sample derived from the calcined SBA-15 with the same *** space in the AS and the strong interactions caused by the abundant hydroxyl groups are responsible for the dispersion of CuO and *** bimetallic materials were employed for the adsorptive separation of propene and *** samples prepared from the as-prepared SBA-15 showed superior performance to their counterparts from the calcined SBA-15 in terms of both adsorption capacity of propene and selectivity for propene/propane.

关键词： bimetallic adsorbents confined space mesoporous silica propene propane separation

Fabrication of Cu^(+) sites in confined spaces for adsorptive desulfurization by series connection double-solvent strategy

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Green Energy & Environment 2022年第2期7卷 345-351页

作者： Shu Shi Yu-Xia Li Shuai-Shuai 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 University30 South Puzhu RoadNanjing 211816China

Cu^(+)-containing materials have shown various application prospects especially in adsorption and catalysis,because they are versatile,nontoxic and low *** date,developing a mild and controllable approach for the fabrication of Cu^(+) sites has remained a pronounced ***,we report a series connection double-solvent strategy(SCDS) for fabricating Cu^(+)sites within MIL-101(Cr),a typical metal–organic *** employing the SCDS in which vitamin C is chosen as the environmentally benign reducing agent,Cu^(2+) was incorporated in the pores and then transformed to Cu^(+) in the confined *** to the conventional high-temperature autoreduction method conducted under harsh environment(700°C for 12 h) with a low Cu^(+) yield(less than 50%),SCDS can selectively reduce Cu^(2+)to Cu^(+) at room temperature without generating any *** resulting Cu^(+)modified MIL-101(Cr) exhibits good desulfurization performance in view of both uptake and recyclability.

关键词： confined double generating

Low-energy-consumption temperature swing system for CO_(2) capture by combining passive radiative cooling and solar heating

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Green Energy & Environment 2024年第3期9卷 507-515页

作者： Ying-Xi Dang Peng Tan Bin Hu Chen Gu 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 UniversityNanjing211816China

Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is ***,we report a low-energy-consumption system by combining passive radiative cooling and solar heating for the uptake of CO_(2) on commercial activated carbons(CACs).During adsorption,the adsorbents are coated with a layer of hierarchically porous poly(vinylidene fluoride-co-hexafluoropropene)[P(VdF-HFP)HP],which cools the adsorbents to a low temperature under sunlight through radiative *** desorption,CACs with broad absorption of the solar spectrum are exposed to light irradiation for *** heating and cooling processes are completely driven by solar *** tests under mimicked sunlight using the CACs show that the performance of this system is comparable to that of the traditional ***,under real sunlight irradiation,the adsorption capacity of the CACs can be well maintained after multiple *** present work may inspire the development of new temperature swing procedures with little energy consumption.

关键词： CO_(2)capture Solar heating Passive radiative cooling Temperature swing adsorption

Fabrication of azobenzene-functionalized porous polymers for selective CO_(2) capture

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Chinese Journal of Chemical Engineering 2022年第3期35卷 24-30页

作者： Ding-Ming Xue Wen-Juan Zhang Xiao-Qin Liu Shi-Chao Qi 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

Many solid adsorbents have been prepared for the CO_(2)*** particular,the photoresponsive adsorbents have attracted extensive interests because of their tunable pore structure and variable responsive behaviors provoked by the external ***,it is challenging to fabricate the photoresponsive adsorbents featured the big CO_(2)capacity and high CO_(2)***,copolymerized between 4-phenylazobenzoyl chloride,2,4,6-trichloro-1,3,5-triazine and melamine,a series of azobenzenefunctionalized porous polymers(PTM-AZOs)are successfully *** PTM-AZOs are verified in possession of proper pore structures,large surface area and photoconductive properties through a series of *** PTM-AZO-2 with the trans-isomerization exhibits the best CO_(2)adsorption amount of 2.7 mmol·g^(-1)(273 K and 0.1 MPa),while the CO_(2)/N_(2)selectivity can reach 2459 and 607 on the trans-and cis-isomerization,*** regulatable pore structures controlled by the photoresponsive azobenzene groups affect the CO_(2)capture performance of the PTM-AZOs.

关键词： Adsorption CO_(2)capture Selectivity Azobenzene Photoresponse

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

Enhancing photoresponsiveness of metal-organic polyhedra by modifying microenvironment

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Nano Research 2024年第6期17卷 5712-5717页

作者： Long Zheng Peng Tan Qian Song Sheng-Tao Wang Min 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

Photoresponsiveness of materials is critical to their tunability and efficiency in terminal *** metal-organic polyhedra(PMOPs)feature intrinsic pores and remote controllability,but aggregation of PMOPs in solid state hampers their photoresponsiveness ***,we report the construction of a new PMOP(Cu_(24)(C_(16)H_(12)N_(2)O_(4))_(12)(C_(18)H_(22)O_(5))12,denoted as MOP-PR-LA),where long alkyl(LA)chains act as the intermolecular poles,propping against adjacent PMOP molecules to create individual microenvironment benefiting the isomerization of photoresponsive(PR)*** ultraviolet(UV)-and visible-light irradiation,MOP-PR-LA is much easier to isomerize than the counterpart MOP-PR without *** propylene adsorption,MOP-PR has a low change of adsorption capacity(9.9%),while that of MOP-PR-LA reaches 58.6%.Density functional theory calculations revealed that PR in the cis state has a negative effect on adsorption,while the trans state of PR favors *** work might open an avenue for the construction of photoresponsive materials with high responsiveness and controllability.

关键词： photoresponsive adsorption metal-organic polyhedra azobenzene long alkyl chains propylene capture

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

Rational fabrication of ordered porous solid strong bases by utilizing the inherent reducibility of metal-organic frameworks

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Nano Research 2022年第4期15卷 2905-2912页

作者： Song-Song Peng Xiang-Bin Shao Yu-Xia Li Yao Jiang Chen Gu Manish Kumar Dinker 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

Ordered porous solid strong bases(OPSSBs)have attracted great research interest due to the excellent performance as heterogeneous catalysts in various *** main obstacle for fabricating OPSSBs is the requirement of high temperature to produce strong basicity on ordered porous *** example,the temperatures of 600-650℃ are required for the decomposition of base precursor NaNO_(3)to basic sites on mesoporous silica SBA-15 and zeolite *** high decomposition temperatures are energy-intensive and harmful to the structure of ***,we report the fabrication of OPSSBs by utilizing the redox interaction between base precursor and low-valence metal centers(e.g.,Cr^(3+))in metal-organic frameworks(MOFs).The base precursor NaNO_(3)on MIL-101(Cr)can be converted to basic sites entirely at 300℃,which is quite lower than those of the conventional thermal conversion on SBA-15 and zeolite Y(600-650℃).The exploration on decomposition mechanism reveals that the valence change of Cr^(3+)to Cr^(6+)takes place during the conversion of NaNO_(3)to basic *** this way,MOFs-derived base catalysts have been synthesized successfully by the host-guest redox strategy and exhibit high catalytic activity in typical base-catalyzed reactions.

关键词： metal-organic frameworks ordered porous solid strong bases host–guest redox interaction transesterification reaction Cr centers