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学者姓名：李坚
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Abstract ：
Cyclohexane (Cy), commonly produced by the catalytic hydrogenation of benzene (Bz), is used in large quantities as a solvent or feedstock for nylon polymers. Removing trace unreacted Bz from the Cy product is technically difficult due to their similar molecular structures and physical properties. Herein, we report that a metal-organic framework (MOF) adsorbent shows a molecular sieving effect for Bz and Cy with record-high Bz/Cy adsorption selectivities (216, 723, and 1027) in their liquid mixtures (v/v = 1:1, 1:10, and 1:20), and traps Bz molecules effectively even at low partial pressure in the vapor phase (e.g., 2.49 mmol/g at 8.2 Pa) or at low content in liquid-phase Cy (e.g., 128 mg/g at 20 ppm). Over 99% removal of trace Bz (1000 ppm) from liquid Cy could be achieved in one simple stripping step at room temperature using this sorbent, producing a Cy with >99.999% purity. Single-crystal structure analyses for guest-free and Bz-loaded phases of the MOF disclosed that a narrow slit-like pore aperture and the strong uniting of multiple weak host-guest and guest-guest interactions are the co-origin of its distinct adsorption property for Bz and Cy.
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| GB/T 7714 | Zhao, Rui-Chao , Xie, Lin-Hua , Liu, Xiao-Min et al. Removal of Trace Benzene from Cyclohexane Using a MOF Molecular Sieve [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 . |
| MLA | Zhao, Rui-Chao et al. "Removal of Trace Benzene from Cyclohexane Using a MOF Molecular Sieve" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2024) . |
| APA | Zhao, Rui-Chao , Xie, Lin-Hua , Liu, Xiao-Min , Liu, Zhe , Li, Xiang-Yu , Li, Jian-Rong . Removal of Trace Benzene from Cyclohexane Using a MOF Molecular Sieve . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 . |
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Abstract ：
Due to the unique photophysical and electrochemical properties of porphyrins, porphyrin-based metal-organic frameworks (PMOFs) offer an excellent platform for heterogeneous catalysis applications and the fundamental study of structure-property relationships based on their crystalline nature. In this study, we investigate the impact of porphyrin ligands with different substituents on the structural diversity of derived Zr(iv)-based PMOFs (Zr-PMOFs), with a particular emphasis on the advantage of a bifunctional pyridyl-carboxylate porphyrinic ligand in tuning the structure and catalysis performance of resultant PMOFs. Two highly stable and porous Zr-PMOFs (BUT-229 and -230) prepared from the bifunctional porphyrinic ligand have similar constituents but different structural topology due to their ligands adopting different conformations. Noteworthily, the catalytic performance of Zr-PMOFs could be profoundly affected by the conformation of their porphyrinic ligands, which determines not only the topology, porosity, and catalytically active center density of the PMOFs, but also their photoelectric properties, including visible-light absorption, bandgap, electron transfer and charge separation efficiency. As a rare example of PMOFs with the flu topology, BUT-229 afforded obviously higher catalytic activity than BUT-230 as well as some benchmark PMOFs in the photo-oxidation reaction of benzyl alcohol. Moreover, with Lewis base sites (free pyridyl N atoms) on pore surfaces, BUT-229 could efficiently catalyze the tandem reactions between aromatic alcohols and active methylene compounds under mild conditions. Its catalytic activity was further enhanced by partially appending covalently the cocatalyst TEMPO (TEMPO = 2,2,6,6-tetramethylpiperidinooxy) to the free pyridyl groups via the Zincke reaction. These results provide insights into the development of high-performance porphyrin-based catalysts for tandem organic reactions. High catalytic performance of porphyrin-based MOFs has been achieved by introducing multiple functionality into their ligands and modulating their conformation.
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| GB/T 7714 | Wu, Wei , Lv, Xiu-Liang , He, Tao et al. Boosting structural variety and catalytic activity of porphyrinic metal-organic frameworks by harnessing bifunctional ligands [J]. | INORGANIC CHEMISTRY FRONTIERS , 2024 , 11 (8) : 2281-2289 . |
| MLA | Wu, Wei et al. "Boosting structural variety and catalytic activity of porphyrinic metal-organic frameworks by harnessing bifunctional ligands" . | INORGANIC CHEMISTRY FRONTIERS 11 . 8 (2024) : 2281-2289 . |
| APA | Wu, Wei , Lv, Xiu-Liang , He, Tao , Si, Guang-Rui , Huang, Hongliang , Xie, Lin-Hua et al. Boosting structural variety and catalytic activity of porphyrinic metal-organic frameworks by harnessing bifunctional ligands . | INORGANIC CHEMISTRY FRONTIERS , 2024 , 11 (8) , 2281-2289 . |
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Abstract ：
Decades of research unveiled the unlimited potential of metal-organic frameworks (MOFs). Nevertheless, the hazardous and expensive production involving massive amounts of organic solvents has severely limited their widespread industrial adoption. Herein, the advantages of two eco-friendly strategies, base-assisted synthesis and modulated hydrothermal chemistry, were complementarily integrated, with the acetate anion introduced as a mild and efficacious modulator to regulate the coordination and tailor the crystallization pathway(s). The green, rapid, and scalable synthesis of a dual-ligand Zn-MOF was thereby achieved in water media, featuring an unprecedented space-time yield of 24 ton per m(3) per day and a batch size exceeding a kilogram (i.e., 1.2 kg). Owing to its strong affinity toward CH4, the acquired Zn-MOF demonstrated a considerable CH4/N-2 separation capacity under ambient conditions. This study not only facilitates the green and scalable production of MOFs but also offers a cost-effective adsorbent for CH4 recovery.
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| GB/T 7714 | Han, Zhang-Ye , Bai, Xuefeng , Zhao, Yan-Long et al. Green and scalable synthesis of a dual-ligand Zn-MOF with unprecedented space-time yield in aqueous media and efficient CH4/N2 separation [J]. | GREEN CHEMISTRY , 2024 , 26 (21) : 10867-10875 . |
| MLA | Han, Zhang-Ye et al. "Green and scalable synthesis of a dual-ligand Zn-MOF with unprecedented space-time yield in aqueous media and efficient CH4/N2 separation" . | GREEN CHEMISTRY 26 . 21 (2024) : 10867-10875 . |
| APA | Han, Zhang-Ye , Bai, Xuefeng , Zhao, Yan-Long , Li, Wen-Liang , Sun, Quanyou , Xie, Zheng-He et al. Green and scalable synthesis of a dual-ligand Zn-MOF with unprecedented space-time yield in aqueous media and efficient CH4/N2 separation . | GREEN CHEMISTRY , 2024 , 26 (21) , 10867-10875 . |
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Abstract ：
Designing an adsorbent that can simultaneously trap acetylene (C2H2) and ethane (C2H6) impurities for the one-step purification of ethylene (C2H4) remains a challenge. Herein, we constructed a novel Cu-based metal-organic framework (MOF), BUT-321, which exhibits the selective adsorption of C2H2 and C2H6 over C2H4. It was found that the high density of oxygen binding sites within the pore channels of BUT-321 can build an optimal environment for stronger interactions with C2H6, compared to the isostructural MOF BUT-320. Column breakthrough experiments confirm the exceptional C2H4 separation performance of BUT-321 from both binary (1:1 for C2H2/C2H4 or C2H6/C2H4) and ternary (1:1:1 for C2H2/C2H4/C2H6) gas mixtures in a single step. In addition, BUT-321 exhibits good chemical stability in water and an alkaline solution, combined with its synthesis scalability, economic viability, and recyclability, thus facilitating the application for the one-step C2H4 purification.
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| GB/T 7714 | Zhang, Peng-Dan , Wu, Xue-Qian , Shuai, Qi et al. Optimizing the Microenvironment of Pores in an MOF for Boosting Ethylene Purification from a Ternary-Component Mixture [J]. | ACS MATERIALS LETTERS , 2024 , 6 (10) : 4632-4638 . |
| MLA | Zhang, Peng-Dan et al. "Optimizing the Microenvironment of Pores in an MOF for Boosting Ethylene Purification from a Ternary-Component Mixture" . | ACS MATERIALS LETTERS 6 . 10 (2024) : 4632-4638 . |
| APA | Zhang, Peng-Dan , Wu, Xue-Qian , Shuai, Qi , Yu, Jiamei , Zhang, Xin , Li, Jian-Rong . Optimizing the Microenvironment of Pores in an MOF for Boosting Ethylene Purification from a Ternary-Component Mixture . | ACS MATERIALS LETTERS , 2024 , 6 (10) , 4632-4638 . |
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Abstract ：
The overuse of antibiotics poses a serious threat to human health and ecosystems. Therefore, the development of high-performance antibiotic removal materials has attracted increasing attention. However, the adsorption and removal of trace amounts of antibiotics in aqueous systems still face significant challenges. Taking tetracycline (TC) as a representative antibiotic and based on its structural characteristics, a series of TC adsorbents are prepared by grafting alkyl groups to the framework of MIL-101(Cr). The adsorptive capacity of the modified materials for tetracycline markedly surpasses that of MIL-101(Cr), with MIL-101-dod achieving the best adsorption performance. MIL-101-dod demonstrated an outstanding ability to adsorb tetracycline at low concentrations, where a 5.0 mg sample of MIL-101-dod can reduce the concentration of a 90 mL 5 ppm tetracycline solution to below 1 ppb, significantly superior to other sorbents. XPS and IR tests indicate that MIL-101-dod has multiple weak interactions with tetracycline molecules, including C & horbar;H & mldr;O and C & horbar;H & mldr;pi. This work provides theoretical and experimental support for the development of adsorbents for low-concentration antibiotics. A series of tetracycline adsorbents are prepared by grafting an alkyl group onto the MIL-101 skeleton. Among these, MIL-101-dod has the best adsorption capacity for low-concentration tetracycline, with 5.0 mg of MIL-101-dod capable of reducing the concentration of 90 mL 5 ppm tetracycline solution to below 1 ppb. This study provides theoretical and experimental support for the development of low-concentration antibiotic adsorbents. image
Keyword ：
MIL-101(Cr) MIL-101(Cr) pollutant adsorption pollutant adsorption metal-organic frameworks metal-organic frameworks postsynthetic modification postsynthetic modification tetracycline antibiotics tetracycline antibiotics
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| GB/T 7714 | Li, Yi , Peng, Haoxin , Li, Heming et al. Elimination of Trace Tetracycline with Alkyl Modified MIL-101 in Water [J]. | SMALL , 2024 , 20 (48) . |
| MLA | Li, Yi et al. "Elimination of Trace Tetracycline with Alkyl Modified MIL-101 in Water" . | SMALL 20 . 48 (2024) . |
| APA | Li, Yi , Peng, Haoxin , Li, Heming , Ma, Qianhui , Zhang, Xin , Chen, Qiang et al. Elimination of Trace Tetracycline with Alkyl Modified MIL-101 in Water . | SMALL , 2024 , 20 (48) . |
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Abstract ：
Adsorptive C2H2/C2H4 separation using metal-organic frameworks (MOFs) has emerged as a promising technology for the removal of C2H2 (acetylene) impurity (1 %) from C2H4 (ethylene). The practical application of these materials involves the optimization of separation performance as well as development of scalable and green production protocols. Herein, we report the efficient C2H2/C2H4 separation in a MOF, Cu(OH)INA (INA: isonicotinate) which achieves a record C2H2 packing density of 351 mg cm-3 at 0.01 bar through high affinity towards C2H2. DFT (density functional theory) calculations reveal the synergistic binding mechanism through pore confinement and the oxygen sites in pore wall. The weakly basic nature of binding sites leads to a relatively low heat of adsorption (Qst) of approximately 36 kJ/mol, which is beneficial for material regeneration and thermal management. Furthermore, a scalable and environmentally friendly synthesis protocol with a high space-time yield of 544 kg m-3 day-1 has been developed without using any modulating agents. This material also demonstrates enduring separation performance for multiple cycles, maintaining its efficacy after exposure to water or air for three months.
Keyword ：
ethylene ethylene green synthesis green synthesis packing density packing density metal-organic frameworks metal-organic frameworks acetylene removal acetylene removal
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| GB/T 7714 | Zhang, Xin , Chen, Qiancheng , Bai, Xuefeng et al. Achieving Record C2H2 Packing Density for Highly Efficient C2H2/C2H4 Separation with a Metal-Organic Framework Prepared by a Scalable Synthesis in Water [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (45) . |
| MLA | Zhang, Xin et al. "Achieving Record C2H2 Packing Density for Highly Efficient C2H2/C2H4 Separation with a Metal-Organic Framework Prepared by a Scalable Synthesis in Water" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 45 (2024) . |
| APA | Zhang, Xin , Chen, Qiancheng , Bai, Xuefeng , Zhao, Yan-Long , Li, Jian-Rong . Achieving Record C2H2 Packing Density for Highly Efficient C2H2/C2H4 Separation with a Metal-Organic Framework Prepared by a Scalable Synthesis in Water . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (45) . |
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Abstract ：
Tailoring a MOF with suitable pore windows for the sieving C3H6/C3H8 separation is attractive but challenging, where controlling the local framework flexibility by introducing functionality provides a solution. In this work, four isoreticular ultramicroporous Zn-triazolate-dicarboxylate frameworks, Zn-ATZ-IP(R) (R = -F, -OH, -NH2, and -CH3) (HATZ = 3-amino-1,2,4-triazole; H2IP-R = R group functionalized isophthalic acid) with variable pore apertures, were targeted as platforms to study the effect of functional groups on their separation performance. Single-component adsorption isotherms uncovered the potential of Zn-ATZ-IP(OH)-a with hydroxyl groups as a sieving adsorbent. Single X-ray diffraction (SXRD) measurements revealed that strong intraframework hydrogen bonds hinder the free torsion of ATZ(-) ligand in Zn-ATZ-IP(OH)-a, defining rigid pore windows that admit C3H6 while exclude C3H8, whereas other groups give adaptive larger pores that allow both C3H6 and C3H8 in. Further, in situ XRD measurements suggested that temperature alters the strength of hydrogen bonds, making Zn-ATZ-IP(OH)-a ideal for room-temperature sieving of C3H6/C3H8. This work highlights the superiority of customizing sieving pores sustained by hydrogen bonds, which advances the rational design of smart adsorbents for energy-efficient light hydrocarbon separations.
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| GB/T 7714 | Kong, Xiang-Jing , Xu, Ming-Ming , He, Tao et al. Hydrogen Bonds Defined Pore Windows Enable Sieving Separation of Propylene from Propane in an Ultramicroporous Metal-Organic Framework [J]. | CHEMISTRY OF MATERIALS , 2024 , 36 (21) : 10710-10719 . |
| MLA | Kong, Xiang-Jing et al. "Hydrogen Bonds Defined Pore Windows Enable Sieving Separation of Propylene from Propane in an Ultramicroporous Metal-Organic Framework" . | CHEMISTRY OF MATERIALS 36 . 21 (2024) : 10710-10719 . |
| APA | Kong, Xiang-Jing , Xu, Ming-Ming , He, Tao , Xie, Lin-Hua , Liu, Yu-Hui , Zhang, Xin et al. Hydrogen Bonds Defined Pore Windows Enable Sieving Separation of Propylene from Propane in an Ultramicroporous Metal-Organic Framework . | CHEMISTRY OF MATERIALS , 2024 , 36 (21) , 10710-10719 . |
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Abstract ：
Separation of natural products from their mixture of structurally similar compounds is an important process for drug development and application. Borneol is a natural product widely used in the treatment of the cardiovascular and cerebrovascular diseases, and its production always involve the challenging separation from the diastereomer isoborneol (about 50 %). Herein, elven types of metal-organic frameworks (MOFs) with diverse pore structure and functionalities (-F, -NH2, -SO3H, and -OH) are utilized to evaluate their borneol/isoborneol separation performance, as the first attempt to use MOFs for diastereomers separation. Among these MOFs, UiO66-F4 exhibits the best performance with the borneol/isoborneol selectivity of 2.23 and the maximum borneol adsorption capacity of 106.88 mg center dot g 1 at 298 K, owing to the efficient pore confinement of borneol molecule confirmed by molecular simulation. Subsequent column breakthrough experiment demonstrates good separation performance under dynamic conditions. After five-stage purification unit process, high-purity borneol (>96 %) can be obtained. Furthermore, good reusability and scale-up synthesis suggest a high potential of the UiO-66-F4 materials for practical application.
Keyword ：
Borneol purification Borneol purification Metal-organic frameworks (MOFs) Metal-organic frameworks (MOFs) Diastereomer Separation Diastereomer Separation
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| GB/T 7714 | Lu, Mu-Yao , Xie, Yabo , Huang, Hongliang et al. Purification of borneol from its isomeric mixture by using metal-organic frameworks [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 304 . |
| MLA | Lu, Mu-Yao et al. "Purification of borneol from its isomeric mixture by using metal-organic frameworks" . | SEPARATION AND PURIFICATION TECHNOLOGY 304 (2023) . |
| APA | Lu, Mu-Yao , Xie, Yabo , Huang, Hongliang , Zhao, Yan-Long , An, Hao-Tian , Zhang, Xin et al. Purification of borneol from its isomeric mixture by using metal-organic frameworks . | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 304 . |
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Currently, the elimination of gaseous pollutants-particularly nitrogen oxides-has emerged as a significant concern. Among various deNO(x) technologies, selective catalytic reduction (SCR) has gained prominence as the primary approach for NOx abatement, owing to its superior performance. In this study, novel low-temperature SCR catalysts were developed by regulating the pH value and doping cobalt based on a V2O5-MoO3/TiO2 (VMT) catalyst. The results show an increased SCR performance with 82.8% and 91.1% for catalysts after pH (=10) modification (VMT-10) and (1 wt%) Co/pH (=10) modification (1CoVMT-10), respectively. H-2-TPR, NH3-TPD, XPS and DRIFTS confirmed that the pH regulation transformed polymerization V species into isolated V5+=O, thus leading to an increase in the number of acid sites, which enhanced the NH3 and NO2 adsorption capacity. Furthermore, the DRIFTS study indicated that the NH3-SCR reaction over 1CoVMT-10 followed the E-R and L-H mechanism.
Keyword ：
modified catalyst modified catalyst low temperature low temperature cobalt doping cobalt doping pH regulation pH regulation selective catalyst reduction selective catalyst reduction
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| GB/T 7714 | Wang, Ruonan , Zhang, Yanli , Fan, Xing et al. Cobalt-/pH-Modified V2O5-MoO3/TiO2 Catalyst with Enhanced Activity for the Low-Temperature Selective Catalytic Reduction Process [J]. | CATALYSTS , 2023 , 13 (5) . |
| MLA | Wang, Ruonan et al. "Cobalt-/pH-Modified V2O5-MoO3/TiO2 Catalyst with Enhanced Activity for the Low-Temperature Selective Catalytic Reduction Process" . | CATALYSTS 13 . 5 (2023) . |
| APA | Wang, Ruonan , Zhang, Yanli , Fan, Xing , Li, Jian . Cobalt-/pH-Modified V2O5-MoO3/TiO2 Catalyst with Enhanced Activity for the Low-Temperature Selective Catalytic Reduction Process . | CATALYSTS , 2023 , 13 (5) . |
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Abstract ：
Biotrickling filters (BTFs) for volatile organic compounds (VOCs) have attracted tremendous research attention in the field of environmental engineering. However, the problem of clogging occurred during the long-term operation limits their practical applications. To alleviate the clogging, an integral polypropylene (PP) packing coated with polydimethylsiloxane (PDMS) was prepared, and in combination with fungus, its performance was investigated for toluene elimination. Two laboratory-scale BTFs were started at low toluene concentrations of 200-900 mg.m(-3). Subsequently, a series of experiments were conducted at toluene concentrations of 47-2906 mg.m(-3), with empty bed residence time (EBRT) values of 50 and 40 s. Toluene removal efficiency reached 100 % at the inlet toluene concentration of 296-560 mg.m(-3) for EBRT of 50 s. The maximum elimination capacity (EC) of 98 g.m(-3).h(-1) was obtained at an inlet toluene load of 117.67 g.m(-3).h(-1). Clogging was relieved by manual cleanup, and the BTFs were operated steadily for nearly 8 months. CO2 production was monitored during the whole operation, and toluene mineralization was evaluated simultaneously. Furthermore, the biofilm structure and microbial diversity were analyzed.
Keyword ：
Integral packing Integral packing Mineralization Mineralization Biotrickling filter Biotrickling filter Polydimethylsiloxane Polydimethylsiloxane Clogging Clogging
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| GB/T 7714 | Lv, Ruitong , Kang, Jia , Fan, Xing et al. Performance of integral polypropylene packing coated with polydimethylsiloxane in biotrickling filter for toluene elimination [J]. | PROCESS SAFETY AND ENVIRONMENTAL PROTECTION , 2023 , 169 : 199-211 . |
| MLA | Lv, Ruitong et al. "Performance of integral polypropylene packing coated with polydimethylsiloxane in biotrickling filter for toluene elimination" . | PROCESS SAFETY AND ENVIRONMENTAL PROTECTION 169 (2023) : 199-211 . |
| APA | Lv, Ruitong , Kang, Jia , Fan, Xing , Li, Jian . Performance of integral polypropylene packing coated with polydimethylsiloxane in biotrickling filter for toluene elimination . | PROCESS SAFETY AND ENVIRONMENTAL PROTECTION , 2023 , 169 , 199-211 . |
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