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学者姓名：李坚
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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 . |
| MLA | Li, Yi et al. "Elimination of Trace Tetracycline with Alkyl Modified MIL-101 in Water" . | SMALL (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 . |
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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 . |
| 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 (2024) . |
| 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 . |
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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 ：
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 ：
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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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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Abstract ：
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 ：
The illegal usage of antibiotics as veterinary drugs is an increasing threat for human health. The specific sensing of antibiotics with different toxicity levels is of high challenge, and mainly relies on expensive, time-consuming, and complex instruments. To realize specific sensing by rapid and handy optical sensors, a metal-organic framework (MOF) based dual sensor system is herein developed using two MOF materials BUT-128 and BUT-129 with high sensing selectivity and sensitivity. BUT-128 and BUT-129 exhibit the lowest limit of detection (LOD) towards chloramphenicol and furazolidone among reported MOF sensors. The corresponding dual sensor system with enriched signal readouts realized specific sensing of the strictly forbidden antibiotics (chloramphenicol and nitrofurans) from other regulated veterinary drugs including thiamphenicol, a structural analog of chloramphenicol. Besides, the strategy of this work is expected to flourish the development of optical sensors with high specificity for environment and food safety purposes.
Keyword ：
dual sensor dual sensor metal-organic frameworks metal-organic frameworks fluorescence quenching fluorescence quenching antibiotics antibiotics specific sensing specific sensing
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| GB/T 7714 | Zhao, Yan-Long , Chen, Qiang , Lv, Jie et al. Specific sensing of antibiotics with metal-organic frameworks based dual sensor system [J]. | NANO RESEARCH , 2022 , 15 (7) : 6430-6437 . |
| MLA | Zhao, Yan-Long et al. "Specific sensing of antibiotics with metal-organic frameworks based dual sensor system" . | NANO RESEARCH 15 . 7 (2022) : 6430-6437 . |
| APA | Zhao, Yan-Long , Chen, Qiang , Lv, Jie , Xu, Ming-Ming , Zhang, Xin , Li, Jian-Rong . Specific sensing of antibiotics with metal-organic frameworks based dual sensor system . | NANO RESEARCH , 2022 , 15 (7) , 6430-6437 . |
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Abstract ：
With the guidance of the hard/soft acid/base principle, we adopt a strategy to construct a novel robust metal-organic framework (MOF) by using a dual-functional ligand to coordinate with different types of metal ions in a onepot reaction through coordination self-selection. A bimetallic MOF, namely BUT-85 (BUT = Beijing University of Technology), has been successfully synthesized with a rationally designed pyrazolate-carboxylate ligand. Its robust [Ni-2(OH)(H2O)(2)Pz(3)],, chain (Pz = pyrazolate) with bridging OH-/H2O and pyrazolate groups is reported for the first time. This material shows good chemical stability in water and aqueous solutions with a pH range from 3 to 13. In addition, BUT-85 exhibits preferential adsorption behavior of C2H2 over CO2. It is proposed to be attributed to the abundant exposed bridging OH-/H2O sites in [Ni-2(OH)(H2O)(2)Pz(3)],, chains, which is supported by the results of molecular simulations. Column breakthrough experiments further confirm that this MOF can realize efficient C2H2/ CO2 separation. This strategy can not only enrich the structural library of MOFs but also optimize their properties and functions for promoting applications.
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| GB/T 7714 | Si, Guang-Rui , Wu, Wei , He, Tao et al. Stable Bimetallic Metal-Organic Framework with Dual-Functional Pyrazolate-Carboxylate Ligand: Rational Construction and C2H2/CO2 Separation [J]. | ACS MATERIALS LETTERS , 2022 , 4 (6) : 1032-1036 . |
| MLA | Si, Guang-Rui et al. "Stable Bimetallic Metal-Organic Framework with Dual-Functional Pyrazolate-Carboxylate Ligand: Rational Construction and C2H2/CO2 Separation" . | ACS MATERIALS LETTERS 4 . 6 (2022) : 1032-1036 . |
| APA | Si, Guang-Rui , Wu, Wei , He, Tao , Xu, Zi-Chao , Wang, Kecheng , Li, Jian-Rong . Stable Bimetallic Metal-Organic Framework with Dual-Functional Pyrazolate-Carboxylate Ligand: Rational Construction and C2H2/CO2 Separation . | ACS MATERIALS LETTERS , 2022 , 4 (6) , 1032-1036 . |
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Abstract ：
Novel metal clusters and coordinatively unsaturated sites are important features of metal-organic frameworks (MOFs) for many applications such as catalysis, gas storage and separation. Herein, two isostructural MOFs, BUT-150 and BUT-151 with unprecedented binuclear nickel clusters have been developed, using tetracarboxylate linkers containing chelating bipyridine-type units. The nickel cluster is coordinated with four carboxylate groups, one bipyridine unit, and one bridging water, leading to two open nickel sites per cluster. Interestingly, the two MOFs show selective adsorption of C2H2 and C2H6 over C2H4, representing two rare examples of MOFs with open metal sites for such ternary separation. Especially, BUT-151 with a phenanthroline unit has a high C2H2/C2H4 selectivity of 2.31 and C2H6/C2H4 selectivity of 1.36 at 273 K, being higher or comparable to current benchmark materials. The overall good separation performance of BUT-151 may be attributed to its high acetylene affinity from open metal sites and efficient confinement of ethane molecules by the open window with rich oxygen sites. Column breakthrough experiments confirm the good separation performance of binary or ternary gas mixtures by BUT-151 under dynamic conditions.
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| GB/T 7714 | Wang, Hao-Tian , Chen, Qiang , Zhang, Xin et al. Two isostructural metal-organic frameworks with unique nickel clusters for C2H2/C2H6/C2H4 mixture separation [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2022 , 10 (23) : 12497-12502 . |
| MLA | Wang, Hao-Tian et al. "Two isostructural metal-organic frameworks with unique nickel clusters for C2H2/C2H6/C2H4 mixture separation" . | JOURNAL OF MATERIALS CHEMISTRY A 10 . 23 (2022) : 12497-12502 . |
| APA | Wang, Hao-Tian , Chen, Qiang , Zhang, Xin , Zhao, Yan-Long , Xu, Ming-Ming , Lin, Rui-Biao et al. Two isostructural metal-organic frameworks with unique nickel clusters for C2H2/C2H6/C2H4 mixture separation . | JOURNAL OF MATERIALS CHEMISTRY A , 2022 , 10 (23) , 12497-12502 . |
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