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学者姓名:李建荣
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摘要 :
重金属离子污染问题一直备受关注。开发利用多孔材料吸附去除水中重金属离子一直是材料、环境等相关学科领域的研究热点之一。金属有机框架材料(metal-organic frameworks,MOFs)是一类新型的多孔材料,具有结构多样、比表面积大、孔径可调、孔表面特征易设计调控等特点,在气体分离、催化、传感等领域表现出极大的应用潜力。近年来,高稳定MOF材料的构筑取得了许多重大突破,大量研究工作探索了这类材料在水中的应用,包括水中重金属离子的吸附去除。Cr(Ⅵ)离子是一类毒性大、分布广的重金属离子,不同条件下存在形态多样,其吸附去除研究具有理论和实际意义。本文主要综述了近年来利用MOF材料吸附去除水...
关键词 :
多孔材料 多孔材料 吸附去除 吸附去除 六价铬Cr(Ⅵ) 六价铬Cr(Ⅵ) 金属有机框架 金属有机框架 重金属污染 重金属污染
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GB/T 7714 | 李茹霞 , 钟文彬 , 谢林华 et al. 金属有机框架材料对Cr(Ⅵ)离子的吸附去除研究进展 [J]. | 无机化学学报 , 2021 , 37 (03) : 385-400 . |
MLA | 李茹霞 et al. "金属有机框架材料对Cr(Ⅵ)离子的吸附去除研究进展" . | 无机化学学报 37 . 03 (2021) : 385-400 . |
APA | 李茹霞 , 钟文彬 , 谢林华 , 谢亚勃 , 李建荣 . 金属有机框架材料对Cr(Ⅵ)离子的吸附去除研究进展 . | 无机化学学报 , 2021 , 37 (03) , 385-400 . |
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摘要 :
金属有机框架材料对Cr(Ⅵ)离子的吸附去除研究进展
关键词 :
六价铬Cr(Ⅵ) 六价铬Cr(Ⅵ) 吸附去除 吸附去除 多孔材料 多孔材料 重金属污染 重金属污染 金属有机框架 金属有机框架
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GB/T 7714 | 李茹霞 , 钟文彬 , 谢林华 et al. 金属有机框架材料对Cr(Ⅵ)离子的吸附去除研究进展 [J]. | 李茹霞 , 2021 , 37 (3) : 385-400 . |
MLA | 李茹霞 et al. "金属有机框架材料对Cr(Ⅵ)离子的吸附去除研究进展" . | 李茹霞 37 . 3 (2021) : 385-400 . |
APA | 李茹霞 , 钟文彬 , 谢林华 , 谢亚勃 , 李建荣 , 无机化学学报 . 金属有机框架材料对Cr(Ⅵ)离子的吸附去除研究进展 . | 李茹霞 , 2021 , 37 (3) , 385-400 . |
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摘要 :
Metal-organic frameworks (MOFs) have been attracting tremendous attention owing to their great structural diversity and functional tunability. Despite numerous inherent merits and big progress in the fundamental research (synthesizing new compounds, discovering new structures, testing associated properties, etc.), poor chemical stability of most MOFs severely hinders their involvement in practical applications, which is the final goal for developing new materials. Therefore, constructing new stable MOFs or stabilizing extant labile MOFs is quite important. As with them, some "potential" applications would come true and a lot of new applications under harsh conditions can be explored. Efficient strategies are being pursued to solve the stability problem of MOFs and thereby achieve and expand their applications. In this Account, we summarize the research advance in the design and synthesis of chemically stable MOFs, particularly those stable in acidic, basic, and aqueous systems, as well as in the exploration of their applications in several expanding fields of environment, energy, and food safety, which have been dedicated in our lab over the past decade. The strategies for accessing stable MOFs can be classified into: (a) assembling high-valent metals (hard acid, such as Zr4+, Al3+) with carboxylate ligands (hard base) for acid-stable MOFs; (b) combining low-valent metals (soft acid, such as Co2+, Ni2+) and azolate ligands (soft base, such as pyrazolate) for alkali-resistant MOFs; (c) enhancing the connectivity of the building unit; (d) contracting or rigidifying the ligand; (e) increasing the hydrophobicity of the framework; and (f) substituting liable building units with stable ones (such as metal metathesis) to obtain robust MOFs. In addition, other factors, including the geometry and symmetry of building units, framework-framework interaction, and so forth, have also been taken into account in the design and synthesis of stable MOFs. On the basis of these approaches, the stability of resulting MOFs under corresponding conditions has been remarkably enhanced. With high chemical stability achieved, the MOFs have found many new and significant applications, aiming at addressing global challenges related to environmental pollution, energy shortage, and food safety. A series of stable MOFs have been constructed for detecting and eliminating contaminations. Various fluorescent MOFs were rationally customized to be powerful platforms for sensing hazardous targets in food and water, such as dioxins, antibiotics, veterinary drugs, and heavy metal ions. Some hydrophobic MOFs even showed effective and specific capture of low-concentration volatile organic compounds. Novel MOFs with record-breaking acid/base/nucleophilic regent resistance have expanded their application scope under harsh conditions. BUT-8(Cr)A, as the most acid-stable MOF yet, showed reserved structural integrity in concentrated H2SO4 and recorded high proton conductivity; the most alkali-resistant MOF, PCN-601, retained crystallinity even in boiling saturated NaOH aqueous solution, and such base-stable MOFs composed of non-noble metal clusters and poly pyrazolate ligands also demonstrated great potential in heterogeneous catalysis in alkaline/nucleophilic systems for the first time. It is believed that this Account will provide valuable references on stable MOFs' construction as well as application expansion toward harsh conditions, thereby being helpful to promote MOF materials to step from fundamental research to practical applications.
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GB/T 7714 | He, Tao , Kong, Xiang-Jing , Li, Jian-Rong . Chemically Stable Metal-Organic Frameworks: Rational Construction and Application Expansion [J]. | ACCOUNTS OF CHEMICAL RESEARCH , 2021 , 54 (15) : 3083-3094 . |
MLA | He, Tao et al. "Chemically Stable Metal-Organic Frameworks: Rational Construction and Application Expansion" . | ACCOUNTS OF CHEMICAL RESEARCH 54 . 15 (2021) : 3083-3094 . |
APA | He, Tao , Kong, Xiang-Jing , Li, Jian-Rong . Chemically Stable Metal-Organic Frameworks: Rational Construction and Application Expansion . | ACCOUNTS OF CHEMICAL RESEARCH , 2021 , 54 (15) , 3083-3094 . |
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摘要 :
The pollution of heavy metal ions has long been a big concern to the society. The development and utilization of porous materials for the adsorptive removal of heavy metal ions in water represents one of the hottest research subjects in related areas, such as materials science and environmental science. Due to their structural variety, large specific surface area, adjustable pore size, and tailorable pore surface characteristics, metal-organic frameworks (MOFs) show great potential in many applications, such as gas separation, catalysis, and sensing. In the past few years, many major breakthroughs have been made in the construction of highly stable MOFs. A lot of research works have been explored for the applications of MOFs in water systems, including the adsorptive removal of heavy metal ions in water. Cr(VI) ions are a kind of wide-distributed heavy metal ions with high toxicity, existing in water in various forms under different conditions. The study on the removal of Cr(VI) ions from water is of significance academically and practically. Herein, the published research works about adsorptive removal of Cr(VI) ions with MOFs or MOF-based materials are reviewed. These materials are classified into four classes: (1) highly stable zirconium-based MOF, (2) cationic MOF, (3) post-modified MOF, and (4) MOF-based composite materials. The adsorption mechanism, adsorption capacity, and regenerability of these materials for Cr(VI) ions are also discussed. The existing problems and the trend of future works for the practical application of MOFs in the removal of heavy metal ions are analyzed at last.
关键词 :
adsorption removal adsorption removal Cd(VI) Cd(VI) heavy metal pollution heavy metal pollution metal-organic frameworks metal-organic frameworks porous materials porous materials
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GB/T 7714 | Li Ru-Xia , Zhong Wen-Bin , Xie Lin-Hua et al. Recent Advances in Adsorptive Removal of Cr(VI) Ions by Metal-Organic Frameworks [J]. | CHINESE JOURNAL OF INORGANIC CHEMISTRY , 2021 , 37 (3) : 385-400 . |
MLA | Li Ru-Xia et al. "Recent Advances in Adsorptive Removal of Cr(VI) Ions by Metal-Organic Frameworks" . | CHINESE JOURNAL OF INORGANIC CHEMISTRY 37 . 3 (2021) : 385-400 . |
APA | Li Ru-Xia , Zhong Wen-Bin , Xie Lin-Hua , Xie Ya-Bo , Li Jian-Rong . Recent Advances in Adsorptive Removal of Cr(VI) Ions by Metal-Organic Frameworks . | CHINESE JOURNAL OF INORGANIC CHEMISTRY , 2021 , 37 (3) , 385-400 . |
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摘要 :
The designability and tunability of the pore structure are the advantage of metal–organic frameworks (MOFs) for adsorptive separation applications. However, it is still challenging to design MOF adsorbent rationally according to industrial demands, because of the complexity in the separation processes and the relative lack of structure-separation relationship information. Herein, we established a contrastive model ingeniously via structural modification at the atom level in three Cu(II)-MOFs constructed from isonicotinic acid (HINA) and its fluorinated analogue 3-fluoro-isonicotinic acid (HFINA), targeting on controlling pore surface fluorination for studying light hydrocarbon separation. Both the fluorinated MOFs (Cu-FINA-1 and 2) show notably enhanced C2H2/C2H4 and C3H4/C3H6 selectivity compared with Cu-INA without increasing regeneration energy consumption. Especially, Cu-FINA-2 exhibits a considerable IAST selectivity (6.3–9.3) for C3H4/C3H6, while Cu-FINA-1 achieves a C3H6 process productivity of 31.6 cm3/g in column breakthrough experiments. Molecular simulations reveal that the polar F sites within the confined pores can interact with gas adsorbates through C-H···F hydrogen bonds, and the tailored pore size and optimal diffusion kinetics mainly contribute to the excellent separation selectivity for Cu-FINA-1. This work highlights how pore surface fluorination and related structural evolution can influence light hydrocarbon adsorption/separation properties in MOFs, and thus promotes the rational design and precise optimization of new adsorbents for alkynes/alkenes separations, even at the atom level. © 2020 Elsevier B.V.
关键词 :
Copper compounds Copper compounds Energy utilization Energy utilization Fluorination Fluorination Halogenation Halogenation Hydrocarbon refining Hydrocarbon refining Hydrocarbons Hydrocarbons Hydrogen bonds Hydrogen bonds Pore size Pore size Pore structure Pore structure Separation Separation Structural design Structural design
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GB/T 7714 | Wu, Xue-Qian , Liu, Jing-Hao , He, Tao et al. Understanding how pore surface fluorination influences light hydrocarbon separation in metal–organic frameworks [J]. | Chemical Engineering Journal , 2021 , 407 . |
MLA | Wu, Xue-Qian et al. "Understanding how pore surface fluorination influences light hydrocarbon separation in metal–organic frameworks" . | Chemical Engineering Journal 407 (2021) . |
APA | Wu, Xue-Qian , Liu, Jing-Hao , He, Tao , Zhang, Peng-Dan , Yu, Jiamei , Li, Jian-Rong . Understanding how pore surface fluorination influences light hydrocarbon separation in metal–organic frameworks . | Chemical Engineering Journal , 2021 , 407 . |
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摘要 :
The exploration of metal-organic frameworks (MOFs) through the rational design of building units with specific sizes, geometries, and symmetries is essential for enriching the structural diversity of porous solids for applications including storage, separation, and conversion. However, it is still a challenge to directly synthesize rare-earth (RE) MOFs with less connected clusters as a thermodynamically favored product. Herein, we report a systematic investigation on the influence of size, rigidity, and symmetry of linkers over the formation of RE-tetracarboxylate MOFs and uncover the critical role of linker desymmetrization in constructing RE-MOFs with eight-connected hexanuclear clusters. Our results on nine new RE-MOFs, PCN-50X (X = 1-9), indicate that utilization of trapezoidal or tetrahedral linkers provides accesses to traditionally unattainable RE-tetracarboxylate MOFs with 8-c hexanuclear nodes, while the introduction of square or rectangular linkers during the assembly of RE-MOFs based on polynuclear clusters typically leads to the MOFs constructed from 12-c nodes with underlying shp topology. By rational linker design, MOFs with two unprecedented (4, 8)-c nets, lxl and jun, can also be obtained. This work highlights linker desymmetrization as a powerful strategy to enhance MOFs' structural complexity and access MOF materials with nondefault topologies that can be potentially used for separation and catalysis.
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GB/T 7714 | Lv Xiu-Liang , Feng Liang , Xie Lin-Hua et al. Linker Desymmetrization: Access to a Series of Rare-Earth Tetracarboxylate Frameworks with Eight-Connected Hexanuclear Nodes. [J]. | Journal of the American Chemical Society , 2021 , 143 (7) : 2784-2791 . |
MLA | Lv Xiu-Liang et al. "Linker Desymmetrization: Access to a Series of Rare-Earth Tetracarboxylate Frameworks with Eight-Connected Hexanuclear Nodes." . | Journal of the American Chemical Society 143 . 7 (2021) : 2784-2791 . |
APA | Lv Xiu-Liang , Feng Liang , Xie Lin-Hua , He Tao , Wu Wei , Wang Kun-Yu et al. Linker Desymmetrization: Access to a Series of Rare-Earth Tetracarboxylate Frameworks with Eight-Connected Hexanuclear Nodes. . | Journal of the American Chemical Society , 2021 , 143 (7) , 2784-2791 . |
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摘要 :
In the past few years, metal-organic frameworks (MOFs) have emerged as a class of fascinating materials for photocatalysis. Herein, a new MOF formulated as [Zn(bpe)(fdc)]center dot 2DMF (BUT-206, bpe = 1,2-bis(4-pyridyl) ethylene, H(2)fdc = 2,5-furan dicarboxylic acid, DMF = N,N-dimethylformamide) is reported, which was synthesized under solvothermal conditions and applied for photocatalytic degradation of dyes (crystal violet and rhodamine B). Noteworthily, BUT-206 exhibited high photocatalytic activity toward the degradation of crystal violet without using any photosensitizer or cocatalyst under UV-irradiation. The photocatalytic degradation of crystal violet by BUT-206 was effective with a degradation efficiency of 92.5% within 120 minutes. The effects of key parameters including pH, amount of photocatalyst and initial concentration of dye on the dye degradation processes were examined, and the kinetics of dye degradation was established by the pseudo-first order kinetic equation. Furthermore, BUT-206 showed good cyclic stability in photocatalytic performance for up to five regeneration cycles, making it a potential green catalyst for dye degradation.
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GB/T 7714 | Alamgir , Talha, Khalid , Wang, Ying-Jie et al. Construction of a mixed ligand MOF as "green catalyst" for the photocatalytic degradation of organic dye in aqueous media [J]. | RSC ADVANCES , 2021 , 11 (38) : 23838-23845 . |
MLA | Alamgir et al. "Construction of a mixed ligand MOF as "green catalyst" for the photocatalytic degradation of organic dye in aqueous media" . | RSC ADVANCES 11 . 38 (2021) : 23838-23845 . |
APA | Alamgir , Talha, Khalid , Wang, Ying-Jie , Ullah, Raza , Wang, Bin , Wang, Lu et al. Construction of a mixed ligand MOF as "green catalyst" for the photocatalytic degradation of organic dye in aqueous media . | RSC ADVANCES , 2021 , 11 (38) , 23838-23845 . |
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摘要 :
Despite numerous inherent merits of metal-organic frameworks (MOFs), structural fragility has imposed great restrictions on their wider involvement in many applications, such as in catalysis. Herein, a strategy for enhancing stability and enabling functionality in a labile Zr(IV)-MOF has been proposed by in situ porphyrin substitution. A size- and geometry-matched robust linear porphyrin ligand 4,4'-(porphyrin-5,15-diyl)dibenzolate (DCPP2- ) is selected to replace the 4,4'-(1,3,6,8-tetraoxobenzo[lmn][3,8]phenanthroline-2,7(1H,3H,6H,8H)-diyl)dibenzoate (NDIDB2- ) ligand in the synthesis of BUT-109(Zr), affording BUT-110 with varied porphyrin contents. Compared to BUT-109(Zr), the chemical stability of BUT-110 series is greatly improved. Metalloporphyrin incorporation endows BUT-110 MOFs with high catalytic activity in the photoreduction of CO2 , in the absence of photosensitizers. By tuning the metal species and porphyrin contents in BUT-110, the resulting BUT-110-50%-Co is demonstrated to be a good photocatalyst for selective CO2 -to-CO reduction, via balancing the chemical stability, photocatalytic efficiency, and synthetic cost. This work highlights the advantages of in situ ligand substitution for MOF modification, by which uniform distribution and high content of the incoming ligand are accessible in the resulting MOFs. More importantly, it provides a promising approach to convert unstable MOFs, which mainly constitute the vast MOF database but have always been neglected, into robust functional materials.
关键词 :
in situ ligand substitution in situ ligand substitution metal-organic frameworks metal-organic frameworks photocatalytic CO 2 reduction photocatalytic CO 2 reduction porphyrin ligands porphyrin ligands stability enhancement stability enhancement
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GB/T 7714 | Kong Xiang-Jing , He Tao , Zhou Jian et al. In Situ Porphyrin Substitution in a Zr(IV)-MOF for Stability Enhancement and Photocatalytic CO2 Reduction. [J]. | Small , 2021 : e2005357 . |
MLA | Kong Xiang-Jing et al. "In Situ Porphyrin Substitution in a Zr(IV)-MOF for Stability Enhancement and Photocatalytic CO2 Reduction." . | Small (2021) : e2005357 . |
APA | Kong Xiang-Jing , He Tao , Zhou Jian , Zhao Chen , Li Tong-Chuan , Wu Xue-Qian et al. In Situ Porphyrin Substitution in a Zr(IV)-MOF for Stability Enhancement and Photocatalytic CO2 Reduction. . | Small , 2021 , e2005357 . |
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Clenbuterol (CLE) and ractopamine (RAC) are two kinds of typical β2-adrenergic agonists which pose a serious threat to the health of human beings. In this work, 10 kinds of metal-organic frameworks (MOFs) with high stability and various pore features are screened to assess adsorption performance for CLE and RAC. An Al(III)-MOF (BUT-19) with abundant ethyl groups exhibits exceptional performance in removing CLE and RAC from water. The maximum adsorption capacity for CLE and RAC are up to 294.1 and 366.3 mg/g under the optimum adsorption conditions, respectively. Meanwhile, the adsorption mechanism effects of pH, temperature, and coexisted ions are investigated systematically. It is found that the MOF pore size and weak hydrogen-bond interactions between CLE/RAC molecules and the MOF are the main causes leading to the extraordinary adsorption. This study provides a new idea for the purposeful design and synthesis of MOFs for removing environmental pollutants and sheds light on the depuration of contaminated water.
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GB/T 7714 | Lv Jie , Chen Qiang , Liu Jing-Hao et al. Effective Removal of Clenbuterol and Ractopamine from Water with a Stable Al(III)-Based Metal-Organic Framework. [J]. | Inorganic chemistry , 2021 , 60 (3) : 1814-1822 . |
MLA | Lv Jie et al. "Effective Removal of Clenbuterol and Ractopamine from Water with a Stable Al(III)-Based Metal-Organic Framework." . | Inorganic chemistry 60 . 3 (2021) : 1814-1822 . |
APA | Lv Jie , Chen Qiang , Liu Jing-Hao , Yang Hao-Sen , Wang Peilong , Yu Jiamei et al. Effective Removal of Clenbuterol and Ractopamine from Water with a Stable Al(III)-Based Metal-Organic Framework. . | Inorganic chemistry , 2021 , 60 (3) , 1814-1822 . |
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摘要 :
Constructing stable palladium(II)-based metal-organic frameworks (MOFs) would unlock more opportunities for MOF chemistry, particularly toward applications in catalysis. However, their availability is limited by synthetic challenges due to the inertness of the Pd-ligand coordination bond, as well as the strong tendency of the Pd(II) source to be reduced under typical solvothermal conditions. Under the guidance of reticular chemistry, herein, we present the first example of an azolate Pd-MOF, BUT-33(Pd), obtained via a deuterated solvent-assisted metal metathesis. BUT-33(Pd) retains the underlying sodalite network and mesoporosity of the template BUT-33(Ni) and shows excellent chemical stability (resistance to an 8 M NaOH aqueous solution). With rich Pd(II) sites in the atomically precise distribution, it also demonstrates good performances as a heterogeneous Pd(II) catalyst in a wide application scope, including Suzuki/Heck coupling reactions and photocatalytic CO2 reduction to CH4. This work highlights a feasible approach to reticularly construct noble metal based MOFs via metal metathesis, in which various merits, including high chemical stability, large pores, and tunable functions, have been integrated for addressing challenging tasks.
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GB/T 7714 | He, Tao , Kong, Xiang-Jing , Zhou, Jian et al. A Practice of Reticular Chemistry: Construction of a Robust Mesoporous Palladium Metal-Organic Framework via Metal Metathesis [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2021 , 143 (26) : 9901-9911 . |
MLA | He, Tao et al. "A Practice of Reticular Chemistry: Construction of a Robust Mesoporous Palladium Metal-Organic Framework via Metal Metathesis" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 143 . 26 (2021) : 9901-9911 . |
APA | He, Tao , Kong, Xiang-Jing , Zhou, Jian , Zhao, Chen , Wang, Kecheng , Wu, Xue-Qian et al. A Practice of Reticular Chemistry: Construction of a Robust Mesoporous Palladium Metal-Organic Framework via Metal Metathesis . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2021 , 143 (26) , 9901-9911 . |
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