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Keywords = heterometallic metal–organic framework

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15 pages, 12174 KiB  
Article
Lanthanide Heterometallic MOFs with 5-Iodosophthalate Linkers: Tuning of Luminescent Properties by Varying of Metal Composition
by Mikhail A. Bondarenko, Roman V. Redkin, Elizaveta A. Pilyukova, Nikita A. Korobeynikov, Alexander S. Zaguzin, Marianna I. Rakhmanova, Tatiana Ya. Guselnikova, Evgeny A. Maksimovsky, Vladimir P. Fedin and Sergey A. Adonin
Inorganics 2025, 13(5), 154; https://doi.org/10.3390/inorganics13050154 - 7 May 2025
Viewed by 599
Abstract
Coordination polymers [Gd2(5-iip)3(DMF)4]·0.4DMF (1) and [Dy2(5-iip)3DMF2]·0.33DMF (2) (5-iip2−—5-iodoisophthalate) feature two different structural types, as follows from X-ray diffractometry data. We prepared and characterized an extended [...] Read more.
Coordination polymers [Gd2(5-iip)3(DMF)4]·0.4DMF (1) and [Dy2(5-iip)3DMF2]·0.33DMF (2) (5-iip2−—5-iodoisophthalate) feature two different structural types, as follows from X-ray diffractometry data. We prepared and characterized an extended series of corresponding heterometallic complexes of the composition [GdxDy2−x(5-iip)3DMF2]·0.33DMF and [EuxDy2−x(5-iip)3DMF2]·0.33DMF, where x = 0.2, 0.4…1.8, and examined the changes of their luminescent properties induced by variations of metal composition, finding the promising white emission sources with high light purity. Full article
(This article belongs to the Section Coordination Chemistry)
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13 pages, 2565 KiB  
Article
The Structure and Optical Properties of Luminescent Terbium Terephthalate Metal–Organic Frameworks Doped with Yttrium, Gadolinium, and Lanthanum Ions
by Anna S. Petrova, Oleg S. Butorlin, Yulia N. Toikka, Ilya E. Kolesnikov, Sergey N. Orlov, Mikhail N. Ryazantsev, Nikita A. Bogachev, Mikhail Yu. Skripkin and Andrey S. Mereshchenko
Crystals 2024, 14(11), 966; https://doi.org/10.3390/cryst14110966 - 8 Nov 2024
Viewed by 1458
Abstract
The structural features and luminescent properties of heterometallic Tb–Gd, Tb–La, and Tb–Y terephthalate metal–organic frameworks, namely (TbxM1−x)2(1,4-bdc)3∙4H2O (M = Gd, La, Y), were studied in detail in a wide concentration range (x = [...] Read more.
The structural features and luminescent properties of heterometallic Tb–Gd, Tb–La, and Tb–Y terephthalate metal–organic frameworks, namely (TbxM1−x)2(1,4-bdc)3∙4H2O (M = Gd, La, Y), were studied in detail in a wide concentration range (x = 0.001–1). The crystalline phase of synthesized compounds corresponds to Ln2(1,4-bdc)3·4H2O. The lifetime of 5D4 decreased with increased Tb3+ concentration, but PLQY depends non-linearly on the Tb3+ concentration. The 50% substitution of Tb3+ for Y3+, Gd3+, or La3+ ions result in the significant enhancement of photoluminescence quantum yield, up to 1.6 times. The morphology, thermal stability, and vibrational structure of the selected homo- and bi-metallic materials is reported as well. Full article
(This article belongs to the Special Issue Synthesis and Crystal Structure of Rare-Earth Metal Compounds)
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14 pages, 2646 KiB  
Article
Heterometallic ZnHoMOF as a Dual-Responsive Luminescence Sensor for Efficient Detection of Hippuric Acid Biomarker and Nitrofuran Antibiotics
by Jingrui Yin, Wenqian Li, Wencui Li, Liying Liu, Dongsheng Zhao, Xin Liu, Tuoping Hu and Liming Fan
Molecules 2023, 28(17), 6274; https://doi.org/10.3390/molecules28176274 - 27 Aug 2023
Cited by 48 | Viewed by 2112
Abstract
Developing efficient and sensitive MOF-based luminescence sensors for bioactive molecule detection is of great significance and remains a challenge. Benefiting from favorable chemical and thermal stability, as well as excellent luminescence performance, a porous Zn(II)Ho(III) heterometallic–organic framework (ZnHoMOF) was selected here as a [...] Read more.
Developing efficient and sensitive MOF-based luminescence sensors for bioactive molecule detection is of great significance and remains a challenge. Benefiting from favorable chemical and thermal stability, as well as excellent luminescence performance, a porous Zn(II)Ho(III) heterometallic–organic framework (ZnHoMOF) was selected here as a bifunctional luminescence sensor for the early diagnosis of a toluene exposure biomarker of hippuric acid (HA) through “turn-on” luminescence enhancing response and the daily monitoring of NFT/NFZ antibiotics through “turn-off” quenching effects in aqueous media with high sensitivity, acceptable selectivity, good anti-interference, exceptional recyclability performance, and low detection limits (LODs) of 0.7 ppm for HA, 0.04 ppm for NFT, and 0.05 ppm for NFZ. Moreover, the developed sensor was employed to quantify HA in diluted urine samples and NFT/NFZ in natural river water with satisfactory results. In addition, the sensing mechanisms of ZnHoMOF as a dual-response chemosensor in efficient detection of HA and NFT/NFZ antibiotics were conducted from the view of photo-induced electron transfer (PET), as well as inner filter effects (IFEs), with the help of time-dependent density functional theory (TD-DFT) and spectral overlap experiments. Full article
(This article belongs to the Special Issue Metal Organic Frameworks (MOFs) for Sensing Applications)
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27 pages, 3497 KiB  
Review
Advantages of Bimetallic Organic Frameworks in the Adsorption, Catalysis and Detection for Water Contaminants
by Jun Luo, Xiao Luo, Yonghai Gan, Xiaoming Xu, Bin Xu, Zhuang Liu, Chengcheng Ding, Yibin Cui and Cheng Sun
Nanomaterials 2023, 13(15), 2194; https://doi.org/10.3390/nano13152194 - 28 Jul 2023
Cited by 34 | Viewed by 4592
Abstract
The binary metal organic framework (MOF) is composed of two heterometallic ions bonded to an organic ligand. Compared with monometallic MOFs, bimetallic MOFs have greatly improved in terms of structure, porosity, active site, adsorption, selectivity, and stability, which has attracted wide attention. At [...] Read more.
The binary metal organic framework (MOF) is composed of two heterometallic ions bonded to an organic ligand. Compared with monometallic MOFs, bimetallic MOFs have greatly improved in terms of structure, porosity, active site, adsorption, selectivity, and stability, which has attracted wide attention. At present, many effective strategies have been designed for the synthesis of bimetallic MOF-based nanomaterials with specific morphology, structure, and function. The results show that bimetallic MOF-based nanocomposites could achieve multiple synergistic effects, which will greatly improve their research in the fields of adsorption, catalysis, energy storage, sensing, and so on. In this review, the main preparation methods of bimetallic MOFs-based materials are summarized, with emphasis on their applications in adsorption, catalysis, and detection of target pollutants in water environments, and perspectives on the future development of bimetallic MOFs-based nanomaterials in the field of water are presented. Full article
(This article belongs to the Topic Nanomaterials for Catalytic Remediation of Environmental Contaminants)
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15 pages, 3133 KiB  
Article
Bis(2,6-pyrazolyl)pyridines as a New Scaffold for Coordination Polymers
by Igor A. Nikovskiy, Pavel V. Dorovatovskii, Valentin V. Novikov and Yulia V. Nelyubina
Molecules 2023, 28(11), 4275; https://doi.org/10.3390/molecules28114275 - 23 May 2023
Cited by 1 | Viewed by 2575
Abstract
Two coordination polymers, Fe(LOBF3)(CH3COO)(CH3CN)2]n•nCH3CN and [Fe(LO−)2AgNO3BF4•CH3OH]n•1.75nCH3OH•nH2O (LO− = 3,3′-(4-(4-cyanophenyl)pyridine-2,6-diyl)bis(1-(2,6-dichlorophenyl)-1H-pyrazol-5-olate)), were obtained via a [...] Read more.
Two coordination polymers, Fe(LOBF3)(CH3COO)(CH3CN)2]n•nCH3CN and [Fe(LO−)2AgNO3BF4•CH3OH]n•1.75nCH3OH•nH2O (LO− = 3,3′-(4-(4-cyanophenyl)pyridine-2,6-diyl)bis(1-(2,6-dichlorophenyl)-1H-pyrazol-5-olate)), were obtained via a PCET-assisted process that uses the hydroxy-pyrazolyl moiety of the ligand and the iron(II) ion as sources of proton and electron, respectively. Our attempts to produce heterometallic compounds under mild conditions of reactant diffusion resulted in the first coordination polymer of 2,6-bis(pyrazol-3-yl)pyridines to retain the core N3(L)MN3(L). Under harsh solvothermal conditions, a hydrogen atom transfer to the tetrafluoroborate anion caused the transformation of the hydroxyl groups into OBF3 in the third coordination polymer of 2,6-bis(pyrazol-3-yl)pyridines. This PCET-assisted approach may be applicable to produce coordination polymers and metal–organic frameworks with the SCO-active core N3(L)MN3(L) formed by pyrazolone- and other hydroxy-pyridine-based ligands. Full article
(This article belongs to the Section Inorganic Chemistry)
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17 pages, 8750 KiB  
Article
Two-Dimensional Bimetallic Phthalocyanine Covalent-Organic-Framework-Based Chemiresistive Gas Sensor for ppb-Level NO2 Detection
by Xiyu Chen, Min Zeng, Jianhua Yang, Nantao Hu, Xiaoyong Duan, Wei Cai, Yanjie Su and Zhi Yang
Nanomaterials 2023, 13(10), 1660; https://doi.org/10.3390/nano13101660 - 17 May 2023
Cited by 26 | Viewed by 3900
Abstract
Two-dimensional (2D) phthalocyanine-based covalent organic frameworks (COFs) provide an ideal platform for efficient and rapid gas sensing—this can be attributed to their regular structure, moderate conductivity, and a large number of scalable metal active centers. However, there remains a need to explore structural [...] Read more.
Two-dimensional (2D) phthalocyanine-based covalent organic frameworks (COFs) provide an ideal platform for efficient and rapid gas sensing—this can be attributed to their regular structure, moderate conductivity, and a large number of scalable metal active centers. However, there remains a need to explore structural modification strategies for optimizing the sluggish desorption process caused by the extensive porosity and strong adsorption effect of metal sites. Herein, we reported a 2D bimetallic phthalocyanine-based COF (COF-CuNiPc) as chemiresistive gas sensors that exhibited a high gas-sensing performance to nitrogen dioxide (NO2). Bimetallic COF-CuNiPc with an asymmetric synergistic effect achieves a fast adsorption/desorption process to NO2. It is demonstrated that the COF-CuNiPc can detect 50 ppb NO2 with a recovery time of 7 s assisted by ultraviolet illumination. Compared with single-metal phthalocyanine-based COFs (COF-CuPc and COF-NiPc), the bimetallic structure of COF-CuNiPc can provide a proper band gap to interact with NO2 gas molecules. The CuNiPc heterometallic active site expands the overlap of d-orbitals, and the optimized electronic arrangement accelerates the adsorption/desorption processes. The concept of a synergistic effect enabled by bimetallic phthalocyanines in this work can provide an innovative direction to design high-performance chemiresistive gas sensors. Full article
(This article belongs to the Special Issue Nanomaterials in Gas Sensors)
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12 pages, 2771 KiB  
Article
Brightly Luminescent (TbxLu1−x)2bdc3·nH2O MOFs: Effect of Synthesis Conditions on Structure and Luminescent Properties
by Viktor G. Nosov, Yulia N. Toikka, Anna S. Petrova, Oleg S. Butorlin, Ilya E. Kolesnikov, Sergey N. Orlov, Mikhail N. Ryazantsev, Stefaniia S. Kolesnik, Nikita A. Bogachev, Mikhail Yu. Skripkin and Andrey S. Mereshchenko
Molecules 2023, 28(5), 2378; https://doi.org/10.3390/molecules28052378 - 4 Mar 2023
Cited by 10 | Viewed by 2963
Abstract
Luminescent, heterometallic terbium(III)–lutetium(III) terephthalate metal-organic frameworks (MOFs) were synthesized via direct reaction between aqueous solutions of disodium terephthalate and nitrates of corresponding lanthanides by using two methods: synthesis from diluted and concentrated solutions. For (TbxLu1−x)2bdc3·nH [...] Read more.
Luminescent, heterometallic terbium(III)–lutetium(III) terephthalate metal-organic frameworks (MOFs) were synthesized via direct reaction between aqueous solutions of disodium terephthalate and nitrates of corresponding lanthanides by using two methods: synthesis from diluted and concentrated solutions. For (TbxLu1−x)2bdc3·nH2O MOFs (bdc = 1,4-benzenedicarboxylate) containing more than 30 at. % of Tb3+, only one crystalline phase was formed: Ln2bdc3·4H2O. At lower Tb3+ concentrations, MOFs crystallized as the mixture of Ln2bdc3·4H2O and Ln2bdc3·10H2O (diluted solutions) or Ln2bdc3 (concentrated solutions). All synthesized samples that contained Tb3+ ions demonstrated bright green luminescence upon excitation into the 1ππ* excited state of terephthalate ions. The photoluminescence quantum yields (PLQY) of the compounds corresponding to the Ln2bdc3 crystalline phase were significantly larger than for Ln2bdc3·4H2O and Ln2bdc3·10H2O phases due to absence of quenching from water molecules possessing high-energy O-H vibrational modes. One of the synthesized materials, namely, (Tb0.1Lu0.9)2bdc3·1.4H2O, had one of the highest PLQY among Tb-based MOFs, 95%. Full article
(This article belongs to the Special Issue Multifunctional Metal-Organic Framework Materials)
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11 pages, 3220 KiB  
Article
Heterometallic Europium(III)–Lutetium(III) Terephthalates as Bright Luminescent Antenna MOFs
by Viktor G. Nosov, Arkady S. Kupryakov, Ilya E. Kolesnikov, Aleksandra A. Vidyakina, Ilya I. Tumkin, Stefaniia S. Kolesnik, Mikhail N. Ryazantsev, Nikita A. Bogachev, Mikhail Yu. Skripkin and Andrey S. Mereshchenko
Molecules 2022, 27(18), 5763; https://doi.org/10.3390/molecules27185763 - 6 Sep 2022
Cited by 12 | Viewed by 3134
Abstract
A new series of luminescent heterometallic europium(III)–lutetium(III) terephthalate metal–organic frameworks, namely (EuxLu1−x)2bdc3·nH2O, was synthesized using a direct reaction in a water solution. At the Eu3+ concentration of 1–40 at %, the MOFs [...] Read more.
A new series of luminescent heterometallic europium(III)–lutetium(III) terephthalate metal–organic frameworks, namely (EuxLu1−x)2bdc3·nH2O, was synthesized using a direct reaction in a water solution. At the Eu3+ concentration of 1–40 at %, the MOFs were formed as a binary mixture of the (EuxLu1−x)2bdc3 and (EuxLu1−x)2bdc3·4H2O crystalline phases, where the Ln2bdc3·4H2O crystalline phase was enriched by europium(III) ions. At an Eu3+ concentration of more than 40 at %, only one crystalline phase was formed: (EuxLu1−x)2bdc3·4H2O. All MOFs containing Eu3+ exhibited sensitization of bright Eu3+-centered luminescence upon the 280 nm excitation into a 1ππ* excited state of the terephthalate ion. The fine structure of the emission spectra of Eu3+ 5D0-7FJ (J = 0–4) significantly depended on the Eu3+ concentration. The luminescence quantum yield of Eu3+ was significantly larger for Eu-Lu terephthalates containing a low concentration of Eu3+ due to the absence of Eu-Eu energy migration and the presence of the Ln2bdc3 crystalline phase with a significantly smaller nonradiative decay rate compared to the Ln2bdc3·4H2O. Full article
(This article belongs to the Special Issue Multifunctional Metal-Organic Framework Materials)
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15 pages, 6544 KiB  
Article
Influence of Substituents in Terephthalate Linker on the Structure of MOFs Obtained from Presynthesized Heterometallic Complex
by Marina Barsukova, Evgeny Dudko, Denis Samsonenko, Konstantin Kovalenko, Alexey Ryadun, Aleksandr Sapianik and Vladimir Fedin
Inorganics 2021, 9(1), 4; https://doi.org/10.3390/inorganics9010004 - 2 Jan 2021
Cited by 1 | Viewed by 3610
Abstract
The synthesis of new porous materials with desired properties is a challenging task. It becomes especially difficult if you need to combine several metals in one framework to obtain a heterometallic node. The use of presynthesized complexes for obtaining of new heterometallic metal–organic [...] Read more.
The synthesis of new porous materials with desired properties is a challenging task. It becomes especially difficult if you need to combine several metals in one framework to obtain a heterometallic node. The use of presynthesized complexes for obtaining of new heterometallic metal–organic frameworks could be essential to solve the problem of tailored synthesis. In our study we use presynthesized heterometallic pivalate complex [Li2Zn2(piv)6(py)2] to obtain new MOFs with heterometallic core as a node of the framework. We are managed to obtain four new heterometallic MOFs: [H2N(CH3)2]2[Li2Zn2(bdc)4]·CH3CN·DMF (1), [Li2Zn2(H2Br2-bdc)(Br2-bdc)3]·2DMF (2), [H2N(CH3)2][LiZn2(ndc)3]·CH3CN (3) and [{Li2Zn2(dmf)(py)2}{LiZn(dmf)2}2 (NO2-bdc)6]·5DMF (4). Moreover three of them contain starting tetranuclear core {Li2Zn2} and saves its geometry. We also demonstrate the influence of substituent in terephthalate ring on preservation of tetranuclear core. For compound 1 it was shown that luminescence of the framework could be quenched when nitrobenzene is included in the pores. Full article
(This article belongs to the Special Issue Heterometallic Complexes)
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11 pages, 1164 KiB  
Article
CuII- and CoII-Based MOFs: {[La2Cu3(µ-H2O)(ODA)6(H2O)3]∙3H2O}n and {[La2Co3(ODA)6(H2O)6]∙12H2O}n. The Relevance of Physicochemical Properties on the Catalytic Aerobic Oxidation of Cyclohexene
by Luis Santibáñez, Néstor Escalona, Julia Torres, Carlos Kremer, Patricio Cancino and Evgenia Spodine
Catalysts 2020, 10(5), 589; https://doi.org/10.3390/catal10050589 - 25 May 2020
Cited by 11 | Viewed by 3725
Abstract
The aerobic oxidation of cyclohexene was done using the heterometallic metal organic frameworks (MOFs) {[La2Cu3(μ-H2O)(ODA)6(H2O)3]⋅3H2O}n (LaCuODA)) (1) and {[La2Co3(ODA)6 [...] Read more.
The aerobic oxidation of cyclohexene was done using the heterometallic metal organic frameworks (MOFs) {[La2Cu3(μ-H2O)(ODA)6(H2O)3]⋅3H2O}n (LaCuODA)) (1) and {[La2Co3(ODA)6(H2O)6]∙12H2O}n (LaCoODA) (2) as catalysts, in solvent free conditions (ODA, oxydiacetic acid). After 24 h of reaction, the catalytic system showed that LaCoODA had a better catalytic performance than that of LaCuODA (conversion 85% and 67%). The structures of both catalysts were very similar, showing channels running along the c axis. The physicochemical properties of both MOFs were determined to understand the catalytic performance. The Langmuir surface area of LaCoODA was shown to be greater than that of LaCuODA, while the acid strength and acid sites were greater for LaCuODA. On the other hand, the redox potential of the active sites was related to CoII/CoIII in LaCoODA and CuII/CuI in LaCuODA. Therefore, it is concluded that the Langmuir surface area and the redox potentials were more important than the acid strength and acid sites of the studied MOFs, in terms of the referred catalytic performance. Finally, the reaction conditions were also shown to play an important role in the catalytic performance of the studied systems. Especially, the type of oxidant and the way to supply it to the reaction medium influenced the catalytic results. Full article
(This article belongs to the Special Issue MOFs for Advanced Applications)
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13 pages, 3058 KiB  
Article
A Heterometallic Three-Dimensional Metal−Organic Framework Bearing an Unprecedented One-Dimensional Branched-Chain Secondary Building Unit
by Jing Chen, Meng-Yao Chao, Yan Liu, Bo-Wei Xu, Wen-Hua Zhang and David J. Young
Molecules 2020, 25(9), 2190; https://doi.org/10.3390/molecules25092190 - 7 May 2020
Cited by 7 | Viewed by 3606
Abstract
A heterometallic metal−organic framework (MOF) of [Cd6Ca4(BTB)6(HCOO)2(DEF)2(H2O)12]∙DEF∙xSol (1, H3BTB = benzene-1,3,5-tribenzoic acid; DEF = N,N′-diethylformamide; xSol. = undefined solvates [...] Read more.
A heterometallic metal−organic framework (MOF) of [Cd6Ca4(BTB)6(HCOO)2(DEF)2(H2O)12]∙DEF∙xSol (1, H3BTB = benzene-1,3,5-tribenzoic acid; DEF = N,N′-diethylformamide; xSol. = undefined solvates within the pore) was prepared by solvothermal reaction of Cd(NO3)2·4H2O, CaO and H3BTB in a mixed solvent of DEF/H2O/HNO3. The compatibility of these two divalent cations from different blocks of the periodic table results in a solid-state structure consisting of an unusual combination of a discrete V-shaped heptanuclear cluster of [Cd2Ca]2Ca′ and an infinite one-dimensional (1D) chain of [Cd2CaCa′]n that are orthogonally linked via a corner-shared Ca2+ ion (denoted as Ca′), giving rise to an unprecedented branched-chain secondary building unit (SBU). These SBUs propagate via tridentate BTB to yield a three-dimensional (3D) structure featuring a corner-truncated P41 helix in MOF 1. This outcome highlights the unique topologies possible via the combination of carefully chosen s- and d-block metal ions with polydentate ligands. Full article
(This article belongs to the Section Molecular Structure)
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11 pages, 3130 KiB  
Article
Bifunctional Heterometallic Metal-Organic Frameworks for Solvent-Free Heterogeneous Cascade Catalysis
by Mingming Zheng, Yanxiang Wang and Pingyun Feng
Catalysts 2020, 10(3), 309; https://doi.org/10.3390/catal10030309 - 8 Mar 2020
Cited by 12 | Viewed by 4098
Abstract
A family of heterometallic metal-organic frameworks (MOFs) (CPM200s) harmoniously coexisting as Lewis acids and base (azo) sites were prepared. Seven CPM200s were employed as multifunctional heterogeneous cascade catalysts for the one-pot deacetalization-Knoevenagel reaction in a solvent-free system. Benefiting from the cooperation between Lewis [...] Read more.
A family of heterometallic metal-organic frameworks (MOFs) (CPM200s) harmoniously coexisting as Lewis acids and base (azo) sites were prepared. Seven CPM200s were employed as multifunctional heterogeneous cascade catalysts for the one-pot deacetalization-Knoevenagel reaction in a solvent-free system. Benefiting from the cooperation between Lewis acids from the open metal sites and base sites from the ligands, the CPM200s showed high activity and selectivity for the tandem reaction. The heterometallic 3D porous framework reported here not only offers a combination of two opposite active sites in the same framework of materials but also increases mass transfer of the substrate, thus maximizing the efficiency and substrate selectivity of the bifunctional catalysts. The CPM200s showed the highest turnover frequency (TOF), outperforming that of the reported MOFs in tandem with the deacetalization-Knoevenagel reaction. A strong correlation between the TOF and charge-to-radius ratio (z/r) of metal ions in the CPM200s was observed for the first time. The bifunctional CPM200s catalysts can be reused five times without significant loss of activity. Full article
(This article belongs to the Special Issue Multifunctional Heterogeneous Catalysis)
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