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1. Producing cold from heat with aluminum carboxylate-based metal-organic frameworks

Author

Effrosyni Gkaniatsou, Chaoben Chen, Frédéric S. Cui, Xiaowei Zhu, Paul Sapin, Farid Nouar, Cédric Boissière, Christos N. Markides, Jan Hensen, and Christian Serre

Subjects
metal-organic frameworks, sorption cooling, solar cooling, thermally driven, aluminum carboxylate, upscale synthesis, Physics, QC1-999
Abstract

Summary: Worldwide cooling energy demands will increase by four times by 2050. Thermally driven cooling technology is an alternative solution to electric heat pumps in removing hazardous refrigerants and harnessing renewables and waste heat. We highlight the advantages of water-stable microporous aluminum-carboxylate-based metal-organic frameworks, or Al-MOFs, as sorbents in the application of producing cold from heat. Here, we synthesize the Al-MOFs with green and scalable processes, which are prerequisites for exploring various industrial and civil applications. A proof-of-concept full-scale adsorption chiller with different Al-MOFs is built up with optimized configurations derived from various characterization techniques. The tested Al-MOFs achieve thermal efficiency above 0.6 and specific cooling power over 1 kW/kg in typical cooling scenarios. Notably, when solar thermal energy is used as the heat source in an outdoor validation, Al-MOFs are weather-resilient solutions that exhibit a stable energy conversion efficiency under fluctuating operating conditions (ambient temperature and solar irradiation).

Published
2022
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2. In Situ Synthesis of a Mesoporous MIL-100(Fe) Bacteria Exoskeleton

Author

Anastasia Permyakova, Alshaba Kakar, Jonathan Bachir, Effrosyni Gkaniatsou, Bernard Haye, Nicolas Menguy, Farid Nouar, Christian Serre, Nathalie Steunou, Thibaud Coradin, Francisco M. Fernandes, Clémence Sicard, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Matériaux et Biologie (LCMCP-MATBIO), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), ANR-19-CE08-0023,EMERGE,Conception de matériaux bio-hybrides associant entités biologiques et Metal-Organic Frameworks pour des applications environnementales(2019), and ANR-17-CE08-0009,CellsInFoams,Mousses macroporeuses cœur-coquille pour l'encapsulation de bactéries(2017)

Subjects
Synthesised, Two-component, Bacteria, Pseudomonas putida, General Chemical Engineering, Biomedical Engineering, Membrane integrity, Mesoporous, MIL-100, In-situ synthesis, Aqueous media, Exoskeleton (Robotics), Polycarboxylates, [CHIM]Chemical Sciences, General Materials Science, Cytology, Condition
Abstract

International audience; The mesoporous iron polycarboxylate MIL-100(Fe) was synthesized in the presence of Pseudomonas putida bacteria. The synthesis was performed under green conditions, i.e., pure aqueous media at 30 °C that were compatible with the preservation of the cell membrane integrity. Interestingly, the resulting biohybrid exhibited a very different microstructure than a physical mixture of the two components, as it led to the formation of a novel living material featuring an exoskeleton encapsulating individual bacteria cell. Remarkably, TEM and STEM observations on cross sections revealed that this shell was not directly in contact with the cell wall, suggesting the exopolysaccharides network promotes strong interactions with the MOF precursors, leading to high proximity between the two components.

Published
2022

3. Robust ionic liquid@MOF composite as a versatile superprotonic conductor

Author

Effrosyni Gkaniatsou, Carine Livage, Kiran Taksande, Nathalie Steunou, Sabine Devautour-Vinot, Guillaume Maurin, Corine Simonnet-Jégat, Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and ANR-11-LABX-0039,CHARMMMAT,CHimie des ARchitectures MoléculairesMultifonctionnelles et des MATériaux(2011)

Subjects
Materials science, Composite number, Proton exchange membrane fuel cell, 02 engineering and technology, Conductivity, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 7. Clean energy, 0104 chemical sciences, Inorganic Chemistry, chemistry.chemical_compound, Chemical engineering, chemistry, Ionic liquid, Anhydrous, [CHIM]Chemical Sciences, Chemical stability, 0210 nano-technology, Mesoporous material, Proton conductor
Abstract

International audience; A highly performing proton conducting composite was prepared through the impregnation of EMIMCl ionic liquid in the mesoporous MIL-101(Cr)–SO3H MOF. The resulting EMIMCl@MIL-101(Cr)–SO3H composite displays high thermal and chemical stability, alongside retention of a high amount of EMIMCl even at temperatures as high as 500 K, as well as under moisture conditions. Remarkably, this composite exhibits outstanding proton conductivity not only at the anhydrous state (σ473 K = 1.5 × 10−3 S cm−S) but also under humidity (σ(343 K/60%–80%RH) ≥ 0.10 S cm−1) conditions. This makes EMIMCl@MIL-101(Cr)–SO3H a unique candidate to act as a solid state proton conductor for PEMFC applications under versatile conditions.

Published
2021

4. Moisture-participating MOF thermal battery for heat reallocation between indoor environment and building-integrated photovoltaics

Author

Effrosyni Gkaniatsou, Jan Hensen, Frédéric S. Cui, Christian Serre, Farid Nouar, Rcgm Roel Loonen, Bin Meng, Building Performance, EIRES System Integration, and EAISI High Tech Systems

Subjects
Materials science, 02 engineering and technology, Environment, Thermal energy, 010402 general chemistry, 01 natural sciences, Automotive engineering, Added value, General Materials Science, SDG 7 - Affordable and Clean Energy, Electrical and Electronic Engineering, Built environment, Nano-porous, Moisture, Renewable Energy, Sustainability and the Environment, business.industry, Photovoltaic system, BIPV, Metal-organic frameworks, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Electricity generation, Built, Sorption, Building-integrated photovoltaics, 0210 nano-technology, business, SDG 7 – Betaalbare en schone energie, Thermal Battery
Abstract

The present deployment of photovoltaic (PV) panels on the rooftop has been far below its potential. Stakeholders often see the PV as a strong design constraint, isolated from the built environment and not adapted to their requirements. Here, we propose a new design that combines the PV panels with a metal-organic framework basedsorptive thermal battery, which serves as a multi-functional building element and is more actively involved in the indoor environment regulation. The open-loop thermal battery can stock moisture from air with 105 times its volume so that the built environment with high humidity at night is dried to a comfortable and healthy level. The moisture is removed at daytime with unpleasant solar heat, thereby cools the PV panels simultaneously,improving electricity generation by 5%. The benefits of this design can be translated into economic added value to facilitate investment decisions of building-integrated PV projects.

Published
2021

5. New Hybrid Fe-based MOF/polymer Composites for the photodegradation of organic dyes

Author

Fabrice Morlet-Savary, Effrosyni Gkaniatsou, Chaima Brahmi, Aissam Airoudj, Clémence Sicard, Mahmoud Benltifa, Frédéric Dumur, Latifa Bousselmi, Laure Michelin, Jacques Lalevée, Cyril Vaulot, Institut de Science des Matériaux de Mulhouse (IS2M), Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Centre de Recherche et Technologies des Eaux (CERTE), Institut de Chimie Radicalaire (ICR), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), and Dumur, Frederic

Subjects
[CHIM.MATE] Chemical Sciences/Material chemistry, Materials science, 02 engineering and technology, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Photopolymer, Chemical engineering, Polymer composites, Fe based, 0210 nano-technology, Photodegradation, Photocatalytic degradation
Abstract

International audience; Metals Organic Frameworks (MOFs) are promising crystalline, embrittled materials generally produced in powdering form with varied remarkably functionalities. In contrary, polymer are flexible and processable materials. Therefore, obtaining shaped solids gathering polymer malleability and MOFs properties such as their photocatalytic activities, have attracked many reasearchers attention. This work, report the successful fruitful incorporation of two different Fe-based MOFs into a polymer matrix via a facile and cheap photopolymerization process upon mild visible light irradiation at 405 nm. The as-prepared photocomposites displayed excellent stability and photocalytic performance for several Acid Black degradation cycles. Hence, approximatively, 95% of this model dye was decomposed by the two MIL-100(Fe)/polymer and MIL-88A(Fe)/polymer composites under juste 30 min of UV lamp irradiation. Incorporation of the MOFs into the polymer was confirmed by several techniques including Scanning Electron Microscopy (SEM), Energy-dispersive X-ray analysis 2 (EDX), Transmission Electron Microscopy (TEM), X-Ray Diffraction analysis (DRX), Fourier-Transform Infrared Spectroscopy (FTIR). Furthermore, these photocatalysts exhibited a high thermal stability, excellent rigidity and low band gap energy characterized by Thermogravimetric Analysis (TGA) Atomic Force Microscopy (AFM), Dynamic Mechanical Analysis (DMA) and UV-Visible diffuse reflectance spectroscopy, respectively.

Published
2021

6. Metal–Organic Framework Based 1D Nanostructures and Their Superstructures: Synthesis, Microstructure, and Properties

Author

Subharanjan Biswas, Clémence Sicard, Eddy Dumas, Nicolas Menguy, Ali Saad, Effrosyni Gkaniatsou, Nathalie Steunou, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), and Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Nanostructure, Materials science, General Chemical Engineering, Metal organic frameworks, Nanotechnology, 02 engineering and technology, General Chemistry, Superstructures, 010402 general chemistry, 021001 nanoscience & nanotechnology, Microstructure, 01 natural sciences, 0104 chemical sciences, Nanostructures, Materials Chemistry, Genetics, [CHIM]Chemical Sciences, Metal-organic framework, 0210 nano-technology, Crystallization
Abstract

International audience; Owing to their high and tunable porosity as well as great chemical diversity, metal–organic frameworks (MOFs) have shown great promise over the past 20 years for a wide range of applications, including gas storage/separation, catalysis, and biomedicine. To date, MOF nanoparticles (NPs) have mostly been obtained as polycrystalline powders or spherical nanocrystals while anisotropic MOFs nanocrystals have been less explored and are of interest in the fields of catalysis, sensing, and electronics. One of the main challenges for the practical application of MOFs is thus to control the crystal size, morphology, and multiscale porosity of these materials while developing adequate shaping strategies. In this review, we cover recent advances in the different synthetic strategies of one-dimensional (1D) MOF nanocrystals as well as hierarchical porous superstructures based on tubular MOFs. We describe the architectures based on MOFs nanotubes (NTs), nanowires (NWs), and nanorods (NRs). Our discussion is focused on the synthetic approaches that drive the structure, crystallinity, size, and morphology of these hierarchical porous hybrid materials. Finally, their potential for different applications is presented.

Published
2021

7. MOFs industrialization: a complete assessment of production costs

Author

Moisés L. Pinto, Christian Serre, Effrosyni Gkaniatsou, Farid Nouar, Maria Inês Severino, Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), and Universidade de Lisboa (ULISBOA)

Subjects
Waste management, Production cost, Scale (chemistry), Industrial scale, 02 engineering and technology, Raw material, [SHS.ECO]Humanities and Social Sciences/Economics and Finance, 010402 general chemistry, 021001 nanoscience & nanotechnology, Investment (macroeconomics), 01 natural sciences, 7. Clean energy, Bioplastic, 0104 chemical sciences, [CHIM.GENI]Chemical Sciences/Chemical engineering, 8. Economic growth, Environmental science, Production (economics), Industrial Development, Physical and Theoretical Chemistry, 0210 nano-technology, Batch production, JEL: L - Industrial Organization/L.L6 - Industry Studies: Manufacturing/L.L6.L65 - Chemicals • Rubber • Drugs • Biotechnology, Metal-Organic Frameworks
Abstract

International audience; The potential of safe and low-cost batch production processes for Metal-Organic Frameworks (MOFs) at an industrial scale has been evaluated based on the prototypical MOF MIL-160(Al), a bio-derived material of high practical interest that can be made with a high space-time yield using green ambient pressure conditions. A simple method to calculate the production cost of this material has been determined based on a simulated process constructed with the data collected from laboratory pilot largescale tests taking into account for the first time in MOF cost evaluation all the process parameters such as the scale, the cost of the raw materials, recirculation, and washing. The investment for a production plant established the ground for the estimation of the complete cost. The expected cost ranged from ca. 55 $ per kg at 100 tons per year down to 29.5 $ per kg for 1 kton per year production with longer term perspectives of reaching costs below 10 $ per kg once the bio-derived ligand is considered for the large-scale production of bioplastics.

Published
2021

8. Enhancing microperoxidase activity and selectivity: immobilization in metal-organic frameworks

Author

Nathalie Steunou, Christian Serre, Rémy Ricoux, Effrosyni Gkaniatsou, Clémence Sicard, Jean-Pierre Mahy, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), UMR 8124 Laboratoire de Chimie Bioorganique et Bioinorganique, Université Paris Sud (Paris 11), Chimie bio-organique et bio-inorganique (CBOBI), and Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Cytochrome, biology, 010405 organic chemistry, Chemistry, Proteolytic enzymes, General Chemistry, 010402 general chemistry, 01 natural sciences, Combinatorial chemistry, 0104 chemical sciences, 13. Climate action, Biocatalysis, biology.protein, [CHIM]Chemical Sciences, Metal-organic framework, Selectivity, ComputingMilieux_MISCELLANEOUS
Abstract

Microperoxidases 8 (MP8) and 11 (MP11) are heme-containing peptides obtained by the proteolytic digestion of Cytochrome c. They act as mini-enzymes that combine both peroxidase-like and Cytochrome P450-like activities that may be useful in the synthesis of fine chemicals or in the degradation of environmental pollutants. However, their use is limited by their instability in solution due to (i) the bleaching of the heme in the presence of an excess of H2O2, (ii) the decoordination of the distal histidine ligand of the iron under acidic conditions and, (iii) their tendency to aggregate in aqueous alkaline solutions, even at low concentrations. Additionally, both MP8 and MP11 show relatively low selectivity, due to the lack of control of the substrates by a specific catalytic pocket on the distal face of the heme. Both stability and selectivity issues can be effectively addressed by immobilization of microperoxidases in solid matrices, which can also lead to their possible recycling from the reaction medium. Considering their relatively small size, the pore inclusion of MPs into Metal-Organic Frameworks appeared to be more adequate compared to other immobilization methods that have been widely investigated for decades. The present minireview describes the catalytic activities of MP8 and MP11, their limitations, and various results describing their immobilization into MOFs which led to MP11- or MP8@MOF hybrid materials that display good activity in the oxidation of dyes and phenol derivatives, with remarkable recyclability due to the stabilization of the MPs inside the MOF cavities. An example of selective oxidation of dyes according to their charge by MP8@MOF hybrid materials is also highlighted.

Published
2019

10. Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction

Author

Sergio Navalón, Mercedes Alvaro, Andrea Santiago-Portillo, Jean-Marc Greneche, Effrosyni Gkaniatsou, Christian Serre, Nathalie Steunou, Clémence Sicard, Mónica Giménez-Marqués, Cristina Vallés-García, Hermenegildo Garcia, Ministerio de Economía y Competitividad (España), Ministerio de Ciencia, Innovación y Universidades (España), Generalitat Valenciana, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Instituto de Tecnología Química (ITQ), Universitat Politècnica de València (UPV)-Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), Le Mans Université (UM)-Centre National de la Recherche Scientifique (CNRS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP UMR8004 FRE2000), and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris)

Subjects
Crystal structure, 010402 general chemistry, 01 natural sciences, Hydrothermal circulation, Ion, Catalysis, QUIMICA ORGANICA, QUIMICA ANALITICA, [CHIM]Chemical Sciences, General Materials Science, Lewis acids and bases, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], Materials, ComputingMilieux_MISCELLANEOUS, Mossbauer spectrometry, [PHYS]Physics [physics], 010405 organic chemistry, Renewable Energy, Sustainability and the Environment, Chemistry, General Chemistry, Prins reaction, 0104 chemical sciences, Chemical stability, Química orgànica, Nuclear chemistry
Abstract

[EN] This work highlights the benefit of designing mixed-metal (Cr/Fe) MOFs for enhanced chemical stability and catalytic activity. A robust and stable mixed-metal MIL-101(Cr/Fe) was prepared through a HF-free direct hydrothermal route with Fe(3+)content up to 21 wt%. The incorporation of Fe(3+)cations in the crystal structure was confirmed by(57)Fe Mossbauer spectrometry. The catalytic performance of the mixed metal MIL-101(Cr/Fe) was evaluated in the Prins reaction. MIL-101(Cr/Fe) exhibited a higher catalytic activity compared to MIL-101(Cr), improved chemical stability compared to MIL-101(Fe) and a higher catalytic activity for bulky substrates compared to MIL-100(Fe).In situinfra-red spectroscopy study suggests that the incorporation of Fe(3+)ions in MIL-101 structure leads to an increase in Lewis acid sites. It was thus concluded that the predominant role of Cr(3+)ions was to maintain the crystal structure, while Fe(3+)ions enhanced the catalytic activity., Financial support by the Spanish Ministry of Economy and Competitiveness (Severo Ochoa, CTQ2018-890237-CO2-R1 and Maria de Maeztu, CEX2019-000919-M), is gratefully acknowledged. Generalidad Valenciana is also thanked for funding (Prometeo 2017/083). S. N. thanks financial support by the Ministerio de Ciencia, Innovacion y Universidades (RTI 2018-099482-A-I00 project), Fundacion Ramon Areces (XVIII Concurso Nacional para la Adjudicacion de Ayudas a la Investigacion en Ciencias de la Vida y de la Materia, 2016), and Generalitat Valenciana grupos de investigacion consolidables 2019 (ref: AICO/2019/214) project. E. G. thanks the ANR-11-LABEX-0039 (LabEx CHARM3AT) for financial support. M. G.-M thanks support from "la Caixa" Foundation (LCF/BQ/PI19/11690022) and Generalitat Valenciana (SEJI/2020/036).

Published
2020

11. Encapsulation of Microperoxidase-8 in MIL-101(Cr)-X Nanoparticles: Influence of Metal-Organic Framework Functionalization on Enzymatic Immobilization and Catalytic Activity

Author

Christian Serre, Kalani Kariyawasam, Jean-Pierre Mahy, Nathalie Steunou, Effrosyni Gkaniatsou, Samanta Salas, Clémence Sicard, I. Stenger, Benhui Fan, Narjes Ayoub, Rémy Ricoux, Gilles Patriarche, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie Moléculaire et des Matériaux d'Orsay (ICMMO), Institut de Chimie du CNRS (INC)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Groupe d'Etude de la Matière Condensée (GEMAC), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Centre de Nanosciences et de Nanotechnologies (C2N), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), LabEx ASLAN, and This work was supported by the ANR-11-LABEX-0039 (LabEx charm 3 at).

Subjects
Immobilized enzyme, biocatalysis, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Catalysis, chemistry.chemical_compound, [CHIM]Chemical Sciences, General Materials Science, metal-organic frameworks, ComputingMilieux_MISCELLANEOUS, enzyme immobilization, Thioanisole, peroxidase activity, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 021001 nanoscience & nanotechnology, 0104 chemical sciences, enzyme, Monomer, chemistry, Biocatalysis, immobilization, Surface modification, functionalization, Metal-organic framework, 0210 nano-technology, Nuclear chemistry
Abstract

International audience; Microperoxidase 8 (MP8) was immobilized within MIL-101(Cr) bearing terephthalate linkers with functionalized groups (-NH2 and -SO3H). A synthesis protocol for MIL-101(Cr)-SO3H that avoids the use of toxic Cr(VI) and HF was developed. The electrostatic interactions between the MP8 molecules and the MOF matrices were found to be crucial for a successful immobilization. Raman spectroscopy revealed the dispersion of the immobilized MP8 molecules in MIL-101(Cr)-X matrices as monomers without aggregation. The presence of functional groups resulted in higher amounts of immobilized MP8 in comparison to the bare MIL-101(Cr). The catalytic activity of MP8@MIL-101(Cr)-NH2 per material mass was higher than that for MP8@MIL-101(Cr). The presence of free amino groups can thus improve the immobilization efficiency, leading to a higher amount of catalytically active species and improving the subsequent catalytic activity of the heterogeneous biocatalysts. MP8@MIL(Cr)-X also successfully catalyzed the selective oxidation of thioanisole derivatives into sulfoxides.

Published
2020

12. Metal–organic frameworks: a novel host platform for enzymatic catalysis and detection

Author

Christian Serre, Jean-Pierre Mahy, Nathalie Steunou, Effrosyni Gkaniatsou, Rémy Ricoux, and Clémence Sicard

Subjects
Materials science, Process Chemistry and Technology, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Enzyme catalysis, Mechanics of Materials, General Materials Science, Metal-organic framework, Electrical and Electronic Engineering, 0210 nano-technology, Host (network)
Abstract

The use of metal–organic frameworks (MOFs) as immobilization matrices for enzymes as a platform for emerging applications is reported. In addition to an overview of strategies developed to prepare enzyme–MOF biocomposites, the features that render MOFs interesting matrices for bio-immobilization are highlighted along with their potential benefits beyond a solid-state support in the design of innovative biocomposites.

Published
2017

13. Multivariable Sieving and Hierarchical Recognition for Organic Toxics in Nonhomogeneous Channel of MOFs

Author

Charlotte Martineau, Mohammad Wahiduzzaman, Qi Zhang, Stefan Henfling, Christian Serre, Narjes Ayoub, Yuanjing Cui, Guodong Qian, Effrosyni Gkaniatsou, Farid Nouar, Sujing Wang, Clémence Sicard, Guillaume Maurin, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Zhejiang University, Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), and Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, multivariable sieving, General Chemical Engineering, hierarchical recognition, 02 engineering and technology, 010402 general chemistry, Molecular sieve, 01 natural sciences, Biochemistry, Materials Chemistry, Environmental Chemistry, Molecule, [CHIM]Chemical Sciences, Surface charge, Porosity, metal-organic frameworks, Multivariable calculus, heterogeneous channels, Biochemistry (medical), General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, Potential energy surface, Metal-organic framework, 0210 nano-technology, Communication channel
Abstract

Highlights • Hierarchical recognition strategy established with heterogeneous channels in MOFs • Ultrafine regulation of aperture size from 3.2 to 7.2 Å based on MIL-140s • Heterogeneous electronic distribution induces various non-covalent interactions • Hierarchical recognition strategy shows multivariable separation for organic toxics; International audience; Developing optimal molecular sieves, which are able to perform multivariable aqueous sieving of diverse harmful organics, is of practical significance in chemistry and environmental protection. Current porous sieves, however, can only recognize organics on the basis of two variables (charge and size), which is far from enough because of the multi-complexity of the toxics. Herein, we report a series of isostructural metal-organic frameworks, MIL-140s [ZrO(O 2C–R–CO 2)], with triangular hydrophobic channels for the separation of dyes and practical toxics, such as high carcinogenic pesticides and persistent organic pollutants. Theoretical calculations demonstrate the key role of nonhomogeneous electron distribution within channels for recognition of various guest molecules. Multivariable sieving for both dyes and practical toxics has been validated by both separation experiments and DFT calculation. The sieving mechanisms are revealed through presenting an outside-in theoretical model, hierarchical recognition, by the regulation of surface charge, pore size, and potential energy surface of MIL-140s.

Published
2019

14. Influence of Filler Pore Structure and Polymer on the Performance of MOF-Based Mixed-Matrix Membranes for CO 2 Capture

Author

Paul A. Wright, Timothy Johnson, Xinlei Liu, Effrosyni Gkaniatsou, Marvin Benzaqui, Freek Kapteijn, Jorge Gascon, Angelica Orsi, Christian Serre, Nathalie Steunou, Magdalena M. Lozinska, Clémence Sicard, Anahid Sabetghadam, Catalysis Engineering - ChemE, Delft University of Technology, Van der Maasweg 9, 2629HZ Delft, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), EaStCHEM School of Chemistry, University of St Andrews [Scotland], Johnson Matthey Technology Centre, Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), European Commission, University of St Andrews. School of Chemistry, and University of St Andrews. EaSTCHEM

Subjects
Filler (packaging), Metal-organic framework, Polymers, NDAS, 02 engineering and technology, 010402 general chemistry, Thermal diffusivity, 01 natural sciences, Catalysis, [CHIM]Chemical Sciences, QD, Gas separation, Solubility, Porosity, chemistry.chemical_classification, Membranes, Chemistry, Organic Chemistry, General Chemistry, Polymer, Composite materials, Metal-organic frameworks, QD Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Membrane, Chemical engineering, Pore structure, 0210 nano-technology
Abstract

International audience; Membrane gas separation units are gaining increasing attention owing to their relatively low energy consumption, ease of operation and environmental aspects. Metal-organic framework (MOF)-mixed matrix membranes (MMMs) are proposed as alternative materials delivering both the promising performance benefits from embedded MOF fillers and the processing features of polymers. In order to gain insight into the influence of MOF filler and polymer on membrane performance, eight different composites are studied by combining four MOFs and two polymers. MOF materials (NH2-MIL-53(Al), MIL-69(Al), MIL-96(Al) and ZIF-94(Zn)) with various chemical functionalities, topologies, and dimensionalities of porosity were employed as fillers, while two typical polymers with different permeability-selectivity properties (6FDA-DAM and Pebax) were deliberately selected as matrices. Separation results are rationalized on the basis of thorough characterization of the main components of the composites. The observed differences in membrane performance in the separation of CO2 from N2 are explained on the basis of gas solubility, diffusivity properties and compatibility between the filler and polymer phases.

Published
2018

15. Influence of Filler Pore Structure and Polymer on the Performance of MOF-Based Mixed-Matrix Membranes for CO

Author

Anahid, Sabetghadam, Xinlei, Liu, Marvin, Benzaqui, Effrosyni, Gkaniatsou, Angelica, Orsi, Magdalena M, Lozinska, Clemence, Sicard, Timothy, Johnson, Nathalie, Steunou, Paul A, Wright, Christian, Serre, Jorge, Gascon, and Freek, Kapteijn

Abstract

To gain insight into the influence of metal-organic framework (MOF) fillers and polymers on membrane performance, eight different composites were studied by combining four MOFs and two polymers. MOF materials (NH

Published
2018

16. Enzyme Encapsulation in Mesoporous Metal–Organic Frameworks for Selective Biodegradation of Harmful Dye Molecules

Author

Nathalie Steunou, Linda Benahmed, Clémence Sicard, Christian Serre, Effrosyni Gkaniatsou, Qi Zhang, Jean-Pierre Mahy, Flavien Bourdreux, Rémy Ricoux, Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie Moléculaire et des Matériaux d'Orsay (ICMMO), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Institut des Matériaux Poreux de Paris (IMAP ), Département de Chimie - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Ecole Superieure de Physique et de Chimie Industrielles de la Ville de Paris (ESPCI Paris), and Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Models, Molecular, Immobilized enzyme, Surface Properties, 02 engineering and technology, 010402 general chemistry, Redox, 01 natural sciences, Catalysis, chemistry.chemical_compound, Methyl orange, Particle Size, Coloring Agents, Metal-Organic Frameworks, Molecular Structure, Chemistry, [SDE.IE]Environmental Sciences/Environmental Engineering, fungi, General Chemistry, General Medicine, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, Hydrogen-Ion Concentration, Enzymes, Immobilized, 021001 nanoscience & nanotechnology, Combinatorial chemistry, 0104 chemical sciences, Peroxidases, Biocatalysis, Nanoparticles, Metal-organic framework, Selectivity, Mesoporous material, 0210 nano-technology, Porosity
Abstract

Microperoxidase-8, a small, peroxidase-type enzyme was immobilized into nanoparticles of the mesoporous and ultra-stable metal-organic framework (MOF) MIL-101(Cr). The immobilized enzyme fully retained its catalytic activity and exhibited enhanced resistance to acidic conditions. The biocatalyst was reusable and showed a long-term stability. By exploiting the properties of the MOF's framework, we demonstrated, for the first time, that the MOF matrix could act in synergy with the enzyme (Microperoxidase-8) and enhance selectivity the oxidation reaction of dyes. The oxidation rate of the harmful negatively charged dye (methyl orange) was significantly increased after enzyme immobilization, probably as a result of the pre-concentration of the methyl orange reactant owing to a charge matching between this dye and the MOF.

Published
2018

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