Periodic Reporting for period 1 - LIVINGPORE (Bringing Nanospace to Life by Adapting Pore Environments to Chemical Complexity)
Période du rapport: 2023-01-01 au 2025-06-30
Porous materials play a critical role in chemical separation, catalysis, and biotechnological applications, yet existing frameworks often lack the ability to dynamically respond to their environment. Metal-Organic Frameworks (MOFs), a class of crystalline porous materials, offer tunable structures and high surface areas, but their potential remains largely untapped due to their typically rigid architectures.
LIVINGPORE is an ERC-funded research project that introduces a paradigm shift in porous material design by developing adaptive MOFs with programmable porosity. By integrating amino acid sequences within MOF structures, we aim to create materials that selectively recognize and transform molecular guests. This approach leverages principles of protein folding and molecular recognition, providing a new level of structural and functional control in crystalline materials.
The project is built upon two complementary concepts:
• Transformable Porosity – The ability of MOFs to adjust their pore geometry and chemical environment in response to specific guest molecules, enabling selective separation of enantiomers, biomolecules, or industrially relevant compounds.
• Transformative Porosity – The capacity of MOFs to actively modify the conformation and function of encapsulated molecules, particularly enzymes, facilitating applications in biocatalysis and biomolecular engineering.
To achieve these objectives, LIVINGPORE integrates high-throughput computational modeling, synthetic chemistry, and advanced characterization techniques. The development of a topology-templated algorithm allows for the predictive design of hypothetical MOF structures, accelerating the discovery process through iterative feedback between computational simulations and experimental synthesis. Additionally, x-ray and electron diffraction structural analysis combined with molecular dynamics simulations are employed to elucidate host-guest interactions at an atomic level.
The expected impact of LIVINGPORE spans multiple scientific and technological domains:
• Pharmaceutical Science – Enabling enantioselective separation and targeted drug delivery, enhancing the efficiency of therapeutic molecule production.
• Sustainable Chemistry – Developing porous materials for selective adsorption and catalytic conversion of pollutants, contributing to greener chemical processes.
• Biotechnology – Advancing enzyme stabilization and functional enhancement within confined environments, with potential applications in industrial biocatalysis and biofuel production.
By redefining the functional capabilities of porous molecular frameworks, LIVINGPORE bridges the gap between synthetic materials and biological systems, unlocking new pathways for precision molecular recognition and catalysis. This research not only advances fundamental scientific understanding but also holds promise for technological innovations in medicine, environmental science, and chemical engineering.
LIVINGPORE is an ERC-funded research project that introduces a paradigm shift in porous material design by developing adaptive MOFs with programmable porosity. By integrating amino acid sequences within MOF structures, we aim to create materials that selectively recognize and transform molecular guests. This approach leverages principles of protein folding and molecular recognition, providing a new level of structural and functional control in crystalline materials.
The project is built upon two complementary concepts:
• Transformable Porosity – The ability of MOFs to adjust their pore geometry and chemical environment in response to specific guest molecules, enabling selective separation of enantiomers, biomolecules, or industrially relevant compounds.
• Transformative Porosity – The capacity of MOFs to actively modify the conformation and function of encapsulated molecules, particularly enzymes, facilitating applications in biocatalysis and biomolecular engineering.
To achieve these objectives, LIVINGPORE integrates high-throughput computational modeling, synthetic chemistry, and advanced characterization techniques. The development of a topology-templated algorithm allows for the predictive design of hypothetical MOF structures, accelerating the discovery process through iterative feedback between computational simulations and experimental synthesis. Additionally, x-ray and electron diffraction structural analysis combined with molecular dynamics simulations are employed to elucidate host-guest interactions at an atomic level.
The expected impact of LIVINGPORE spans multiple scientific and technological domains:
• Pharmaceutical Science – Enabling enantioselective separation and targeted drug delivery, enhancing the efficiency of therapeutic molecule production.
• Sustainable Chemistry – Developing porous materials for selective adsorption and catalytic conversion of pollutants, contributing to greener chemical processes.
• Biotechnology – Advancing enzyme stabilization and functional enhancement within confined environments, with potential applications in industrial biocatalysis and biofuel production.
By redefining the functional capabilities of porous molecular frameworks, LIVINGPORE bridges the gap between synthetic materials and biological systems, unlocking new pathways for precision molecular recognition and catalysis. This research not only advances fundamental scientific understanding but also holds promise for technological innovations in medicine, environmental science, and chemical engineering.
During this period, LIVINGPORE has made significant progress in both transformable and transformative porosity, achieving key milestones in the synthesis and characterization of adaptive frameworks The most significant technical and scientific advancements include:
• Development of Organic Platforms for synthesis of bispyrazolate oligopeptides: a high-yield synthetic platform for bispyrazole peptides was established, enabling gram-scale production of organic ligands with the general formula Pz-X-Pz (single amino acid) and Pz-XY-Pz (dipeptide).
• High-Throughput (HT) Synthetic Chemistry for Transformable Porosity : systematic synthetic screening led to the development of peptide bispyrazolate frameworks, which exhibit both high chemical stability and tunable conformational flexibility. These materials have been functionalized with multiple amino acids, demonstrating their broad versatility and potential for molecular recognition.
• Advanced Crystallographic Studies and Electron Diffraction: Optimization of electron diffraction techniques enabled structural characterization of MOFs in different structural states confirming the dynamic flexibility of these materials to guest uptake/removal.
• Surface Functionalization for Synthetic Chaperones: To develop MOFs as synthetic chaperones, a click-chemistry-based functionalization method was implemented. This innovative strategy allows for the systematic and stable grafting of amino acids onto mesoporous frameworks, enhancing their compatibility with protein encapsulation and molecular recognition.
• Generation of Ultraporous MOFs: We have discovered a methodology that utilizes our own MOF families based on heterometallic Ti2Ca2 clusters as templates. The reaction of these microporous frameworks with metal solutions results in a change in the cluster’s nuclearity, inducing the formation of mesoporous crystals with cavities close to 4 nm and yields approaching 100%. The availability of this synthetic tool will enable the synthesis of multiple porous crystals compatible with the encapsulation of enzymes with varying sizes.
• Development of Organic Platforms for synthesis of bispyrazolate oligopeptides: a high-yield synthetic platform for bispyrazole peptides was established, enabling gram-scale production of organic ligands with the general formula Pz-X-Pz (single amino acid) and Pz-XY-Pz (dipeptide).
• High-Throughput (HT) Synthetic Chemistry for Transformable Porosity : systematic synthetic screening led to the development of peptide bispyrazolate frameworks, which exhibit both high chemical stability and tunable conformational flexibility. These materials have been functionalized with multiple amino acids, demonstrating their broad versatility and potential for molecular recognition.
• Advanced Crystallographic Studies and Electron Diffraction: Optimization of electron diffraction techniques enabled structural characterization of MOFs in different structural states confirming the dynamic flexibility of these materials to guest uptake/removal.
• Surface Functionalization for Synthetic Chaperones: To develop MOFs as synthetic chaperones, a click-chemistry-based functionalization method was implemented. This innovative strategy allows for the systematic and stable grafting of amino acids onto mesoporous frameworks, enhancing their compatibility with protein encapsulation and molecular recognition.
• Generation of Ultraporous MOFs: We have discovered a methodology that utilizes our own MOF families based on heterometallic Ti2Ca2 clusters as templates. The reaction of these microporous frameworks with metal solutions results in a change in the cluster’s nuclearity, inducing the formation of mesoporous crystals with cavities close to 4 nm and yields approaching 100%. The availability of this synthetic tool will enable the synthesis of multiple porous crystals compatible with the encapsulation of enzymes with varying sizes.
• Systematic Programming of Pore Response in Transformable Frameworks: We have advanced the design of metal-peptide frameworks by integrating peptide-based linkers with rigid building blocks, creating highly controlled, modular materials. Unlike conventional supramolecular assembly, our approach enhances mechanical robustness, stability, and adaptability while ensuring precise pore responsiveness. This innovation addresses key limitations in biomimetic materials, such as framework collapse and solvent-induced degradation, enabling their broader application in molecular recognition, separation, and catalysis.
• Dynamic Bonding in Molecular Frameworks: Our results reveal that coordination bonds in soft-metal frameworks can be reversibly broken and reformed by guest molecule interactions, demonstrating a solid-state equivalent of dynamic covalent bonding. This discovery introduces adaptive reorganization mechanisms in porous crystals, a feature previously exclusive to supramolecular chemistry. It challenges the conventional rigidity of zeolites and activated carbons, paving the way for new dynamic sorbents with tunable porosity and function.
• Dynamic Bonding in Molecular Frameworks: Our results reveal that coordination bonds in soft-metal frameworks can be reversibly broken and reformed by guest molecule interactions, demonstrating a solid-state equivalent of dynamic covalent bonding. This discovery introduces adaptive reorganization mechanisms in porous crystals, a feature previously exclusive to supramolecular chemistry. It challenges the conventional rigidity of zeolites and activated carbons, paving the way for new dynamic sorbents with tunable porosity and function.