jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Natalie Hanheiser | Yina Jiang | Christian Zoister | Mathias Dimde | Katharina Achazi | Chuanxiong Nie | Yuanyuan Li | Rainer Haag | Abhishek Kumar Singh
Source: Angewandte Chemie International Edition (article, 2025-03-20)
Field: Chemistry — Organic Chemistry

Modular Synthesis of Dendritic Oligo‐Glycerol Cationic Surfactants for Enhanced Antibacterial Efficacy Bacterial infections and antibiotic resistance present an ever-increasing threat to human health worldwide, and medicine urgently needs new alternatives for the successful treatment of bacterial infections. Cationic surfactants have proven to be effective antibacterial agents due to their ability to disrupt bacterial membranes, inhibit biofilm formation, and combat a broad spectrum of pathogens. We employed a orthogonal click chemistry strategy for the efficient modular synthesis of six novel cationic surfactants. Our results emphasize the strong correlation between the surfactant design and its antibacterial potential. Among these six cationic surfactants we identified a prime candidate, which possessed an impressive antibacterial effect against gram-positive and gram-negative bacteria, including drug-resistant strains. We found that our surfactant can prevent biofilm formation and eradicate already existing biofilms. Cryo-TEM imaging was used to reveal the membrane-disrupting properties of the surfactant. In-vivo wound healing experiments underline the surfactants' ability to inhibit wound infections. Cationic surfactants often face the challenge of balancing strong antibacterial activity with minimal cytotoxicity. Our strategic design and orthogonal click chemistry approach have enabled precise fine-tuning of molecular structures to achieve an optimal balance between antibacterial efficacy and biocompatibility, effectively overcoming this critical limitation. Cationic polymerization ; Antibacterial activity ; Pulmonary surfactant ; Biofilm ; Chemistry ; Biocompatibility ; Combinatorial chemistry ; Bacteria ; Click chemistry ; Bacterial cell structure ; Nanotechnology ; Materials science ; Biology ; Organic chemistry ; Biochemistry Antimicrobial agents and applications ; Antimicrobial Peptides and Activities ; Click Chemistry and Applications
Authors: Isaac Alcón | Aron W. Cummings | Esteve Ribas | Stephan Roche | Aitor Mugarza
Source: Nanoscale Advances (review, 2025-01-01)
Field: Materials Science — Materials Chemistry

Progress on quantum transport engineering in atomically precise anisotropic nanoporous graphene Bottom-up on-surface synthesis has demonstrated an impressive capability to realize desired carbon nanomaterials with atomic precision, also referred to as carbon nanoarchitectures. By using chemically tailored organic building blocks, it is possible to obtain virtually any carbon nanoarchitecture, with equally tunable electronic and magnetic properties. Among all known carbon nanoarchitectures, graphene nanoribbons (GNRs) have become the most extensively studied for nanoelectronics, due to their conductive π-conjugated structure and semiconducting nature. In this review, we summarize the progress made on a particular type of nanoporous graphenes (NPGs), conceived as 2D arrays of laterally bonded GNRs. Due to their relative novelty, these GNR-based NPGs have not yet acquired the same global attention as their predecessors (GNRs). However, recent progress suggests that these nanomaterials may play a central role in future carbon nanoelectronics and spintronics. This is due in large part to the ability to fine tune, both by chemical design and by external means, the electronic coupling between neighbouring GNRs within the NPG, thereby enabling precise control over the anisotropic properties of these materials, as demonstrated by various theoretical studies. In this review, we summarize the different approaches that have been proposed to tune such inter-ribbon coupling and, thus, the anisotropy. Overall, these studies underscore the unique platform that GNR-based NPGs provide for tailoring quantum electronic properties and two-dimensional anisotropy. As the field progresses, this capability could be harnessed for targeted applications at the molecular scale or even the atomic scale. Graphene ; Nanoporous ; Nanomaterials ; Nanotechnology ; Materials science ; Carbon fibers ; Quantum ; Carbon quantum dots ; Quantum dot ; Physics ; Composite number ; Composite material Graphene research and applications ; Surface Chemistry and Catalysis ; Nanomaterials for catalytic reactions
Authors: Evan A. Bisirri | Joel L. Kaar | Daniel K. Schwartz
Source: Langmuir (article, 2025-02-20)
Field: Materials Science — Surfaces, Coatings and Films

High-Throughput Screening Identifies Anionic Polymer Supports that Improve Enzyme Activity at Low pH and High Temperature Elevated temperatures and nonoptimal pH can destabilize enzyme structure or change the protonation state of catalytic residues resulting in attenuated catalytic performance. Enzyme immobilization on polymer supports enables the fine-tuning of highly varied vicinal chemistries to improve enzyme performance by promoting correctly folded enzyme structure and adjusting the local microenvironment to more favorable conditions. Herein, we sought to investigate how multicomponent random copolymer brushes composed of monomers with anionic, cationic, neutral (zwitterionic, and mixed-charge), and aromatic properties stabilize covalently tethered lipase A from<i>Bacillus subtilis</i> at low pH and high temperature. Polymer brush compositions were screened using a high-throughput approach involving the combinatorial synthesis of random copolymer brushes and in situ characterization of immobilized lipase function. Although cationic supports provided a modest improvement over soluble lipase in maximum activity and thermal stability at low pH, more substantial enhancements in lipase stability were observed for anionic and neutral zwitterionic polymer supports, resulting in increases in temperature optima as great as 40 °C (from 40 to 80 °C) and an increase in maximum activity by more than 300%. These observations were counter to expectations regarding the role of surface charge on local pH and were attributed instead to the preservation of enzyme structure due to stabilizing electrostatic interactions between negatively charged polymer moieties and the net positively charged surface of lipase A. Our findings suggest that the stabilization of enzyme structure by charged polymers may offset unfavorable local changes in pH in certain situations, while in other situations these effects may be synergistic. Throughput ; Chemistry ; High-throughput screening ; Polymer ; Enzyme ; Enzyme assay ; Chemical engineering ; Biochemistry ; Organic chemistry ; Computer science Polymer Surface Interaction Studies ; Electrochemical sensors and biosensors ; Enzyme Catalysis and Immobilization
Authors: Deepak Bansal | Adel Nada | Samrat Ghosh | Indresh Kumar Pandey | Nicolas D. Boscher
Source: Materials Advances (article, 2025-01-01)
Field: Materials Science — Polymers and Plastics

Porphyrin-based polyimide 2D porous organic polymers: band engineering for bifunctional electrocatalytic OER and HER The development of bifunctional catalysts for overall water splitting is a rapidly advancing area of research. In this study, we report the synthesis of novel porphyrin-based polyimide polymers for electrocatalytic oxygen (OER) and hydrogen evolution reactions (HER). By assembling aminophenyl porphyrins with naphthalenetetracarboxylic dianhydride (NTCDA) linkers, donor-acceptor (D-A) architectures that enable extended π-electron delocalization and tailored frontier molecular orbitals conducive to water splitting were formed. FTIR, XPS and XRD analyses confirmed successful imidization between aminophenyl porphyrins (TAPP, NiTAPP, and CuTAPP) and NTCDA, resulting in π-π stacked two-dimensional polymer networks POP-1, POP-2, and POP-3, respectively. Band structure studies <i>via</i> XPS revealed that both imidization and metal incorporation significantly influence the electronic properties and enable the fine-tuning of the HOMO-LUMO levels for enhanced electrocatalytic activity. Electrochemical evaluations demonstrated the bifunctional nature of the polymers, with the Ni(ii)-based polymer, <i>i.e.</i>POP-2, showing the best performance. POP-2 exhibited a lower OER onset potential (1.45 V <i>vs.</i> RHE) and smaller Tafel slope (167 mV dec<sup>-1</sup>) compared to its metal-free (POP-1) and Cu(ii)-based (POP-3) analogues. Similarly, in the HER, POP-2 displayed a reduced onset potential (<i>ca.</i> 159 mV) and a lower Tafel slope (<i>ca.</i> 82 mV dec<sup>-1</sup>), attributed to the favorable redox behavior of Ni, optimal hydrogen binding energy, and enhanced charge delocalization. Electrochemical impedance spectroscopy confirmed its superior conductivity, while Mott-Schottky and XPS analyses revealed beneficial band alignment and increased charge carrier density. Long-term stability tests further validated the durability of POP-2. This work highlights the potential of metal-coordinated conjugated polymers as efficient and robust heterogeneous bifunctional electrocatalysts for overall water splitting. Bifunctional ; Polyimide ; Porphyrin ; Porosity ; Materials science ; Polymer ; Electrocatalyst ; Polymer chemistry ; Chemical engineering ; Nanotechnology ; Catalysis ; Organic chemistry ; Chemistry ; Composite material ; Electrode ; Electrochemistry ; Engineering ; Physical chemistry ; Layer (electronics) Conducting polymers and applications ; Covalent Organic Framework Applications
Authors: Abhijeet S. Gangan | Ekin D. Cubuk | Samuel S. Schoenholz | Mathieu Bauchy | N. M. Anoop Krishnan
Source: Journal of Chemical Theory and Computation (article, 2025-06-05)
Field: Materials Science — Materials Chemistry

Force-Field Optimization by End-to-End Differentiable Atomistic Simulation The accuracy of atomistic simulations depends on the precision of the force fields. Traditional numerical methods often struggle to optimize the empirical force-field parameters for reproducing the target properties. Recent approaches rely on training these force fields based on forces and energies from first-principle simulations. However, it is unclear whether these approaches will enable the capture of complex material responses such as vibrational or elastic properties. To this extent, we introduce a framework employing inner loop simulations and outer loop optimization that exploits automatic differentiation for both property prediction and force-field optimization by computing gradients of the simulation analytically. We demonstrate the approach by optimizing classical potentials such as Stillinger-Weber and EDIP for silicon and BKS for SiO<sub>2</sub> to reproduce properties like the elastic constants, vibrational density of states, and phonon dispersion. We also demonstrate how a machine-learned potential can be fine-tuned using automatic differentiation to reproduce any target property such as radial distribution functions. Interestingly, the resulting force field exhibits improved accuracy and generalizability to unseen temperatures compared to those fine-tuned on energies and forces. Finally, we demonstrate the extension of the approach to optimize the force fields toward multiple target properties. Altogether, differentiable simulations, through the analytical computation of their gradients, offer a powerful tool for both theoretical exploration and practical applications toward understanding physical systems and materials. Force field (fiction) ; Computer science ; Differentiable function ; Molecular dynamics ; End-to-end principle ; Field (mathematics) ; Computational science ; Physics ; Statistical physics ; Mathematics ; Artificial intelligence ; Mathematical analysis ; Quantum mechanics Machine Learning in Materials Science ; Nuclear Materials and Properties ; Ion-surface interactions and analysis
Authors: Dongye Li | Binbin Wang | Kunpeng Zheng | Hongni Chen | Yali Xing | Yanzhi Xia | Xiaojing Long
Source: iScience (article, 2025-02-12)
Field: Materials Science — Polymers and Plastics

Precisely tuning the electronic states of organic polymer electrocatalysts via thiophene-based moieties for enhanced oxygen reduction reaction Optimizing molecular structures in oxygen reduction reaction (ORR) is crucial for enhancing catalytic efficiency and stability, particularly with respect to the effective adsorption and conversion of reaction intermediates. Sulfur-containing heterocyclic compound thiophene can precisely modulate the electronic states and local charge densities, thereby fine-tuning the adsorption and reactivity of microporous polymers, yet, it remains a largely unexplored area. Herein, thiophene-based building blocks featuring diversified linkers into a phenyl-containing model Ph-CMP are developed, affording the thiophene-fused BPT-CMP and the thiophene-linked BCT-CMP. The electron density and adsorption capacity of the frameworks are well regulated through condensation and connecting modification, showing excellent half-wave potentials compared to the reversible hydrogen electrode, surpassing even most metal-free polymer electrocatalysts. Through theoretical calculations and experimental results, we have validated that the thiophene-fused skeleton (BPT-CMP) triggers the activation of thiophene units, with the exposed pentatomic heterocyclic carbon atom (site-3) serving as the catalytic active site. Thiophene ; Oxygen reduction ; Oxygen reduction reaction ; Polymer ; Chemistry ; Oxygen ; Combinatorial chemistry ; Reduction (mathematics) ; Nanotechnology ; Materials science ; Chemical engineering ; Organic chemistry ; Electrochemistry ; Electrode ; Physical chemistry Conducting polymers and applications ; Fuel Cells and Related Materials ; Electrocatalysts for Energy Conversion
Authors: Anna F. A. Peacock
Source: Journal of Inorganic Biochemistry (review, 2025-03-23)
Field: Materials Science — Materials Chemistry

Coiled coils as ligands for inclusion in the inorganic chemist's toolbox – For advances in MRI contrast agent design Ligands are essential tools in synthetic inorganic chemistry, enabling the fine-tuning of metal ion properties to optimize performance. Spanning from small molecules to macromolecular proteins, ligands vary widely in structure and function. De novo designed coiled coils serve as a unique bridge between these extremes, offering precise control over metal coordination. Here, we explore the application of coiled coil ligands in MRI contrast agent design, leveraging their versatility to systematically modulate the coordination chemistry and hydration state of gadolinium - the metal used in most clinical MRI contrast agents. This novel class of gadolinium-based agents demonstrates superior performance compared to existing clinical agents, highlighting the potential of coiled coil ligands. Furthermore, when coordinated to copper, these ligands form complexes that challenge the conventional notion that copper is unsuitable for MRI contrast agents. These findings establish coiled coil ligands as a powerful platform for advancing contrast agent design. Chemistry ; Toolbox ; Inclusion (mineral) ; Contrast (vision) ; Chemist ; Combinatorial chemistry ; Nanotechnology ; Organic chemistry ; Mineralogy ; Artificial intelligence ; Computer science Lanthanide and Transition Metal Complexes ; Advanced MRI Techniques and Applications ; Radioactive element chemistry and processing
Authors: Alexander Huber | Tobias Thiele | Tobias Rex | Constantin G. Daniliuc | Christoph Wölper | Rick Y. Lorberg | L. Hofmann | Cristian A. Strassert | Michael Giese | Jens Voskuhl
Source: Chemical Science (article, 2025-01-01)
Field: Materials Science — Materials Chemistry

Steric pressure in heteropentacenes modulates the photophysical properties – a molecular design strategy for functional materials Discovering the versatile ability of environment-independent solution and solid-state emission (SSSE) enabled new possibilities of fine-tuning photophysical properties, targeting specific organelles, or developing remarkable materials. Herein, we report an unprecedented design concept for SSSE by employing the "magic methyl" effect in a series of alkylated heteropentacyclic luminophores R8, Y8, and G8. Implementing an increasing amount of <i>ortho</i>-methyl groups influences the vertical electronic transitions, tuning the emission colors from red over yellow to green and inverting the preferred state of luminescence from solution to solely the solid-state or even both. An in-depth analysis was performed using X-ray diffractometric structure elucidation, packing analysis and density functional theory calculations to correlate the photophysical properties with the steric pressure induced by the methyl groups. Additionally, the application scope of these new materials was investigated. Mesoporous silica nanoparticles loaded with the three new luminophores were prepared and employed as additives for 3D printing using digital light processing. Ultimately, these stimuli-responsive molecules performed as optical sensors of microenvironmental temperature and phase transition changes in liquid crystals. Steric effects ; Luminescence ; Time-dependent density functional theory ; Density functional theory ; Materials science ; Molecule ; Photochemistry ; Solid-state ; Mesoporous material ; Chemical physics ; Nanotechnology ; Chemistry ; Optoelectronics ; Computational chemistry ; Organic chemistry ; Physical chemistry Luminescence and Fluorescent Materials ; Synthesis and Properties of Aromatic Compounds ; Organic Light-Emitting Diodes Research
Authors: Wim Hectors | Tom Delmulle | Wim Soetaert
Source: Polymers (review, 2025-07-31)
Field: Materials Science — Biomaterials

Metabolic Engineering Strategies for Enhanced Polyhydroxyalkanoate (PHA) Production in Cupriavidus necator The environmental burden of conventional plastics has sparked interest in sustainable alternatives such as polyhydroxyalkanoates (PHAs). However, despite ample research in bioprocess development and the use of inexpensive waste streams, production costs remain a barrier to widespread commercialization. Complementary to this, genetic engineering offers another avenue for improved productivity. <i>Cupriavidus necator</i> stands out as a model host for PHA production due to its substrate flexibility, high intracellular polymer accumulation, and tractability to genetic modification. This review delves into metabolic engineering strategies that have been developed to enhance the production of poly(3-hydroxybutyrate) (PHB) and related copolymers in <i>C. necator</i>. Strategies include the optimization of central carbon flux, redox and cofactor balancing, adaptation to oxygen-limiting conditions, and fine-tuning of granule-associated protein expression and the regulatory network. This is followed by outlining engineered pathways improving the synthesis of PHB copolymers, PHBV, PHBHHx, and other emerging variants, emphasizing genetic modifications enabling biosynthesis based on unrelated single-carbon sources. Among these, enzyme engineering strategies and the establishment of novel artificial pathways are widely discussed. In particular, this review offers a comprehensive overview of promising engineering strategies, serving as a resource for future strain development and positioning <i>C. necator</i> as a valuable microbial chassis for biopolymer production at an industrial scale. Cupriavidus necator ; Polyhydroxyalkanoates ; Synthetic biology ; Bioplastic ; Metabolic engineering ; Biochemical engineering ; Bioprocess ; Biopolymer ; Biotechnology ; Chemistry ; Engineering ; Biology ; Biochemistry ; Computational biology ; Bacteria ; Polymer ; Waste management ; Enzyme ; Chemical engineering biodegradable polymer synthesis and properties ; Microplastics and Plastic Pollution ; Electrospun Nanofibers in Biomedical Applications
Authors: Jedsada Jaroensan | Jitlada Vichapong
Source: Journal of Food Composition and Analysis (article, 2025-05-08)
Field: Chemistry — Analytical Chemistry

An eco-friendly method for enrichment using melamine sponge impregnated hydrophobic deep eutectic solvents prior to HPLC quantitation of sulfonamide residues Melamine ; Sulfonamide ; Chemistry ; Chromatography ; High-performance liquid chromatography ; Sponge ; Environmentally friendly ; Organic chemistry ; Biology Analytical chemistry methods development ; Analytical Chemistry and Chromatography ; Analytical Methods in Pharmaceuticals
Authors: Fantan Kong | Fu-Xin Ma | Cun‐Guang Liang | Bin Hao | Qianru Li | Akram Yasin | Rui Wang | Chongjiang Lv | Peng‐Cheng Ma
Source: Separation and Purification Technology (article, 2025-05-26)
Field: Materials Science — Surfaces, Coatings and Films

Preparation of hydrophobic/oleophilic stainless steel felt and its separation performance for water-in-oil emulsion under various conditions Emulsion ; Materials science ; Chemical engineering ; Separation (statistics) ; Chromatography ; Chemistry ; Engineering ; Mathematics Surface Modification and Superhydrophobicity ; Electrospun Nanofibers in Biomedical Applications ; Pickering emulsions and particle stabilization
Authors: Changqing Li | Zhaoying Wang | Yucheng Jin | Zhongping Li | Jong‐Pil Jeon | Songlin Zhao | Yanhua Shao | Feng Tang | Won-Yeong Kim | Runnan Guan | Jeong-Min Seo | Zonghoon Lee | Sang‐Young Lee | Jong‐Beom Baek
Source: Angewandte Chemie (article, 2025-01-22)
Field: Materials Science — Materials Chemistry

Tunable Catalytic Vertex Wall Chemistry in Metal‐free Covalent Organic Frameworks for Enhanced Oxygen Reduction Abstract Metal‐free covalent organic frameworks (COFs) have emerged as promising catalysts for the oxygen reduction reaction (ORR) because of their unique structural properties and notable stability. To enhance both catalytic activity and selectivity, a variety of linkers and linkages have been investigated in efforts to precisely engineer COFs. However, the impact of vertex structures within COFs on ORR catalysis remains largely underexplored. Here, to modulate COF catalytic performance, we introduce tunable catalytic vertex wall chemistry by introducing diverse triazine and thiophene units. The catalytic vertex wall approach allows the fine‐tuning of electronic surface states, leading to improved intermediate adsorption characteristics and accelerated ORR activity. Remarkably, the engineered COF achieved a half‐wave potential of 0.76 V, surpassing COFs modified by linker or linkage strategies. Theoretical calculations suggest that this enhanced activity arises from the strong binding affinity of OOH* intermediates to carbon atoms adjacent to the thiophene vertex, facilitating OOH* reduction to a O 2 molecule, which is the rate‐limiting step of the ORR. These findings reveal the pivotal role of vertex wall engineering in conjugated COF frameworks, and offer critical insights to advance COFs design toward superior ORR performance. Oxygen reduction ; Chemistry ; Covalent bond ; Catalysis ; Oxygen ; Metal-organic framework ; Metal ; Photochemistry ; Organic chemistry ; Adsorption Covalent Organic Framework Applications ; Electrocatalysts for Energy Conversion ; Fuel Cells and Related Materials