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2,887 result(s) for "Physiochemistry"
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Orthogonal-array dynamic molecular sieving of propylene/propane mixtures
Rigid molecular sieving materials work well for small molecules with the complete exclusion of large ones 1 – 3 , and molecules with matching physiochemical properties may be separated using dynamic molecular sieving materials 4 – 6 . Metal–organic frameworks (MOFs) 7 – 9 are known for their precise control of structures and functions on a molecular level 10 – 15 . However, the rational design of local flexibility in the MOF framework for dynamic molecular sieving remains difficult and challenging. Here we report a MOF material (JNU-3a) featuring one-dimension channels with embedded molecular pockets opening to propylene (C 3 H 6 ) and propane (C 3 H 8 ) at substantially different pressures. The dynamic nature of the pockets is revealed by single-crystal-to-single-crystal transformation upon exposure of JNU-3a to an atmosphere of C 3 H 6 or C 3 H 8 . Breakthrough experiments demonstrate that JNU-3a can realize high-purity C 3 H 6 (≥99.5%) in a single adsorption–desorption cycle from an equimolar C 3 H 6 /C 3 H 8 mixture over a broad range of flow rates, with a maximum C 3 H 6 productivity of 53.5 litres per kilogram. The underlying separation mechanism—orthogonal-array dynamic molecular sieving—enables both large separation capacity and fast adsorption–desorption kinetics. This work presents a next-generation sieving material design that has potential for applications in adsorptive separation. A dynamic molecular sieve made from a metal–organic framework with orthogonally arrayed pockets is capable of separating propylene (C 3 H 6 ) from a propylene (C 3 H 6 )/propane (C 3 H 8 ) gas mixture.
Iron-mediated organic matter decomposition in humid soils can counteract protection
Soil organic matter (SOM) is correlated with reactive iron (Fe) in humid soils, but Fe also promotes SOM decomposition when oxygen (O 2 ) becomes limited. Here we quantify Fe-mediated OM protection vs. decomposition by adding 13 C dissolved organic matter (DOM) and 57 Fe II to soil slurries incubated under static or fluctuating O 2 . We find Fe uniformly protects OM only under static oxic conditions, and only when Fe and DOM are added together: de novo reactive Fe III phases suppress DOM and SOM mineralization by 35 and 47%, respectively. Conversely, adding 57 Fe II alone increases SOM mineralization by 8% following oxidation to 57 Fe III . Under O 2 limitation, de novo reactive 57 Fe III phases are preferentially reduced, increasing anaerobic mineralization of DOM and SOM by 74% and 32‒41%, respectively. Periodic O 2 limitation is common in humid soils, so Fe does not intrinsically protect OM; rather reactive Fe phases require their own physiochemical protection to contribute to OM persistence. Reactive iron minerals protect vast amounts of terrestrial carbon from decomposition and release as CO 2 . Here the authors show that reactive iron alone does not provide sufficient protection except under strict oxic conditions—instead, iron itself promotes carbon decomposition.
Diversifying crop rotation increases food production, reduces net greenhouse gas emissions and improves soil health
Global food production faces challenges in balancing the need for increased yields with environmental sustainability. This study presents a six-year field experiment in the North China Plain, demonstrating the benefits of diversifying traditional cereal monoculture (wheat–maize) with cash crops (sweet potato) and legumes (peanut and soybean). The diversified rotations increase equivalent yield by up to 38%, reduce N 2 O emissions by 39%, and improve the system’s greenhouse gas balance by 88%. Furthermore, including legumes in crop rotations stimulates soil microbial activities, increases soil organic carbon stocks by 8%, and enhances soil health (indexed with the selected soil physiochemical and biological properties) by 45%. The large-scale adoption of diversified cropping systems in the North China Plain could increase cereal production by 32% when wheat–maize follows alternative crops in rotation and farmer income by 20% while benefiting the environment. This study provides an example of sustainable food production practices, emphasizing the significance of crop diversification for long-term agricultural resilience and soil health. Food production systems need to balance yield and sustainability. Here, the authors conduct 6 years long crop diversification field experiments in the North China Plain, showing that diversifying cereal monocultures with cash crops and legumes cand improve yield and reduce GHG emissions.
Structural parameters of nanoparticles affecting their toxicity for biomedical applications: a review
Rapidly growing interest in using nanoparticles (NPs) for biomedical applications has increased concerns about their safety and toxicity. In comparison with bulk materials, NPs are more chemically active and toxic due to the greater surface area and small size. Understanding the NPs’ mechanism of toxicity, together with the factors influencing their behavior in biological environments, can help researchers to design NPs with reduced side effects and improved performance. After overviewing the classification and properties of NPs, this review article discusses their biomedical applications in molecular imaging and cell therapy, gene transfer, tissue engineering, targeted drug delivery, Anti-SARS-CoV-2 vaccines, cancer treatment, wound healing, and anti-bacterial applications. There are different mechanisms of toxicity of NPs, and their toxicity and behaviors depend on various factors, which are elaborated on in this article. More specifically, the mechanism of toxicity and their interactions with living components are discussed by considering the impact of different physiochemical parameters such as size, shape, structure, agglomeration state, surface charge, wettability, dose, and substance type. The toxicity of polymeric, silica-based, carbon-based, and metallic-based NPs (including plasmonic alloy NPs) have been considered separately.
Hydrogels for RNA delivery
RNA-based therapeutics have shown tremendous promise in disease intervention at the genetic level, and some have been approved for clinical use, including the recent COVID-19 messenger RNA vaccines. The clinical success of RNA therapy is largely dependent on the use of chemical modification, ligand conjugation or non-viral nanoparticles to improve RNA stability and facilitate intracellular delivery. Unlike molecular-level or nanoscale approaches, macroscopic hydrogels are soft, water-swollen three-dimensional structures that possess remarkable features such as biodegradability, tunable physiochemical properties and injectability, and recently they have attracted enormous attention for use in RNA therapy. Specifically, hydrogels can be engineered to exert precise spatiotemporal control over the release of RNA therapeutics, potentially minimizing systemic toxicity and enhancing in vivo efficacy. This Review provides a comprehensive overview of hydrogel loading of RNAs and hydrogel design for controlled release, highlights their biomedical applications and offers our perspectives on the opportunities and challenges in this exciting field of RNA delivery.RNA-based therapeutics hold promise for the treatment of several diseases. This Review provides an overview of hydrogels for RNA delivery, discussing how the chemical nature and physical properties of hydrogels can be explored for tailored RNA loading and release, and highlighting the use of these materials in biomedical applications.
O-glycosylation and its role in therapeutic proteins
Protein glycosylation is ubiquitous throughout biology. From bacteria to humans, this post translational modification with sophisticated carbohydrate structures plays a profound role in the interaction of proteins with cells and changes the physiochemical properties of the proteins that carry them. When the glycans are linked to Ser or Thr residues, they are known as O-linked glycans, as the glycosidic linkage is through oxygen. O-glycans are perhaps best known as part of the mucin proteins, however many soluble proteins carry these types of glycans, and that their roles in biology are still being discovered. Many of the soluble proteins that carry O-glycans have a role as therapeutic proteins, and in the 21st century, the application of synthetic biology is starting to be applied to improving these proteins through manipulation of the glycans. This review will explore the role of these O-linked glycans in proteins with pharmaceutical significance, as well as recent advancements in recombinant glycoprotein therapeutics.
Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode
The physiochemical properties of the solid-electrolyte interphase, primarily governed by electrolyte composition, have a profound impact on the electrochemical cycling of metallic lithium. Herein, we discover that the effect of nitrate anions on regulating lithium deposition previously known in ether-based electrolytes can be extended to carbonate-based systems, which dramatically alters the nuclei from dendritic to spherical, albeit extremely limited solubility. This is attributed to the preferential reduction of nitrate during solid-electrolyte interphase formation, and the mechanisms behind which are investigated based on the structure, ion-transport properties, and charge transfer kinetics of the modified interfacial environment. To overcome the solubility barrier, a solubility-mediated sustained-release methodology is introduced, in which nitrate nanoparticles are encapsulated in porous polymer gel and can be steadily dissolved during battery operation to maintain a high concentration at the electroplating front. As such, effective dendrite suppression and remarkably enhanced cycling stability are achieved in corrosive carbonate electrolytes. The solid-electrolyte interphase (SEI) is one of the governing factors for the reversibility of Li metal anode. Here, the authors reveal the impact of nitrate additive on the SEI in carbonate electrolytes, and demonstrate a method to overcome the solubility limitation of nitrate.
The protein corona from nanomedicine to environmental science
The protein corona spontaneously develops and evolves on the surface of nanoscale materials when they are exposed to biological environments, altering their physiochemical properties and affecting their subsequent interactions with biosystems. In this Review, we provide an overview of the current state of protein corona research in nanomedicine. We next discuss remaining challenges in the research methodology and characterization of the protein corona that slow the development of nanoparticle therapeutics and diagnostics, and we address how artificial intelligence can advance protein corona research as a complement to experimental research efforts. We then review emerging opportunities provided by the protein corona to address major issues in healthcare and environmental sciences. This Review details how mechanistic insights into nanoparticle protein corona formation can broadly address unmet clinical and environmental needs, as well as enhance the safety and efficacy of nanobiotechnology products. Understanding the protein corona can advance nanomedicinal developments and elucidate how nanomaterials impact the environment. This Review discusses the evolution and challenges in characterizing the protein corona, explores how artificial intelligence can supplement experimental efforts and exposes emerging opportunities in nanomedicine and the environment.
Solvent-derived defects suppress adsorption in MOF-74
Defects in metal-organic frameworks (MOFs) have great impact on their nano-scale structure and physiochemical properties. However, isolated defects are easily concealed when the frameworks are interrogated by typical characterization methods. In this work, we unveil the presence of solvent-derived formate defects in MOF-74, an important class of MOFs with open metal sites. With multi-dimensional solid-state nuclear magnetic resonance (NMR) investigations, we uncover the ligand substitution role of formate and its chemical origin from decomposed N,N-dimethylformamide (DMF) solvent. The placement and coordination structure of formate defects are determined by 13 C NMR and density functional theory (DFT) calculations. The extra metal-oxygen bonds with formates partially eliminate open metal sites and lead to a quantitative decrease of N 2 and CO 2 adsorption with respect to the defect concentration. In-situ NMR analysis and molecular simulations of CO 2 dynamics elaborate the adsorption mechanisms in defective MOF-74. Our study establishes comprehensive strategies to search, elucidate and manipulate defects in MOFs. Defects in metal-organic frameworks impact their structure and properties. Here authors uncover formate defects in MOF-74 that originate from decomposed DMF solvent. NMR shows that the defects partially eliminate open metal sites and lead to a decrease of gas adsorption; the adsorption mechanism of CO 2 in defective MOF is also elucidated.