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美利体育登录入口官网:刊期编辑部信息

Issue Editorial Masthead

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DOI：https://doi.org/10.1021/arv058i020_1996910

发表时间：2025年

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美利体育登录入口官网:摘要

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美利体育登录入口官网:Abstract

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美利体育登录入口官网:Biological Polymers: Evolution, Function, and Significance

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusA holistic description of biopolymers and their evolutionary origins will contribute to our understanding of biochemistry, biology, the origins of life, and signatures of life outside our planet. While biopolymer sequences evolve through known Darwinian processes, the origins of the backbones of polypeptides, polynucleotides, and polyglycans are less certain. We frame this topic through two questions: (i) Do the characteristics of biopolymer backbones indicate evolutionary origins? (ii) Are there reasonable mechanistic models of such pre-Darwinian evolutionary processes? To address these questions, we have established criteria to distinguish chemical species produced by evolutionary mechanisms from those formed by nonevolutionary physical, chemical, or geological processes. We compile and evaluate properties shared by all biopolymer backbones rather than isolating a single type. Polypeptide, polynucleotide, and polyglycan backbones are kinetically trapped and thermodynamically unstable in aqueous media. Each biopolymer forms a variety of elaborate assemblies with diverse functions, a phenomenon we call polyfunction. Each backbone changes structure and function upon subtle chemical changes such as the reduction of ribose or a change in the linkage site or stereochemistry of polymerized glucose, a phenomenon we call function-switching. Biopolymers display homo- and heterocomplementarity, enabling atomic-level control of structure and function. Biopolymer backbones access recalcitrant states, where assembly modulates kinetics and thermodynamics of hydrolysis. Biopolymers are emergent; the properties of biological building blocks change significantly upon polymerization. In cells, biopolymers compose mutualistic networks; a cell is an Amazon Jungle of molecules. We conclude that biopolymer backbones exhibit hallmarks of evolution. Neither chemical, physical, nor geological processes can produce molecules consistent with observations. We are faced with the paradox that Darwinian evolution relies on evolved backbones but cannot alter biopolymer backbones. This Darwinian constraint is underlined by the observation that across the tree of life, ribosomes are everywhere and always have been composed of RNA and protein. Our data suggest that chemical species on the Hadean Earth underwent non-Darwinian coevolution driven in part by hydrolytic stress, ultimately leading to biopolymer backbones. We argue that highly evolved biopolymer backbones facilitated a seamless transition from chemical to Darwinian evolution. This model challenges convention, where backbones are products of direct prebiotic synthesis. In conventional models, biopolymer backbones retain vestiges of prebiotic chemistry. Our findings, however, align with models where chemical species underwent iterative and recursive sculpting, selection, and exaptation. This model supports Orgel’s “gloomy” prediction that modern biochemistry has discarded vestiges of prebiotic chemistry. But there is hope. We believe an understanding of biopolymer origins will progress during the challenging and exciting integration of chemical sciences and evolutionary theory. These efforts can provide new perspectives on pre-Darwinian mechanisms and can deepen our understanding of evolution and of chemical sciences. Our working definition of chemical evolution is continuous chemical change with exploration of new chemical spaces and avoidance of equilibrium. In alignment with our model, we observe chemical evolution in complex mixtures undergoing wet–dry cycling, which does appear to undergo continuous chemical change and exploration of new chemical spaces while avoiding equilibrium.This publication is licensed underCC-BY 4.0 . License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator.View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. ACS PublicationsCopyright ? 2025 The Authors. Published by American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Biopolymers Dietary fiber Genetics Molecules Peptides and proteins

引用量：120发表时间：2025年
美利体育登录入口官网:AI-Driven Antimicrobial Peptide Discovery: Mining and Generation

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusThe escalating threat of antimicrobial resistance (AMR) poses a significant global health crisis, potentially surpassing cancer as a leading cause of death by 2050. Traditional antibiotic discovery methods have not kept pace with the rapidly evolving resistance mechanisms of pathogens, highlighting the urgent need for novel therapeutic strategies. In this context, antimicrobial peptides (AMPs) represent a promising class of therapeutics due to their selectivity toward bacteria and slower induction of resistance compared to classical, small molecule antibiotics. However, designing effective AMPs remains challenging because of the vast combinatorial sequence space and the need to balance efficacy with low toxicity. Addressing this issue is of paramount importance for chemists and researchers dedicated to developing next-generation antimicrobial agents.Artificial intelligence (AI) presents a powerful tool to revolutionize AMP discovery. By leveraging AI, we can navigate the immense sequence space more efficiently, identifying peptides with optimal therapeutic properties. This Account explores the emerging application of AI in AMP discovery, focusing on two primary strategies: AMP mining, and AMP generation, as well as the use of discriminative methods as a valuable toolbox.AMP mining involves scanning biological sequences to identify potential AMPs. Discriminative models are then used to predict the activity and toxicity of these peptides. This approach has successfully identified numerous promising candidates, which were subsequently validated experimentally, demonstrating the potential of AI in AMP design and discovery.AMP generation, on the other hand, creates novel peptide sequences by learning from existing data through generative modeling. This class of models optimizes for desired properties, such as increased activity and reduced toxicity, potentially producing synthetic peptides that surpass naturally occurring ones. Despite the risk of generating unrealistic sequences, generative models hold the promise of accelerating the discovery of highly effective and highly novel and diverse AMPs.In this Account, we describe the technical challenges and advancements in these AI-based approaches. We discuss the importance of integrating various data sources and the role of advanced algorithms in refining peptide predictions. Additionally, we highlight the future potential of AI to not only expedite the discovery process but also to uncover peptides with unprecedented properties, paving the way for next-generation antimicrobial therapies.In conclusion, the synergy between AI and AMP discovery opens new frontiers in the fight against AMR. By harnessing the power of AI, we can design novel peptides that are both highly effective and safe, offering hope for a future where AMR is no longer a looming threat. Our paper underscores the transformative potential of AI in drug discovery, advocating for its continued integration into biomedical research.This publication is licensed underCC-BY 4.0 . License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator.View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. ACS PublicationsCopyright ? 2025 The Authors. Published by American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Antimicrobial agents Assays Bacteria Peptides and proteins Toxicity

引用量：118发表时间：2025年
美利体育登录入口官网:Heterogeneous Frustrated Lewis Pair Catalysts: Rational Structure Design and Mechanistic Elucidation Based on Intrinsic Properties of Supports

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusThe discovery of reversible hydrogenation using metal-free phosphoborate species in 2006 marked the official advent of frustrated Lewis pair (FLP) chemistry. This breakthrough revolutionized homogeneous catalysis approaches and paved the way for innovative catalytic strategies. The unique reactivity of FLPs is attributed to the Lewis base (LB) and Lewis acid (LA) sites either in spatial separation or in equilibrium, which actively react with molecules. Since 2010, heterogeneous FLP catalysts have gained increasing attention for their ability to enhance catalytic performance through tailored surface designs and improved recyclability, making them promising for industrial applications. Over the past 5 years, our group has focused on investigating and strategically modifying various types of solid catalysts with FLPs that are unique from classic solid FLPs. We have explored systematic characterization techniques to unravel the underlying mechanisms between the active sites and reactants. Additionally, we have demonstrated the critical role of catalysts’ intrinsic electronic and geometric properties in promoting FLP formation and stimulating synergistic effects. The characterization of FLP catalysts has been greatly enhanced by the use of advanced techniques such as synchrotron X-ray diffraction, neutron powder diffraction, X-ray photoelectron spectroscopy, extended X-ray absorption fine structure, elemental mapping in scanning transmission electron microscopy, electron paramagnetic resonance spectroscopy, diffuse-reflectance infrared Fourier transform spectroscopy, and solid-state nuclear magnetic resonance spectroscopy. These techniques have provided deeper insights into the structural and electronic properties of FLP systems for the future design of catalysts.Understanding electron distribution in the overlapping orbitals of LA and LB pairs is essential for inducing FLPs in operando in heterogeneous catalysts through target electron reallocation by external stimuli. For instance, in silicoaluminophosphate-type zeolites with weak orbital overlap, the adsorption of polar gas molecules leads to heterolytic cleavage of the Alδ+–Oδ? bond, creating unquenched LA–LB pairs. In a Ru-doped metal–organic framework, the Ru–N bond can be polarized through metal–ligand charge transfer under light, forming Ru+–N– pairs. This activation of FLP sites from the framework represents a groundbreaking innovation that expands the catalytic potential of existing materials. For catalysts already employing FLP chemistry to dynamically generate products from substrates, a complete mechanistic interpretation requires a thorough examination of the surface electronic properties and the surrounding environment. The hydrogen spillover ability on the Ru-doped FLP surfaces improves conversion efficiency by suppressing hydrogen poisoning at metal sites. In situ H2–H2O conditions enable the production of organic chemicals with excellent activity and selectivity by creating new bifunctional sites via FLP chemistry. By highlighting the novel FLP systems featuring FLP induction and synergistic effects and the selection of advanced characterization techniques to elucidate reaction mechanisms, we hope that this Account will offer innovative strategies for designing and characterizing FLP chemistry in heterogeneous catalysts to the research community.This publication is licensed underCC-BY 4.0 . License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator.View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. ACS PublicationsCopyright ? 2025 The Authors. Published by American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Adsorption Catalysts Frustrated Lewis pairs Hydrogen Materials

引用量：112发表时间：2025年
美利体育登录入口官网:Advances in Proximity-Assisted Bioconjugation

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusProximity-induced chemistry (PIC) refers to the transient reactivity between two or more molecules upon physical closeness which are otherwise unreactive. Harnessed by nature to control fundamental biological processes such as transcription and signal transduction, PIC increases the probability of correctly oriented, effective collisions, facilitating fundamental cellular processes. Within the field of chemical biology, PIC has been employed for several clinically relevant purposes, including the degradation of aberrant biomolecules and construction of protein therapeutics. This Account focuses on the application of PIC strategies for the development of site-specific bioconjugation techniques, termed proximity-assisted bioconjugation (PAB). Site-specific bioconjugation refers to the precise modification of biomolecules to generate homogeneous products. Such techniques are vital for the development of protein therapeutics including antibody–drug conjugates (ADCs), the investigation of the biological mechanisms of post-translational modifications (PTMs), and the visualization of biomolecular interactions in vitro and in vivo. While numerous strategies have been developed, many suffer from poor yields, limited product stability, demanding experimental procedures, and/or a lack of regioselectivity. Thus, PIC principles have been implemented to address these limitations, leading to the development of PAB strategies which achieve precise, regioselective modification of biomolecules. In this Account, we describe the development of PAB techniques within our group at the University of Cambridge and Instituto de Medicina Molecular (iMM) over the past five years. Our journey with PAB began serendipitously while investigating maleic acid derivatives for cysteine bioconjugation. Here, we discovered the secondary participation of proximal lysines on Trastuzumab-V205C and Gemtuzumab-V205C, conjugatable THIOMAB antibodies commonly used in ADCs, leading to the formation of distinct bioconjugate products relative to IgGs without such lysines. Further investigation into the proximal lysine (K207) of Trastuzumab-V205C revealed that residue 207 could be harnessed directly or mutated to precisely tune the stability of ADCs due to proximity interactions between K207 and covalent modifications of C205. Considering that two Trastuzumab drug conjugates are approved for clinical use, these findings have contributed to the evolving understanding of the chemical landscape of this antibody and help inform future ADC design and development. Further, we describe efforts from our group to develop two distinct PAB approaches: regioselective lysine acetylation of histone H3 and phage display-compatible peptide cyclization. These strategies combine induced-proximity with traditional bioconjugation techniques to enable regioselective modification of biomolecules which are historically difficult to selectively modify. These methods are readily adaptable to related systems and serve as representative examples of how to successfully develop PAB strategies for desired applications. In short, this Account highlights our group’s contributions to and insights on PAB methodologies wherein we illustrate how PIC can be thoughtfully applied to bioconjugation techniques for various aims including regioselective bioconjugation and enhanced bioconjugate stability. We expect that PAB approaches will continue to diversify bioconjugation applications and greatly expand the toolkit of chemical biologists.This publication is licensed underCC-BY 4.0 . License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator.View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. ACS PublicationsCopyright ? 2025 The Authors. Published by American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Chemical biology Conjugate acid-base pairs Modification Monomers Organic reactions Peptides and proteins Viruses

引用量：111发表时间：2025年
美利体育登录入口官网:Discovery of Stable Extra-large Pore Zeolites Based on Rational Design of Structure-directing Agents

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusAluminosilicate zeolites possess ordered pore structures and tunable acidities as well as remarkable thermal/hydrothermal stabilities, which render them highly suitable for industrial applications in petroleum refining, in organic chemical synthesis, as catalysts, and in gas separation technologies as adsorbents. Computational predictions indicate that millions of theoretical zeolite framework types may be realizable; however, the International Zeolite Association (IZA) has authenticated only 260 zeolite framework types to date. Among these, approximately 20 types have found industrial applications, and their pore systems are generally confined to not exceeding the 12-membered ring (MR). There is an intense demand in industry to develop novel, stable, three-dimensional (3D) zeolites with extra-large pores, which are essential for heavy oil conversion and macromolecular catalysis.Over the past 30 years, more than 30 extra-large pore zeolites have been synthesized by using bulky organic structure-directing agents (SDAs) as templates. Nevertheless, their utilization has been restricted by various factors, like inferior thermal and hydrothermal stability, unexpected interrupted frameworks, and limitation of 3D connectivity. Research on the exploration of stable 3D extra-large pore zeolites has advanced sluggishly, and there has been a persistent inability to achieve breakthroughs along this direction. Recently, we reported the ZEO series of 3D stable silica-based extra-large pore zeolites, which represents a synthetic breakthrough in this area. This Account focuses on the timeline and comprehensively introduces our decade-long efforts in developing novel 3D stable extra-large pore zeolites, especially for the progressive innovation of designing SDAs. Starting with the semirigid imidazole salts as SDAs, we successfully synthesized NUD-1/2/3, a series of new large and extra-large pore germanosilicate zeolites; later efforts were extended to highly rigid benzimidazole-based SDAs, which led to the successful synthesis of high silica and pure silica extra-large pore zeolites NUD-5/6. Although imidazole salts were found to be much more efficient, their lower stability under alkaline and high temperature conditions limited their application. At the same time, most of the as-synthesized zeolites have only 1D extra-large pores due to the strong molecular interactions between the SDAs caused by their aromatic rings. To address this issue, bulky and stable SDAs derived from cycloalkyl phosphines were subsequently developed. With tricyclohexylmethylphosphonium (TCyMP) as the SDA, we synthesized the first 3D stable extra-large pore aluminosilicate zeolite, ZEO-1, which is a breakthrough in zeolite synthesis. Furthermore, a new 1D to 3D topotactic condensation mechanism stemming from a novel 1D chain silicate, ZEO-2, was discovered, by which the 3D stable extra-large pore zeolites ZEO-3 and ZEO-5 were synthesized, continuously expanding the pore size limits of 3D stable zeolites. The ZEO series, along with the recently reported ZMQ-1, fills the existing gap in 3D stable zeolites between large pore zeolites and mesoporous materials. This achievement paves the way for the selective catalysis of macromolecules in the future. The discovery of these extra-large pore zeolites benefits from not only the synthetic advancements but also the technological advancements in structural characterizations. Furthermore, machine learning as an emerging technique is expected to play a pivotal role in propelling the development of zeolite science.This publication is licensed for personal use by The American Chemical Society. ACS PublicationsCopyright ? 2025 American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Cations Chemical structure Imidazoles Silica Zeolites

引用量：105发表时间：2025年
美利体育登录入口官网:Recent Advances in Bioinspired Cu-Directed C–H Hydroxylation Reactions

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusCu-dependent metalloenzymes catalyze a wide array of oxidative transformations using O2 as an oxidant under mild conditions. These include the hydroxylation of challenging organic substrates (e.g., oxidation of methane to methanol in particulate methane monooxygenase) and the regio- and enantioselective hydroxylation of complex molecules (e.g., benzylic hydroxylation of dopamine to noradrenaline in dopamine-β-monooxygenase). Lytic polysaccharide monooxygenase enzymes (LPMOs) promote the C–H hydroxylation and subsequent cleavage of the polysaccharide chains found in natural materials such as cellulose or chitin. Recent reports on the reactivity of LPMOs suggest that, instead of O2, these Cu-dependent metalloenzymes utilize H2O2 as an oxidant. In 2015, our research lab reported that the catalytic hydroxylation of strong C–H bonds (e.g., cyclohexane) using Cu and H2O2 proceeded via formation of nonselective Fenton-like oxidants (hydroxyl and hydroperoxyl radicals). To achieve regioselectivity, LPMOs bind the organic substrate before exposing the Cu center to the oxidant, a reaction that leads to the formation of a highly organized ternary complex prior to substrate hydroxylation (i.e., metal–substrate–oxidant adduct). Based on this concept, our research lab has pioneered the use of Cu, directing groups, and green oxidants to promote the site-selective hydroxylation of ketones and aldehydes. In our first report on this topic, we carried out an extensive mechanistic analysis on the Cu-directed sp3 C–H hydroxylation reactions developed by Sch?necker and co-workers. Our findings suggested that the reaction between CuI and O2 did not lead to the formation of dinuclear Cu2O2 (as it was previously suggested) but produced CuII and H2O2, which generated mononuclear CuII-hydroperoxide oxidants. Based on our mechanistic analysis, we redesigned the reaction conditions to utilize CuII and H2O2, which improved the yield, cost, and practicability of the Sch?necker oxidations. Since then, our research lab has broadened the scope of substrates that can be oxidized using Cu, H2O2, and bidentate directing groups to include the γ-hydroxylation of sp2 C–H bonds and β-hydroxylation of sp3 C–H bonds. Our latest reports have focused on the regioselective hydroxylation of substituted unsymmetrical benzophenones (which occurred via the formation of an electrophilic CuOOH species) and, for the first time, enantioselective C–H hydroxylation reactions via the formation of Cu/O2 species. Our work highlights the importance of a mechanistic understanding to improve oxidation processes as well as underlines the use of metal-directed transformations to study the mechanisms by which metalloenzymes functionalize organic molecules.This publication is licensed underCC-BY 4.0 . License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator.View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. ACS PublicationsCopyright ? 2025 The Authors. Published by American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Aromatic compounds Hydrocarbons Organic reactions Oxidation Oxidation reactions

引用量：82发表时间：2025年
美利体育登录入口官网:High-Pressure Synthesis of Pnictogen Nitrides

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusNitrides represent a class of chemical compounds of high scientific and technological relevance. Nevertheless, due to the challenging synthetic conditions, essentially related to the stability of the N2 molecule, nitrides have remained largely unexplored compared with the corresponding oxides.The laser-heated diamond anvil cell (LH-DAC), providing access to the GPa pressure range and temperatures as high as several thousands of K, has dramatically changed the rules of the game, unveiling thermodynamic conditions in which N2 becomes unstable and polymerizes into extended crystalline phases. A variety of N-compounds have been indeed synthesized by laser-heating the corresponding elements in a N2 environment under high-pressure (HP) conditions.Nevertheless, only recently group 15 elements heavier than N have been targeted by this method, and excluding α-P3N5 and γ-P3N5, crystalline pnictogen nitrides have remained essentially unknown.Since the discovery of phosphorene, while the quest for 2D materials has raised the interest for group 15 xenes and their N-doping as a key development, the inherent tendency of pnictogens to adopt crystalline layered structures persisting at high pressure has increased focus on binary N-compounds with heavier pnictogens, with implications for fundamental chemistry and potential applications.In this scenario, the discovery of the pseudo simple-cubic (p-sc) structure in the phase diagram of P, and, a few years later, the high-pressure–high-temperature (HP-HT) synthesis of PH3 from the elements and the discovery of the crystalline van der Waals (vdW) compound (PH3)2H2 have further reconnected the HP behavior of P to that of lighter N.These experimental studies, highlighting consistency in the structural and reactive properties of group 15 elements at high pressure, together with additional theoretical and computational insights, have opened new perspectives and motivated further investigations about the existence of crystalline pnictogen nitrides.Indeed, not only α- and γ-P3N5, but also three other crystalline polymorphs of phosphorus nitride (δ-P3N5, PN2, and α′-P3N5), have been synthesized by the direct HP-HT chemical reaction of P and N2 in a LH-DAC.Moving down in group 15, the same method has led to the discovery of the first crystalline nitrides of arsenic (AsN) and antimony (Sb3N5), whose existence has always represented an open question in inorganic chemistry, and to the structural characterization of two crystalline polymorphs of bismuth nitride (BiN).This Account provides an overview of the recent progress in the high-pressure and high-temperature synthesis of crystalline pnictogen nitrides, demonstrating the effective activation of a direct chemistry between N and heavier pnictogens. The presented results mark fundamental advancements in the chemistry of group 15 elements and pioneer the discovery of new advanced pnictogen-based materials of energetic and technological relevance, potentially recoverable under ambient conditions as stable or metastable systems.This publication is licensed underCC-BY 4.0 . License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator.View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. ACS PublicationsCopyright ? 2025 The Authors. Published by American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Crystal structure Diffraction Elements Nitrides Nitrogen Phosphorus Pnictides

引用量：81发表时间：2025年
美利体育登录入口官网:Mainstream and Sidestream Modeling in Oxygen Evolution Electrocatalysis

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusThe oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are key in numerous electrochemical technologies, such as water electrolyzers, CO2 electrolyzers, low-temperature fuel cells, regenerative fuel cells and some metal-air batteries. The OER and ORR tend to be sluggish and catalyzed by scarce and expensive materials, the durability of which is often insufficient. For two decades, computational methods have been regarded as a cost-effective means to explain experimental observations, test hypothesis, and design new materials for these two reactions.Currently, the most widely used computational model is based on the free energies of the intermediates (*O, *OH, *OOH) and the scaling relations among them. Since the publication of two seminal papers in 2011, the scaling relation between the adsorption energies of *OOH and *OH was assigned all the responsibility for the experimental inefficiencies of OER and ORR electrocatalysts. This triggered a research paradigm based on breaking such scaling relation that still lasts until this day (see the diagram next to this text). After noting in 2018 that breaking the scaling relation between *OOH and *OH does not necessarily entail an improvement of the OER overpotential, my group moved away from the mainstream and has since been devising alternative descriptors and methods to enhance OER electrocatalysts and bifunctional OER/ORR electrocatalysts.In this Account, I will describe when and why we introduced the concepts of electrochemical symmetry, delta-epsilon optimization, bifunctional volcano plot, and error awareness, among others, aiming to provide quantitative tools for the computational design and optimization of electrocatalysts.This publication is licensed underCC-BY 4.0 . License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator.View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. ACS PublicationsCopyright ? 2025 The Author. Published by American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Catalysts Electrocatalysts Materials Radiology Redox reactions

引用量：80发表时间：2025年
美利体育登录入口官网:Precision Phototherapy Enabled by Decoding Complex Microenvironments

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusThe complex and dynamic microenvironments of pathological sites, including infections, tumors, and neurological disorders, impose formidable challenges on conventional therapies due to features such as iron dysregulation, localized acidity, biofilm barriers, and thermal adaptation. Harnessing these microenvironmental cues to design light-activated, microenvironment-responsive therapeutic platforms offers a promising strategy for precise, spatiotemporally controlled treatments.Nutritional immunity restricts iron availability to suppress pathogen proliferation, while bacteria deploy specialized siderophore-mediated uptake systems to circumvent this restriction. By exploiting this vulnerability, “Trojan horse” nanoplatforms such as a multifunctional nanocomposite (Ga-CT@P) can hijack bacterial iron uptake pathways, induce iron starvation, and exert potent antimicrobial effects. DFT calculations revealed that Ga3+ exhibits stronger, more uniform binding to enterobactin than Fe3+, leading to stable, redox-inert complexes that mislead bacterial transport systems.Beyond metal ion interference, acid-responsive photodynamic therapy (PDT) offers spatiotemporally precise activation at infectious sites while minimizing off-target toxicity. Our development of DHTPA, a pH-responsive AIE photosensitizer, enables robust reactive oxygen species (ROS) generation exclusively under mildly acidic conditions, enhancing bactericidal efficacy. This platform demonstrated strong antibacterial effects against drug-resistant pathogens and effectively promoted wound healing in vivo, showcasing the potential of lesion-specific “on-demand” PDT.To address biofilm barriers, OMV-camouflaged nanodisguisers synergistically integrate photothermal heating, ion interference, and ROS generation to dismantle biofilms while inducing metabolic collapse in pathogens. Simultaneously, OMV-coated nanodisguisers exploit bacterial adhesion pathways for targeted delivery, enabling photonic disruption of pathogen metabolism.In thermosensitive microenvironments, where heat-shock-protein-mediated thermal tolerance limits photothermal therapy (PTT), we developed dual-laser PTT strategies using NIR-II AIEgens (PM331@F127) to achieve precise, stepwise thermal regulation. This strategy rapidly suppresses heat tolerance mechanisms at higher temperatures and maintains moderate thermal ablation, maximizing efficacy while reducing collateral damage.In high-barrier systems such as the central nervous system (CNS), crossing the blood–brain barrier (BBB) is essential for effective phototherapy. We designed DK@RA-PEG, an NIR-II photosensitizer platform functionalized with RVG peptides and nucleic acid aptamers, to enable BBB penetration, virus-specific targeting, and ROS-mediated viral eradication under NIR light. This approach demonstrated effective treatment of rabies virus infection in vivo while maintaining neurocompatibility.Collectively, these advances establish a versatile framework for microenvironment-responsive, light-controlled therapies that decode and harness biochemical and physical signatures within diseased tissues, achieving spatiotemporal precision beyond conventional modalities. By integrating chemical signaling modulation, smart molecular design, and physiological barrier penetration, these platforms illuminate a path toward intelligent, personalized phototherapies for complex disease landscapes.This publication is licensed for personal use by The American Chemical Society. ACS PublicationsCopyright ? 2025 American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Biofilms Cancer therapy Infectious diseases Iron Tumors

引用量：80发表时间：2025年
美利体育登录入口官网:Bistable Functions and Signaling Motifs in Systems Chemistry: Taking the Next Step Toward Synthetic Cells

AbstractClick to copy section linkSection link copied!High Resolution ImageDownload MS PowerPoint SlideConspectusA key challenge in modern chemistry research is to mimic life-like functions using simple molecular networks and the integration of such networks into the first functional artificial cell. Central to this endeavor is the development of signaling elements that can regulate the cell function in time and space by producing entities of code with specific information to induce downstream activity. Such artificial signaling motifs can emerge in nonequilibrium systems, exhibiting complex dynamic behavior like bistability, multistability, oscillations, and chaos. However, the de novo, bottom-up design of such systems remains challenging, primarily because the kinetic characteristics and energy aspects yielding bifurcation have not yet been globally defined. We herein review our recent work that focuses on the design and functional analysis of peptide-based networks, propelled by replication reactions and exhibiting bistable behavior. Furthermore, we rationalize and discuss their exploitation and implementation as variable signaling motifs in homogeneous and heterogeneous environments.The bistable reactions constitute reversible second-order autocatalysis as positive feedback to generate two distinct product distributions at steady state (SS), the low-SS and high-SS. Quantitative analyses reveal that a phase transition from simple reversible equilibration dynamics into bistability takes place when the system is continuously fueled, using a reducing agent, to keep it far from equilibrium. In addition, an extensive set of experimental, theoretical, and simulation studies highlight a defined parameter space where bistability operates.Analogous to the arrangement of protein-based bistable motifs in intracellular signaling pathways, sequential concatenation of the synthetic bistable networks is used for signal processing in homogeneous media. The cascaded network output signals are switched and erased or transduced by manipulating the order of addition of the components, allowing it to reach “on demand” either the low-SS or high-SS. The pre-encoded bistable networks are also useful as a programming tool for the downstream regulation of nanoscale materials properties, bridging together the Systems Chemistry and Nanotechnology fields. In such heterogeneous cascade pathways, the outputs of the bistable network serve as input signals for consecutive nanoparticle formation reaction and growth processes, which–depending on the applied conditions–regulate various features of (Au) nanoparticle shape and assembly.Our work enables the design and production of various signaling apparatus that feature higher complexity than previously observed in chemical networks. Future studies, briefly discussed at the end of the Account, will be directed at the design and analysis of more elaborate functionality, such as bistability under flow conditions, multistability, and oscillations. We propose that a profound understanding of the design principles facilitating the replication-based bistability and related functions bear implications for exploring the origin of protein functionality prior to the highly evolved replication–translation–transcription machinery. The integration of our peptide-based signaling motifs within future synthetic cells seems to be a straightforward development of the two alternating states as memory and switch elements for controlling cell growth and division and even communication among different cells. We furthermore suggest that such systems can be introduced into living cells for various biotechnology applications, such as switches for cell temporal and spatial manipulations.This publication is licensed underCC-BY 4.0 . License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator.View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. License Summary*You are free to share(copy and redistribute) this article in any medium or format and to adapt(remix, transform, and build upon) the material for any purpose, even commercially within the parameters below: Creative Commons (CC): This is a Creative Commons license. Attribution (BY): Credit must be given to the creator. View full license *DisclaimerThis summary highlights only some of the key features and terms of the actual license. It is not a license and has no legal value. Carefully review the actual license before using these materials. ACS PublicationsCopyright ? 2025 The Authors. Published by American Chemical SocietySubjectswhat are subjects Article subjects are automatically applied from the ACS Subject Taxonomy and describe the scientific concepts and themes of the article. Bistability Cell signaling Chemical reactions DNA replication Oscillation

引用量：79发表时间：2025年

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