Accounts of materials research最新文献

{"title":"Reframing Sustainable Agriculture with Precision Materials Chemistry","authors":"Jing-Hang Wu, Kong Chen, Yuen Wu","doi":"10.1021/accountsmr.6c00118","DOIUrl":"10.1021/accountsmr.6c00118","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 7","pages":"646–649"},"PeriodicalIF":14.1,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148624944","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Coordination-Driven Design of Single-Atom Nanozymes: Bridging Mechanistic Insights and Multimetal Applications","authors":"Eslam M. Hamed,&nbsp;Yanyan Zhu,&nbsp;Fun Man Fung,&nbsp;Sam F. Y. Li","doi":"10.1021/accountsmr.5c00337","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00337","url":null,"abstract":"<p>Single-atom nanozymes (SANs)represent a transformative frontierin artificial enzymes, addressing limitations of natural enzymes andconventional nanomaterial-based catalysts. Natural enzymes are fragileand costly, and traditional nanozymes often lack well-defined activesites. Our research leverages single-atom catalysis to engineer highlyefficient and stable enzyme mimics for biosensing and environmentalremediation.</p><p>SANs exhibit a diverse range of enzyme-like activities,includingperoxidase, catalase, oxidase (OXD), and superoxide dismutase (SOD)mimetic functions. By focusing on atomically dispersed metal centers,SANs maximize atomic utilization and provide well-defined active sites,enabling unprecedented control over catalytic performance, e.g., copper-basedsystems that exhibit remarkable OXD-like activity mimicking galactoseoxidase.</p><p>To decode the active site and clarify the underlyingcatalyticmechanism, we combined experimental techniques and theoretical modeling.Kinetic assays revealed ultrahigh substrate affinity and catalyticefficiency, and advanced characterization provided direct evidencefor high-valent metal-oxo intermediate formation, mirroring naturalheme-containing enzymes. However, this pathway is not universal; SANmechanisms are highly coordination-dependent, with alternative routesincluding surface-confined redox cycling, radical-mediated processes,and metal–ligand cooperative pathways. Density functional theorycalculations confirmed that the precise electronic structure and coordinationenvironment endowed the SANs with biomimetic catalytic mechanisms.</p><p>These mechanistic insights formed the bedrock for rational designprinciples: judicious choice of metal, strategic selection of supportmaterials, and precise control of the coordination environment. UsingMOF-derived and wet-chemistry approaches, we developed a zinc-centeredSAN (Zn-SAN) that mimics the CO₂ hydration activity ofcarbonic anhydrase and bimetallic Cu/Zn-SANs mimicking SOD, with enhancedstability and recyclability.</p><p>SANs offer robust, cost-effectiveplatforms for sensitive biosensing,controlled ROS generation for antibacterial treatments, and CO₂ capture and conversion, with applications in point-of-carediagnostics, food safety monitoring, and therapeutics. Challengesin long-term stability, scalable synthesis, and ultrahigh selectivityremain, but integrating AI and advanced computational design promisesto accelerate discovery toward multifunctional SANs with cascade catalyticcapabilities.</p><p>Rather than a discrete subclass of nanozymes,SANs should be viewedas atomically engineered catalytic materials bridging heterogeneouscatalysis and biological redox chemistry. Continued integration ofoperando characterization, theoretical modeling, and rational coordinationdesign will be essential for establishing structure–mechanism–functionrelationships that guide translational applications.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 7","pages":"673–685"},"PeriodicalIF":14.1,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148651009","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Nickel Catalysts at the Crossroads: Sabatier Methanation, Carbide Phases, and Prospects for Methanol Synthesis","authors":"Jean C. da Cruz,&nbsp;Bruno H. Arpini,&nbsp;Adriano H. Braga,&nbsp;Nágila E. C. Maluf,&nbsp;Liane M. Rossi","doi":"10.1021/accountsmr.5c00315","DOIUrl":"10.1021/accountsmr.5c00315","url":null,"abstract":"&lt;p&gt;Nickel is a cornerstone of heterogeneouscatalysis and remainsone of the most practical metals for hydrogenation chemistry. In CO&lt;sub&gt;2&lt;/sub&gt; hydrogenation, however, Ni has long been associated withthe Sabatier reaction, favoring the formation of CH&lt;sub&gt;4&lt;/sub&gt;. Whilemethane is relevant for energy storage and compatible with existentinfrastructure, it is often less desirable than CO or oxygenates aschemical feedstocks. As the field of CO&lt;sub&gt;2&lt;/sub&gt; utilization evolvestoward a circular carbon economy, this raises a critical question:can nickel catalysts be reengineered to move beyond methanation andenable access to more valuable products? This Account addresses thatquestion by revisiting Ni catalysis from a broader and more forward-lookingperspective. Although methanation remains the most studied reactionwith Ni, the continued focus on CH&lt;sub&gt;4&lt;/sub&gt; as the primary productno longer reflects the full potential of this metal. Instead, selectiveformation of CO and methanol offers more versatile pathways for downstreamchemical synthesis and fuel production. Achieving such selectivityrequires overcoming the intrinsic tendency of Ni to strongly bindand hydrogenate CO intermediates, leading preferentially to methane.We examine how Ni can be repurposed for alternative CO&lt;sub&gt;2&lt;/sub&gt; valorization pathways by controlling the features that most stronglydetermine selectivity: (i) particle size and surface-site distributions,which regulate the extent of deep hydrogenation, (ii) carbon incorporationin and on Ni, ranging from surface-carburized states to carbide-likemotifs that weakens CO adsorption and shifts selectivity toward CO,(iii) carbon/metal interfaces, such as N-doped carbon coatings, whichmodify adsorption properties and interfacial reaction environments,and (iv) alloy and intermetallic chemistry, particularly Zn- and Ga-containingphases, which impose new adsorption energetics and can enable methanolsynthesis under appropriate conditions. Beyond these established strategies,emerging insights into nickel carbide phases introduce an underexploreddimension in catalyst design. Their distinct electronic and structuralproperties provide opportunities to tune selectivity in ways not accessiblewith metallic Ni alone. At the same time, advances in operando characterizationand computational modeling are beginning to reveal the dynamic natureof Ni surfaces under reaction conditions, offering new pathways forrational catalyst design. Throughout this Account, we highlight lessonsfrom our laboratory alongside complementary advances in the field,emphasizing unifying design principles that can guide the identificationof the targeted active state for CO&lt;sub&gt;2&lt;/sub&gt; hydrogenation. Byintegrating these perspectives, we propose that nickel should notbe viewed solely as a methanation catalyst, but as a versatile andtunable platform for CO&lt;sub&gt;2&lt;/sub&gt; conversion. This Account summarizespreviously published results from our group and others; no new experimentaldata are pr","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 7","pages":"661–672"},"PeriodicalIF":14.1,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148651102","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Understanding Adsorption and Reactions at Aqueous Oxide Interfaces with Neural Network Potential Molecular Dynamics","authors":"Sanghyun J. Park,&nbsp;Abhinav S. Raman,&nbsp;Annabella Selloni","doi":"10.1021/accountsmr.6c00001","DOIUrl":"10.1021/accountsmr.6c00001","url":null,"abstract":"&lt;p&gt;Chemical processes at metaloxide–waterinterfaces are ofcentral importance in geochemistry, biology, and energy technologies.A better understanding of these processes would allow us to make asignificant step toward optimizing and controlling them, which couldin turn lead to broader impacts. Computational modeling is indispensableto accomplishing this task because complexity and disorder often makeit difficult to extract atomistic information from experiments. Balancingcomputational cost and accuracy, simulation schemes based on efficientmachinelearning representations of the potential energy surface (PES) predictedby ab initio calculations have become increasingly popular over thepast decade. In particular, several studies have demonstrated theability of machine learning models to accurately reproduce the complexab initio PESs of aqueous oxide interfaces, allowing simulations ofsystems and processes that are not accessible with ab initio methods.&lt;/p&gt;&lt;p&gt;In this Account, we review our recent efforts to understand adsorptionprocesses and reactions at aqueous oxide interfaces using deep potentialmolecular dynamics (DPMD), a simulation scheme employing deep neuralnetworks (DNNs), which has proven to be quite successful in accuratelydescribing many different systems in the condensed phase. After summarizingthe DPMD methodology, we first review our work on the acid–basechemistry of oxide surfaces in contact with water, a fundamental characteristicthat controls proton transfer and surface charge at the interface.We focus on the aqueous interface of rutile IrO&lt;sub&gt;2&lt;/sub&gt;, an oxidematerial thus far considered the best catalyst for the oxygen evolutionreaction (OER). We show that this interface is characterized by alarge fraction of dissociated water and a strong Brønsted acidityof the surface sites, in good agreement with the experimentally measuredvalue of the point of zero proton charge.&lt;/p&gt;&lt;p&gt;In our second example,we investigate how the adsorption of organicspecies from ambient air or water affects the structure and wettabilityof the aqueous interfaces of TiO&lt;sub&gt;2&lt;/sub&gt;, a prototypical photocatalyticmaterial. This is a question that is relevant to understanding theUV-induced hydrophilicity of TiO&lt;sub&gt;2&lt;/sub&gt; surfaces, a propertyat the basis of self-cleaning windows and related applications. Specificallyfocusing on formic and acetic acids, the two most common atmosphericorganic acids, our simulations reveal that these acids control thewettability of TiO&lt;sub&gt;2&lt;/sub&gt; largely through acid–base chemistryat the interface rather than chemisorption on the oxide surface, afinding that could help improve the design of self-cleaning surfacesand photocatalytic devices.&lt;/p&gt;&lt;p&gt;Finally, we review our recent studyof methanol at TiO&lt;sub&gt;2&lt;/sub&gt;–water interfaces, a system whoseinterest is largely motivatedby the role of methanol in enhancing photocatalytic hydrogen evolutionon TiO&lt;sub&gt;2&lt;/sub&gt;. Our simulations provide mechanistic insights intothe coupled roles of the ","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 7","pages":"699–709"},"PeriodicalIF":14.1,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148612863","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Toward Autonomous Electrochemical Sensing: Advances and Challenges in Calibration-Free and Long-Duration Technologies","authors":"Le Jing,&nbsp;Qianqian Li,&nbsp;Shaoguang Li,&nbsp;Hui Li,&nbsp;Fan Xia","doi":"10.1021/accountsmr.6c00038","DOIUrl":"10.1021/accountsmr.6c00038","url":null,"abstract":"<p>Electrochemical biosensors holdpromise for autonomous molecularmonitoring owing to their sensitivity, electronic compatibility, andsuitability for wearable, implantable, and point-of-care platforms.However, conventional operation relies on external calibration thaterodes with batch-to-batch variability and environmental fluctuations,ultimately compromising long-term accuracy in complex biofluids andin vivo environments. Calibration-free electrochemical sensing addressesthis challenge through three complementary strategies. First, intrinsicdual-signal encoding strategy embeds two distinct redox-reportersto generate ratiometric outputs that convert absolute faradaic currentsinto self-normalized readouts, thereby eliminating the need for externalcalibration. Second, operationally programmed self-referencing strategyextracts drift-differentiated kinetics from a single reporter by varyingmeasurement parameters or environmental conditions. Third, interfacialengineering slows signal decay and drift at its molecular origin throughcoordinated optimization of redox reporters, self-assembled monolayers,protective layers and nuclease-resistant nucleic-acid scaffolds. ThisAccount summarizes recent advances, outlines these signal- and interface-leveldesigns and their principles, and discusses opportunities toward long-lastingautonomous biosensing in clinical settings.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 7","pages":"721–734"},"PeriodicalIF":14.1,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148656338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"From Molecules to the Field: Iron Oxides Controlling Pharmaceutical Fate and Remediation","authors":"Muhammad Usman,&nbsp;Tao Luo,&nbsp;Wei Cheng,&nbsp;Huichun Zhang,&nbsp;Jean-François Boily,&nbsp;Khalil Hanna","doi":"10.1021/accountsmr.6c00017","DOIUrl":"10.1021/accountsmr.6c00017","url":null,"abstract":"<p>Iron oxide (nano)minerals are abundant and reactivecomponentsof natural systems, exerting a profound influence on the environmentalfate of contaminants. Among these, pharmaceutical pollutants havegained increasing attention due to their ubiquitous presence in aquaticand terrestrial environments, their persistence, and their potentialto harm ecosystems and human health, particularly through contributionsto antimicrobial resistance.</p><p>Iron oxides play a dual role inmitigating pharmaceutical pollution:they serve as adsorptive surfaces and as redox-active materials capableof transforming pharmaceutical compounds. Adsorption is governed bythe affinity between pharmaceutical functional groups and specificiron oxide surface sites, while redox-active pharmaceuticals may undergoabiotic transformations upon electron transfer with Fe(III) or mixed-valent(Fe(II)–Fe(III)) minerals. These interactions can yield breakdownproducts with altered bioactivity and toxicity, adding complexityto environmental risk assessments. However, these processes remainpoorly understood due to experimental limitations and the absenceof reliable predictive models. Predicting pharmaceutical behaviorunder environmentally relevant conditions requires bridging multiplespatial and temporal scales.</p><p>In this Account, we provide a multiscaleevaluation of how ironoxides influence the fate and remediation potential of pharmaceuticalpollutants, integrating findings from experimental and modeling studiesat molecular, interface, pore, column, and field levels. We also explorehow Machine Learning can link across scales and uncover emergent patternsin complex data sets. Environmental factors, including solution chemistry,mineral properties, and co-occurring components, significantly influencethese interactions.</p><p>This approach allows us to identify keyknowledge gaps, draw connectionsbetween molecular-scale reactivity and macroscale environmental processes,and highlight opportunities for developing predictive tools for environmentalrisk assessment. The insights gained extend beyond pharmaceuticalsto a wide range of emerging organic contaminants. Advancing this fieldrequires interdisciplinary collaboration at the intersection of moleculargeochemistry, environmental materials science, mineralogy, hydrology,and microbiology.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 7","pages":"710–720"},"PeriodicalIF":14.1,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148651063","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Supramolecular Architecture of Chiral Macrocycles: Hierarchical Assembly and Confinement Effect for Enhanced Circularly Polarized Luminescence","authors":"Xin Song,&nbsp;Xuefeng Zhu,&nbsp;Shengfu Wu,&nbsp;Weili Shang,&nbsp;Liangyu Hu,&nbsp;Minghua Liu","doi":"10.1021/accountsmr.6c00071","DOIUrl":"10.1021/accountsmr.6c00071","url":null,"abstract":"&lt;p&gt;Circularly polarized luminescencehas emerged as a cutting-edgeresearch field owing to its dual significance in advancing the fundamentalunderstanding of chiral excited states and enabling the design ofnovel functional materials. A central challenge in realizing efficientCPL lies in the effective integration of chirality with the luminescentmoieties. Conventional strategies, often based on covalent bondingbetween chiral and luminescent units in small molecules, frequentlylead to systems that show either no or only weak CPL. Meaningfully,supramolecular assembly offers a transformative alternative by facilitatingchiral transfer and amplifying the CPL signals. In a broader context,supramolecular assembly serves as a foundational methodology for constructingmacroscopic functional supramolecular architectures from molecular-scalebuilding blocks. More importantly, by regulating noncovalent interactions,supramolecular approaches enable efficient chirality transfer fromchiral sites to assembled luminescent architecture, even allowingachiral luminophores to display stronger CPL activity through simplemixing or doping. Moreover, such an assembled architecture can significantlyenhance CPL intensity, greatly broadening the scope of high-performanceCPL-active materials.&lt;/p&gt;&lt;p&gt;Macrocycles are fundamental to supramolecularchemistry owing totheir critical roles in molecular recognition. However, most macrocyclesare intrinsically achiral or exhibit poor chirality in their isolatedmolecular state, posing a significant challenge for effective integrationof chirality with luminophores and subsequent amplification of CPL.This Account presents an innovative strategy to address this issuethrough a hierarchical confinement effect at both molecular and supramolecularassembly levels. We demonstrate how chirality can be introduced ortransferred within a macrocycle-based hierarchical assembled architectureto generate and enhance CPL signals. Key advances discussed includethe successful induction and propagation of chirality via hierarchicalassembly of the macrocyclic supramolecular architecture under a multipleconfinement effect, leading to efficient activation and substantialamplification of CPL within the supramolecular system. Specific approachesencompass (1) steering CPL by organizing macrocycles into helicalarchitecture for supramolecular chirality induction, transfer, andsignal amplification; (2) tuning CPL through spatial confinement ofachiral luminophores within chiral inner cavities of the hierarchicalmacrocyclic assembled architecture; and (3) modulating CPL via macrocycleoutward surface-mediated coassembly of guests for precise controlof the morphology and CPL. Collectively, these multiple confinementeffects establish a systematic framework for manipulating the chiropticalproperties of the hierarchically assembled nanoarchitectures. Beyondadvancing the fundamental understanding of chiral luminescence, thesemethodologies enable the rational design of high-perfor","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 7","pages":"750–764"},"PeriodicalIF":14.1,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148675540","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synchrotron X-ray Probes of Transition-Metal Carbides/Nitrides: From Structure Tuning to In-Situ Synthesis Control","authors":"Shiqiang Wei,&nbsp;Jialin Shi,&nbsp;Changda Wang,&nbsp;Shuangming Chen,&nbsp;Li Song","doi":"10.1021/accountsmr.5c00351","DOIUrl":"10.1021/accountsmr.5c00351","url":null,"abstract":"<p>Two-dimensional(2D) transition-metal carbides and nitrides, collectivelyknown as MXenes, have emerged as a highly promising class of layeredmaterials owing to their tunable physicochemical properties and broadapplicability in electrochemical energy storage. However, their practicaldeployment is still limited by structural instability and the difficultyof achieving precise structural control, both of which stem from complexand insufficiently understood phase-evolution pathways during synthesisand operation. In this Account, we present a review on recent progressin MXenes structural engineering and synthesis regulation, emphasizingthe important role of synchrotron X-ray techniques in revealing structure–propertyrelationships and phase-evolution mechanisms. We first summarize keypostetching structural regulation strategies, including intercalation,surface termination engineering, and atomic-scale configuration control.Synchrotron-based X-ray characterization enables quantitative identificationof structural features that are difficult to probe by conventionalmethods, including the local coordination environments of intercalantsand the spatial distributions of surface terminations and defects.Meanwhile, advances in in situ and operando synchrotron techniquesallow direct observation of microstructural evolution under realisticoperating conditions. These studies demonstrate that structural regulationstrongly influences ion transport, redox behavior, and mechanicalstability, thereby governing MXenes performance in diverse electrochemicalenergy-storage systems. We further discuss an emerging paradigm shiftin the field: from postsynthetic structural tuning to active controlof structural evolution during synthesis. This shift offers a moredeterministic pathway toward MXenes with controlled microstructuresand improved quality. In particular, synchrotron-based operando studiesenable real-time monitoring of the top-down etching of MAX phases,making it possible to capture the formation of MXenes frameworks,identify transient intermediates, and elucidate the evolution of surfaceterminations and defects─information that is difficult to obtainusing conventional ex situ methods. Finally, we highlight future opportunitiesin MXenes research. A deeper understanding of MXenes microstructures,their dynamic evolution, and the associated synthesis mechanisms willprovide the foundation for controllable synthesis, precise structuralregulation, and the scalable production of high-performance MXenes.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 7","pages":"765–776"},"PeriodicalIF":14.1,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148634034","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mussel Foot Proteins: From Molecular Mechanisms to Production Strategy and Application","authors":"Zhongxin Cui,&nbsp;Chuntao Ji,&nbsp;Qiuyue Yin,&nbsp;Yani Zhao,&nbsp;Lei Zhang,&nbsp;Haishan Qi","doi":"10.1021/accountsmr.6c00043","DOIUrl":"10.1021/accountsmr.6c00043","url":null,"abstract":"<p>Achieving strong and durableadhesion in aquatic,dynamic environmentsis a significant challenge. Marine mussels address this through byssalthreads secured by Mussel Foot Proteins (Mfps). Comprising severalmain variants (Mfp-1 to Mfp-6) with distinct structures, Mfps serveas an important model in bioadhesion, providing key insights for syntheticmaterial design. Their functionality is due to 3,4-dihydroxyphenylalanine(DOPA), which is “A significant yet not the sole chemical factor”and “one of the key sources of inspiration” within complexadhesion systems. These catechol groups of DOPA mediate a two-stageadhesion process. Initially, they facilitate rapid surface wettingand attachment through noncovalent interactions such as hydrogen bonding,cation-π interactions, and hydrophobic effects. Subsequently,oxidation can convert catechols to quinones, which enable covalentcross-linking for cohesion and stable substrate anchoring via reactionswith nucleophiles or metal ion coordination. This combination of reversibleand irreversible interactions underpins the robust adhesion of Mfpsin marine settings.</p><p>Understanding these natural mechanisms hassignificantly advancedadhesive technology, leading to diverse Mfp materials. Beyond mimickingnatural proteins, synthetic biology and polymer chemistry have beenemployed to replicate and extend these principles. Recombinant expressionallows the production of tailored proteins, while synthetic peptidescapture core functional motifs. This approach has led to a range offunctional biomaterials with applications extending beyond adhesion,including tissue adhesives, antifouling coatings, drug delivery systems,self-healing hydrogels, and biosensors.</p><p>Current research isexploring more dynamic and multifunctionalsystems based on the Mfps principles. Future efforts may focus onenvironmentally responsive materials that offer spatiotemporal controlover the adhesion. Integrating Mfp designs with synthetic biologycould also contribute to developing engineered living materials. Keyresearch directions include the computational design of adhesive peptides,protein engineering for stability, optimization of microbial expressionsystems for production, and improved purification strategies. Realizingthe practical potential of Mfp-based technologies will require addressingpersistent challenges in scalable production and controlling catecholoxidation through interdisciplinary efforts in molecular design, materialsscience, and engineering.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 7","pages":"735–749"},"PeriodicalIF":14.1,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148666658","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Recasting the Catalytic Legacy of Reverse Water–Gas Shift Reaction: Rational Design Strategies for Selective CO2 Valorization","authors":"Muhammad Asif Nawaz,José Antonio Odriozola,Tomas Ramirez Reina","doi":"10.1021/accountsmr.5c00275","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00275","url":null,"abstract":"ConspectusRising atmospheric CO2 and climate pressures have intensified interest in carbon capture and utilization (CCU). The reverse water–gas shift (RWGS) reaction offers a direct route to convert CO2 into CO, a versatile syngas component for Fischer–Tropsch, methanol synthesis, and other downstream processes, thereby supporting a circular carbon economy. RWGS is inherently challenging: it is endothermic and favored only at high temperatures (&gt;600 °C), which promotes catalyst sintering and high energy demand, while at lower temperatures the competing Sabatier reaction dominates, producing CH4 over Ni. Catalyst selection further complicates implementation: noble metals (Au, Pt, Rh) offer high CO selectivity but are costly, whereas base metals (Ni, Fe, Cu) are more abundant yet prone to methanation, sintering, or phase instability. Industrial deployment also demands resilience under water-rich environments, high space velocities, and thermal cycling associated with variable renewable H2 supply.This Account presents our efforts to address these challenges through rational catalyst design guided by three central principles: electronic modulation via promoters to control adsorption and reaction pathways; active phase engineering to tune catalytic functionality and suppress undesired reactions, and structural and interfacial design to enhance stability and durability under realistic conditions. These principles are systematically explored using Ni- and Fe-based catalysts as model systems for scalable CO2 valorization. Alkali-promoted Ni catalysts, particularly Cs-modified Ni/CeO2, demonstrate how electronic tuning and metal–support interactions suppress methanation and enable CO-selective RWGS across a wide temperature range. Phase engineering further transforms Ni into phosphide intermetallic (Ni2P, Ni12P5), introducing active sites that favor CO formation while minimizing hydrogenation pathways. Complementary strategies in Fe-based systems, including MOF-derived Fe/carbon composites and Fe–Cu bimetallics, highlight the role of metal–support and metal–metal interactions in stabilizing active phases and enhancing CO yields. To address deactivation, nanoscale architectural control, such as core–shell and yolk–shell structures, has been employed to mitigate sintering and carbon deposition. Beyond single-function catalysts, dual-function and switchable materials integrate CO2 capture with catalytic conversion and enable dynamic operation across RWGS, methanation, and dry reforming, providing flexibility under variable process conditions. Mechanistic insights derived from operando spectroscopy reveal how surface defects, promoters, and support redox properties govern reaction pathways, including formate-mediated and redox mechanisms, thereby linking catalyst structure to function. Collectively, these studies demonstrate how integrating electronic, compositional, and structural design strategies can reconcile the competing demands of activity, selectivity","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"21 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148385135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}