ACS Materials Au最新文献

{"title":"The Nexus of Innovation: Electrochemically Synthesizing H2O2 and Its Integration with Downstream Reactions","authors":"Qiu Jiang,&nbsp;Yuan Ji,&nbsp;Tingting Zheng,&nbsp;Xu Li and Chuan Xia*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00070","DOIUrl":"10.1021/acsmaterialsau.3c00070","url":null,"abstract":"<p >Hydrogen peroxide (H₂O₂) represents a chemically significant oxidant that is prized for its diverse applicability across various industrial domains. Recent innovations have shed light on the electrosynthesis of H₂O₂ through two-electron oxygen reduction reactions (2e^– ORR) or two-electron water oxidation reactions (2e^– WOR), processes that underscore the attractive possibility for the on-site production of this indispensable oxidizing agent. However, the translation of these methods into practical utilization within chemical manufacturing industries remains an aspiration rather than a realized goal. This Perspective intends to furnish a comprehensive overview of the latest advancements in the domain of coupled chemical reactions with H₂O₂, critically examining emergent strategies that may pave the way for the development of new reaction pathways. These pathways could enable applications that hinge on the availability and reactivity of H₂O₂, including, but not limited to the chemical synthesis coupled with H₂O₂ and waste water treatment byFenton-like reactions. Concurrently, the Perspective acknowledges and elucidates some of the salient challenges and opportunities inherent in the coupling of electrochemically generated H₂O₂, thereby providing a scholarly analysis that might guide future research.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 2","pages":"133–147"},"PeriodicalIF":0.0,"publicationDate":"2023-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00070","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138580926","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"2D MOFs and Zeolites for Composite Membrane and Gas Separation Applications: A Brief Review","authors":"Minsu Kim,&nbsp;Wooyoung Choi,&nbsp;Choong Hoo Lee and Dae Woo Kim*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00072","DOIUrl":"10.1021/acsmaterialsau.3c00072","url":null,"abstract":"<p >Commercial membranes have predominantly been fabricated from polymers due to their economic viability and processability. This choice offers significant advantages in energy efficiency, cost-effectiveness, and operational simplicity compared to conventional separation techniques like distillation. However, polymeric membranes inherently exhibit a trade-off between their permeability and selectivity, which is summarized in the Robeson upper bound. To potentially surpass these limitations, mixed-matrix membranes (MMMs) can be an alternative solution, which can be constructed by combining polymers with inorganic additives such as metal–organic frameworks (MOFs) and zeolites. Incorporating high-aspect-ratio fillers like MOF nanosheets and zeolite nanosheets is of significant importance. This incorporation not only enhances the efficiency of separation processes but also reinforces the mechanical robustness of the membranes. We outline synthesis techniques for producing two-dimensional (2D) crystals (including nanocrystals with high aspect ratio) and provide examples of their integration into membranes to customize separation performances. Moreover, we propose a potential trajectory for research in the area of high-aspect-ratio materials-based MMMs, supported by a mathematical-model-based performance prediction.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 2","pages":"148–161"},"PeriodicalIF":0.0,"publicationDate":"2023-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00072","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138580790","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Combined First-Principles and Experimental Investigation into the Reactivity of Codeposited Chromium–Carbon under Pressure","authors":"Paul V. Marshall,&nbsp;Scott D. Thiel,&nbsp;Elizabeth E. Cote,&nbsp;Rostislav Hrubiak,&nbsp;Matthew L. Whitaker,&nbsp;Yue Meng and James P. S. Walsh*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00086","DOIUrl":"10.1021/acsmaterialsau.3c00086","url":null,"abstract":"<p >High-pressure synthesis in the diamond anvil cell suffers from the lack of a general approach for the control of precursor stoichiometry and homogeneity. Here, we present results from a new method we have developed that uses magnetron cosputtering to prepare stoichiometrically precise and atomically mixed amorphous films of Cr:C. Laser-heated diamond anvil cell experiments carried out on a flake of this sample at pressures between 13.5 and 24.3 GPa lead to the observation of Cr₃C (<i>Pnma</i>) over the entire pressure range─in good agreement with our in-house theoretical predictions─but also reveal two other metastable phases that were not expected: a novel monoclinic chromium carbide phase and the NaCl-type CrC (<i>Fm</i>3̅<i>m</i>) phase. The unexpected stability of CrC is investigated by using first-principles methods, revealing a large stabilizing effect tied to substoichiometry at the carbon site. These results offer an important case study into the current limitations of crystal structure prediction methods with regard to phase complexity and bolster the growing need for advanced theoretical approaches that can more completely survey experimentally unexplored phase space.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 4","pages":"393–402"},"PeriodicalIF":5.7,"publicationDate":"2023-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00086","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138555777","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electron Spin Selective Iridium Electrocatalysts for the Oxygen Evolution Reaction","authors":"Carlos J. Mingoes*,&nbsp;Bob C. Schroeder and Ana B. Jorge Sobrido*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00084","DOIUrl":"10.1021/acsmaterialsau.3c00084","url":null,"abstract":"<p >Highly efficient electrocatalysts for water electrolysis are crucial to the widespread commercialization of the technology and an important step forward toward a sustainable energy future. In this study, an alternative method for boosting the electrocatalytic activity toward the oxygen evolution reaction (OER) of a well-known electrocatalyst (iridium) is presented. Iridium nanoparticles (2.1 ± 0.2 nm in diameter) functionalized with chiral molecules were found to markedly enhance the activity of the OER when compared to unfunctionalized and achiral functionalized iridium nanoparticles. At a potential of 1.55 V vs Reference Hydrogen Electrode (RHE), chiral functionalized iridium nanoparticles exhibited an average 85% enhancement in activity with respect to unfunctionalized iridium nanoparticles compared to an average 13% enhancement for the achiral functionalized iridium nanoparticle. This activity enhancement is attributed to a spin-selective electron transfer mechanism taking place on the chiral functionalized catalysts, a characteristic induced by the chirality of the ligand. This alternative path for the OER drastically reduces the production of hydrogen peroxide, which was confirmed via a colorimetric method.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 2","pages":"204–213"},"PeriodicalIF":0.0,"publicationDate":"2023-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00084","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138525929","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Activating Mn Sites by Ni Replacement in α-MnO2","authors":"Sami M. Alharbi,&nbsp;Mohammed A. Alkhalifah,&nbsp;Benjamin Howchen,&nbsp;Athi N. A. Rahmah,&nbsp;Veronica Celorrio and David J. Fermin*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00051","DOIUrl":"10.1021/acsmaterialsau.3c00051","url":null,"abstract":"<p >Transition metal oxides are characterized by an acute structure and composition dependent electrocatalytic activity toward the oxygen evolution (OER) and oxygen reduction (ORR) reactions. For instance, Mn containing oxides are among the most active ORR catalysts, while Ni based compounds tend to show high activity toward the OER in alkaline solutions. In this study, we show that incorporation of Ni into α-MnO₂, by adding Ni precursor into the Mn-containing hydrothermal solution, can generate distinctive sites with different electronic configurations and contrasting electrocatalytic activity. The structure and composition of the Ni modified hollandite α-MnO₂ phase were investigated by X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), transmission electron microscopy coupled to energy-dispersive X-ray spectroscopy (TEM-EDX), inductively coupled plasma–optical emission spectroscopy (ICP-OES), and X-ray photoelectron spectroscopy (XPS). Our analysis suggests that Mn replacement by Ni into the α-MnO₂ lattice (site A) occurs up to approximately 5% of the total Mn content, while further increasing Ni content promotes the nucleation of separate Ni phases (site B). XAS and XRD show that the introduction of sites A and B have a negligible effect on the overall Mn oxidation state and bonding characteristics, while very subtle changes in the XPS spectra appear to suggest changes in the electronic configuration upon Ni incorporation into the α-MnO₂ lattice. On the other hand, changes in the electronic structure promoted by site A have a significant impact in the pseudocapacitive responses obtained by cyclic voltammetry in KOH solution at pH 13, revealing the appearance of Mn 3d orbitals at the energy (potential) range relevant to the ORR. The evolution of Mn 3d upon Ni replacement significantly increases the catalytic activity of α-MnO₂ toward the ORR. Interestingly, the formation of segregated Ni phases (site B) leads to a decrease in the ORR activity while increasing the OER rate.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 1","pages":"74–81"},"PeriodicalIF":0.0,"publicationDate":"2023-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00051","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138525896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Advancing PFAS Sorbent Design: Mechanisms, Challenges, and Perspectives","authors":"Yutong He,&nbsp;Xinrong Cheng,&nbsp;Samruddhi Jayendra Gunjal and Cheng Zhang*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00066","DOIUrl":"10.1021/acsmaterialsau.3c00066","url":null,"abstract":"<p >Per- and polyfluoroalkyl substances (PFAS) are a group of synthetic chemicals characterized with persistence and multisurface resistance. Their accumulation in the environment and toxicity to human beings have contributed to the rapid development of regulations worldwide since 2002. The sorption strategy, taking advantage of intermolecular interactions for PFAS capture, provides a promising and efficient solution to the treatment of PFAS contaminated sources. Hydrophobic and electrostatic interactions are the two commonly found in commercially available PFAS sorbents, with the fluorous interaction being the novel mechanism applied for sorbent selectivity. The main object of this Perspective is to provide a critical review on the current design criteria of PFAS sorbents, with particular focus on their sorption and interaction mechanisms as well as limitations. An outlook on future innovative design for efficient PFAS sorbents is also provided.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 2","pages":"108–114"},"PeriodicalIF":0.0,"publicationDate":"2023-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00066","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135192610","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Seeing the Supracolloidal Assemblies in 3D: Unraveling High-Resolution Structures Using Electron Tomography","authors":"Nonappa*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00067","DOIUrl":"10.1021/acsmaterialsau.3c00067","url":null,"abstract":"<p >Transmission electron microscopy (TEM) imaging has revolutionized modern materials science, nanotechnology, and structural biology. Its ability to provide information about materials’ structure, composition, and properties at atomic-level resolution has enabled groundbreaking discoveries and the development of innovative materials with precision and accuracy. Electron tomography, single particle reconstruction, and microcrystal electron diffraction techniques have paved the way for the three-dimensional (3D) reconstruction of biological samples, synthetic materials, and hybrid nanostructures at near atomic-level resolution. TEM tomography using a series of two-dimensional (2D) projections has been used extensively in biological science, but in recent years it has become an important method in synthetic nanomaterials and soft matter research. TEM tomography offers unprecedented morphological details of 3D objects, internal structures, packing patterns, growth mechanisms, and self-assembly pathways of self-assembled colloidal systems. It complements other analytical tools, including small-angle X-ray scattering, and provides valuable data for computational simulations for predictive design and reverse engineering of nanomaterials with the desired structure and properties. In this perspective, I will discuss the importance of TEM tomography in the structural understanding and engineering of self-assembled nanostructures with specific emphasis on colloidal capsids, composite cages, biohybrid superlattices with complex geometries, polymer assemblies, and self-assembled protein-based superstructures.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 3","pages":"238–257"},"PeriodicalIF":0.0,"publicationDate":"2023-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00067","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135241547","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Innovations in Bioengineering Virtual Special Issue","authors":"Stephanie L. Brock*,&nbsp;Maryam Badv,&nbsp;Ali Khademhosseini and Paul S. Weiss,&nbsp;","doi":"10.1021/acsmaterialsau.3c00089","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.3c00089","url":null,"abstract":"","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"3 6","pages":"569–570"},"PeriodicalIF":0.0,"publicationDate":"2023-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00089","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"72202282","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Versatile Design of Organic Polymeric Nanoparticles for Photodynamic Therapy of Prostate Cancer","authors":"Jiacheng Ling,&nbsp;Rongrong Gu,&nbsp;Lulu Liu,&nbsp;Ruixi Chu,&nbsp;Junchao Wu,&nbsp;Rongfang Zhong,&nbsp;Sheng Ye*,&nbsp;Jian Liu* and Song Fan*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00060","DOIUrl":"10.1021/acsmaterialsau.3c00060","url":null,"abstract":"<p >Radical prostatectomy is a primary treatment option for localized prostate cancer (PCa), although high rates of recurrence are commonly observed postsurgery. Photodynamic therapy (PDT) has demonstrated efficacy in treating nonmetastatic localized PCa with a low incidence of adverse events. However, its limited efficacy remains a concern. To address these issues, various organic polymeric nanoparticles (OPNPs) loaded with photosensitizers (PSs) that target prostate cancer have been developed. However, further optimization of the OPNP design is necessary to maximize the effectiveness of PDT and improve its clinical applicability. This Review provides an overview of the design, preparation, methodology, and oncological aspects of OPNP-based PDT for the treatment of PCa.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 1","pages":"14–29"},"PeriodicalIF":0.0,"publicationDate":"2023-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00060","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135589302","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tunable High Entropy Lanthanide Oxide Microspheres via Confined Electroprecipitation in Emulsion Droplet Scaffolds","authors":"Charles H. Laber,&nbsp;Austin R. Scircle,&nbsp;Zachary P. Mouton,&nbsp;Travis Thornell,&nbsp;Ashly Antony,&nbsp;Jonah W. Jurss and Matthew W. Glasscott*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00062","DOIUrl":"10.1021/acsmaterialsau.3c00062","url":null,"abstract":"<p >Emergent high entropy nanomaterials and their associated complex surface structure hold promise to unlock unique catalytic intermediate pathways and photonic/plasmonic interactions; however, synthetic strategies to tune the size, morphological, and stoichiometric properties remain limited. This work demonstrates a confined electro-precipitation mechanism for the formation of tunable, high-entropy oxide microspheres within emulsion droplet scaffolds. This mechanism complements a traditional confined electrodeposition mechanism and explains the previously observed anomalous formation of thermodynamically unfavorable particles, including lanthanide species. Mass transfer studies reveal that microsphere coverage over a surface may be tuned and modeled by using a time-dependent modified Levich equation. Additionally, morphological tuning was demonstrated as a function of experimental conditions, such as rotation rate and precursor concentration. Finally, extension to multimetallic species permitted the generation of high-entropy lanthanide oxide microspheres, which were confirmed to have equimolar stoichiometries via energy dispersive spectroscopy and inductively coupled plasma mass spectrometry. This novel method promises to generate tunable, complex oxides with applications to thermal catalysis, optics, and applications yet unknown.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 2","pages":"179–184"},"PeriodicalIF":0.0,"publicationDate":"2023-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00062","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135589697","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}