ACS Materials Au最新文献

{"title":"Embracing Nature’s Clockwork: Crafting Plastics for Degradation in Plant Agricultural Systems","authors":"Danila Merino*,&nbsp;","doi":"10.1021/acsmaterialsau.4c0003110.1021/acsmaterialsau.4c00031","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00031https://doi.org/10.1021/acsmaterialsau.4c00031","url":null,"abstract":"<p >In the 21st century, global agriculture confronts the urgent challenge of increasing food production by 70% by 2050 while simultaneously addressing environmental and health concerns. Plastics, integral to agricultural innovation, present sustainability challenges due to their non-biodegradable nature and contribution to pollution. This perspective examines the transition to bioplastics, emphasizing their bio-based origin and their crucial characteristic of being readily biodegradable in the soil. Key bioplastics such as poly(lactic acid) (PLA), polyhydroxyalkanoates (PHAs), and biomass-derived polymers are discussed, particularly regarding the microplastic generation in soil resulting from their use in specific applications like mulch films, delivery systems, and soil conditioners. Embracing bioplastics signifies a significant step forward in achieving sustainable agriculture and addressing plastic waste. However, it is highlighted that while some bioplastics can be recovered and recycled, special applications where the plastic is in intimate contact with soil pose challenges for recovery. In these cases, that represent more than the 50% of plastics used in agriculture, meticulous design for biodegradation in soil synchronized with agricultural cycles is necessary. This approach ensures minimal environmental impact and promotes a circular approach to plastic use in agriculture.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00031","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161502","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":"Embracing Nature’s Clockwork: Crafting Plastics for Degradation in Plant Agricultural Systems","authors":"Danila Merino","doi":"10.1021/acsmaterialsau.4c00031","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00031","url":null,"abstract":"In the 21st century, global agriculture confronts the urgent challenge of increasing food production by 70% by 2050 while simultaneously addressing environmental and health concerns. Plastics, integral to agricultural innovation, present sustainability challenges due to their non-biodegradable nature and contribution to pollution. This perspective examines the transition to bioplastics, emphasizing their bio-based origin and their crucial characteristic of being readily biodegradable in the soil. Key bioplastics such as poly(lactic acid) (PLA), polyhydroxyalkanoates (PHAs), and biomass-derived polymers are discussed, particularly regarding the microplastic generation in soil resulting from their use in specific applications like mulch films, delivery systems, and soil conditioners. Embracing bioplastics signifies a significant step forward in achieving sustainable agriculture and addressing plastic waste. However, it is highlighted that while some bioplastics can be recovered and recycled, special applications where the plastic is in intimate contact with soil pose challenges for recovery. In these cases, that represent more than the 50% of plastics used in agriculture, meticulous design for biodegradation in soil synchronized with agricultural cycles is necessary. This approach ensures minimal environmental impact and promotes a circular approach to plastic use in agriculture.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141612708","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":"Synthesis Route to Single-Walled Zeolite Nanotubes Enabled by Tetrabutylammonium Hydroxide","authors":"Anthony Vallace,&nbsp;Dhrumil R. Shah,&nbsp;Enerelt Burentugs,&nbsp;Atticus J. Tucker,&nbsp;Ashley E. Cavanagh and Christopher W. Jones*,&nbsp;","doi":"10.1021/acsmaterialsau.4c0003010.1021/acsmaterialsau.4c00030","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00030https://doi.org/10.1021/acsmaterialsau.4c00030","url":null,"abstract":"<p >Single-walled zeolite nanotubes (ZNT) were recently synthesized in a narrow compositional window. ZNT structural features─thin zeolitic walls and large mesopores─can allow for easy access of small molecules to zeolite micropores, but they also impart processing limitations for these materials, such as challenges with conventional aqueous ion-exchange conditions. Conventional solid- and liquid-phase ion exchange of calcined NaOH-derived ZNT (NaH-ZNT) results in structural degradation to either 2D sheet-like phases, 3D nanocrystals, or amorphous phases, motivating different direct synthesis routes and unconventional ion-exchange procedures of uncalcined ZNT precursors. Here, a modified synthesis route for ZNT synthesis is introduced that facilitates facile ion exchange as well as incorporation of additional non-Al heteroatoms in the zeolite framework. Tetrabutylammonium hydroxide (TBAOH) is used as a hydroxide source and co-OSDA, enabling synthesis of new compositions of ZNT, otherwise unachievable by post-modification of previously reported NaH-ZNT. By varying the gel composition, synthesis temperature, crystallization time, hydroxide source, silicon source, and aluminum source, productive conditions for the new TBAOH synthesis are developed, leading to increased strong acid site density in the ZNT. The collected results demonstrate the sensitivity of the ZNT synthesis to many key parameters and show that the ZNT forms only when Si/(Al + T) ∼ 30 in these synthesis gels and with specific Si and Al sources, and always in the presence of trace Na⁺. Catalytic testing, via the tandem CO₂ hydrogenation to methanol and methanol to aromatics reaction, shows that ZNTs provide adequate catalytic activity (acidity), relative to their conventional 3D counterparts in converting methanol to aromatic compounds.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00030","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161460","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":"Synthesis Route to Single-Walled Zeolite Nanotubes Enabled by Tetrabutylammonium Hydroxide","authors":"Anthony Vallace, Dhrumil R. Shah, Enerelt Burentugs, Atticus J. Tucker, Ashley E. Cavanagh, Christopher W. Jones","doi":"10.1021/acsmaterialsau.4c00030","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00030","url":null,"abstract":"Single-walled zeolite nanotubes (ZNT) were recently synthesized in a narrow compositional window. ZNT structural features─thin zeolitic walls and large mesopores─can allow for easy access of small molecules to zeolite micropores, but they also impart processing limitations for these materials, such as challenges with conventional aqueous ion-exchange conditions. Conventional solid- and liquid-phase ion exchange of calcined NaOH-derived ZNT (NaH-ZNT) results in structural degradation to either 2D sheet-like phases, 3D nanocrystals, or amorphous phases, motivating different direct synthesis routes and unconventional ion-exchange procedures of uncalcined ZNT precursors. Here, a modified synthesis route for ZNT synthesis is introduced that facilitates facile ion exchange as well as incorporation of additional non-Al heteroatoms in the zeolite framework. Tetrabutylammonium hydroxide (TBAOH) is used as a hydroxide source and co-OSDA, enabling synthesis of new compositions of ZNT, otherwise unachievable by post-modification of previously reported NaH-ZNT. By varying the gel composition, synthesis temperature, crystallization time, hydroxide source, silicon source, and aluminum source, productive conditions for the new TBAOH synthesis are developed, leading to increased strong acid site density in the ZNT. The collected results demonstrate the sensitivity of the ZNT synthesis to many key parameters and show that the ZNT forms only when Si/(Al + T) ∼ 30 in these synthesis gels and with specific Si and Al sources, and always in the presence of trace Na⁺. Catalytic testing, via the tandem CO₂ hydrogenation to methanol and methanol to aromatics reaction, shows that ZNTs provide adequate catalytic activity (acidity), relative to their conventional 3D counterparts in converting methanol to aromatic compounds.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141612760","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":"Viscoelasticity in 3D Cell Culture and Regenerative Medicine: Measurement Techniques and Biological Relevance","authors":"Payam Eliahoo,&nbsp;Hesam Setayesh,&nbsp;Tyler Hoffman,&nbsp;Yifan Wu,&nbsp;Song Li and Jennifer B. Treweek*,&nbsp;","doi":"10.1021/acsmaterialsau.3c00038","DOIUrl":"10.1021/acsmaterialsau.3c00038","url":null,"abstract":"<p >The field of mechanobiology is gaining prominence due to recent findings that show cells sense and respond to the mechanical properties of their environment through a process called mechanotransduction. The mechanical properties of cells, cell organelles, and the extracellular matrix are understood to be viscoelastic. Various technologies have been researched and developed for measuring the viscoelasticity of biological materials, which may provide insight into both the cellular mechanisms and the biological functions of mechanotransduction. Here, we explain the concept of viscoelasticity and introduce the major techniques that have been used to measure the viscoelasticity of various soft materials in different length- and timescale frames. The topology of the material undergoing testing, the geometry of the probe, the magnitude of the exerted stress, and the resulting deformation should be carefully considered to choose a proper technique for each application. Lastly, we discuss several applications of viscoelasticity in 3D cell culture and tissue models for regenerative medicine, including organoids, organ-on-a-chip systems, engineered tissue constructs, and tunable viscoelastic hydrogels for 3D bioprinting and cell-based therapies.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.3c00038","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141500878","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":"Impact of Nickel on Iridium–Ruthenium Structure and Activity for the Oxygen Evolution Reaction under Acidic Conditions","authors":"Erlend Bertheussen, Simon Pitscheider, S. Cooper, Rebecca Pittkowski, Katrine L. Svane, Aline Bornet, Erik M. Wisaeus, Kirsten M. Ø. Jensen, Jan Rossmeisl, Matthias Arenz, Christian Kallesøe, Christoffer M. Pedersen","doi":"10.1021/acsmaterialsau.4c00025","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00025","url":null,"abstract":"","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141336725","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":"Impact of Nickel on Iridium–Ruthenium Structure and Activity for the Oxygen Evolution Reaction under Acidic Conditions","authors":"Erlend Bertheussen,&nbsp;Simon Pitscheider,&nbsp;Susan R. Cooper,&nbsp;Rebecca Pittkowski,&nbsp;Katrine L. Svane,&nbsp;Aline Bornet,&nbsp;Erik M. Wisaeus,&nbsp;Kirsten M. Ø. Jensen,&nbsp;Jan Rossmeisl,&nbsp;Matthias Arenz,&nbsp;Christian Kallesøe and Christoffer M. Pedersen*,&nbsp;","doi":"10.1021/acsmaterialsau.4c0002510.1021/acsmaterialsau.4c00025","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00025https://doi.org/10.1021/acsmaterialsau.4c00025","url":null,"abstract":"<p >Proton exchange membrane water electrolysis (PEMWE) is a promising technology to produce hydrogen directly from renewable electricity sources due to its high power density and potential for dynamic operation. Widespread application of PEMWE is, however, currently limited due to high cost and low efficiency, for which high loading of expensive iridium catalyst and high OER overpotential, respectively, are important reasons. In this study, we synthesize highly dispersed IrRu nanoparticles (NPs) supported on antimony-doped tin oxide (ATO) to maximize catalyst utilization. Furthermore, we study the effect of adding various amounts of Ni to the synthesis, both in terms of catalyst structure and OER activity. Through characterization using various X-ray techniques, we determine that the presence of Ni during synthesis yields significant changes in the structure of the IrRu NPs. With no Ni present, metallic IrRu NPs were synthesized with Ir-like structure, while the presence of Ni leads to the formation of IrRu oxide particles with rutile/hollandite structure. There are also clear indications that the presence of Ni yields smaller particles, which can result in better catalyst dispersion. The effect of these differences on OER activity was also studied through rotating disc electrode measurements. The IrRu-supported catalyst synthesized with Ni exhibited OER activity of up to 360 mA mg_PGM^–1 at 1.5 V vs RHE. This is ∼7 times higher OER activity than the best-performing IrO_<i>x</i> benchmark reported in the literature and more than twice the activity of IrRu-supported catalyst synthesized without Ni. Finally, density functional theory (DFT) calculations were performed to further elucidate the origin of the observed activity enhancement, showing no improvement in intrinsic OER activity for hollandite Ir and Ru compared to the rutile structures. We, therefore, hypothesize that the increased activity measured for the IrRu supported catalyst synthesized with Ni present is instead due to increased electrochemical surface area.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-06-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00025","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161258","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":"In Vivo Assessment of a Triple Periodic Minimal Surface Based Biomimmetic Gyroid as an Implant Material in a Rabbit Tibia Model","authors":"Pearlin Amaan Khan,&nbsp;Ansheed Raheem,&nbsp;Cheirmadurai Kalirajan,&nbsp;Konda Gokuldoss Prashanth and Geetha Manivasagam*,&nbsp;","doi":"10.1021/acsmaterialsau.4c0001610.1021/acsmaterialsau.4c00016","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00016https://doi.org/10.1021/acsmaterialsau.4c00016","url":null,"abstract":"<p >Biomimetic approaches to implant construction are a rising frontier in implantology. Triple Periodic Minimal Surface (TPMS)-based additively manufactured gyroid structures offer a mean curvature of zero, rendering this structure an ideal porous architecture. Previous studies have demonstrated the ability of these structures to effectively mimic the mechanical cues required for optimal implant construction. The porous nature of gyroid materials enhances bone ingrowth, thereby improving implant stability within the body. This enhancement is attributed to the increased surface area of the gyroid structure, which is approximately 185% higher than that of a dense material of the same form factor. This larger surface area allows for enhanced cellular attachment and nutrient circulation facilitated by the porous channels. This study aims to evaluate the biological performance of a gyroid-based Ti6Al-4V implant material compared to a dense alloy counterpart. Cellular viability was assessed using the lactate dehydrogenase (LDH) assay, which demonstrated that the gyroid surface allowed marginally higher viability than dense material. The <i>in vivo</i> integration was studied over 6 weeks using a rabbit tibia model and characterized using X-ray, micro-CT, and histopathological examination. With a metal volume of 8.1%, the gyroid exhibited a bone volume/total volume (BV/TV) ratio of 9.6%, which is 11-fold higher than that of dense metal (0.8%). Histological assessments revealed neovascularization, in-bone growth, and the presence of a Haversian system in the gyroid structure, hinting at superior osteointegration.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00016","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161257","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":"In Vivo Assessment of a Triple Periodic Minimal Surface Based Biomimmetic Gyroid as an Implant Material in a Rabbit Tibia Model","authors":"Pearlin Amaan Khan, Ansheed Raheem, Cheirmadurai Kalirajan, K. Prashanth, Geetha Manivasagam","doi":"10.1021/acsmaterialsau.4c00016","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00016","url":null,"abstract":"","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141351141","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":"Electrocatalytic and Selective Oxidation of Glycerol to Formate on 2D 3d-Metal Phosphate Nanosheets and Carbon-Negative Hydrogen Generation","authors":"Inderjeet Chauhan,&nbsp;Pothoppurathu M. Vijay,&nbsp;Ravi Ranjan,&nbsp;Kshirodra Kumar Patra and Chinnakonda S. Gopinath*,&nbsp;","doi":"10.1021/acsmaterialsau.4c0002410.1021/acsmaterialsau.4c00024","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00024https://doi.org/10.1021/acsmaterialsau.4c00024","url":null,"abstract":"<p >In the landscape of green hydrogen production, alkaline water electrolysis is a well-established, yet not-so-cost-effective, technique due to the high overpotential requirement for the oxygen evolution reaction (OER). A low-voltage approach is proposed to overcome not only the OER challenge by favorably oxidizing abundant feedstock molecules with an earth-abundant catalyst but also to reduce the energy input required for hydrogen production. This alternative process not only generates carbon-negative green H₂ but also yields concurrent value-added products (VAPs), thereby maximizing economic advantages and transforming waste into valuable resources. The essence of this study lies in a novel electrocatalyst material. In the present study, unique and two-dimensional (2D) ultrathin nanosheet phosphates featuring first-row transition metals are synthesized by a one-step solvothermal method, and evaluated for the electrocatalytic glycerol oxidation reaction (GLYOR) in an alkaline medium and simultaneous H₂ production. Co₃(PO₄)₂ (CoP), Cu₃(PO₄)₂ (CuP), and Ni₃(PO₄)₂ (NiP) exhibit 2D sheet morphologies, while FePO₄ (FeP) displays an entirely different snowflake-like morphology. The 2D nanosheet morphology provides a large surface area and a high density of active sites. As a GLYOR catalyst, CoP ultrathin (∼5 nm) nanosheets exhibit remarkably low onset potential at 1.12 V (vs RHE), outperforming that of NiP, FeP, and CuP around 1.25 V (vs RHE). CoP displays 82% selective formate production, indicating a superior capacity for C–C cleavage and concurrent oxidation; this property could be utilized to valorize larger molecules. CoP also exhibits highly sustainable electrochemical stability for a continuous 200 h GLYOR operation, yielding 6.5 L of H₂ production with a 4 cm² electrode and 98 ± 0.5% Faradaic efficiency. The present study advances our understanding of efficient GLYOR catalysts and underscores the potential of sustainable and economically viable green hydrogen production methodologies.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00024","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161259","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}