ACS Materials Au最新文献

{"title":"Electrochemical Reduction of Nitrogen to Ammonia Using Zinc Telluride","authors":"Sham J. Mane, Nesta B. Joseph, Rekha Kumari, Awadhesh Narayan, Aninda J. Bhattacharyya","doi":"10.1021/acsmaterialsau.4c00014","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00014","url":null,"abstract":"Electrosynthesis of ammonia (NH₃), an important constituent molecule of various commercial fertilizers, is a promising and sustainable alternative strategy compared with the century-old Haber-Bosch process. Herein, zinc telluride (ZnTe) is demonstrated as an efficient electrocatalyst for reducing nitrogen (N₂) under ambient conditions to NH₃. In this simple chemical strategy, Zn preferentially binds N₂ over hydrogen (H₂), and Te, by virtue of its superior electronic properties, enhances the electrocatalytic activity of ZnTe. The analysis of the X-ray diffraction data using the Bravais-Friedel-Donnay-Harker (BFDH) theory predicted a crystal geometry with the active electrocatalytic sites predominantly confined to the (111) planes of ZnTe. The preferential binding of nitrogen (N₂; adsorption energy = −0.043 eV) over hydrogen (H₂, adsorption energy = −0.028 eV) to Zn on the (111) plane of ZnTe is further confirmed by density functional theory. The ZnTe catalyst is observed to be stable in the acidic medium and delivers a very high yield of NH₃ (19.85 μg/h^–1 mg_cat^–1) and a Faradaic efficiency of 6.24% at −0.6 V (versus RHE). Additional verification experiments do not reveal the formation of side products (such as NH₂–NH₂) during N₂ reduction by ZnTe. Further, density functional theory calculations strongly predict that the electrocatalytic reduction of N₂ to NH₃ by ZnTe preferentially occurs via the alternate pathway.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"28 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141933577","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":"Realizing the Potential of Commercial E-Textiles for Wearable Glucose Biosensing Application","authors":"Moshfiq-Us-Saleheen Chowdhury, Sutirtha Roy, Krishna Prasad Aryal, Henry Leung, Richa Pandey","doi":"10.1021/acsmaterialsau.4c00033","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00033","url":null,"abstract":"Advancements in wearable technology have enabled noninvasive health monitoring using biosensors. This research focuses on developing a textile-based sweat glucose sensor using commercially available conductive textiles, evading the complexity of traditional fabrication methods. A comparative analysis of three low-cost conductive textiles, Adafruit 1364, 1167, and 4762, has been conducted for electrochemical glucose detection with glucose-specific enzymes such as glucose oxidase (GOx) and glucose dehydrogenase (GDH). Adafruit 1364 outperformed others in morphological, electrochemical, and wearable properties. Cyclic voltammetry shows that Adafruit 1364 and 4762 effectively detect glucose at the potential of 0.23 and 0.08 V using glucose oxidase and 0.1 and 0.08 V using glucose dehydrogenase enzymes, respectively. Furthermore, chronoamperometry has been conducted to confirm the presence of glucose at 1 μM concentration. Differential pulse voltammetry was conducted to assess the sensitivity of the Adafruit 1364 fabric electrode using glucose solutions with concentrations of 0.05, 0.15, 0.25, and 0.5 mM. The electrode immobilized with GOx showed a sensitivity of 0.005 μA μM⁻¹ and a limit of detection (LOD) of 41.3 μM, while the electrode immobilized with GDH exhibited a sensitivity of 0.0019 μA μM⁻¹ and an LOD of 63.1 μM. The study also highlighted the reproducibility, effect of interferents, and advantageous wearable properties of these sensors.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"60 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141776058","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":"Self-Diffusion of Ge in Amorphous GexSi1–x Films Studied In Situ by Neutron Reflectometry","authors":"Erwin Hüger*,&nbsp;Jochen Stahn and Harald Schmidt,&nbsp;","doi":"10.1021/acsmaterialsau.4c0004610.1021/acsmaterialsau.4c00046","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00046https://doi.org/10.1021/acsmaterialsau.4c00046","url":null,"abstract":"<p >Ge_<i>x</i>Si_1–<i>x</i> alloys are gaining renewed interest for many applications in electronics and optics, especially for miniaturized devices showing quantum size effects. Point defects and atomic diffusion play a crucial role in miniaturized and metastable systems. In the present work, Ge self-diffusion in sputter deposited amorphous Ge_<i>x</i>Si_1–<i>x</i> alloys is studied in situ as a function of Ge content <i>x</i> = 0.13, 0.43, 0.8, and 1.0 by neutron reflectometry. The determined Ge self-diffusivities obey the Arrhenius law in the investigated temperature ranges. The higher the Ge content <i>x</i>, the higher the Ge self-diffusivity at the same temperature. The activation enthalpy decreases with <i>x</i> from 4.4 eV for self-diffusion in pure silicon films to about 2 eV self-diffusion in Ge_0.8Si_0.2 and Ge. The decrease of the activation enthalpy for amorphous Ge_<i>x</i>Si_1–<i>x</i> is similar to the case of crystalline Ge_<i>x</i>Si_1–<i>x</i>. Possible explanations are discussed.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 5","pages":"537–546 537–546"},"PeriodicalIF":5.7,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00046","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142166919","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":"Self-Diffusion of Ge in Amorphous GexSi1–x Films Studied In Situ by Neutron Reflectometry","authors":"Erwin Hüger, Jochen Stahn, Harald Schmidt","doi":"10.1021/acsmaterialsau.4c00046","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00046","url":null,"abstract":"Ge_<i>x</i>Si_1–<i>x</i> alloys are gaining renewed interest for many applications in electronics and optics, especially for miniaturized devices showing quantum size effects. Point defects and atomic diffusion play a crucial role in miniaturized and metastable systems. In the present work, Ge self-diffusion in sputter deposited amorphous Ge_<i>x</i>Si_1–<i>x</i> alloys is studied in situ as a function of Ge content <i>x</i> = 0.13, 0.43, 0.8, and 1.0 by neutron reflectometry. The determined Ge self-diffusivities obey the Arrhenius law in the investigated temperature ranges. The higher the Ge content <i>x</i>, the higher the Ge self-diffusivity at the same temperature. The activation enthalpy decreases with <i>x</i> from 4.4 eV for self-diffusion in pure silicon films to about 2 eV self-diffusion in Ge_0.8Si_0.2 and Ge. The decrease of the activation enthalpy for amorphous Ge_<i>x</i>Si_1–<i>x</i> is similar to the case of crystalline Ge_<i>x</i>Si_1–<i>x</i>. Possible explanations are discussed.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"85 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141785444","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":"In Vitro Osteo-Immunological Responses of Bioactive Calcium Phosphate-Containing Urethane Dimethacrylate-Based Composites: A Potential Alternative to Poly(methyl methacrylate) Bone Cement","authors":"Weerachai Singhatanadgit, Piyarat Sungkhaphan, Boonlom Thavornyutikarn, Setthawut Kitpakornsanti, Anne Young, Wanida Janvikul","doi":"10.1021/acsmaterialsau.4c00037","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00037","url":null,"abstract":"This investigation developed new composite bone cements using urethane dimethacrylate (UDMA), poly(propylene glycol) dimethacrylate (PPGDMA), and hydroxyethyl methacrylate (HEMA), with micrometer-sized aluminosilicate glass filler. Monocalcium phosphate monohydrate (MCPM) and hydroxyapatite (HA) particles were added to enhance biological performance, particularly osteo-immunomodulation. Free radical polymerization was triggered by mixing two pastes containing either benzoyl peroxide (BPO, an initiator) or N-tolyglycine glycidyl methacrylate (NTGGMA, an activator). Increasing butylated hydroxytoluene (BHT, an inhibitor) enabled a suitable delay after mixing at 25 °C for placement. At 37 °C, the delay time was reduced and the final conversion was enhanced. Findings also demonstrated the biocompatibility of the developed bone cement toward osteo-immunological cell lineages, including mesenchymal stem cells (MSCs), fibroblasts, osteoclast precursor RAW 246.7 cells, and peripheral blood mononuclear cells (PBMCs). Notably, the cement with both MCPM and HA combined facilitated sufficient MSC growth, enabling subsequent mineralization while concurrently suppressing the proliferation of fibroblasts, osteoclast progenitors, and PBMCs. Furthermore, composite cement exhibited the capacity to differentially regulate osteoblast differentiation, cell-(in)dependent mineralization, osteoclastogenesis, and PBMC-mediated inflammatory responses at both cellular and molecular levels in vitro. These observations suggested their potential use for bone repair, especially in cases of inflammation-associated bone defects.","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"342 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141754024","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":"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":"4 5","pages":"450–458 450–458"},"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":"8 1","pages":""},"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":"4 5","pages":"523–536 523–536"},"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":"81 1","pages":""},"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":"4 4","pages":"354–384"},"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}