Displaying publications 21 - 40 of 73 in total

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  1. Saidi NM, Omar FS, Numan A, Apperley DC, Algaradah MM, Kasi R, et al.
    ACS Appl Mater Interfaces, 2019 Aug 21;11(33):30185-30196.
    PMID: 31347822 DOI: 10.1021/acsami.9b07062
    To overcome the critical limitations of liquid-electrolyte-based dye-sensitized solar cells, quasi-solid-state electrolytes have been explored as a means of addressing long-term device stability, albeit with comparatively low ionic conductivities and device performances. Although metal oxide additives have been shown to augment ionic conductivity, their propensity to aggregate into large crystalline particles upon high-heat annealing hinders their full potential in quasi-solid-state electrolytes. In this work, sonochemical processing has been successfully applied to generate fine Co3O4 nanoparticles that are highly dispersible in a PAN:P(VP-co-VAc) polymer-blended gel electrolyte, even after calcination. An optimized nanocomposite gel polymer electrolyte containing 3 wt % sonicated Co3O4 nanoparticles (PVVA-3) delivers the highest ionic conductivity (4.62 × 10-3 S cm-1) of the series. This property is accompanied by a 51% enhancement in the apparent diffusion coefficient of triiodide versus both unmodified and unsonicated electrolyte samples. The dye-sensitized solar cell based on PVVA-3 displays a power conversion efficiency of 6.46% under AM1.5 G, 100 mW cm-2. By identifying the optimal loading of sonochemically processed nanoparticles, we are able to generate a homogenous extended particle network that effectively mobilizes redox-active species through a highly amorphous host matrix. This effect is manifested in a selective 51% enhancement in photocurrent density (JSC = 16.2 mA cm-2) and a lowered barrier to N719 dye regeneration (RCT = 193 Ω) versus an unmodified solar cell. To the best of our knowledge, this work represents the highest known efficiency to date for dye-sensitized solar cells based on a sonicated Co3O4-modified gel polymer electrolyte. Sonochemical processing, when applied in this manner, has the potential to make meaningful contributions toward the ongoing mission to achieve the widespread exploitation of stable and low-cost dye-sensitized solar cells.
  2. Halilu A, Hayyan M, Aroua MK, Yusoff R, Hizaddin HF
    ACS Appl Mater Interfaces, 2019 Jul 24;11(29):25928-25939.
    PMID: 31305059 DOI: 10.1021/acsami.9b05962
    Climate engineering solutions with emphasis on CO2 removal remain a global open challenge to balancing atmospheric CO2 equilibrium levels. As a result, warnings of impending climate disasters are growing every day in urgency. Beyond ordinary CO2 removal through natural CO2 sinks such as oceans and forest vegetation, direct CO2 conversion into valuable intermediaries is necessary. Here, a direct electrosynthesis of the peroxydicarbonate anion (C2O62-) was investigated by the reaction of CO2 with the superoxide ion (O2·-), electrochemically generated from O2 reduction in bis(trifluoromethylsulfonyl)imide [TFSI-] anion derived ionic liquid (IL) media. This is the first time that the IL media were employed successfully for CO2 conversion into C2O62-. Moreover, the charge transfer coefficient for the O2·- generation process in the ILs was less than 0.5, indicating that the process was irreversible. Voltammetry experiments coupled with global electrophilicity index analysis revealed that, when CO2/O2 was contacted simultaneously in the IL medium, O2·- was generated in situ first at a potential of approximately -1.0 V. Also, CO2 was more susceptible to attack by O2·- before any possible interaction with the IL except for [PMIm+][TFSI-]. This was because CO2 has a higher global electrophilicity index (ωCO2 = 0.489 eV) than those for the [EDMPAmm+][TFSI-] and [MOEMMor+][TFSI-]. By further COSMO-RS modeling, CO2 absorption was proven feasible at the COSMO-surface of the [TFSI-] IL-anion where the charge densities were σ = -1.100 and 1.1097 e/nm2. Therefore, the susceptible competitiveness of either IL cations or CO2 to the nucleophilic effects of O2·- was a function of their positive character as estimated by their electrophilicity indices. As determined by experimental attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and DFT-FTIR computation, the reaction yielded C2O62- in the ILs. Consequently, the presence of O=O symmetric stretching FTIR vibrational mode at ∼844 cm-1 coupled with the disappearance of the oxidative cyclic voltammetry waves when sparging CO2 and O2 confirmed the presence of C2O62-. Moreover, based on DFT/B3LYP/6-31G, pure C2O62- has symmetric O=O stretching at ∼805 and ∼844 cm-1 when it is in association with the IL-cation. This was the first spectroscopic observation of C2O62- in ILs, and the O=O symmetric stretching vibration has peculiarity for identifying C2O62- in ILs. This will open new doors to utilize CO2 in industrial applications with the aid of reactive oxygen species.
  3. Steiner JD, Cheng H, Walsh J, Zhang Y, Zydlewski B, Mu L, et al.
    ACS Appl Mater Interfaces, 2019 Oct 16;11(41):37885-37891.
    PMID: 31589393 DOI: 10.1021/acsami.9b14729
    Elemental doping represents a prominent strategy to improve interfacial chemistry in battery materials. Manipulating the dopant spatial distribution and understanding the dynamic evolution of the dopants at the atomic scale can inform better design of the doping chemistry for batteries. In this work, we create a targeted hierarchical distribution of Ti4+, a popular doping element for oxide cathode materials, in LiNi0.8Mn0.1Co0.1O2 primary particles. We apply multiscale synchrotron/electron spectroscopy and imaging techniques as well as theoretical calculations to investigate the dynamic evolution of the doping chemical environment. The Ti4+ dopant is fully incorporated into the TMO6 octahedral coordination and is targeted to be enriched at the surface. Ti4+ in the TMO6 octahedral coordination increases the TM-O bond length and reduces the covalency between (Ni, Mn, Co) and O. The excellent reversibility of Ti4+ chemical environment gives rise to superior oxygen reversibility at the cathode-electrolyte interphase and in the bulk particles, leading to improved stability in capacity, energy, and voltage. Our work directly probes the chemical environment of doping elements and helps rationalize the doping strategy for high-voltage layered cathodes.
  4. Navaneethan B, Vijayakumar GP, Ashang Luwang L, Karuppiah S, Jayarama Reddy V, Ramakrishna S, et al.
    ACS Appl Mater Interfaces, 2021 Mar 03;13(8):9691-9701.
    PMID: 33605136 DOI: 10.1021/acsami.0c22028
    Electrospinning is a promising technique for the fabrication of bioscaffolds in tissue engineering applications. Pertaining issues of multiple polymer jets and bending instabilities result in random paths which lend poor controllability over scaffolds morphology for affecting the porosity and mechanical stability. The present study alleviates these challenges by demonstrating a novel self-directing single jet taking a specifically patterned path to deposit fibers into circular and uniform scaffolds without tuning any externally controlled parameters. High-speed camera observation revealed that the charge retention and dissipation on the collected fibers caused rapid autojet switching between the two jetting modes, namely, a microcantilever-like armed jet motion and a whipping motion, which sequentially expand the area and thickness of the scaffolds, respectively, in a layered-like fashion. The physical properties showed that the self-switching dual-jet modes generated multilayered microfibrous scaffolds (MFSs) with dual morphologies and varied fiber packing density, thereby establishing the gradient porosity and mechanical strength (through buckled fibers) in the scaffolds. In vitro studies showed that as-spun scaffolds are cell-permeable hierarchical 3D microporous structures enabling lateral cell seeding into multiple layers. The cell proliferation on days 6 and 9 increased 21% and 38% correspondingly on MFSs than on nanofibrous scaffolds (NFSs) done by conventional multijets electrospinning. Remarkably, this novel and single-step process is highly reproducible and tunable for developing fibrous scaffolds for tissue engineering applications.
  5. Cheng Y, Lai OM, Tan CP, Panpipat W, Cheong LZ, Shen C
    ACS Appl Mater Interfaces, 2021 Jan 27;13(3):4146-4155.
    PMID: 33440928 DOI: 10.1021/acsami.0c17134
    Immobilization can be used to improve the stability of lipases and enhances lipase recovery and reusability, which increases its commercial value and industrial applications. Nevertheless, immobilization frequently causes conformational changes of the lipases, which decrease lipase catalytic activity. in the present work, we synthesized UIO-66 and grafted UIO-66 crystals with proline for immobilization of Candida rugosa lipase (CRL). As indicated by steady-state fluorescence microscopy, grafting of proline onto UIO-66 crystals induced beneficial conformational change in CRL. CRL immobilized on UIO-66/Pro (CRL@UIO-66/Pro) demonstrated higher enzyme activity and better recyclability than that immobilized on UIO-66 (CRL@UIO-66) in both hydrolysis (CRL@UIO-66/Pro: 0.34 U; CRL@UIO-66: 0.15 U) and transesterification (CRL@UIO-66/Pro: 0.93 U; CRL@UIO-66: 0.25 U) reactions. The higher values of kcat and kcat/Km of CRL@UIO-66/Pro also showed that it had better catalytic efficiency as compared to CRL@UIO-66. It is also worth noting that CRL@UIO-66/Pro (0.93 U) demonstrated a much higher transesterification activity as compared to free CRL (0.11 U), indicating that UIO-66/Pro has increased the solvent stability of CRL. Both CRL@UIO-66 and CRL@UIO-66/Pro were also used for the fabrication of biosensors for nitrofen with a wide linear range (0-100 μM), lower limit of detection, and good recovery rate.
  6. Foroozandeh P, Aziz AA, Mahmoudi M
    ACS Appl Mater Interfaces, 2019 Oct 30;11(43):39672-39687.
    PMID: 31633323 DOI: 10.1021/acsami.9b15533
    Clinical translation of nanotechnologies has limited success, at least in part, due to the existence of several overlooked factors on the nature of the nanosystem (e.g., physicochemical properties of nanoparticles), nanobio interfaces (e.g., protein corona composition), and the cellular characteristics (e.g., cell type). In the past decade, several ignored factors including personalized and disease-specific protein corona (a layer of formed biomolecules at the surface of nanoparticles upon their entrance into a biological fluid), incubating temperature, local temperature gradient, cell shape, and cell sex has been introduced. Here, it was hypothesized and validated cell age as another overlooked factor in the field of nanomedicine. To test our hypothesis, cellular toxicity and uptake profiles of our model nanoparticles (i.e., PEGylated quantum dots, QDs) were probed in young and senescent cells (i.e., IMR90 fibroblast cells from human fetal lung and CCD841CoN epithelial cells from human fetal colon) and the outcomes revealed substantial dependency of cell-nanoparticles interactions to the cell age. For example, it was observed that the PEGylated QDs were acutely toxic to senescent IMR90 and CCD841CoN cells, leading to lysosomal membrane permeabilization which caused cell necrosis; in contrast, the young cells were resilient to the exact same amount of QDs and the same incubation time. It was also found that the formation of protein corona could delay the QDs' toxicity on senescent cells. These findings suggest that the cellular aging process have a capacity to cause deteriorative effects on their organelles and normal functions. The outcomes of this study suggest the proof-of-concept that cell age may have critical role in biosystem responses to nanoparticle technologies. Therefore, the effect of cell age should be carefully considered on the nanobio interactions and the information about cellular age (e.g., passage number and age of the cell donor) should be included in the nanomedicine papers to facilitate clinical translation of nanotechnologies and to help scientists to better design and produce safe and efficient diagnostic/therapeutic age-specific nanoparticles.
  7. Mohammad Haniff MAS, Zainal Ariffin NH, Hafiz SM, Ooi PC, Syono MI, Hashim AM
    ACS Appl Mater Interfaces, 2019 Jan 30;11(4):4625-4636.
    PMID: 30618229 DOI: 10.1021/acsami.8b19043
    We demonstrated a simple and scalable fabrication route of a nitrogen-doped reduced graphene oxide (N-rGO) photodetector on an 8 in. wafer-scale. The N-rGO was prepared through in situ plasma treatment in an acetylene-ammonia atmosphere to achieve an n-type semiconductor with substantial formation of quaternary-N substituted into the graphene lattice. The morphology, structural, chemical composition, and electrical properties of the N-rGO were carefully characterized and used for the device fabrication. The N-rGO devices were fabricated in a simple metal-semiconductor-metal structure with unconventional metal-on-bottom configuration to promote high-performance photodetection. The N-rGO devices exhibited enhanced photoresponsivity as high as 0.68 A W-1 at 1.0 V, which is about 2 orders of magnitude higher compared to a pristine graphene and wide-band photoinduced response from the visible to the near-infrared region with increasing sensitivity in the order of 785, 632.8, and 473 nm excitation wavelengths. We also further demonstrated a symmetric characteristic of the photoinduced response to any position of local laser excitation with respect to the electrodes. The excellent features of wafer-scale N-rGO devices suggest a promising route to merge the current silicon technology and two-dimensional materials for future optoelectronic devices.
  8. Tan KH, Chen YW, Van CN, Wang H, Chen JW, Lim FS, et al.
    ACS Appl Mater Interfaces, 2019 Jan 09;11(1):1655-1664.
    PMID: 30561192 DOI: 10.1021/acsami.8b17758
    The ability of band offsets at multiferroic/metal and multiferroic/electrolyte interfaces in controlling charge transfer and thus altering the photoactivity performance has sparked significant attention in solar energy conversion applications. Here, we demonstrate that the band offsets of the two interfaces play the key role in determining charge transport direction in a downward self-polarized BFO film. Electrons tend to move to BFO/electrolyte interface for water reduction. Our experimental and first-principle calculations reveal that the presence of neodymium (Nd) dopants in BFO enhances the photoelectrochemical performance by reduction of the local electron-hole pair recombination sites and modulation of the band gap to improve the visible light absorption. This opens a promising route to the heterostructure design by modulating the band gap to promote efficient charge transfer.
  9. Wang D, Wong SI, Sunarso J, Xu M, Wang W, Ran R, et al.
    ACS Appl Mater Interfaces, 2021 May 05;13(17):20105-20113.
    PMID: 33886260 DOI: 10.1021/acsami.1c02502
    Hydrocarbon-fueled solid oxide fuel cells (SOFCs) that can operate in the intermediate temperature range of 500-700 °C represent an attractive SOFC device for combined heat and power applications in the industrial market. One of the ways to realize such a device relies upon exploiting an in situ steam reforming process in the anode catalyzed by an anti-carbon coking catalyst. Here, we report a new Ni and Ru bimetal-doped perovskite catalyst, Ba(Zr0.1Ce0.7Y0.1Yb0.1)0.9Ni0.05Ru0.05O3-δ (BZCYYbNRu), with enhanced catalytic hydrogen production activity on n-butane (C4H10), which can resist carbon coking over extended operation durations. Ru in the perovskite lattice inhibits Ni precipitation from perovskite, and the high water adsorption capacity of proton conducting perovskite improves the coking resistance of BZCYYbNRu. When BZCYYbNRu is used as a steam reforming catalyst layer on a Ni-YSZ-supported anode, the single fuel cell not only achieves a higher power density of 1113 mW cm-2 at 700 °C under a 10 mL min-1 C4H10 continuous feed stream at a steam to carbon (H2O/C) ratio of 0.5 but also shows a much better operational stability for 100 h at 600 °C compared with those reported in the literature.
  10. Ge S, Ma NL, Jiang S, Ok YS, Lam SS, Li C, et al.
    ACS Appl Mater Interfaces, 2020 Jul 08;12(27):30824-30832.
    PMID: 32544314 DOI: 10.1021/acsami.0c07448
    We used an innovative approach involving hot pressing, low energy consumption, and no adhesive to transform bamboo biomass into a natural sustainable fiber-based biocomposite for structural and furniture applications. Analyses showed strong internal bonding through mechanical "nail-like" nano substances, hydrogen, and ester and ether bonds. The biocomposite encompasses a 10-fold increase in internal bonding strength with improved water resistance, fire safety, and environmentally friendly properties as compared to existing furniture materials using hazardous formaldehyde-based adhesives. As compared to natural bamboo material, this new biocomposite has improved fire and water resistance, while there is no need for toxic adhesives (mostly made from formaldehyde-based resin), which eases the concern of harmful formaldehyde-based VOC emission and ensures better indoor air quality. This surpasses existing structural and furniture materials made by synthetic adhesives. Interestingly, our approach can 100% convert discarded bamboo biomass into this biocomposite, which represents a potentially cost reduction alternative with high revenue. The underlying fragment riveting and cell collapse binding are obviously a new technology approach that offers an economically and sustainable high-performance biocomposite that provides solutions to structural and furniture materials bound with synthetic adhesives.
  11. Alias N, Ali Umar A, Malek NAA, Liu K, Li X, Abdullah NA, et al.
    ACS Appl Mater Interfaces, 2021 Jan 20;13(2):3051-3061.
    PMID: 33410652 DOI: 10.1021/acsami.0c20137
    A deficiency in the photoelectrical dynamics at the interface due to the surface traps of the TiO2 electron transport layer (ETL) has been the critical factor for the inferiority of the power conversion efficiency (PCE) in the perovskite solar cells. Despite its excellent energy level alignment with most perovskite materials, its large density of surface defect as a result of sub lattice vacancies has been the critical hurdle for an efficient photovoltaic process in the device. Here, we report that atoms thick 2D TiS2 layer grown on the surface of a (001) faceted and single-crystalline TiO2 nanograss (NG) ETL have effectively passivated the defects, boosting the charge extractability, carrier mobility, external quantum efficiency, and the device stability. These properties allow the perovskite solar cells (PSCs) to produce a PCE as high as 18.73% with short-circuit current density (Jsc), open-circuit voltage (Voc), and fill-factor (FF) values as high as 22.04 mA/cm2, 1.13 V, and 0.752, respectively, a 3.3% improvement from the pristine TiO2-NG-based PSCs. The present approach should find an extensive application for controlling the photoelectrical dynamic deficiency in perovskite solar cells.
  12. Walle KZ, Musuvadhi Babulal L, Wu SH, Chien WC, Jose R, Lue SJ, et al.
    ACS Appl Mater Interfaces, 2021 Jan 20;13(2):2507-2520.
    PMID: 33406841 DOI: 10.1021/acsami.0c17422
    Although solid-state Li-metal batteries (LMBs) featuring polymer-based solid electrolytes might one day replace conventional Li-ion batteries, the poor Li-ion conductivity of solid polymer electrolytes at low temperatures has hindered their practical applications. Herein, we describe the first example of using a co-precipitation method in a Taylor flow reactor to produce the metal hydroxides of both the Ga/F dual-doped Li7La3Zr2O12 (Ga/F-LLZO) ceramic electrolyte precursors and the Li2MoO4-modified Ni0.8Co0.1Mn0.1O2 (LMO@T-LNCM 811) cathode materials for LMBs. The Li/Nafion (LiNf)-coated Ga/F-LLZO (LiNf@Ga/F-LLZO) ceramic filler was finely dispersed in the poly(vinylidene fluoride)/polyacrylonitrile/lithium bis(trifluoromethanesulfonimide)/succinonitrile matrix to give a trilayer composite polymer electrolyte (denoted "Tri-CPE") through a simple solution-casting. The bulk ionic conductivity of the Tri-CPE at room temperature was approximately 4.50 × 10-4 S cm-1 and exhibited a high Li+ ion transference number (0.84). It also exhibits a broader electrochemical window of 1-5.04 V versus Li/Li+. A full cell based on a CR2032 coin cell containing the LMO@T-LNCM811-based composite cathode, when cycled under 1 C/1 C at room temperature for 300 cycles, achieved an average Columbic efficiency of 99.4% and a capacity retention of 89.8%. This novel fabrication strategy for Tri-CPE structures has potential applications in the preparation of highly safe high-voltage cathodes for solid-state LMBs.
  13. Zainol Abidin MN, Goh PS, Said N, Ismail AF, Othman MHD, Hasbullah H, et al.
    ACS Appl Mater Interfaces, 2020 Jul 22;12(29):33276-33287.
    PMID: 32589391 DOI: 10.1021/acsami.0c08947
    The development of wearable artificial kidney demands an efficient dialysate recovery, which relies upon the adsorption process. This study proposes a solution to solve the problem of competitive adsorption between the uremic toxins by employing two adsorptive components in a membrane separation process. Dual-layer hollow fiber (DLHF) membranes, which are composed of a polysulfone (PSf)/activated carbon (AC) inner layer and a PSf/poly(methyl methacrylate) (PMMA) outer layer, were prepared for co-adsorptive removal of creatinine and urea from aqueous solution. The DLHF membranes were characterized in terms of morphological, physicochemical, water transport, and creatinine adsorption properties. The membrane was then subjected to an ultrafiltration adsorption study for performance evaluation. The incorporation of AC in membrane, as confirmed by microscopic and surface analyses, has improved the pure water flux up to 25.2 L/(m2 h). A membrane with optimum AC loading (9 wt %) demonstrated the highest maximum creatinine adsorption capacity (86.2 mg/g) based on the Langmuir adsorption isotherm model. In the ultrafiltration adsorption experiment, the membrane removed creatinine and urea with a combined average percent removal of 29.3%. Moreover, the membrane exhibited creatinine and urea uptake recoveries of 98.8 and 81.2%, respectively. The combined action of PMMA and AC in the PSf DLHF membrane has made the adsorption of multiple uremic toxins possible during dialysate recovery.
  14. Ali MK, Moshikur RM, Wakabayashi R, Moniruzzaman M, Goto M
    ACS Appl Mater Interfaces, 2021 May 05;13(17):19745-19755.
    PMID: 33891816 DOI: 10.1021/acsami.1c03111
    Chemotherapeutic cytotoxic agents such as paclitaxel (PTX) are considered essential for the treatment of various cancers. However, PTX injection is associated with severe systemic side effects and high rates of patient noncompliance. Micelle formulations (MFs) are nano-drug delivery systems that offer a solution to these problems. Herein, we report an advantageous carrier for the transdermal delivery of PTX comprising a new MF that consists of two biocompatible surfactants: cholinium oleate ([Cho][Ole]), which is a surface-active ionic liquid (SAIL), and sorbitan monolaurate (Span-20). A solubility assessment confirmed that PTX was readily solubilized in the SAIL-based micelles via multipoint hydrogen bonding and cation-π and π-π interactions between PTX and SAIL[Cho][Ole]. Dynamic light scattering (DLS) and transmission electron microscopy revealed that in the presence of PTX, the MF formed spherical PTX-loaded micelles that were well-distributed in the range 8.7-25.3 nm. According to DLS, the sizes and size distributions of the micelle droplets did not change significantly over the entire storage period, attesting to their physical stability. In vitro transdermal assessments using a Franz diffusion cell revealed that the MF absorbed PTX 4 times more effectively than a Tween 80-based formulation and 6 times more effectively than an ethanol-based formulation. In vitro and in vivo skin irritation tests revealed that the new carrier had a negligible toxicity profile compared with a conventional ionic liquid-based carrier. Based on these findings, we believe that the SAIL[Cho][Ole]-based MF has potential as a biocompatible nanocarrier for the effective transdermal delivery of poorly soluble chemotherapeutics such as PTX.
  15. Hama M, Ishima Y, Chuang VTG, Ando H, Shimizu T, Ishida T
    ACS Appl Mater Interfaces, 2021 May 05;13(17):19736-19744.
    PMID: 33881292 DOI: 10.1021/acsami.1c03065
    Abraxane, an albumin-bound paclitaxel nanoparticle formulation, is superior to conventional paclitaxel preparations because it has better efficacy against unresectable pancreatic cancer. Previous reports suggest that this better efficacy of Abraxane than conventional paclitaxel preparation is probably due to its transport through Gp60, an albumin receptor on the surface of vascular endothelial cells. The increased tumor accumulation of Abraxane is also caused by the secreted protein acid and rich in cysteine in the tumor stroma. However, the uptake mechanism of Abraxane remains poorly understood. In this study, we demonstrated that the delivery of Abraxane occurred via different receptor pathways from that of endogenous albumin. Our results showed that the uptake of endogenous albumin was inhibited by a Gp60 pathway inhibitor in the process of endocytosis through endothelial cells or tumor cells. In contrast, the uptake of Abraxane-derived HSA was less affected by the Gp60 pathway inhibitor but significantly reduced by denatured albumin receptor inhibitors. In conclusion, these data indicate that Abraxane-derived HSA was taken up into endothelial cells or tumor cells by a mechanism different from normal endogenous albumin. These new data on distinct cellular transport pathways of denatured albumin via gp family proteins different from those of innate albumin shed light on the mechanisms of tumor delivery and antitumor activity of Abraxane and provide new scientific rationale for the development of a novel albumin drug delivery strategy via a denatured albumin receptor.
  16. Robin Chang YH, Jiang J, Khong HY, Saad I, Chai SS, Mahat MM, et al.
    ACS Appl Mater Interfaces, 2021 Jun 02;13(21):25121-25136.
    PMID: 34008948 DOI: 10.1021/acsami.1c04759
    Transition metal chalcogenides (TMCs) have gained worldwide interest owing to their outstanding renewable energy conversion capability. However, the poor mechanical flexibility of most existing TMCs limits their practical commercial applications. Herein, triggered by the recent and imperative synthesis of highly ductile α-Ag2S, an effective approach based on evolutionary algorithm and ab initio total-energy calculations for determining stable, ductile phases of bulk and two-dimensional Ag
    x
    Se1-x and Ag
    x
    Te1-x compounds was implemented. The calculations correctly reproduced the global minimum bulk stoichiometric P212121-Ag8Se4 and P21/c-Ag8Te4 structures. Recently reported metastable AgTe3 was also revealed but it lacks dynamical stability. Further single-layered screening unveiled two new monolayer P4/nmm-Ag4Se2 and C2-Ag8Te4 phases. Orthorhombic Ag8Se4 crystalline has a narrow, direct band gap of 0.26 eV that increases to 2.68 eV when transforms to tetragonal Ag4Se2 monolayer. Interestingly, metallic P21/c-Ag8Te4 changes to semiconductor when thinned down to monolayer, exhibiting a band gap of 1.60 eV. Present findings confirm their strong stability from mechanical and thermodynamic aspects, with reasonable Vickers hardness, bone-like Young's modulus (E) and high machinability observed in bulk phases. Detailed analysis of the dielectric functions ε(ω), absorption coefficient α(ω), power conversion efficiency (PCE) and refractive index n(ω) of monolayers are reported for the first time. Fine theoretical PCE (SLME method ∼11-28%), relatively high n(0) (1.59-1.93), and sizable α(ω) (104-105 cm-1) that spans the infrared to visible regions indicate their prospects in optoelectronics and photoluminescence applications. Effective strategies to improve the temperature dependent power factor (PF) and figure of merit (ZT) are illustrated, including optimizing the carrier concentration. With decreasing thickness, ZT of p-doped Ag-Se was found to rise from approximately 0.15-0.90 at 300 K, leading to a record high theoretical conversion efficiency of ∼12.0%. The results presented foreshadow their potential application in a hybrid device that combines the photovoltaic and thermoelectric technologies.
  17. Haddadi SA, Hu S, Ghaderi S, Ghanbari A, Ahmadipour M, Pung SY, et al.
    ACS Appl Mater Interfaces, 2021 Sep 08;13(35):42074-42093.
    PMID: 34428889 DOI: 10.1021/acsami.1c13055
    MXene sheets, as new 2D nanomaterials, have been used in many advanced applications due to their superior thin-layered architecture, as well as their capability to be employed as novel nanocontainers for advanced applications. In this research, intercalated Ti3C2 MXene sheets were synthesized through an etching method, and then they were modified with 3-aminopropyltriethoxysilane (APTES). Cerium cations (Ce3+) as an eco-friendly corrosion inhibitor were encapsulated within Ti3C2 MXene sheets to fabricate novel self-healing epoxy nanocomposite coatings. The corrosion protection performance (CPP) of Ce3+-doped Ti3C2 MXene nanosheets (Ti3C2 MXene-Ce3+) in a 3.5 wt % sodium chloride (NaCl) solution was studied on bare mild steel substrates using electrochemical impedance spectroscopy (EIS) and potentiodynamic polarization measurements. The self-healing CPP of epoxy coatings loaded with 1 wt % undoped and doped Ti3C2 MXene was evaluated using EIS, salt spray, and field emission scanning electron microscopy (FE-SEM) techniques. The introduction of Ti3C2 MXene-Ce3+ into the corrosive solution and artificially scribed epoxy coating enhanced the total impedance from 717 to 6596 Ω cm2 and 8876 to 32092 Ω cm2, respectively, after 24 h of immersion compared to the control samples.
  18. Derakhshankhah H, Hajipour MJ, Barzegari E, Lotfabadi A, Ferdousi M, Saboury AA, et al.
    ACS Appl Mater Interfaces, 2016 Nov 16;8(45):30768-30779.
    PMID: 27766857
    EMT-type zeolite nanoparticles (EMT NPs) with particle size of 10-20 nm and external surface area of 200 m2/g have shown high selective affinity toward plasma protein (fibrinogen). Besides, the EMT NPs have demonstrated no adverse effect on blood coagulation hemostasis. Therefore, it was envisioned that the EMT NPs could inhibit possible β-amyloid (Aβ)-fibrinogen interactions that result in the formation of structurally abnormal clots, which are resistant to lysis, in cerebral vessels of patients with Alzheimer disease (AD). To evaluate this hypothesis, the clot formation and degradation of Aβ-fibrinogen in the presence and absence of the EMT zeolite NPs were assessed. The results clearly showed that the delay in clot dissolution was significantly reduced in the presence of zeolite NPs. By formation of protein corona, the EMT NPs showed a negligible reduction in their inhibitory strength. Docking of small molecules (Aβ-fibrinogen) introduced a novel potential inhibitory candidate. The zeolite NPs showed similar inhibitory effects on binding of fibrinogen to both Aβ(25-35) and/or Aβ(1-42). This indicates that the inhibitory strength of these NPs is independent of Aβ sequence, and it is suggested that the zeolite NPs adsorb fibrinogen and specifically obstruct their Aβ binding sites. Therefore, the zeolite NPs can be the safe and effective inhibitors in preventing Aβ-fibrinogen interaction and consequent cognitive damage.
  19. Haniff MASM, Hafiz SM, Huang NM, Rahman SA, Wahid KAA, Syono MI, et al.
    ACS Appl Mater Interfaces, 2017 May 03;9(17):15192-15201.
    PMID: 28418234 DOI: 10.1021/acsami.7b02833
    This paper presents a straightforward plasma treatment modification of graphene with an enhanced piezoresistive effect for the realization of a high-performance pressure sensor. The changes in the graphene in terms of its morphology, structure, chemical composition, and electrical properties after the NH3/Ar plasma treatment were investigated in detail. Through a sufficient plasma treatment condition, our studies demonstrated that plasma-treated graphene sheet exhibits a significant increase in sensitivity by one order of magnitude compared to that of the unmodified graphene sheet. The plasma-doping introduced nitrogen (N) atoms inside the graphene structure and was found to play a significant role in enhancing the pressure sensing performance due to the tunneling behavior from the localized defects. The high sensitivity and good robustness demonstrated by the plasma-treated graphene sensor suggest a promising route for simple, low-cost, and ultrahigh resolution flexible sensors.
  20. Esro M, Kolosov O, Jones PJ, Milne WI, Adamopoulos G
    ACS Appl Mater Interfaces, 2017 01 11;9(1):529-536.
    PMID: 27933760 DOI: 10.1021/acsami.6b11214
    Silicon dioxide (SiO2) is the most widely used dielectric for electronic applications. It is usually produced by thermal oxidation of silicon or by using a wide range of vacuum-based techniques. By default, the growth of SiO2 by thermal oxidation of silicon requires the use of Si substrates whereas the other deposition techniques either produce low quality or poor interface material and mostly require high deposition or annealing temperatures. Recent investigations therefore have focused on the development of alternative deposition paradigms based on solutions. Here, we report the deposition of SiO2 thin film dielectrics deposited by spray pyrolysis in air at moderate temperatures of ≈350 °C from pentane-2,4-dione solutions of SiCl4. SiO2 dielectrics were investigated by means of UV-vis absorption spectroscopy, spectroscopic ellipsometry, XPS, XRD, UFM/AFM, admittance spectroscopy, and field-effect measurements. Data analysis reveals smooth (RRMS < 1 nm) amorphous films with a dielectric constant of about 3.8, an optical band gap of ≈8.1 eV, leakage current densities in the order of ≈10(-7) A/cm(2) at 1 MV/cm, and high dielectric strength in excess of 5 MV/cm. XPS measurements confirm the SiO2 stoichiometry and FTIR spectra reveal features related to SiO2 only. Thin film transistors implementing spray-coated SiO2 gate dielectrics and C60 and pentacene semiconducting channels exhibit excellent transport characteristics, i.e., negligible hysteresis, low leakage currents, high on/off current modulation ratio on the order of 10(6), and high carrier mobility.
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