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1.
Small ; 18(19): e2107881, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-35417059

RESUMEN

In contrast to the 2D organic-inorganic hybrid Ruddlesden-Popper halide perovskites (RPP), a new class of 2D all inorganic RPP (IRPP) has been recently proposed by substituting the organic spacers with an optimal inorganic alternative of cesium cations (Cs+ ). Nevertheless, the synthesis of high-membered 2D IRPPs (n > 1) has been a very challenging task because the Cs+ need to act as both spacers and A-site cations simultaneously. This work presents the successful synthesis of stable phase-pure high-membered 2D IRPPs of Csn+1 Pbn Br3n+1 nanosheets (NSs) with n = 3 and 4 by employing the strategy of using additional strong binding bidentate ligands. The structures of the 2D IRPPs (n = 3 and 4) NSs are confirmed by powder X-ray diffraction and high-resolution aberration-corrected scanning transmission electron microscope measurements. These 2D IRPPs NSs exhibit a strong quantum confinement effect with tunable absorption and emission in the visible light range by varying their n values, attributed to their inherent 2D quantum-well structure. The superior structural and optical stability of the phase-pure high-membered 2D IRPPs make them a promising candidate as photocatalysts in CO2 reduction reactions with outstanding photocatalytic performance and long-term stability.

2.
Nature ; 520(7547): 325-8, 2015 Apr 16.
Artículo en Inglés | MEDLINE | ID: mdl-25849777

RESUMEN

The development of new rechargeable battery systems could fuel various energy applications, from personal electronics to grid storage. Rechargeable aluminium-based batteries offer the possibilities of low cost and low flammability, together with three-electron-redox properties leading to high capacity. However, research efforts over the past 30 years have encountered numerous problems, such as cathode material disintegration, low cell discharge voltage (about 0.55 volts; ref. 5), capacitive behaviour without discharge voltage plateaus (1.1-0.2 volts or 1.8-0.8 volts) and insufficient cycle life (less than 100 cycles) with rapid capacity decay (by 26-85 per cent over 100 cycles). Here we present a rechargeable aluminium battery with high-rate capability that uses an aluminium metal anode and a three-dimensional graphitic-foam cathode. The battery operates through the electrochemical deposition and dissolution of aluminium at the anode, and intercalation/de-intercalation of chloroaluminate anions in the graphite, using a non-flammable ionic liquid electrolyte. The cell exhibits well-defined discharge voltage plateaus near 2 volts, a specific capacity of about 70 mA h g(-1) and a Coulombic efficiency of approximately 98 per cent. The cathode was found to enable fast anion diffusion and intercalation, affording charging times of around one minute with a current density of ~4,000 mA g(-1) (equivalent to ~3,000 W kg(-1)), and to withstand more than 7,500 cycles without capacity decay.

3.
Small ; 16(45): e2002885, 2020 11.
Artículo en Inglés | MEDLINE | ID: mdl-32945097

RESUMEN

High demand for green ecosystems has urged the human community to reconsider and revamp the traditional way of synthesis of several compounds. Ammonia (NH3 ) is one such compound whose applications have been extended from fertilizers to explosives and is still being synthesized using the high energy inhaling Haber-Bosch process. Carbon free electrocatalytic nitrogen reduction reaction (NRR) is considered as a potential replacement for the Haber-Bosch method. However, it has few limitations such as low N2 adsorption, selectivity (competitive HER reactions), low yield rate etc. Since it is at the early stage, tremendous efforts have been devoted in understanding the reaction mechanism and screening of the electrocatalysts and electrolytes. In this review, the electrocatalysts are classified based on the periodic table with heat maps of Faraday efficiency and yield rate of NH3 in NRR and their electrocatalytic properties toward NRR are discussed. Also, the activity of each element is discussed and short tables and concise graphs are provided to enable the researchers to understand recent progress on each element. At the end, a perspective is provided on countering the current challenges in NRR. This review may act as handbook for basic NRR understandings, recent progress in NRR, and the design and development of advanced electrocatalysts and systems.

4.
Phys Chem Chem Phys ; 22(43): 24842-24855, 2020 Nov 21.
Artículo en Inglés | MEDLINE | ID: mdl-33125020

RESUMEN

Global population explosion has led to the rapid revolution of science and technology, and the high energy demand has necessitated new and efficient energy conversion and storage systems. Lithium ion batteries (LIBs) have a high potential window, high capacity, and high stability, but suffer from high cost and low safety. Therefore, many alternative batteries, including sodium ion batteries (NIBs), potassium (KIBs), aluminum (AIBs), and dual ion batteries (DIBs), have been introduced. One of the key working principles of these batteries is based on cation or anion intercalation in the graphite layers, and leads to the formation of graphite intercalation compounds (GICs). Recently, studies based on determining a reaction mechanism to improve the performance of the batteries have been conducted. In this review, an overview of the work on the reaction mechanism of polyatomic ions intercalated into GICs, the structure of intercalated polyatomic ions, the structure of the accommodated GICs, and their staging is provided. In other words, this review focuses on unraveling and understanding the reaction mechanisms for the intercalation of polyatomic ions into GICs by in situ and ex situ techniques, correlated with computational studies. The current limitations and future prospects of polyatomic ions intercalation batteries are also discussed.

5.
Small ; 15(49): e1904723, 2019 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-31657122

RESUMEN

The generation of ammonia, hydrogen production, and nitrogen purification are considered as energy intensive processes accompanied with large amounts of CO2 emission. An electrochemical method assisted by photoenergy is widely utilized for the chemical energy conversion. In this work, earth-abundant iron pyrite (FeS2 ) nanocrystals grown on carbon fiber paper (FeS2 /CFP) are found to be an electrochemical and photoactive catalyst for nitrogen reduction reaction under ambient temperature and pressure. The electrochemical results reveal that FeS2 /CFP achieves a high Faradaic efficiency (FE) of ≈14.14% and NH3 yield rate of ≈0.096 µg min-1 at -0.6 V versus RHE electrode in 0.25 m LiClO4 . During the electrochemical catalytic reaction, the crystal structure of FeS2 /CFP remains in the cubic pyrite phase, as analyzed by in situ X-ray diffraction measurements. With near-infrared laser irradiation (808 nm), the NH3 yield rate of the FeS2 /CFP catalyst can be slightly improved to 0.1 µg min-1 with high FE of 14.57%. Furthermore, density functional theory calculations demonstrate that the N2 molecule has strong chemical adsorption energy on the iron atom of FeS2 . Overall, iron pyrite-based materials have proven to be a potential electrocatalyst with photoactive behavior for ammonia production in practical applications.

6.
Anal Bioanal Chem ; 411(13): 2793-2802, 2019 May.
Artículo en Inglés | MEDLINE | ID: mdl-30931506

RESUMEN

A powerful technique to detect bone biomarkers has been developed for assessment of osteoporosis at the early stage. Two-dimensional multilayered gold-nanoparticle thin film (MTF-AuNPs) was demonstrated as a promising test platform for detection of bone biomarker, hydroxyproline (HYP), measured by surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS). With strong surface plasmon resonance and excellent homogeneity, facilely prepared, highly ordered, and large-scale MTF-AuNPs revealed high sensitivity of HYP in the SALDI-MS measurement without additional matrixes, such as α-cyano-4-hydroxycinnamic acid (CHCA) and 2,5-dihydroxybenzoic acid (DHB). Furthermore, the mass spectrum of HYP with MTF-AuNPs was significantly improved in signal intensity enhancement, background noise reduction, and signal-to-noise ratio amplification. The excellent reproducibility of HYP spectra with only 9.3% relative signal variation could be attributed to MTF-AuNPs' high absorbance at a wavelength of 337 nm, low heat capacity, superior thermal conductivity, and outstanding homogeneity. The calibration curve showed high linear correlation between mass spectrum intensity and HYP concentration in the range of 1 to 100 µM, covering the whole level in healthy people and osteoporosis patients. In particular, the serum sample was directly deposited onto the MTF-AuNP sample substrate without any pretreatment and its HYP concentration was then successfully determined. We believe that the combination of SALDI-MS and MTF-AuNP sample substrates would be a potential approach for bone biomarker detection in the osteoporosis risk assessment. Graphical abstract.


Asunto(s)
Biomarcadores/sangre , Oro/química , Nanopartículas del Metal/química , Osteoporosis/sangre , Espectrometría de Masa por Láser de Matriz Asistida de Ionización Desorción/métodos , Biomarcadores/análisis , Humanos , Hidroxiprolina/sangre , Límite de Detección , Nanopartículas del Metal/ultraestructura , Osteoporosis/diagnóstico , Reproducibilidad de los Resultados , Medición de Riesgo
7.
Anal Chem ; 90(6): 3974-3980, 2018 03 20.
Artículo en Inglés | MEDLINE | ID: mdl-29466668

RESUMEN

The glucose metabolism rate in cancer cells is a crucial piece of information for the cancer aggressiveness. A feasible method to monitor processes of oncogenic mutations has been demonstrated in this work. The fluorescent gold nanoclusters conjugated with glucose (glucose-AuNCs) were successfully synthesized as a cancer-targeting probe for glucose transporters (Gluts) overexpressed by U-87 MG cancer cells, which can be observed under confocal microscopy. The structural and optical characterizations of fluorescent glucose-AuNCs were confirmed by transmission electron microscope (TEM) and Fourier transform infrared spectroscopy (FTIR). The MTT assay exhibited the high biocompatibility of water-soluble glucose-AuNCs for further biomedical applications. The glucose metabolic cleavage of glucose-AuNCs by glycolytic enzymes from U-87 MG cancer cell was measured by fluorescence change of glucose-AuNCs. The fluorescence change based on the integrated area under fluorescence spectra ( A t) of glucose-AuNCs was plotted as a function of different reaction time ( t) with glycolytic enzymes. The fitted curve of A t versus t showed the first-order kinetics to explain the mechanism of glucose metabolic cleavage rate of glucose-AuNCs by glycolytic enzymes. The rate constant k could be utilized to determine the glucose metabolism rate of glucose-AuNCs for the quantitative analysis of cancer aggressiveness. Our work provides a practical application of target-specific glucose-AuNCs as a fluorescence probe to analyze the glucose metabolism in Gluts overexpressed cancer cells.


Asunto(s)
Colorantes Fluorescentes/química , Proteínas Facilitadoras del Transporte de la Glucosa/metabolismo , Glucosa/metabolismo , Glucólisis , Oro/química , Nanopartículas del Metal/química , Neoplasias/metabolismo , Técnicas Biosensibles/métodos , Línea Celular Tumoral , Glucosa/química , Proteínas Facilitadoras del Transporte de la Glucosa/análisis , Humanos , Microscopía Confocal/métodos , Microscopía Fluorescente/métodos , Neoplasias/enzimología
8.
Small ; 13(8)2017 02.
Artículo en Inglés | MEDLINE | ID: mdl-27982540

RESUMEN

Hydrogen is considered as sustainable and environmentally friendly energy for global energy demands in the future. Here a Co-FeS2 catalyst with surface phosphide doping (P/Co-FeS2 ) for hydrogen evolution reaction (HER) in acidic solutions is developed. The P/Co-FeS2 exhibits superior HER electrochemical performance with overpotential of -90 mV at 100 mA cm-2 and Tafel slope of 41 mV/decade and excellent durability.

9.
J Am Chem Soc ; 137(4): 1587-92, 2015 Feb 04.
Artículo en Inglés | MEDLINE | ID: mdl-25588180

RESUMEN

Hydrogen evolution reaction (HER) from water through electrocatalysis using cost-effective materials to replace precious Pt catalysts holds great promise for clean energy technologies. In this work we developed a highly active and stable catalyst containing Co doped earth abundant iron pyrite FeS(2) nanosheets hybridized with carbon nanotubes (Fe(1-x)CoxS(2)/CNT hybrid catalysts) for HER in acidic solutions. The pyrite phase of Fe(1-x)CoxS(2)/CNT was characterized by powder X-ray diffraction and absorption spectroscopy. Electrochemical measurements showed a low overpotential of ∼0.12 V at 20 mA/cm(2), small Tafel slope of ∼46 mV/decade, and long-term durability over 40 h of HER operation using bulk quantities of Fe(0.9)Co(0.1)S(2)/CNT hybrid catalysts at high loadings (∼7 mg/cm(2)). Density functional theory calculation revealed that the origin of high catalytic activity stemmed from a large reduction of the kinetic energy barrier of H atom adsorption on FeS(2) surface upon Co doping in the iron pyrite structure. It is also found that the high HER catalytic activity of Fe(0.9)Co(0.1)S(2) hinges on the hybridization with CNTs to impart strong heteroatomic interactions between CNT and Fe(0.9)Co(0.1)S(2). This work produces the most active HER catalyst based on iron pyrite, suggesting a scalable, low cost, and highly efficient catalyst for hydrogen generation.

10.
Small ; 11(24): 2929-37, 2015 Jun 24.
Artículo en Inglés | MEDLINE | ID: mdl-25703342

RESUMEN

Energy scavenging has become a fundamental part of ubiquitous sensor networks. Of all the scavenging technologies, solar has the highest power density available. However, the energy source is erratic. Integrating energy conversion and storage devices is a viable route to obtain self-powered electronic systems which have long-term maintenance-free operation. In this work, we demonstrate an integrated-power-sheet, consisting of a string of series connected organic photovoltaic cells (OPCs) and graphene supercapacitors on a single substrate, using graphene as a common platform. This results in lighter and more flexible power packs. Graphene is used in different forms and qualities for different functions. Chemical vapor deposition grown high quality graphene is used as a transparent conductor, while solution exfoliated graphene pastes are used as supercapacitor electrodes. Solution-based coating techniques are used to deposit the separate components onto a single substrate, making the process compatible with roll-to-roll manufacture. Eight series connected OPCs based on poly(3-hexylthiophene)(P3HT):phenyl-C61-butyric acid methyl ester (PC60 BM) bulk-heterojunction cells with aluminum electrodes, resulting in a ≈5 V open-circuit voltage, provide the energy harvesting capability. Supercapacitors based on graphene ink with ≈2.5 mF cm(-2) capacitance provide the energy storage capability. The integrated-power-sheet with photovoltaic (PV) energy harvesting and storage functions had a mass of 0.35 g plus the substrate.

11.
Angew Chem Int Ed Engl ; 54(41): 11989-93, 2015 Oct 05.
Artículo en Inglés | MEDLINE | ID: mdl-26307213

RESUMEN

The rising H2 economy demands active and durable electrocatalysts based on low-cost, earth-abundant materials for water electrolysis/photolysis. Here we report nanoscale Ni metal cores over-coated by a Cr2 O3 -blended NiO layer synthesized on metallic foam substrates. The Ni@NiO/Cr2 O3 triphase material exhibits superior activity and stability similar to Pt for the hydrogen-evolution reaction in basic solutions. The chemically stable Cr2 O3 is crucial for preventing oxidation of the Ni core, maintaining abundant NiO/Ni interfaces as catalytically active sites in the heterostructure and thus imparting high stability to the hydrogen-evolution catalyst. The highly active and stable electrocatalyst enables an alkaline electrolyzer operating at 20 mA cm(-2) at a voltage lower than 1.5 V, lasting longer than 3 weeks without decay. The non-precious metal catalysts afford a high efficiency of about 15 % for light-driven water splitting using GaAs solar cells.

12.
ACS Appl Mater Interfaces ; 15(1): 1748-1761, 2023 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-36576167

RESUMEN

Electroluminescence (EL) from the singlet-excited (S1) state is the ideal choice for stable, high-performing deep-blue organic light-emitting diodes (OLEDs) owing to the advantages of an adequately short radiative lifetime, improved device durability, and low cost, which are the most important criteria for their commercialization. Herein, we present the design and synthesis of three donor-acceptor-donor (D-A-D)-configured deep-blue fluorescent materials (denoted as TC-1, TC-2, and TC-3) composed of a thioxanthone or diphenyl sulfonyl acceptor and phenyl carbazolyl donor. These systems exhibit strong deep-blue photoluminescence (422-432 nm) in solutions and redshifted emission (472-486 nm) in thin films. The solid-state photoluminescence quantum yield (PLQY) was estimated to be 78 and 94% for TC-2 and TC-3, respectively. TC-2 and TC-3 possess good molecular packing and large molecular cross-sectional areas, which not only improves the PLQY but enhances the triplet-triplet annihilation up-conversion (TTAUC) efficiency of fluorescent emitters. Furthermore, both compounds were applied as an acceptor for confirming their TTAUC property using bis(2-methyldibenzo[f,h]quinoxaline)(acetylacetonate)iridium(III) (Ir(MDQ)2acac) as the sensitizer. Non-doped OLEDs based on TC-2 and TC-3 exhibit blue EL in the 461-476 nm range. In particular, TC-3 exhibits a maximum external quantum efficiency (EQEmax) of 5.1%, and its EL maximum is 476 nm. In addition, the three emitters were employed as hosts in red OLEDs using bis(1-phenylisoquinoline)(acetylacetonate)iridium(III) (Ir(piq)2acac) as the phosphorescent dopant. The red phosphorescent OLEDs based on TC-1, TC-2, and TC-3 achieve excellent EQEmax values of 21.6, 22.9, and 21.9%, respectively, and peak luminance efficiencies of 12.0, 14.0, and 12.3 cd A-1. These results highlight these fluorophores' versatility and promising prospects in practical OLED applications.

13.
ACS Nano ; 17(5): 4261-4278, 2023 03 14.
Artículo en Inglés | MEDLINE | ID: mdl-36706095

RESUMEN

Triple-negative breast cancer (TNBC) is considered more aggressive with a poorer prognosis than other breast cancer subtypes. Through systemic bioinformatic analyses, we established the ferroptosis potential index (FPI) based on the expression profile of ferroptosis regulatory genes and found that TNBC has a higher FPI than non-TNBC in human BC cell lines and tumor tissues. To exploit this finding for potential patient stratification, we developed biologically amenable phototheranostic iron pyrite FeS2 nanocrystals (NCs) that efficiently harness near-infrared (NIR) light, as in photovoltaics, for multispectral optoacoustic tomography (MSOT) and photothermal ablation with a high photothermal conversion efficiency (PCE) of 63.1%. Upon NIR irradiation that thermodynamically enhances Fenton reactions, dual death pathways of apoptosis and ferroptosis are simultaneously triggered in TNBC cells, comprehensively limiting primary and metastatic TNBC by regulating p53, FoxO, and HIF-1 signaling pathways and attenuating a series of metabolic processes, including glutathione and amino acids. As a unitary phototheranostic agent with a safe toxicological profile, the nanocrystal represents an effective way to circumvent the lack of therapeutic targets and the propensity of multisite metastatic progression in TNBC in a streamlined workflow of cancer management with an integrated image-guided intervention.


Asunto(s)
Nanopartículas , Fármacos Fotosensibilizantes , Terapia Fototérmica , Neoplasias de la Mama Triple Negativas , Humanos , Muerte Celular , Línea Celular Tumoral , Hierro/administración & dosificación , Hierro/uso terapéutico , Nanopartículas/administración & dosificación , Nanopartículas/uso terapéutico , Neoplasias de la Mama Triple Negativas/tratamiento farmacológico , Neoplasias de la Mama Triple Negativas/genética , Neoplasias de la Mama Triple Negativas/radioterapia , Femenino , Rayos Infrarrojos/uso terapéutico , Terapia Fototérmica/métodos , Sulfuros/administración & dosificación , Sulfuros/uso terapéutico , Fármacos Fotosensibilizantes/administración & dosificación , Fármacos Fotosensibilizantes/uso terapéutico , Apoptosis/efectos de los fármacos , Apoptosis/efectos de la radiación , Ferroptosis/efectos de los fármacos , Ferroptosis/efectos de la radiación
14.
J Am Chem Soc ; 134(24): 10011-20, 2012 Jun 20.
Artículo en Inglés | MEDLINE | ID: mdl-22646012

RESUMEN

The finding of new metal alloyed nanocrystals (NCs) with high catalytic activity and low cost to replace PtRu NCs is a critical step toward the commercialization of fuel cells. In this work, a simple cation replacement reaction was utilized to synthesize a new type of ternary Fe(1-x)PtRu(x) NCs from binary FePt NCs. The detailed structural transformation from binary FePt NCs to ternary Fe(1-x)PtRu(x) NCs was analyzed by X-ray absorption spectroscopy (XAS). Ternary Fe(35)Pt(40)Ru(25), Fe(31)Pt(40)Ru(29), and Fe(17)Pt(40)Ru(43) NCs exhibit superior catalytic ability to withstand CO poisoning in methanol oxidation reaction (MOR) than do binary NCs (FePt and J-M PtRu). Also, the Fe(31)Pt(40)Ru(29) NCs had the highest alloying extent and the lowest onset potential among the ternary NCs. Furthermore, the origin for the superior CO resistance of ternary Fe(1-x)PtRu(x) NCs was investigated by determining the adsorption energy of CO on the NCs' surfaces and the charge transfer from Fe/Ru to Pt using a simulation based on density functional theory. The simulation results suggested that by introducing a new metal into binary PtRu/PtFe NCs, the anti-CO poisoning ability of ternary Fe(1-x)PtRu(x) NCs was greatly enhanced because the bonding of CO-Pt on the NCs' surface was weakened. Overall, our experimental and simulation results have indicated a simple route for the discovery of new metal alloyed catalysts with superior anti-CO poisoning ability and low usage of Pt and Ru for fuel cell applications.

15.
Nanomaterials (Basel) ; 12(11)2022 May 26.
Artículo en Inglés | MEDLINE | ID: mdl-35683671

RESUMEN

Various types of 2D organic-inorganic perovskite solar cells have been developed and investigated due to better electron transport behavior and environmental stability. Controlling the formation of phases in the 2D perovskite films has been considered to play an important role in influencing the stability of perovskite materials and their performance in optoelectronic applications. In this work, Lewis base urea was used as an effective additive for the formation of 2D Ruddlesden-Popper (RP) perovskite (BA)2(MA)n-1PbnI3n+1 thin film with mixed phases (n = 2~4). The detailed structural morphology of the 2D perovskite thin film was investigated by in situ X-ray diffraction (XRD), grazing-incidence small-angle X-ray scattering (GISAXS) and photoluminescence mapping. The results indicated that the urea additive could facilitate the formation of 2D RP perovskite thin film with larger grain size and high crystallinity. The 2D RP perovskite thin films for solar cells exhibited a power conversion efficiency (PCE) of 7.9% under AM 1.5G illumination at 100 mW/cm2.

16.
Mater Horiz ; 9(9): 2433-2442, 2022 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-35848594

RESUMEN

Two-dimensional (2D) all-inorganic Ruddlesden-Popper (RP) perovskite Cs7Pb6I19 nanosheets (NSs) were successfully developed for the first time by employing a structural recrystallization process with additional passivation of small organic sulfide molecules. The structure of Cs7Pb6I19 NSs is confirmed by powder X-ray diffraction measurements, atomically-resolved STEM measurements and atomic force microscopy (AFM) studies. Cs7Pb6I19 NSs with a specific n value of 6 exhibits unique absorption and emission spectra with intense excitons at 560 nm due to quantum confinement effects in 2D perovskite slabs. The formation mechanisms of 2D Cs7Pb6I19 NSs and 3D γ-CsPbI3 phases were investigated by in situ photoluminescence (PL) spectroscopy and the activation energies of their formation reactions were calculated to be 151 kJ mol-1 and 95.3 kJ mol-1, respectively. The phase stability of 2D Cs7Pb6I19 NSs can be maintained at temperatures below 14 °C for more than 4 weeks. The overall results indicate that 2D Cs7Pb6I19 NSs demonstrate unique optical properties and structural stability compared with other 3D perovskite materials. We have opened a new path to the future discovery of 2D perovskite structures with metastable phases by using this recrystallization method and the assistance of sulfur-derived organic molecules.

17.
ACS Appl Mater Interfaces ; 13(8): 10279-10286, 2021 Mar 03.
Artículo en Inglés | MEDLINE | ID: mdl-33599486

RESUMEN

This work demonstrates the strong excitonic magneto-optic (MO) effects of magnetic circular dichroism (MCD) and Faraday rotation (FR) in nonmagnetic two-dimensional (2D) organic-inorganic hybrid Ruddlesden-Popper perovskites (RPPs) at room temperature. Due to their strong and sharp excitonic absorption as a result of unique quantum well structures of 2D RPPs, sizeable linear excitonic MO effects of MCD and FR can be observed at room temperature under a low magnetic field (<1 T) compared with their three-dimensional counterpart. In addition, since the band gaps of 2D organic-inorganic hybrid perovskites can be manipulated either by changing the number n of inorganic octahedral slabs per unit cell or through halide engineering, linear excitonic MO effects of 2D-RPPs can be observed through the broadband spectral ranges of visible light. Our result may pave the way for the promising research field of MO and magneto-optoelectronic applications based on 2D organic-inorganic hybrid perovskites with facile solution processes.

18.
J Phys Chem Lett ; 12(33): 8121-8128, 2021 Aug 26.
Artículo en Inglés | MEDLINE | ID: mdl-34410136

RESUMEN

Nitrate (NO3-) reduction reaction (NtRR) is considered as a green alternative method for the conventional method of NH3 synthesis (Haber-Bosch process), which is known as a high energy consuming and large CO2 emitting process. Herein, the copper nanodendrites (Cu NDs) grown along with the {200} facet as an efficient NtRR catalyst have been successfully fabricated and investigated. It exhibited high Faradaic efficiency of 97% at low potential (-0.3 V vs RHE). Furthermore, the 15NO3- isotope labeling method was utilized to confirm the formation of NH3. Both experimental and theoretical studies showed that NtRR on the Cu metal nanostructure is a facet dependent process. Dissociation of NO bonding is supposed to be the rate-determining step as NtRR is a spontaneously reductive and protonation process for all the different facets of Cu. Density functional theory (DFT) calculations revealed that Cu{200} and Cu{220} offer lower activation energy for dissociation of NO compared to that of Cu{111}.

19.
J Phys Chem Lett ; 12(36): 8763-8769, 2021 Sep 16.
Artículo en Inglés | MEDLINE | ID: mdl-34491065

RESUMEN

Metal halide perovskites have attracted great attention for their superior light energy conversion applications. Herein, we demonstrated a facile synthesis of zero-dimensional Sn2+ perovskite Cs4-xMxSnBr6(M = K+ and Rb+) material through the cation transformation reaction at room temperature. Cs4SnBr6 NCs was mixed with pure metal bromide salts (KBr and RbBr) via the mechanochemical process to successfully synthesize Cs4-xMxSnBr6 perovskite where transformation of Cs to mixed Cs/Rb and mixed Cs/K was achieved. By substituting different cations, the bright fluorescence of the Cs4-xMxSnBr6 was tuned from dim green to greenish-cyan while achieving the photoluminescence (PL) quantum yield of ∼39%. The crystal structure of Sn based perovskite with the substitution of K+ or Rb+ cations was determined by X-ray diffraction (XRD). Moreover, the Cs4-xMxSnBr6 demonstrated superior air stability and exhibited a better photocatalytic activity for CO2 reduction reaction (CO2RR) with high selectivity of CH4 gas with a higher yield rate compared to the pristine Cs4SnBr6 NCs.

20.
Nanomaterials (Basel) ; 10(4)2020 Mar 30.
Artículo en Inglés | MEDLINE | ID: mdl-32235565

RESUMEN

An outbreak of a bacterial contagion is a critical threat for human health worldwide. Recently, light-activated heterostructured nanomaterials (LAHNs) have shown potential as antibacterial agents, owing to their unique structural and optical properties. Many investigations have revealed that heterostructured nanomaterials are potential antibacterial agents under light irradiation. In this review, we summarize recent developments of light-activated antibacterial agents using heterostructured nanomaterials and specifically categorized those agents based on their various light harvesters. The detailed antibacterial mechanisms are also addressed. With the achievements of LAHNs as antibacterial agents, we further discuss the challenges and opportunities for their future clinical applications.

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