Ammonium Molecules Research Articles

Oral Bioavailability of Deuterated L‐carnitine in Healthy Volunteers

BACKGROUND Deuterium, the stable isotope of hydrogen was discovered in 1931. Since then the use of deuterated molecules have allowed several advancements in the field of chemical biology. For example: in elucidating mechanisms of reactions, tracking metabolic products, and more recently, the enhancement of pharmacokinetic parameters in already existing drugs. L-carnitine is an amino acid derivative, quaternary ammonium molecule with hygroscopic properties that displays an essential role in the fatty acid metabolism in mammals. L-carnitine is an example of a molecule that is both endogenously synthetized and exogenously administered in the forms of dietary products, supplements, and medicine. This poses a challenge differentiating the source of L-carnitine measured in plasma. OBJECTIVES Our study, aims to use deuterated molecules in pharmacokinetics, for distinguishing endogenous synthesized molecules from exogenously administered ones, like L-carnitine. We have developed a method based on deuteration and posterior detection of L- carnitine using high performance liquid chromatography coupled to tandem mass spectrometry (HPLC-MS/MS). METHODS The study was conducted over an open, four period with a 1-week washout interval and six healthy subjects were recruited. Capsules containing 500 mg of L-carnitine which contained different doses of deuterated (D3) L-carnitine (10,30,100 and 100mg of D3 L-carnitine and 490,470 and 400mg of L-carnitine) in each period were administered to each participant. Plasma L-carnitine D3 concentrations were analysed by liquid chromatography coupled to tandem mass spectrometry (HPLC-MS/MS) with multiple reactions monitoring (MRM). The method linearity ranged from 10 to 1000 ng/mL. RESULTS The following pharmacokinetic parameters were obtained from the L-carnitine D3 plasma concentration vs. time curves: AUClast (72.16, 613.48, 2450.29ng*h/mL [mean]), Cmax (19.25, 75.59, 216.79 ng/mL[mean]) and Tmax (3.5, 3.5, 3.5 h [median]) for 10 mg, 30 mg and 100 mg, respectively. The coefficient of variation for rate and extent of absorption were 55.37% and 65.10% (ratio 3/4 period; 100 mg), respectively. Linearity between the pharmacokinetic parameters was demonstrated by Pearson Correlation. The plasma concentrations showed correlation with dose (10, 30 and 100 mg). CONCLUSION This shows that deuterated L-carnitine displays a high variability coefficient and demonstrates linearity among doses of 10, 30 and 100 mg. These results are consistent with previous literature. The method presented here adds to the existing consensus that deuteration is valuable in studying the pharmacokinetics of endogenously synthesized substances.

Tunable Superhydrophobic Aluminum Surfaces with Anti-Biofouling and Antibacterial Properties

Surfaces in a hygiene critical environment can become potential reservoirs for transmission of pathogenic infections. Engineering surfaces with the tunable anti-biofouling and antibacterial properties could reduce infections particularly in hospitals and public transport hubs. In the present work, a facile two-step process has been deployed to fabricate a superhydrophobic and antibacterial aluminum surface by chemical etching, followed by passivation with low surface energy octyltriethoxysilane (OTES) molecules. The wettability and antibacterial properties of the OTES passivated aluminum was monotonically tuned by adding quaternary ammonium (QUATs) molecules. An anti-biofouling property of 99.9% against Staphylococcus aureus, 99% against Pseudomonas aeruginosa and 99% against E. coli bacteria, was achieved.

Imprinting Ferromagnetism and Superconductivity in Single Atomic Layers of Molecular Superlattices

Ferromagnetism and superconductivity are two antagonistic phenomena since ferromagnetic exchange fields tend to destroy singlet Cooper pairs. Reconciliation of these two competing phases has been achieved in vertically stacked heterostructures where these two orders are confined in different layers. However, controllable integration of these two phases in one atomic layer is a longstanding challenge. Here, an interlayer-space-confined chemical design (ICCD) is reported for the synthesis of dilute single-atom-doped TaS2 molecular superlattice, whereby ferromagnetism is observed in the superconducting TaS2 layers. The intercalation of 2H-TaS2 crystal with bulky organic ammonium molecule expands its van der Waals gap for single-atom doping via co-intercalated cobalt ions, resulting in the formation of quasi-monolayer Co-doped TaS2 superlattices. Isolated Co atoms are decorated in the basal plane of the TaS2 via substituting the Ta atom or anchoring at a hollow site, wherein the orbital-selected p-d hybridization between Co and neighboring Ta and S atoms induces local magnetic moments with strong ferromagnetic coupling. This ICCD approach can be applied to various metal ions, enabling the synthesis of a series of crystal-size TaS2 molecular superlattices.

Small Pore Aluminosilicate EMM-37: Synthesis and Structure Determination Using Continuous Rotation Electron Diffraction.

A new aluminosilicate zeolite, denoted EMM-37, with a 3D small pore channel system, has been synthesized using a diquaternary ammonium molecule as the structure directing agent (SDA) and metakaolin as the aluminum source. The structures of both as-made and calcined forms of EMM-37 were solved and refined using continuous rotation electron diffraction (cRED) data. cRED is a powerful method for the collection of 3D electron diffraction data from submicron- and nanosized crystals, which allows for successful solution and refinement of complex structures in symmetry as low as P1̅.

Solution-processable 2D semiconductors for high-performance large-area electronics

Two-dimensional (2D) materials, consisting of atomically thin crystal layers bound by the van der Waals force, have attracted much interest because of their potential in diverse technologies, including electronics, optoelectronics and catalysis1-10. In particular, solution-processable 2D semiconductor (such as MoS2) nanosheets are attractive building blocks for large-area thin-film electronics. In contrast to conventional zero- and one-dimensional nanostructures (quantum dots and nanowires, respectively), which are typically plagued by surface dangling bonds and associated trapping states, 2D nanosheets have dangling-bond-free surfaces. Thin films created by stacking multiple nanosheets have atomically clean van der Waals interfaces and thus promise excellent charge transport11-15. However, preparing high-quality solution-processable 2D semiconductor nanosheets remains a challenge. For example, MoS2 nanosheets and thin films produced using lithium intercalation and exfoliation are plagued by the presence of the metallic 1T phase and poor electrical performance (mobilities of about 0.3 square centimetres per volt per second and on/off ratios of less than 10)2,12, and materials produced by liquid exfoliation exhibit an intrinsically broad thickness distribution, which leads to poor film quality and unsatisfactory thin-film electrical performance (mobilities of about 0.4 square centimetres per volt per second and on/off ratios of about 100)14,16,17. Here we report a general approach to preparing highly uniform, solution-processable, phase-pure semiconducting nanosheets, which involves the electrochemical intercalation of quaternary ammonium molecules (such as tetraheptylammonium bromide) into 2D crystals, followed by a mild sonication and exfoliation process. By precisely controlling the intercalation chemistry, we obtained phase-pure, semiconducting 2H-MoS2 nanosheets with a narrow thickness distribution. These nanosheets were then further processed into high-performance thin-film transistors, with room-temperature mobilities of about 10 square centimetres per volt per second and on/off ratios of 106 that greatly exceed those obtained for previous solution-processed MoS2 thin-film transistors. The scalable fabrication of large-area arrays of thin-film transistors enabled the construction of functional logic gates and computational circuits, including an inverter, NAND, NOR, AND and XOR gates, and a logic half-adder. We also applied our approach to other 2D materials, including WSe2, Bi2Se3, NbSe2, In2Se3, Sb2Te3 and black phosphorus, demonstrating its potential for generating versatile solution-processable 2D materials.

Naphthalene Diimide Ammonium Directed Single-Crystalline Perovskites with “Atypical” Ambipolar Charge Transport Signatures in Two-Dimensional Limit

A single crystal of a lead–iodine-based 2D perovskite having naphthalene diimide ammonium (NDIA) molecules as organic layers was developed, and the charge transport property was studied using field-effect transistors (FETs) measurements. Structure determination reveals the layered alternative stacking of lead iodide sheets and NDIA bilayers. The presence of NDIA promoted the lead iodide octahedron to form the unique three-point co-planar [Pb3I10]4– unit, which then connected into the 2D network in a corner-sharing manner. The NDIA cations closely stacked into 1D chains within the bilayers that were being sandwiched between the inorganic layers. FET characteristics of the single crystal obtained at room temperature demonstrate VDS-dependent electron and hole transport behavior with mobilities reaching up to more than 5 × 10–3 cm2 V–1 s–1. The 1D stack of NDIAs contributes greatly to the performance improvement for both the charge transport and the stability.

Structure of natural and NH4-exchanged Sasbach faujasite: a single-crystal study

The interest for the environmental, industrial and technological applications of Si-rich zeolites is very high. Among the large-pore zeolites, faujasite is one of the most exploited. The aim of this paper is to obtain detailed structural information on natural and NH4 -exchanged faujasite before using this zeolite for dealumination tests, targeting the realization of large single crystals of allsilica faujasite. As one of the most Si-rich natural samples, faujasite from Sasbach (Na13.64 K0.87 Mg10.46 Ca8.89 Sr0.34 (Al51.95 Si139.57 ) O384 ·272.29 H2 O; space group Fd-3 m; a = 24.6906(2) A) was chosen for study. Single-crystal X-ray diffraction structural refinements of both natural and NH4 -exchanged samples are reported and discussed. In the natural faujasite sample, almost all the extraframework species could be located for the first time. In the NH4 -exchanged sample the ammonium and water molecule sites were located. Ammonium cations occupy two of the sites occupied by the extraframework species in the original mineral.

Monolayer atomic crystal molecular superlattices.

Artificial superlattices, based on van der Waals heterostructures of two-dimensional atomic crystals such as graphene or molybdenum disulfide, offer technological opportunities beyond the reach of existing materials. Typical strategies for creating such artificial superlattices rely on arduous layer-by-layer exfoliation and restacking, with limited yield and reproducibility. The bottom-up approach of using chemical-vapour deposition produces high-quality heterostructures but becomes increasingly difficult for high-order superlattices. The intercalation of selected two-dimensional atomic crystals with alkali metal ions offers an alternative way to superlattice structures, but these usually have poor stability and seriously altered electronic properties. Here we report an electrochemical molecular intercalation approach to a new class of stable superlattices in which monolayer atomic crystals alternate with molecular layers. Using black phosphorus as a model system, we show that intercalation with cetyl-trimethylammonium bromide produces monolayer phosphorene molecular superlattices in which the interlayer distance is more than double that in black phosphorus, effectively isolating the phosphorene monolayers. Electrical transport studies of transistors fabricated from the monolayer phosphorene molecular superlattice show an on/off current ratio exceeding 107, along with excellent mobility and superior stability. We further show that several different two-dimensional atomic crystals, such as molybdenum disulfide and tungsten diselenide, can be intercalated with quaternary ammonium molecules of varying sizes and symmetries to produce a broad class of superlattices with tailored molecular structures, interlayer distances, phase compositions, electronic and optical properties. These studies define a versatile material platform for fundamental studies and potential technological applications.

Lead bromide-based layered perovskite Langmuir–Blodgett films having π-conjugated molecules as organic layer prepared by using squeezed out technique

Using the squeezed out technique, we successfully prepared PbBr-based layered perovskite Langmuir–Blodgett (LB) films, which have π-conjugated materials as an organic layer (i.e., a phenylenevinylene oligomer, a dithienylethene derivative, and a π-conjugated polyfluorene derivative). The mixed monolayers of π-conjugated materials and octadecylammonium bromide were spread on an aqueous subphase containing saturated PbBr2. During pressing, octadecylammonium molecules were squeezed from the mixed monolayer, and the squeezed ammonium molecules formed the PbBr-based layered perovskite structure at the air-aqueous subphase interface. The monolayers with the PbBr-based layered perovskite structure could be deposited on fused quartz substrates by the LB technique. In addition to the preparation procedure, the structural and optical properties of the layered perovskite LB films and their formation mechanism are reported in this paper.

UV-Curable Contact Active Benzophenone Terminated Quaternary Ammonium Antimicrobials for Applications in Polymer Plastics and Related Devices.

A series of UV active benzophenone ([C6H5COC6H4-O-(CH2)n-N+Me2R][X-]; 4, R = C12H25, n = 3, X- = Br-; 5a-c, R = C18H37, n = 3, X- = Cl-, Br-, I-; 6a-c, R = C18H37, n = 4, X- = Cl-, Br-, I-; 7a-c, R = C18H37, n = 6, X- = Cl-, Br-, I-) terminated C12 and C18 quaternary ammonium salts (QACs) were prepared by thermal or microwave-driven Menshutkin protocols of the appropriate benzophenone alkyl halide (1a-c, 2a-c, 3a-c) with the corresponding dodecyl- or octadecyl N,N-dimethylamine. All new compounds were characterized by NMR spectroscopy, HRMS spectrometry, and, in one instance (4), by single-crystal X-ray crystallography. Representative C12 and C18 benzophenone QACs were formulated into 1% (w/v) water or water/ethanol-based aerosol spray coatings and then UV-cured onto plastic substrates (polypropylene, polyethylene, polystyrene, polyvinyl chloride, and polyether ether ketone) with exposure to low to moderate doses of UV (20-30 J cm-2). Confirmation as to the presence of the coatings was detected by advancing water contact angle measurements, which revealed a more hydrophilic surface after coating. Further confirmation was gained by X-ray photoelectron spectroscopy analysis, time of flight secondary ion mass spectrometry, and bromophenol blue staining, all of which showed the presence of the attached quaternary ammonium molecule. Analysis of surfaces treated with the C18 benzophenone 5b by atomic force microscopy and surface profilometry revealed a coating thickness of ∼350 nm. The treated samples along with controls were then evaluated for their antimicrobial efficacy against Gram-positive (Arthrobacter sp., Listeria monocytogenes) and Gram-negative (Pseudomonas aeruginosa) bacteria at a solid/air interface using the large drop inoculum protocol; this technique gave no evidence for cell adhesion after a 3 h time frame. These antimicrobial materials show promise for their use as coatings on plastic biomedical devices with the aim of preventing biofilm formation and preventing the spread of hospital acquired infections.

Application of Victorian brown coal for removal of ammonium and organics from wastewater

ABSTRACTBrown coal is a relatively abundant and low-cost material, which has been used as an effective ion-exchanger to remove ammonium from wastewater. In this study, the influences of pH, ammonium concentration and brown coal dose were investigated for removal of ammonium content from synthetic wastewater. Raw brown coal (RBC) treated with base solution has superior ammonium removal efficiency compared to RBC, which was due to chemical alterations and thus greater attachment of ammonium molecules to base-washed brown coal (BWBC), confirmed by Fourier transform infra-red spectroscopy. Scanning electron microscopy-electron diffraction scattering has identified the augmented sodium content in BWBC, which was subsequently replaced with nitrogen upon wastewater treatment. Crystallographic analysis showed a higher crystallinity formed in BWBC compared to RBC, which was likely due to formation of sodium salt crystals during NaOH treatment. Fitting batch experimental results to adsorption kinetic models suggested that the removal of ammonium was mainly governed by the reaction process rather than the physical diffusion mechanism. Both kinetic and isotherm studies confirmed higher adsorption capacity for BWBC compared to RBC. RBC in column mode was also experimented with to show organics removal from a secondary effluent. A comparatively lower removal of organics was obtained due to inability of charge neutralization as both brown coal and organics are positively charged.

Effects of surface modification of halloysite nanotubes on the morphology and the thermal and rheological properties of polypropylene/halloysite composites

Abstract Effects of unmodified halloysite nanotubes (HNTs) and hexadecyl trimethyl ammonnium bromide treated halloysite nanotubes (CTAB-HNTs) on the morphology as well as the thermal and rheological properties of the HNT-filled polypropylene (PP) composites were investigated. The composites were melt-blended with a novel vane mixer dominated by extensional deformation. Fourier transform infrared spectroscopy well demonstrated that ammonium molecules were successfully interacted with halloysite groups. Compared with unmodified HNTs, the modified HNTs had a better dispersion in the PP matrix. The degree of crystallinity increased with the introduction of HNTs into the PP matrix. Thermal analyses revealed that CTAB-HNTs can improve the composites’ thermal stability compared with unmodified HNTs. As for dynamic shear rheology, the PP/CTAB-HNT composites showed higher viscoelaticity than neat PP in most frequency regimes, and that the raw HNT/PP composites presented the opposite phenomenon. The relaxation time of PP melt and the availability of heterogeneous PP domains increased with the presence of CTAB-HNTs.

Waterborne polyurethane molecular structure designed and its acetic acid and ammonia absorption efficiency

In this study, waterborne polyurethane (WPU) resins consisted of carboxylic acid and side-chained EO (ethylene oxide) functional groups were prepared via a prepolymer ion-hybrid reaction process. After dipping the WPU on fabrics, the dipped fabrics showed promising deodorization properties for both basic and acidic odors and also showed good wash durability because of the presence of those characteristic groups. Basic odors were neutralized via carboxylic acid groups on the WPU, whereas acidic odors were absorbed by the EO groups through hydrogen bonding. Fourier transform infrared spectroscopy (FT-IR) was used to examine the functional groups of carboxylic acid and EO groups, before and after dipping the WPU on the fabrics. The deodorization properties of the dipped fabrics were associated with the content of the functional groups existing on the WPU molecular chain. Scanning electron microscope (SEM) analysis also revealed that the dipped fabrics had a promising wash durability and deodorization properties after 5 times of laundering because WPU particles were still strongly adhered to the fabrics. More side-chain EO groups, more acetic acid molecules were absorbed; while more-COOH groups in polymer chain, more ammonium molecules were absorbed. Table 2 shows that the synthesized WPU’s possess very highly washed durability.

The ammonium ion in a silicate under compression: infrared spectroscopy and powder X-ray diffraction of NH4AlSi3O8—buddingtonite to 30 GPa

The behavior of the ammoniated feldspar buddingtonite, NH4AlSi3O8, has been studied using infrared (IR) spectroscopy up to ~30 GPa and using synchrotron powder X-ray diffraction to 10 GPa at room temperature. We examine the bonding of the ammonium ion under pressure and in particular whether hydrogen bonding is enhanced by compaction, as well as probe how the ammonium ion affects the elasticity and behavior of the aluminosilicate framework at pressure. Powder diffraction data yield a bulk modulus of 49 GPa for a pressure derivative of 4, implying that the ammonium ion substitution may induce a modest softening of the feldspar lattice relative to the potassium ion. Under compression, the N–H vibrations are remarkably insensitive to pressure throughout the pressure range of these experiments. However, the vibrations of the aluminosilicate framework of buddingtonite undergo changes in their slope at ~13 GPa, implying that a change in compressional mechanism occurs near this pressure, but the vibrational modes of the ammonium molecule show little response to this change. These results show that (1) there is little, if any, enhancement of hydrogen bonding between the ammonium ion and the oxygen ions of the silica and aluminum tetrahedral framework under pressure, as manifested by the slight (and mostly positive) shifts in the N–H stretching vibrations of the ammonium ion; (2) ordering of the ammonium ion is not observed under compression, as no changes in peak width or in the general appearance of the spectra are observed under compression; and (3) structural changes induced by pressure in the aluminosilicate framework do not produce significant changes in the bonding of the ammonium ion. Hence, it appears that the ammonium ion interacts minimally with its surrounding lattice, even at high pressures: Its behavior is compatible with it being, aside from Coulombic attraction to the oxygen-dominated matrix, a largely non-interactive guest molecule within the silicate framework. This lack of interaction with the surrounding oxide lattice under compression may impact the stability of ammoniated minerals at high pressures and temperatures and ultimately likely favors nitrides or fluid phases as the dominant nitrogen carriers within the deeper mantle.

Enhancement of Exciton Emission in Lead Halide-Based Layered Perovskites by Cation Mixing.

Spin-coated films of a lead halide, PbX: X = I and Br, layered perovskites having cyclohexenylethyl ammonium molecule as an organic layer, which were mixed with other metal halide-based layered perovskites consisting of various divalent metal halides (for example, Ca2, Cdl2, FeI2, SnBr2 and so on), were prepared. The results of X-ray diffraction measurements exhibited that solid solution formation between PbX-based layered perovskite and other divalent metal halide-based layered perovskites was observed up to very high molar concentration of 50 molar% in the mixed film samples when divalent cations having ionic radius close to that of Pb2+ were employed. In the solid solution films, the exciton emission was much enhanced at room temperature. Exciton emission intensity of Pbl-based layered perovskite mixed with Cal-based layered perovskite (20 molar%) is about 5 times large that of the pristine Pbl-based layered perovskite, and that of PbBr-based layered perovskite mixed with SnBr-based layered perovskite (20 molar%) was also about 5 times large that of the pristine PbBr-based layered perovskite at room temperature.

PbBr-Based Layered Perovskite Organic-Inorganic Superlattice Having Carbazole Chromophore; Hole-Mobility and Quantum Mechanical Calculation.

We have successfully evaluated hole mobility in a spin-coated film of a lead-bromide based layered perovskite having carbazole chromophore-linked ammonium molecules as organic layer by using FET measurement. The values of hole mobility, threshold voltage and on/off ratio at room temperature were evaluated.to.be 1.7 x 10(-6) cm2 V-1 s-1, 27 V and 28 V, respectively. However, the spin-coated films on Si substrates were not so uniform compared with those on fused quartz substrates. To improve the film uniformity, we examined the relationship between substrate temperature during spin-coating and film morphology in the layered perovskite spin-coated films. The mean roughness of the spin-coated films on Si substrates was dependent on the substrate temperature. At 353 K, the mean roughness was minimized and the carrier mobility was enhanced by one order of magnitude; the values of hole mobility and threshold voltage were .estimated to be 3.4 x 10(-5) cm2 V-1 s-1, and 22 V at room temperature in a preliminary FET evaluation, respectively. In addition, we determined a crystal structure of the layered perovskite by X-ray diffraction analysis. To gain a better understanding of the observed hole transports, we conducted quantum mechanical calculations using the obtained crystal structure information. The calculated band structure of the layered organic perovskite showed that the valence band is composed of the organic carbazole layer, which confirms that.the measured hole mobility is mainly derived from the organic part of the layered perovskite. Band and hopping transport mechanisms were discussed by calculating the effective masses and transfer integrals for the 2D periodic system of the organic layer in isolation.

New phase of ammonium nitrate: A monoclinic distortion of AN-IV.

A new phase of ammonium nitrate (AN) is found using first principles evolutionary crystal structure search. It is this polymorph that is associated with the phase transition to previously unidentified phase, which was detected in experiment at 17 GPa upon appearance of the two extra peaks in Raman spectrum. The new phase has a monoclinic unit cell in the P21/m space group symmetry (AN-P21/m) and is similar to the known phase IV of AN (AN-IV) except the ammonium molecules are oriented differently relative to the nitrate molecules. The calculated free energy of AN-P21/m is found to be lower than AN-IV at pressures above 10.83 GPa. The equation of state of both AN-P21/m and AN-IV phases (volume vs hydrostatic pressure at room temperature) has been obtained within the quasi-harmonic approximation. The calculated Raman spectrum of both AN-P21/m and AN-IV as a function of pressure is in a good agreement with experiment. The energetic competitiveness of AN-IV and AN-P21/m at ambient conditions suggests a possibility of the phase transition in a small pressure-temperature range near ambient pressure and temperature.

Antiproliferative activity of O4-benzo[c]phenanthridine alkaloids against HCT-116 and HL-60 tumor cells.

The O4-benzo[c]phenanthridine alkaloids exhibit potent antiproliferative activity against cancer cells, which is derived from their ability to inhibit of topoisomerase I and II. It has been reported that in the alkaloids a cationic quaternary ammonium atom, which results in resonance effects between ring A and B, is necessary for increased antiproliferative activity. These findings indicate the role of their substituents at ring A on inhibition of tumor cell proliferation. In the present study, we systematically assessed the cytotoxic activities of naturally occurring alkaloids and their derivatives containing various ring A substituents against two tumor cell lines, HCT-116 colon tumor cells and HL-60 promyelocytic leukemia cells. Among the cationic iminium alkaloids, which displayed more potent activity than the corresponding neutral derivatives, and the 7,8-oxygenated benzo[c]phenanthridine alkaloids, chelerythrine and NK109, exhibited stronger antiproliferative activity than the 8,9- and 9,10-oxygenated alkaloids. The activity of cationic iminium alkaloids could be correlated with the bond lengths of their ring A substituents and the electrostatic potentials of their ammonium molecules by DFT calculation.

Zwitterionic ammonium and neutral amino molecules as cathode interlayer for inverted polymer solar cells

Cathode interlayer is essential to inverted bulk heterojunction polymer solar cells (PSCs). A series of zwitterionic ammonium and neutral amino organic molecules are introduced into inverted PSCs as cathode interlayer and power conversion efficiency (PCE) as high as 8.07% is demonstrated. Compared to the devices without interlayer, all the devices exhibit significant improvements of the device parameters by reducing the work function of indium tin oxide (ITO) cathode. It is striking that the devices with neutral amino molecules as interlayer exhibit remarkably higher PCEs than the devices with zwitterionic ammonium molecules as interlayer. We attribute the improved performance to the better photoactive morphology induced by the hydrophobic properties of the neutral amino derivatives through research of ultraviolet photoelectron spectroscopy, atomic force microscopy, and contact angle measurements. Interestingly, the PCEs of the inverted PSCs with cathode interlayer are positively correlated with the hydrophobic properties of the interlayer materials, since devices with neutral amino molecules or molecules with a more hydrophobic alkyl pendant (piperidine) as interlayer exhibit higher PCEs. These results pave the way to the design of effective cathode interlayer materials.

Topotactic Phase Transformation of Hexagonal MoO3 to Layered MoO3-II and Its Two-Dimensional (2D) Nanosheets

This study reports a novel strategy to obtain a layered metastable phase of molybdenum trioxide (MoO3). The metastable phase in the layered framework, i.e., MoO3-II, was a result of the topotactic phase transformation of hexagonal-MoO3 (h-MoO3) into MoO3-II. This transformation was realized through the removal of the water and ammonium molecules from the framework of h-MoO3. Next, a facile exfoliation strategy was adopted to prepare MoO3-II nanosheets, consisting of double-layers of MoO6 octahedra. The as-exfoliated MoO3-II nanosheets had measured thicknesses of 1.4, 2.4, and 11.2 nm, as quantified using atomic force microscopy (AFM), equivalent to 2, 3, and 16 double-layers of the MoO6 octahedra in MoO3-II, respectively, after taking into account their respective van der Waals gaps (thickness of a MoO3-II double-layer ∼0.709 nm). This work is the first attempt to synthesize MoO3-II nanosheets and shed light on their formation mechanism.