Dataset Information

Pressure- and Temperature-Induced Insertion of N2, O2 and CH4 to Ag-Natrolite.

ABSTRACT: This paper aimed to investigate the structural and chemical changes of Ag-natrolite (Ag16Al16Si24O80·16H2O, Ag-NAT) in the presence of different pressure transmitting mediums (PTMs), such as N2, O2 and CH4, up to ~8 GPa and 250 °C using in situ synchrotron X-ray powder diffraction and Rietveld refinement. Pressure-induced insertion occurs in two stages in the case of N2 and O2 runs, as opposed to the CH4 run. First changes of the unit cell volume in N2, O2 and CH4 runs are observed at 0.88(5) GPa, 1.05(5) GPa and 1.84(5) GPa with increase of 5.7(1)%, 5.5(1)% and 5.7(1)%, respectively. Subsequent volume changes of Ag-natrolite in the presence of N2 and O2 appear at 2.15(5) GPa and 5.24(5) GPa with a volume increase of 0.8(1)% and a decrease of 3.0(1)%, respectively. The bulk moduli of the Ag-NAT change from 42(1) to 49(7), from 38(1) to 227(1) and from 49(3) to 79(2) in the case of N2, O2 and CH4 runs, respectively, revealing that the Ag-NAT becomes more incompressible after each insertion of PTM molecules. The shape of the channel window of the Ag-NAT changes from elliptical to more circular after the uptake of N2, O2 and CH4. Overall, the experimental results of Ag-NAT from our previous data and this work establish that the onset pressure exponentially increases with the molecular size. The unit cell volumes of the expanded (or contracted) phases of the Ag-NAT have a linear relationship and limit to maximally expand and contract upon pressure-induced insertion.

SUBMITTER: Seoung D

PROVIDER: S-EPMC7560438 | biostudies-literature | 2020 Sep

REPOSITORIES: biostudies-literature

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Pressure- and Temperature-Induced Insertion of N2, O2 and CH4 to Ag-Natrolite.

Seoung Donghoon D Kim Hyeonsu H Kim Pyosang P Lee Yongmoon Y

Materials (Basel, Switzerland) 20200915 18

This paper aimed to investigate the structural and chemical changes of Ag-natrolite (Ag16Al16Si24O80·16H2O, Ag-NAT) in the presence of different pressure transmitting mediums (PTMs), such as N2, O2 and CH4, up to ~8 GPa and 250 °C using in situ synchrotron X-ray powder diffraction and Rietveld refinement. Pressure-induced insertion occurs in two stages in the case of N2 and O2 runs, as o ...[more]

PMID: 32942731

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Project description:We report a combined experimental and modeling study of microwave-activated dilute CH4/N2/H2 plasmas, as used for chemical vapor deposition (CVD) of diamond, under very similar conditions to previous studies of CH4/H2, CH4/H2/Ar, and N2/H2 gas mixtures. Using cavity ring-down spectroscopy, absolute column densities of CH(X, v = 0), CN(X, v = 0), and NH(X, v = 0) radicals in the hot plasma have been determined as functions of height, z, source gas mixing ratio, total gas pressure, p, and input power, P. Optical emission spectroscopy has been used to investigate, with respect to the same variables, the relative number densities of electronically excited species, namely, H atoms, CH, C2, CN, and NH radicals and triplet N2 molecules. The measurements have been reproduced and rationalized from first-principles by 2-D (r, z) coupled kinetic and transport modeling, and comparison between experiment and simulation has afforded a detailed understanding of C/N/H plasma-chemical reactivity and variations with process conditions and with location within the reactor. The experimentally validated simulations have been extended to much lower N2 input fractions and higher microwave powers than were probed experimentally, providing predictions for the gas-phase chemistry adjacent to the diamond surface and its variation across a wide range of conditions employed in practical diamond-growing CVD processes. The strongly bound N2 molecule is very resistant to dissociation at the input MW powers and pressures prevailing in typical diamond CVD reactors, but its chemical reactivity is boosted through energy pooling in its lowest-lying (metastable) triplet state and subsequent reactions with H atoms. For a CH4 input mole fraction of 4%, with N2 present at 1-6000 ppm, at pressure p = 150 Torr, and with applied microwave power P = 1.5 kW, the near-substrate gas-phase N atom concentration, [N]ns, scales linearly with the N2 input mole fraction and exceeds the concentrations [NH]ns, [NH2]ns, and [CN]ns of other reactive nitrogen-containing species by up to an order of magnitude. The ratio [N]ns/[CH3]ns scales proportionally with (but is 102-103 times smaller than) the ratio of the N2 to CH4 input mole fractions for the given values of p and P, but [N]ns/[CN]ns decreases (and thus the potential importance of CN in contributing to N-doped diamond growth increases) as p and P increase. Possible insights regarding the well-documented effects of trace N2 additions on the growth rates and morphologies of diamond films formed by CVD using MW-activated CH4/H2 gas mixtures are briefly considered.

Dataset Information

Pressure- and Temperature-Induced Insertion of N2, O2 and CH4 to Ag-Natrolite.

Publications

Pressure- and Temperature-Induced Insertion of N<sub>2</sub>, O<sub>2</sub> and CH<sub>4</sub> to Ag-Natrolite.

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