In this letter we describe the structural characteristics of nonpolar (112̄0) a-plane GaN thin films grown on (11̄02) r-plane sapphire substrates via metalorganic chemical vapor deposition. Planar growth surfaces have been achieved and the potential for device-quality layers realized by depositing a low temperature nucleation layer prior to high temperature epitaxial growth. The in-plane orientation of the GaN with respect to the r-plane sapphire substrate was confirmed to be [0001]GaN‖[1̄101]sapphire and [1̄100]GaN‖[112̄0]sapphire. This relationship is explicitly defined since the polarity of the a-GaN films was determined using convergent beam electron diffraction. Threading dislocations and stacking faults, observed in plan-view and cross-sectional transmission electron microscope images, dominated the a-GaN microstructure with densities of 2.6×1010 cm−2 and 3.8×105 cm−1, respectively. Submicron pits and crystallographic terraces were observed on the optically specular a-GaN surface with atomic force microscopy.
A better fundamental understanding of the plasma-catalyst interaction and the reaction mechanism is vital for optimizing the design of catalysts for ammonia synthesis by plasma-catalysis. In this work, we report on a hybrid plasma-enhanced catalytic process for the synthesis of ammonia directly from N2 and H2 over transition metal catalysts (M/Al2O3, M = Fe, Ni, Cu) at near room temperature (∼35 °C) and atmospheric pressure. Reactions were conducted in a specially designed coaxial dielectric barrier discharge (DBD) plasma reactor using water as a ground electrode, which could cool and maintain the reaction at near-room temperature. The transparency of the water electrode enabled operando optical diagnostics (intensified charge-coupled device (ICCD) imaging and optical emission spectroscopy) of the full plasma discharge area to be conducted without altering the operation of the reactor, as is often needed when using coaxial reactors with opaque ground electrodes. Compared to plasma synthesis of NH3 without a catalyst, plasma-catalysis significantly enhanced the NH3 synthesis rate and energy efficiency. The effect of different transition metal catalysts on the physical properties of the discharge is negligible, which suggests that the catalytic effects provided by the chemistry of the catalyst surface are dominant over the physical effects of the catalysts in the plasma-catalytic synthesis of ammonia. The highest NH3 synthesis rate of 471 μmol g–1 h–1 was achieved using Ni/Al2O3 as a catalyst with plasma, which is 100% higher than that obtained using plasma only. The presence of a transition metal (e.g., Ni) on the surface of Al2O3 provided a more uniform plasma discharge than Al2O3 or plasma only, and enhanced the mean electron energy. The mechanism of plasma-catalytic ammonia synthesis has been investigated through operando plasma diagnostics combined with comprehensive characterization of the catalysts using N2 physisorption measurements, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), NH3-temperature-programmed desorption (TPD), and N2-TPD. Four forms of adsorbed NH x (x = 0, 1, 2, and 3) species were detected on the surfaces of the spent catalysts using XPS. It was found that metal sites and weak acid sites could enhance the production of NH3 via formation of NH2 intermediates on the surface.
This letter reports on the reduction in extended-defect densities in a-plane (112̄0) GaN films achieved via lateral epitaxial overgrowth (LEO) by hydride vapor phase-epitaxy. A variety of dielectric mask patterns was used to produce 8–125-μm-thick, fully coalesced nonpolar GaN films. The nanometer-scale pit densities in the overgrown regions were less than 3×106 cm−2 compared to ∼1010 cm−2 in the direct-growth a-plane GaN. Cathodoluminescence revealed a fourfold increase in luminous intensity in the overgrown material compared to the window material. X-ray rocking curves indicate the films were free of wing tilt within the sensitivity of the measurements. Whereas non-LEO a-plane GaN exhibits basal plane stacking fault and threading dislocation densities of 105 cm−1 and 109 cm−2, respectively, the overgrown LEO material was essentially free of extended defects. The basal plane stacking fault and threading dislocation densities in the wing regions were below the detection limits of ∼5×106 cm−2 and 3×103 cm−1, respectively.
Recently, carbon dioxide (CO 2 ) conversion into higher-value platform chemicals and synthetic fuels has drawn great attention as a result of global warming. Non-thermal plasma (NTP)-catalytic CO 2 conversion has emerged to significantly reduce the reaction temperature. However, this technology requires a paradigm shift in process design to enhance plasma-catalytic performance. CO 2 conversion using NTP and catalysts has great potential to increase reaction efficiencies due to the synergetic effects between the plasma and catalysts that can provide mutual improvement in their performances. It is crucial to present the recent progress in CO 2 conversion and utilization whilst specifying a research prospects framework and providing future research directions in both industries and laboratories.Herein, a review of encouraging research achievements in CO 2 conversion and utilization using NTP in recent years is provided. The topics reviewed in this work are recent progress in different NTP sources in relation to product selectivity, conversion, and energy efficiency; plasma-based CO 2 reactions and applications; CO 2 conversion integrated with CO 2 capture; and process development of NTP in terms of potential large-scale applications processes. The high market value of the possible products from the NTP process, including chemicals and fuels, make the commercialization of the process feasible. Developing a suitable catalyst with effective sensitivities and performance under intricate conditions can improve the selectivity of these carbon-based liquid chemicals. There is a need for more studies to be performed in this field.
We report on violet-emitting III-nitride light-emitting diodes (LEDs) grown on bulk GaN substrates employing a flip-chip architecture. Device performance is optimized for operation at high current density and high temperature, by specific design consideration for the epitaxial layers, extraction efficiency, and electrical injection. The power conversion efficiency reaches a peak value of 84% at 85 °C and remains high at high current density, owing to low current-induced droop and low series resistance.
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