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Presented at 2020 International Pittsburgh Coal Conference, Pittsburgh, PA (virtual), September 8-11, 2020
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Presented by NETL at Reactive CO2 Capture: Process Integration for the New Carbon Economy Workshop, 02/20
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This is the final technical report for a collaborative project between the Ross Lab at MIT and the Filler Lab at Georgia Tech. The project aimed to combine in situ microscopy and spectroscopy measurements to answer fundamental questions about the physics and chemistry governing the bottom-up vapor-solid-liquid (VLS) growth of one-dimensional (1-D) functional oxides. This work supported one PhD student and 1 postdoc. One paper has been published and 5 others are in preparation. To date, this work has been presented at 5 conferences.
As the world endures environmental crises associated with climate change and the rise of atmospheric CO2 concentrations from anthropogenic CO2 emission, carbon capture and utilization (CCU) technologies are increasingly necessary. Reactive carbon capture (RCC) technologies, in which capture and conversion of CO2 occur in a single reactor, are more energetically and economically attractive by avoiding the need to purify, compress, and transport the captured CO2. To this end, the development of dual function materials (DFM) that enable CO2 capture and conversion to useful C1 products, namely (1) methane, (2) CO, and (3) methanol, are attractive near-term targets for commercial CCU processes for renewable fuels and chemicals. DFM are composed of sorbents and catalysts co-dispersed on the same high surface area carrier. The sorbent component allows for selective capture of CO2 from a gas stream and the catalyst component subsequently performs the in-situ conversion of the adsorbed CO2 upon introduction of a reactive gas (typically H2). The survey of DFM formulations reveals a variety of sorbent+catalyst combinations of interest. There is, however, a lack of depth in fundamental understanding of how the CO2 binds to these materials and how the subsequent reaction mechanisms are affected, which are critical features for the development of next-generation materials with improved performance. To this end, we will describe in this work the CO2 binding characteristics of established and/or new DFM and their sorbent-only counterparts. The surface CO2 binding mechanism and capture capacity will be probed using techniques such as in-situ DRIFTS, operando TGA, and CO2 chemisorption.
46th International Technical Conference on Clean Energy, Clearwater, FL, August 1-4, 2022
A perovskite-based solar cell comprising a transparent electrode disposed on a buffer layer that protects the perovskite from damage during the deposition of the electrode is disclosed. The buffer material is deposited using either low-temperature atomic-layer deposition, chemical-vapor deposition, or pulsed chemical-vapor deposition. In some embodiments, the perovskite material is operative as an absorption layer in a multi-cell solar-cell structure. In some embodiments, the perovskite material is operative as an absorption layer in a single junction solar cell structure.
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As the world endures environmental crises associated with climate change and the rise of atmospheric CO2 concentrations from anthropogenic CO2 emission, carbon capture and utilization (CCU) technologies are increasingly necessary. Reactive carbon capture (RCC) technologies, in which capture and conversion of CO2 occur in a single reactor, are more energetically and economically attractive by avoiding the need to purify, compress, and transport the captured CO2. To this end, dual function materials (DFMs) - composed of sorbents and catalysts co-dispersed on the same high surface area carrier - have been developed. The sorbent component allows for selective capture of CO2 from a gas stream and the catalyst component subsequently performs the in-situ conversion of the adsorbed CO2 upon introduction of a reactive gas (typically H2). The end product of the most established DFM, comprised of Ru and/or Ni with an alkaline sorbent, is methane via the CO2 methanation reaction. While renewable methane would be an excellent transition fuel, fossil methane is inexpensive (averaging $2.57/MMBTU in pre-pandemic 2019) and the economics of renewable methane utilization are noncompetitive. This requires the design and investigation of DFMs that enable CO2 capture and conversion to more valuable and more useful C1 products like CO or methanol (average price of methanol was $20.61/MMBTU in pre-pandemic 2019). These products can then be further upgraded to high energy density synthetic fuels, and related carbonaceous products, for more sustainable alternatives in industries that are difficult to decarbonize, specifically heavy duty vehicles and aviation. Herein, we report various sorbent + catalyst combinations to achieve the production of useful C1 products through reactive capture of CO2.
Higher temperatures and more isothermal heat profiles of solar heat sources are developed. The metal oxide metal sulfate class of cycles were suited for solar heat sources. Electrochemical oxidation of SO2 and thermochemical reactions are presented. Electrolytic oxidation of sulfur dioxide in dilute sulfuric acid solutions were appropriate for metal oxide metal sulfate cycles. The cell voltage at workable current densities required for the oxidation of SO2 was critical to the efficient operation of any metal oxide metal sulfate cycle. A sulfur dioxide depolarized electrolysis cell for the splitting of water via optimization of the anode reaction is discussed. Sulfuric acid concentrations of 30 to 35 weight percent are preferred. Platinized platinum or smooth platinum gave the best anode kinetics at a given potential of the five materials examined.
Equilibrium thermochemical analyses are employed to describe the vaporization processes of metals and metal oxides upon exposure to molecular and atomic oxygen. Specific analytic results for the chromium-, platinum-, aluminum-, and silicon-oxygen systems are presented. Maximum rates of oxidative vaporization predicted from the thermochemical considerations are compared with experimental results for chromium and platinum. The oxidative vaporization rates of chromium and platinum are considerably enhanced by oxygen atoms.
Metal oxides have been an attractive option for a range of applications, including hydrogen sensors, microelectronics, and catalysis, due to their reactivity and tunability. The properties of metal oxides can vary greatly on their precise surface structure; however, few surface science techniques can achieve atomistic-level determinations of surface structure, and fewer yet can do so for insulator surfaces. Low energy ion beam analysis offers a potential insulator-compatible solution to characterizing the surface structure of metal oxides. As a feasibility study, we apply low energy ion beam analysis to investigate the surface structure of a magnetite single crystal, Fe 3 O 4 (100). We obtain multi-angle maps using both forward-scattering low energy ion scattering (LEIS) and backscattering impact-collision ion scattering spectroscopy (ICISS). Both sets of experimental maps have intensity patterns that reflect the symmetries of the Fe 3 O 4 (100) surface structure. However, analytical interpretation of these intensity patterns to extract details of the surface structure is significantly more complex than previous LEIS and ICISS structural studies of one-component metal crystals, which had far more symmetries to exploit. To gain further insight into the surface structure, we model our experimental measurements with ion-trajectory tracing simulations using molecular dynamics. Our simulations provide a qualitative indication that our experimental measurements agree better with a subsurface cation vacancy model than a distorted bulk model.
Oxidation of CO to CO2 is an important reaction technologically and environmentally and a complex and interesting reaction scientifically. In most cases, the reaction is carried out in order to remove CO as an environmental hazard. A major application of heterogeneous catalysts is catalytic oxidation of CO in the exhaust of combustion devices. The reaction over catalysts in exhaust gas is fast and often mass-transfer-limited since exhaust gases are hot and O2/CO ratios are high. The main challenges to catalyst designers are to control thermal sintering and chemical poisoning of the active materials. The effect of the noble metal on the oxide is discussed, followed by the effect of the oxide on the noble metal, the interaction of the noble metal and oxide to form unique catalytic sites, and the possible ways in which the CO oxidation reaction is catalyzed by the NMRO materials.
The work performed in this reporting period has concentrated on the metal-oxide-metal (MOM) diode. The fabrication procedure begins with the deposition of gold probing pads to provide a non-oxidizing contact to test the dc characteristics to the diode accurately. A thin patch capped with an insulating SiO2 layer, is deposited next to form the first half of the diode. The other half of the diode, typically Ni, is deposited completing the conduction path from the oxidized edge of the Ni patch to the opposite gold probing pad. It is important in this step that the last metallization take place without exposing the newly oxidized surface to the atmosphere. Successful production of diodes has been achieved. Work on millimeter wave frequency rectennas incorporating known semiconductor diode technology has been initiated.
Room-temperature ferromagnetic materials with perpendicular magnetic anisotropy are widely sought after for spintronics, magnetic data storage devices, and stochastic computing. To address this need, a new Fe-BaTiO 3 vertically aligned nanocomposite (VAN) has been fabricated—combining both the strong room-temperature ferromagnetic properties of Fe nanopillars and the strong room-temperature ferroelectric properties of the BaTiO 3 matrix. Furthermore, the Fe-BaTiO 3 VAN allows for highly anisotropic magnetic properties with tunable magnetization and coercivity. Additionally, to demonstrate the multiferroic properties of the Fe-BaTiO 3 system, the new metal-oxide hybrid material system has been incorporated in a multilayer stack. Overall, this new multiferroic VAN system possesses great potential in magnetic anisotropy and property tuning and demonstrates a new material family of oxide-metal hybrid systems for room-temperature multiferroic material designs.
Here we present an optics-free CMOS image sensor that incorporates a novel time-gated dual-photodiode pixel design to allow filter- and lens-less image acquisition of near-infrared-excited (NIR-excited) upconverting nanoparticles. Recent biomedical advances have highlighted the benefits of NIR excitation, but NIR interaction with silicon has remained a challenge, even with high-performance optical blocking filters. Using a secondary diode and a dual-photodiode design, this sensor is able to remove the 100s of mV of NIR background on pixels and bring it down to single-digit mV level, nearing its noise floor of 2.2 mV rms, not achievable with any optical filter. Non-linear effects of background cancellation using the diode pair has been mitigated using an initial one-time pixel-level curve fitting and calibration in a post-processing setting. This imager comprises a highly linear 11 fF metal-oxide-metal (MOM) capacitor and includes integrated angle-selective gratings to reject oblique light and enhance sharpness. Each pixel also includes two distinct correlated double sampling schemes, to remove low frequency flicker noise and systematic offset in the datapath. We demonstrate the performance of this imager using pulsed NIR-excited upconverting nanoparticles on standard United-States-Air-Force (USAF) resolution targets and achieve an SNR of 15 dB, while keeping NIR background below 6 mV. This 36-by-80-pixel array measures only 2.3 mm by 4.8 mm and can be thinned down to 25 µm, allowing it to become surgically compatible with intraoperative instruments and equipment, while remaining optics-free.