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NASA NTRS2022

Diffusion in Melts and Magmas

Diffusion results from random motion of particles and entities. Diffusion in melts and magmas is due to thermally excited random motion of atoms, ions, and clusters, and plays a critical role in magmatic and volcanic processes. In melts and magmas, diffusion is one of the two mechanisms of mass transfer; the other being bulk flow (referred to as convection or advection). When both are present, diffusion refers to the dispersive motion relative to the mean bulk flow in a given reference frame (Richter et al. 1998). Diffusion plays critical roles in controlling magma mixing (Watson 1982; Koyaguchi 1985, 1989; Lesher 1994; Huber et al. 2009; Guo and Zhang 2020), mineral growth and dissolution rates in magmas (e.g., Watson 1982; Harrison and Watson 1983; Zhang et al. 1989; Newcombe et al. 2014; Macris et al. 2018), bubble growth and dissolution rate in magmas (Sparks 1978; Proussevitch and Sahagian 1998; Liu and Zhang 2000; Zhang 2013), and elemental and isotope fractionation during mineral 2 growth and dissolution (Jambon 1980; Richter et al. 1999, 2003; Watson and Muller 2009; Chopra et al. 2012; Watkins et al. 2014, 2017; Holycross et al. 2016, 2018). As a result, diffusion also plays an essential role in explosive volcanic eruptions and magma crystallization. Furthermore, diffusion has important applications in geospeedometry (Lasaga 1983, 1998; Zhang 1994, 2008; Trail et al. 2016; Zhang and Xu 2016). Experimental investigation of diffusion in geologically relevant silicate melts began to flourish in the 1970’s when micro-analytical measurements of diffusion profiles became available. In addition to the vast number of papers published since then, numerous books and reviews are available for diffusion in silicate melts. Hofmann et al. (1974) edited a book titled “Geochemical Transport and Kinetics” published by Carnegie Institution of Washington. This was the first landmark book summarizing the field. Lasaga and Kirkpatrick (1981) edited a book “Kinetics of Geochemical Processes” as volume 8 of the Reviews in Mineralogy (later becoming Reviews in Mineralogy and Geochemistry) series. Zhang and Cherniak (2010) edited “Diffusion in Minerals and Melts” as volume 72 of Reviews of Mineralogy and Geochemistry series, in which one chapter focused on diffusion theory, five chapters on diffusion in silicate melts (Behrens 2010; Lesher 2010; Liang 2010; Zhang and Ni 2010; Zhang et al. 2010), and other chapters were on experimental, analytical, and computational methods, and diffusion in minerals. Several textbooks covered the principles and applications of diffusion theories (Kirkaldy and Young 1987; Shewmon 1989; Cussler 1997; Lasaga 1998; Zhang 2008; Vrentas and Vrentas 2016), and two classic books covered the mathematics of diffusion (Carslaw and Jaeger 1959; Crank 1975). In preparing for this review chapter, we thought carefully about what to cover for this vast field, and decided to briefly go through the fundamentals of diffusion (more complete review can be found in Chakraborty 1995; Zhang 2008, 2010) and solutions to often-encountered 3 diffusion problems, and then focus on post-2010 diffusion studies on silicate melts and magmas. Here, melts refer to (mostly natural) silicate liquid, and magmas refer to crystal-bearing and/or bubble-bearing melts in which the continuous phase is the melt. There is a large body of work on diffusion in glasses, especially in the materials science literature, which is not covered in this review.

Youxue Zhang↗

NASA NTRS1999

Origin and Reactivity of the Martian Soil: A 2003 Micromission

The role of water in the development of the martian surface remains a fundamental scientific question. Did Mars have one or more "warm and wet" climatic episodes where liquid water was stable at the surface? If so, the mineral phases present in the soils should be consistent with a history of aqueous weathering. More generally, the formation of hydrated mineral phases on Mars is a strong indicator of past habitable surface environments. The primary purpose of this investigation is to help resolve the question of whether such aqueous indicators are present on Mars by probing the upper meter for diagnostic mineral species. According to Burns [1993], the formation of the ferric oxides responsible for the visible color of Mars are the result of dissolution of Fe (+2) phases from basalts followed by aqueous oxidation and precipitation of Fe" mineral assemblages. These precipitates likely included iron oxyhydroxides such as goethite (a-FeOOH) and lepidocrocite (g-FeOOH), but convincing evidence for these phases at the surface is still absent. The stability of these minerals is enhanced beneath the surface, and thus we propose a subsurface search for hydroxylated iron species as a test for a large-scale chemical weathering process based on interactions with liquid water. It is also possible that the ferric minerals on Mars are not aqueous alteration products of the rocks. A chemical study of the Pathfinder landing site concluded that the soils are not directly derived from the surrounding rocks and are enhanced in Mg and Fe. The additional source of these elements might be from other regions of Mars and transported by winds, or alternatively, from exogenic sources. Gibson [1970] proposed that the spectral reflectivity of Mars is consistent with oxidized meteoritic material. Yen and Murray [1998] further extend Gibson's idea and show, in the laboratory, that metallic iron can be readily oxidized to maghemite and hematite under present-day martian surface conditions (in the absence of liquid water). A test for a meteoritic component of the soil can be conducted, as described below, by searching for the presence of Ni at the martian surface. The average abundance of nickel in an Fe-Ni meteorite is about 7% and, if present at measurable levels in the soil, would be indicative of an exogenic contribution. In addition, it may be possible to directly search for mineral phases common in meteorites. An understanding of the formation and evolution of the martian soil would not be complete without addressing the unusual reactivity discovered by the Viking Landers The presence of an inorganic oxidant, possibly one produced as a results of photochemical processes, is the most widely accepted explanation of the Viking results. Are these chemical species simply adsorbed on soil grains, or have they reacted with the metal oxide substrates and altered the mineral structures? Could a completely different (non-photochemical) process be responsible for the soil reactivity? The various ideas for the nature of this putative oxidant could be constrained by a measurement of the change in reactivity with depth. Different compositions will have different lifetimes and mobilities and thus will have different vertical profiles. Because the oxidizing compounds are believed to actively destroy organic molecules, determination of the reactivity gradient also has significant implications for the search for life on Mars. A DS2-based microprobe system can be instrumented for a 2003 micromission to investigate the origin and reactivity of the martian soil. These measurements would provide invaluable information regarding the climate history and exobiological potential of the planet. The NMR, X ray and chemiresistor measurement approach described embodies a highly synergistic and general set of soil interrogation methods for elements, compounds, and crystal structures and can also be applied to other geologic questions of interest. For example, if the capability for precise targeting of the probes is available, then in-situ investigations of suspected evaporite and hydrothermal deposits would be possible with the same set of instruments. Additional information is contained in the original.

Yen, Albert S.↗

DOE OSTI2020

Atomic-scale constituting stable interface for improved LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathodes of lithium-ion batteries

Ascribed to their higher capacity and lower cost compared to conventional LiCoO 2 , the Ni-rich layered LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) is now considered as one promising cathode for lithium-ion batteries (LIBs). However, it still suffers from some evident performance degradation, especially under high cutoff voltages (i.e., >4.3 V versus Li/Li + ). The performance degradation typically is exhibited as capacity fading and voltage drop, mainly originating from an instable interface between the NMC622 and electrolyte as well as the evolution of the NMC structure. To improve the interfacial and structural stability of NMC cathodes, herein we deposited an ultrathin layer of Al 2 O 3 coatings (<5 nm) conformally over NMC622 composite electrodes directly using atomic layer deposition (ALD). It was found that, under different upper cutoff voltages (4.3, 4.5, and 4.7 V), the ALD Al 2 O 3 coatings enable enhanced performance of NMC622 cathodes with better cyclability and higher capacity. Particularly, the beneficial effects of the ALD Al 2 O 3 coatings are more remarkable at higher upper cutoff voltages (4.5 and 4.7 V). Furthermore, the ALD coatings can significantly improve the rate capability of NMC622. To this end, we utilized a suite of characterization tools and performed a series of electrochemical tests to clarify the effects of the ALD Al 2 O 3 coatings. This study revealed that the beneficial effects of the Al 2 O 3 ALD coatings are multiple: (i) serving as an artificial layer of solid electrolyte interphase to mitigate undesirable interfacial reactions; (ii) acting as a physical barrier to inhibit metal dissolution of NMC; and (iii) forming a reinforced networked overcoating to boost the mechanical integrity of NMC cathodes. This study is favorable for designing high-performance NMC cathodes.

25 ENERGY STORAGE↗