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DOE OSTI2023

Workshop on Addressing Rigor and Reproducibility in Thermal, Heterogeneous Catalysis

Heterogeneous catalysis has long served as the bedrock of the manufacturing of energy carriers, fuels and chemicals, and various technologies for pollution abatement. The significant complexity and variability spanning the entire breadth of catalyst material properties, synthesis methods, characterization techniques, and evaluation procedures, has focused attention on the need to establish community-accepted best practices for ensuring high-quality, benchmarked, and reproducible data. In addition, increased societal urgency to transition to clean energy and reduce greenhouse gas concentrations has incentivized interdisciplinary, convergent, and translational approaches to catalysis research in recent years. Research engineers and scientists with expertise cutting broadly across materials science, chemical synthesis, interfacial science, spectroscopy, and methods of data science and computational simulation, all bring diverse and important perspectives to catalysis research, but often with little awareness of the complexity of catalytic systems, especially in their working environment. As has already occurred in other scientific fields, there has been growing recognition and consensus in the heterogeneous catalysis research community that mechanisms are needed to improve the rigor and reproducibility (R&R) of experimental measurements, to ensure alignment of the broader research community with a common core of best practices specific to the realization of high-quality catalysis research. Similarly, the field is moving rapidly toward computationally informed and data science-driven catalyst design, but the success of implementing such predictive tools hinges on model training and validation rooted in rigorously obtained and reproducible experimental data that are benchmarked to common specifications. As such, this workshop was convened to prepare a report summarizing best practices for reporting data and performing experiments that researchers can use to benchmark, validate, and reproduce data in specific sub-fields of thermal, heterogeneous catalysis. Additionally, we discussed recommendations for future actions that may improve R&R in this field. The workshop organizers and participants include a diverse range of catalysis researchers from various employment sectors (e.g., academia, industry, national laboratory), institutional mission and resources (e.g., PhD-granting research universities, non-PhD-granting teaching universities), career stage (e.g., early, mid and late-career), technical expertise, and demographic background. This diverse group was involved in the discussion of workshop agenda items, writing this report, and discussing possible future action items for the community to consider, which helped ensure that a broad range of perspectives were captured in the description of the problems at hand and the creation of actionable solutions that may be effectively adopted by the diverse practitioners in catalysis research. Importantly, this group of workshop participants also included very early career researchers (e.g., senior PhD students, postdoctoral scholars) who will become the next generation of scientific leaders in various sectors, thus capturing emerging perspectives of newcomers to the field to shape its future while positively impacting the development of its future workforce. We envision that this effort will help advance the field of catalysis science by improving the rigor and reproducibility of experimental data collected by current researchers and future newcomers to the field, which is of broad importance to health and vitality of any scientific discipline. Therefore, best practices identified in this endeavor for thermal heterogeneous catalysis can be translated to such efforts in other areas of catalysis and other scientific fields involving the study of materials, and vice versa. We also envision this to be an ongoing effort, with future workshops that are convened to discuss issues of rigor and reproducibility on technical topics that were unable to be covered in this workshop due to its scope limitations, and as emerging methods and materials become more prevalent in the research community.

36 MATERIALS SCIENCE↗

NASA NTRS2012

Comparison of Inflation Processes at the 1859 Mauna Loa Flow, HI, and the McCartys Flow Field, NM

Basaltic lavas typically form channels or tubes during flow emplacement. However, the importance of sheet flow in the development of basalt ic terrains received recognition over the last 15 years. George Walke r?s research on the 1859 Mauna Loa Flow was published posthumously in 2009. In this paper he discusses the concept of endogenous growth, or inflation, for the distal portion of this otherwise channeldominated lava flow. We used this work as a guide when visiting the 1859 flow to help us better interpret the inflation history of the McCartys flow field in NM. Both well preserved flows display similar clues about the process of inflation. The McCartys lava flow field is among the you ngest (approx.3000 yrs) basaltic lava flows in the continental United States. It was emplaced over slopes of <1 degree, which is similar to the location within the 1859 flow where inflation occurred. Although older than the 1859 flow, the McCartys is located in an arid environ ment and is among the most pristine examples of sheet flow morphologies. At the meter scale the flow surface typically forms smooth, undula ting swales that create a polygonal terrain. The literature for simil ar features includes multiple explanatory hypotheses, original breakouts from adjacent lobes, or inflation related upwarping of crust or sa gging along fractures that enable gas release. It is not clear which of these processes is responsible for polygonal terrains, and it is po ssible that one explanation is not the sole cause of this morphology between all inflated flows. Often, these smooth surfaces within an inflated sheet display lineated surfaces and occasional squeeze-ups alon g swale contacts. We interpret the lineations to preserve original fl ow direction and have begun mapping these orientations to better interpret the emplacement history. At the scale of 10s to 100s of meters t he flow comprises multiple topographic plateaus and depressions. Some depressions display level floors with surfaces as described above, while some are bowl shaped with floors covered in broken lava slabs. Th e boundaries between plateaus and depressions are also typically smoo th, grooved surfaces that have been tilted to angles sometimes approaching vertical. The upper margin of these tilted surfaces displays lar ge cracks, sometimes containing squeeze-ups. The bottom boundary with smooth floored depressions typically shows embayment by younger lavas. It appears that this style of terrain represents the emplacement of an extensive sheet that experiences inflation episodes within prefer red regions where lateral spreading of the sheet is inhibited, thereby forming plateaus. Depressions are often the result of non-inflation and can be clearly identified by lateral squeeze-outs along the pit walls that form when the rising crust exposes the still liquid core of the sheet. Our current efforts are focused on.

Bleacher, Jacob E.↗

NASA NTRS2012

Discovery of a Plains Caldera Complex and Extinct Lava Lake in Arabia Terra, Mars: Implications for the Discovery of Additional Highland Volcanic Source Regions

Several irregularly shaped topographic depressions occur near the dichotomy boundary in northern Arabia Terra, Mars. The geomorphology of these features suggests that they formed by collapse, opposed to meteor impact. At least one depression (approx.55 by 85 km) displays geologic features indicating a complex, multi-stage collapse history. Features within and around the collapse structure indicate volcanic processes. The complex occurs within Hesperian ridged plains of likely volcanic origin and displays no crater rim or evidence for ejecta. Instead the depression consists of a series of circumferential graben and down-dropped blocks which also display upper surfaces similar to ridged plain lavas. Large blocks within the depression are tilted towards the crater center, and display graben that appear to have originally been linked with circumferential graben outside of the complex related to earlier collapse events. A nearly 700 m high mound exists along a graben within the complex that might be a vent. The deepest depression displays two sets of nearly continuous terraces, which we interpret as high-stands of a drained lava lake. These features appear similar to the black ledge described during the Kilauea Iki eruption in 1959. A lacustrine origin for the terraces seems unlikely because of the paucity of channels found in or around the depression that could be linked to aqueous surface processes. In addition, there is no obvious evidence for lacustrine sediments within the basin. Together with the presence of significant faulting that is indicative of collapse we conclude that this crater complex represents a large caldera formed in the Late Noachian to Early Hesperian. Other linear and irregular depressions in the region also might be linked to ancient volcanism. If that hypothesis is correct, it suggests that northern Arabia Terra could contain a large, previously unrecognized highland igneous province. Evacuation of magma via explosive and effusive activity produced localized collapse, might have contributed to nearby ridged plains, and pyroclastic materials erupted from these vents might have supplied sediments in fretted terrain and other deposits. The recognition of volcanoes within Arabia Terra expands the known extent of Noachian-Hesperian volcanism to cover much of the preserved martian highland crust.

Bleacher, Jacob↗

NASA NTRS2016

Africa's Megafans and Their Tectonic Setting

Megafans are a really extensive continental sediment bodies, fluvially derived, and fan-shaped in planform. Only those >80 km long were included in this study. Africa's megafans were mapped for purposes of both comprehensive geomorphic description and as a method of mapping by remote sensing large probable fluvial sediment bodies (we exclude sediment bodies deposited in well defined, modern floodplains and coastal deltas). Our criteria included a length dimension of >80 km and maximum width >40 km, partial cone morphology, and a radial drainage pattern. Visible and especially IR imagery were used to identify the features, combined with topographic SRTM data. We identified 99 megafans most of which are unstudied thus far. Their feeder rivers responsible for depositing megafan sediments rise on, and are consequent drainages oriented down the slopes of the swells that have dominated African landscapes since approximately 34 Ma (the high points in Africa's so-called basin-and-swell topography [1]). Most megafans (66%) have developed along these consequent rivers relatively near the swell cores, oriented radially away from the swells. The vast basins between the swells provide accommodation for megafan sediment wedges. Although clearly visible remotely, most megafans are inactive as a result of incision by the feeder river (which then no longer operates on the fan surface). Two tectonic settings control the location of Africa's megafans, 66% on swell flanks, and 33% related to rifts. (i) Swell flanks Most megafans are apexed relatively near the core of the parent swell, and are often clustered in groups: e.g., six on the west and north flanks of the Hoggar Swell (Algeria), seven on the north and south flanks of the Tibesti Swell (Libya-Chad borderlands), twelve on the west flank of the Ethiopian Swell, four on the east flank of the East African Swell (Kenya), Africa's largest, and eight around Angola's Bié Swell (western Zambia, northern Namibia). A cluster of possible fans lies on the western margin of the Congo Basin (Mayombe Swell), and on the coastal slopes of the Namibia Swell. Sheer size may have militated aginst the recognition of many megafans: the largest in the Sahara are the Teghahart (378 km, Hoggar Swell, Algeria), and the Wadi Albalata (340 km, Uweinat Swell, Egypt). In southern Africa the largest are the Cubango (320 km, Bié Swell, Angola/ Namibia), and the Limpopo (230 km, Mozambique). (ii) Rift zones (a) Steer's horns basins-wide depressions centered on rifts. The largest contiguous group (n=14) developed in a steer's-horns basin occupies the wide Muglad depression (200-350 km, South Sudan). Four rift-related megafans lie SE of Lake Chad (Chad). Nine megafans occupy the complex Anza Rift in Kenya/South Somalia. The Salamat megafan (Chad), is unusual because it oriented parallel with the linked Salamat, Doseo and Doba rift axes, and is consequently one of the longest in Africa (465 km). (b) Rift depressions sensu stricto. Most rifts are too narrow to provide a transverse dimension large enough to accommodate megafans. Although well-known, the Okavango Rift (NW Botswana, NE Namibia) is unique in Africa in hosting three megafans within identifiable faulted margins. The Nile megafan is Africa's largest (476 km) and comprises the vast Sudd wetland (South Sudan). An explanation for its remarkable size may be its location in a depression at the junction of two conducive tectonic zones, the East African Swell margin and the Muglad steer's-horns depression. Discharge of the River Nile, the largest in the region, has allowed the Nile megafan to outcompete neighboring megafans for space.

Wilkinson, M. J.↗

NASA NTRS2002

From following edges to pursuing objects

Primates can generate accurate, smooth eye-movement responses to moving target objects of arbitrary shape and size, even in the presence of complex backgrounds and/or the extraneous motion of non-target objects. Most previous studies of pursuit have simply used a spot moving over a featureless background as the target and have thus neglected critical issues associated with the general problem of recovering object motion. Visual psychophysicists and theoreticians have shown that, for arbitrary objects with multiple features at multiple orientations, object-motion estimation for perception is a complex, multi-staged, time-consuming process. To examine the temporal evolution of the motion signal driving pursuit, we recorded the tracking eye movements of human observers to moving line-figure diamonds. We found that pursuit is initially biased in the direction of the vector average of the motions of the diamond's line segments and gradually converges to the true object-motion direction with a time constant of approximately 90 ms. Furthermore, transient blanking of the target during steady-state pursuit induces a decrease in tracking speed, which, unlike pursuit initiation, is subsequently corrected without an initial direction bias. These results are inconsistent with current models in which pursuit is driven by retinal-slip error correction. They demonstrate that pursuit models must be revised to include a more complete visual afferent pathway, which computes, and to some extent latches on to, an accurate estimate of object direction over the first hundred milliseconds or so of motion.

NASA Discipline Neuroscience↗

NASA NTRS2002

Structure and Dynamics of the Quiet Solar Chromosphere

The grant supported research on the structure of the quiet, nonmagnetic chromosphere and on wave excitation and propagation in both the nonmagnetic chromosphere and the magnetic network. The work on the structure of the chromosphere culminated in the recognition that between two competing views of the solar chromosphere, older models by Avrett and collaborators (referred to as VAL) and the newer, dynamical model by Carlsson & Stein (referred to as CS), the clear decision is in favor of the older models, and this in spite of the evident lack of physics, which does not include wave motion and oscillations. The contrast between the static VAL models and the dynamical CS model can be stated most succinctly by comparing the temperature variation implied by the VAL models and the temperature fluctuations of the CS model, which are, respectively, of the order of 10% for the VAL model (at heights where hydrogen is 50% ionized) and a factor of 10 (at the upper boundary of their chromospheric model). The huge fluctuations of the CS model have never been observed, whereas the smaller temperature variations of the VAL models are consistent with ground-based and space-based observations. While it should be obvious which model describes the Sun and which one fails, the case is far from settled in the minds of solar physicists. Thus, much educational work remains to be done and, of course, more research to develop arguments that make the case more convincing. The research on waves and oscillations has been based on a unified theory of excitation of acoustic waves in the field-free atmosphere and of transverse and longitudinal waves in magnetic flux tubes located in the magnetic network by noting, first, that impulsive excitation of all these waves in gravitationally stratified media leads to oscillations at the respective cutoff frequencies and, second, that the observed oscillation frequencies in the nonmagnetic and magnetic parts of the chromosphere match corresponding cutoff frequencies in the upper solar photosphere. The dynamical simulations by Carlsson and Stein have been most instructive and of fundamental importance for understanding wave propagation in a stratified medium by their "flaws", the most important of which is an intensity excess at the H2v emission peak in the H line of Ca II, which is surprising since the observed intensity should have been an upper limit to the simulated intensity. The only plausible explanation for a predicted intensity that is higher than observed is that energy is spread horizontally in upward propagation in the Sun, but not in the plane-wave modeling of CS (as well as by almost everyone else). Investigations of the horizontal size of the region disturbed by the upward-propagating shock in the acoustic-wave propagation implies that the waves in H2v bright-point oscillations emanate from a point source with a diameter corresponding to the width of an intergranular lane, about 100 km, and reach a size of about 4000 km in the upper layers of the chromosphere. Linear, analytic modeling of waves emanating from a point source in a stratified atmosphere shows that the upward-expanding propagation channel does not have sharp boundaries and that the shape of the wave front depends on the order of the wave behind the initial pulse. Otherwise, the behavior of the linear waves resembles that of the nonlinear shock waves observed in the Sun. Research that needs to be done to firm up the conclusions reached above concerns the numerical simulations of nonlinear waves and oscillations in a three-dimensional stratified atmosphere with impulsive excitation, and observations linking directly the horizontal size of the disturbed area in upward propagation to individual waves.

Kalkofen, Wolfgang↗