Catalytic reactor for operando spatially resolved structure-activity profiling using high-energy X-ray diffraction.

In heterogeneous catalysis, operando measurements probe catalysts in their active state and are essential for revealing complex catalyst structure-activity relationships. The development of appropriate operando sample environments for spatially resolved studies has come strongly into focus in recent years, particularly when coupled to the powerful and multimodal characterization tools available at synchrotron light sources. However, most catalysis studies at synchrotron facilities only measure structural information about the catalyst in a spatially resolved manner, whereas gas analysis is restricted to the reactor outlet. Here, a fully automated and integrated catalytic profile reactor setup is shown for the combined measurement of temperature, gas composition and high-energy X-ray diffraction (XRD) profiles, using the oxidative dehydrogenation of C2H6 to C2H4 over MoO3/γ-Al2O3 as a test system. The profile reactor methodology was previously developed for X-ray absorption spectroscopy and is here extended for operando XRD. The profile reactor is a versatile and accessible research tool for combined spatially resolved structure-activity profiling, enabling the use of multiple synchrotron-based characterization methods to promote a knowledge-based optimization of a wide range of catalytic systems in a time- and resource-efficient way.

Less extreme and earlier outbursts of ice-dammed lakes since 1900.

Episodic failures of ice-dammed lakes have produced some of the largest floods in history, with disastrous consequences for communities in high mountains1-7. Yet, estimating changes in the activity of ice-dam failures through time remains controversial because of inconsistent regional flood databases. Here, by collating 1,569 ice-dam failures in six major mountain regions, we systematically assess trends in peak discharge, volume, annual timing and source elevation between 1900 and 2021. We show that extreme peak flows and volumes (10 per cent highest) have declined by about an order of magnitude over this period in five of the six regions, whereas median flood discharges have fallen less or have remained unchanged. Ice-dam floods worldwide today originate at higher elevations and happen about six weeks earlier in the year than in 1900. Individual ice-dammed lakes with repeated outbursts show similar negative trends in magnitude and earlier occurrence, although with only moderate correlation to glacier thinning8. We anticipate that ice dams will continue to fail in the near future, even as glaciers thin and recede. Yet widespread deglaciation, projected for nearly all regions by the end of the twenty-first century9, may bring most outburst activity to a halt.

Hazard from Himalayan glacier lake outburst floods.

Sustained glacier melt in the Himalayas has gradually spawned more than 5,000 glacier lakes that are dammed by potentially unstable moraines. When such dams break, glacier lake outburst floods (GLOFs) can cause catastrophic societal and geomorphic impacts. We present a robust probabilistic estimate of average GLOFs return periods in the Himalayan region, drawing on 5.4 billion simulations. We find that the 100-y outburst flood has an average volume of 33.5+3.7/-3.7 × 106 m3 (posterior mean and 95% highest density interval [HDI]) with a peak discharge of 15,600+2,000/-1,800 m3⋅s-1 Our estimated GLOF hazard is tied to the rate of historic lake outbursts and the number of present lakes, which both are highest in the Eastern Himalayas. There, the estimated 100-y GLOF discharge (∼14,500 m3⋅s-1) is more than 3 times that of the adjacent Nyainqentanglha Mountains, and at least an order of magnitude higher than in the Hindu Kush, Karakoram, and Western Himalayas. The GLOF hazard may increase in these regions that currently have large glaciers, but few lakes, if future projected ice loss generates more unstable moraine-dammed lakes than we recognize today. Flood peaks from GLOFs mostly attenuate within Himalayan headwaters, but can rival monsoon-fed discharges in major rivers hundreds to thousands of kilometers downstream. Projections of future hazard from meteorological floods need to account for the extreme runoffs during lake outbursts, given the increasing trends in population, infrastructure, and hydropower projects in Himalayan headwaters.

Rare flash floods and debris flows in southern Germany.

Flash floods and debris flows are iconic hazards in mountainous regions with steep relief, high rainfall intensities, rapid snowmelt events, and abundant sediments. The cuesta landscapes of southern Germany hardly come to mind when dealing with such hazards. A series of heavy rainstorms dumping up to 140 mm in 2 h caused destructive flash floods and debris flows in May 2016. The most severe damage occurred in the Braunsbach municipality, which was partly buried by 42,000 m3 of boulders, gravel, mud, and anthropogenic debris from the small catchment of Orlacher Bach (~6 km2). We analysed this event by combining rainfall patterns, geological conditions, and geomorphic impacts to estimate an average sediment yield of 14,000 t/km2 that mostly (~95%) came from some 50 riparian landslides and channel-bed incision of ~2 m. This specific sediment yield ranks among the top 20% globally, while the intensity-duration curve of the rainstorm is similarly in the upper percentile range of storms that had triggered landslides. Compared to similar-sized catchments in the greater region hit by the rainstorms, we find that the Orlacher Bach is above the 95th percentile in terms of steepness, storm-rainfall intensity, and topographic curvatures. The flash flood transported a sediment volume equal to as much as 20-40% of the Pleistocene sediment volume stored in the Orlacher Bach fan, and may have had several predecessors in the Holocene. River control structures from 1903 and records of a debris flow in the 1920s in a nearby catchment indicate that the local inhabitants may have been aware of the debris-flow hazards earlier. Such recurring and destructive events elude flood-hazard appraisals in humid landscapes of gentle relief, and broaden mechanistic views of how landslides and debris flows contribute to shaping small and deeply cut tributaries in the southern Germany cuesta landscape.

Repeated catastrophic valley infill following medieval earthquakes in the Nepal Himalaya.

Geomorphic footprints of past large Himalayan earthquakes are elusive, although they are urgently needed for gauging and predicting recovery times of seismically perturbed mountain landscapes. We present evidence of catastrophic valley infill following at least three medieval earthquakes in the Nepal Himalaya. Radiocarbon dates from peat beds, plant macrofossils, and humic silts in fine-grained tributary sediments near Pokhara, Nepal's second-largest city, match the timing of nearby M > 8 earthquakes in ~1100, 1255, and 1344 C.E. The upstream dip of tributary valley fills and x-ray fluorescence spectrometry of their provenance rule out local sources. Instead, geomorphic and sedimentary evidence is consistent with catastrophic fluvial aggradation and debris flows that had plugged several tributaries with tens of meters of calcareous sediment from a Higher Himalayan source >60 kilometers away.

Glacier and landslide feedbacks to topographic relief in the Himalayan syntaxes.

Despite longstanding research on the age and formation of the Tibetan Plateau, the controls on the erosional decay of its margins remain controversial. Pronounced aridity and highly localized rock uplift have traditionally been viewed as limits to the dissection of the plateau by bedrock rivers. Recently, however, glacier dynamics and landsliding have been argued to retard headward fluvial erosion into the plateau interior by forming dams and protective alluvial fill. Here, we report a conspicuous clustering of hundreds of natural dams along the Indus and the Tsangpo Rivers where these cross the Himalayan syntaxes. The Indus is riddled by hundreds of dams composed of debris from catastrophic rock avalanches, forming the largest concentration of giant landslide dams known worldwide, whereas the Tsangpo seems devoid of comparable landslide dams. In contrast, glacial dams such as river-blocking moraines in the headwaters of both rivers are limited to where isolated mountain ranges intersect the regional snowline. We find that to first-order, high local topographic relief along both rivers corresponds to conspicuously different knickzones and differences in the type and potential longevity of these dams. In both syntaxes, glacier and landslide dams act as a negative feedback in response to fluvial dissection of the plateau margins. Natural damming protects bedrock from river incision and delays headward knickpoint migration, thereby helping stabilize the southwestern and southeastern margins of the Tibetan Plateau in concert with the effects of upstream aridity and localized rock uplift.

Tibetan plateau river incision inhibited by glacial stabilization of the Tsangpo gorge.

A considerable amount of research has focused on how and when the Tibetan plateau formed in the wake of tectonic convergence between India and Asia. Although far less enquiry has addressed the controls on river incision into the plateau itself, widely accepted theory predicts that steep fluvial knick points (river reaches with very steep gradients) in the eastern Himalayan syntaxis at the southeastern plateau margin should erode rapidly, driving a wave of incision back into the plateau. Preservation of the plateau edge thus presents something of a conundrum that may be resolved by invoking either differential rock uplift matching erosional decay, or other mechanisms for retarding bedrock river incision in this region where high stream power excludes the potential for aridity as a simple limit to dissection of the plateau. Here we report morphologic evidence showing that Quaternary depression of the regional equilibrium line altitude, where long-term glacier mass gain equals mass loss, was sufficient to repeatedly form moraine dams on major rivers: such damming substantially impeded river incision into the southeastern edge of the Tibetan plateau through the coupled effects of upstream impoundment and interglacial aggradation. Such glacial stabilization of the resulting highly focused river incision centred on the Tsangpo gorge could further contribute to initiating and accentuating a locus of rapid exhumation, known as tectonic anaeurysm.