An Exceptionally Stable Metal–Organic Framework Supported Molybdenum(VI) Oxide Catalyst for Cyclohexene Epoxidation
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catalysis (heterogeneous), materials and chemistry↗
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Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution
Colloidal quantum dots (QDs) have demonstrated great promise in artificial photosynthesis. However, the ultrasmall size hinders its controllable and effective interaction with cocatalysts. To improve the poor interparticle electronic communication between free QD and cocatalyst, we design here a self-assembled architecture of nanoparticles, QDs and Ptnanoparticles, simply jointed together by molecular polyacrylate to greatly enhance the rate and efficiency of interfacial electron transfer (ET). The enhanced interparticle electronic communication is confirmed by femtosecond transient absorption spectroscopy and X-ray transient absorption. Taking advantage of the enhanced interparticle ET with a time scale of ~65 ps, 5.0 mL assembled CdSe/CdS QDs/cocatalysts solution produces 94 ± 1.5 mL (4183 ± 67 µmol) molecular H 2 in 8 h, giving rise to an internal quantum yield of ~65% in the first 30 min and a total turnover number of >16,400,000 per Pt-nanoparticle. This study demonstrates that self-assembly is a promising way to improve the sluggish kinetics of interparticle ET process, which is the key step for advanced H 2 photosynthesis.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Direct Silyl Ether Metathesis for Vitrimers with Exceptional Thermal Stability
Not provided.
Chemistry↗
Exceptional Charge Transport Properties of Graphene on Germanium
The excellent charge transport properties of graphene suggest a wide range of application in analog electronics. While most practical devices will require that graphene be bonded to a substrate, such bonding generally degrades these transport properties. In contrast, when graphene is transferred to Ge(001) its conductivity is extremely high and the charge carrier mobility derived from the relevant transport measurements is, under some circumstances, higher than that of freestanding, edge-supported graphene. Here, we measure a mobility of ~5 × 10 5 cm 2 V –1 s –1 at 20 K, and ~10 3 cm 2 V –1 s –1 at 300 K. These values are close to the theoretical limit for doped graphene. Carrier densities in the graphene are as high as 10 14 cm –2 at 300 K.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Facile Microwave-Assisted Synthesis of 2D Imine-Linked Covalent Organic Frameworks for Exceptional Iodine Capture
Not Available
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
California's Drought of the Future: A Midcentury Recreation of the Exceptional Conditions of 2012–2017
The California drought of 2012–2016 was a record-breaking event with extensive social, political, and economic repercussions. The impacts were extensive and exposed the difficulty in preparing for the effects of prolonged dry conditions. Although the lessons from this drought drove important changes to state law and policy, there is little doubt that climate change will only exacerbate future droughts. To discern the character of future drought, this paper examines this recent drought period retrospectively and prospectively, that is, as it occurred historically and if similar dynamical conditions to the historical period were to arise 30 years later (2042–2046) subject to the effects of climate change. Simulations were conducted using the Weather Research and Forecasting model using the pseudo global warming method. The simulated historical and future droughts are contrasted in terms of temperature, precipitation, snowpack, soil moisture, evapotranspiration, and forest health. Overall, the midcentury drought is observed to be significantly worse, with many more extreme heat days, record-low snowpack, increased soil drying, and record-high forest mortality. With these findings in mind, the data sets developed in this study provide a means to structure future drought planning around a drought scenario that is realistic and modeled after a memorable historical analog.
54 ENVIRONMENTAL SCIENCES↗
Exceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La 0.5 Sr 1.5 Ni 1– x Fe x O 4±δ Ruddlesden-Popper oxides
The electrolysis of water is of global importance to store renewable energy and the methodical design of next-generation oxygen evolution catalysts requires a greater understanding of the structural and electronic contributions that give rise to increased activities. Herein, we report a series of Ruddlesden–Popper La 0.5 Sr 1.5 Ni 1– x Fe x O 4±δ oxides that promote charge transfer via cross-gap hybridization to enhance electrocatalytic water splitting. Using selective substitution of lanthanum with strontium and nickel with iron to tune the extent to which transition metal and oxygen valence bands hybridize, we demonstrate remarkable catalytic activity of 10 mA cm –2 at a 360 mV overpotential and mass activity of 1930 mA mg –1 ox at 1.63 V via a mechanism that utilizes lattice oxygen. This work demonstrates that Ruddlesden–Popper materials can be utilized as active catalysts for oxygen evolution through rational design of structural and electronic configurations that are unattainable in many other crystalline metal oxide phases.
25 ENERGY STORAGE↗
Exceptional hydrogen storage achieved by screening nearly half a million metal-organic frameworks
Few hydrogen adsorbents balance high usable volumetric and gravimetric capacities. Although metal-organic frameworks (MOFs) have recently demonstrated progress in closing this gap, the large number of MOFs has hindered the identification of optimal materials. Here, a systematic assessment of published databases of real and hypothetical MOFs is presented. Nearly 500,000 compounds were screened computationally, and the most promising were assessed experimentally. Three MOFs with capacities surpassing that of IRMOF-20, the record-holder for balanced hydrogen capacity, are demonstrated: SNU-70, UMCM-9, and PCN-610/NU-100. Analysis of trends reveals the existence of a volumetric ceiling at ~ 40 g H 2 L -1 . Surpassing this ceiling is proposed as a new capacity target for hydrogen adsorbents. Counter to earlier studies of total hydrogen uptake in MOFs, usable capacities in the highest-capacity materials are negatively correlated with density and volumetric surface area. Instead, capacity is maximized by increasing gravimetric surface area and porosity. This suggests that property/performance trends for total capacities may not translate to usable capacities.
36 MATERIALS SCIENCE↗
Exceptional subgenome stability and functional divergence in the allotetraploid Ethiopian cereal teff
Teff (Eragrostis tef) is a cornerstone of food security in the Horn of Africa, where it is prized for stress resilience, grain nutrition, and market value. Here, we report a chromosome-scale assembly of allotetraploid teff (variety Dabbi) and patterns of subgenome dynamics. The teff genome contains two complete sets of homoeologous chromosomes, with most genes maintaining as syntenic gene pairs. TE analysis allows us to estimate that the teff polyploidy event occurred ~1.1 million years ago (mya) and that the two subgenomes diverged ~5.0 mya. Despite this divergence, we detect no large-scale structural rearrangements, homoeologous exchanges, or biased gene loss, in contrast to many other allopolyploids. The two teff subgenomes have partitioned their ancestral functions based on divergent expression across a diverse expression atlas. Together, these genomic resources will be useful for accelerating breeding of this underutilized grain crop and for fundamental insights into polyploid genome evolution.
54 ENVIRONMENTAL SCIENCES↗
Robust and conductive two-dimensional metal-organic frameworks with exceptionally high volumetric and areal capacitance
For miniaturized capacitive energy storage, volumetric and areal capacitances are more important metrics than gravimetric ones because of the constraints imposed by device volume and chip area. Typically used in commercial supercapacitors, porous carbons, although they provide a stable and reliable performance, lack volumetric performance because of their inherently low density and moderate capacitances. In this paper, we report a high-performing electrode based on conductive hexaaminobenzene (HAB)-derived two-dimensional metal-organic frameworks (MOFs). In addition to possessing a high packing density and hierarchical porous structure, these MOFs also exhibit excellent chemical stability in both acidic and basic aqueous solutions, which is in sharp contrast to conventional MOFs. Submillimetre-thick pellets of HAB MOFs showed high volumetric capacitances up to 760 F cm -3 and high areal capacitances over 20 F cm -2 . Furthermore, the HAB MOF electrodes exhibited highly reversible redox behaviours and good cycling stability with a capacitance retention of 90% after 12,000 cycles. In conclusion, these promising results demonstrate the potential of using redox-active conductive MOFs in energy-storage applications.
25 ENERGY STORAGE↗
Exceptional power density and stability at intermediate temperatures in protonic ceramic fuel cells
Not provided.
Energy & Fuels↗
Exceptional activity of sub-nm Pt clusters on CdS for photocatalytic hydrogen production: A combined of experimental and first-principles study
In this work we have explored a new concept of substantially increasing photocatalytic activity for H₂ production of conventional semiconductors by modifying them with sub-nm Pt particles. By combining both experimental and theoretical approaches, we have also developed new mechanistic insights into the 17 times increase in photocatalytic activity of Pt modified CdS catalysts.
29 ENERGY PLANNING, POLICY, AND ECONOMY↗
Achieving an exceptionally high loading of isolated cobalt single atoms on a porous carbon matrix for efficient visible-light-driven photocatalytic hydrogen production
Isolated cobalt single atoms with a high loading of 5.9 wt% are generated through an in situ preparation strategy.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
A single-component water-lean post-combustion CO 2 capture solvent with exceptionally low operational heat and total costs of capture – comprehensive experimental and theoretical evaluation
A comprehensive evaluation of a recently developed water-lean amine-based solvent, namely N-(2-ethoxyethyl)-3-morpholinopropan-1-amine (2-EEMPA), has been performed to analyze its post-combustion CO 2 capture performance. This evaluation comprises (1) fundamental characterization of the solvent–CO 2 interaction using vapor–liquid equilibria, kinetics and viscosity measurements; (2) process characterization of the CO 2 capture performance as measured in a laboratory scale continuous flow system and via Aspen Plus® simulation using a flue gas simulant; as well as (3) a full techno economic analysis of the capture process at industrial scale with corresponding projections of critical metrics. This paper summarizes the many parts of this comprehensive evaluation and shows how the various parts come together to empower validated conclusions about its process performance. Notably, it is projected that this solvent can operate at a regeneration heat rate of 2.0 GJ per tonne CO 2 for post-combustion capture, and at a total cost of capture of $50.6/tonne CO 2 . Overall, with further process optimization significant reductions in the capture cost are predicted.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Tailoring Lewis/Brønsted acid properties of MOF nodes via hydrothermal and solvothermal synthesis: simple approach with exceptional catalytic implications
The Lewis/Brønsted catalytic properties of the Metal–Organic Framework (MOF) nodes can be tuned by simply controlling the solvent employed in the synthetic procedure. In this work, we demonstrate that Hf-MOF-808 can be prepared from a material with a higher amount of Brønsted acid sites, via modulated hydrothermal synthesis, to a material with a higher proportion of unsaturated Hf Lewis acid sites, via modulated solvothermal synthesis. The Lewis/Brønsted acid properties of the resultant metallic clusters have been studied by different characterization techniques, including XAS, FTIR and NMR spectroscopies, combined with a DFT study. The different nature of the Hf-MOF-808 materials allows their application as selective catalysts in different target reactions requiring Lewis, Brønsted or Lewis– Brønsted acid pairs.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Kinetic H 2 S/CO 2 selectivity in an exceptionally sterically hindered amine membrane
Decreasing membrane thickness reduces the reaction time for the competing amine-H 2 S and amine-CO 2 reactions, thus enhancing the selectivity for the “faster”, kinetically favored product, i.e. , hydrosulfide.
Rao, Shraavya↗
Abell 1430: A merging cluster with exceptional diffuse radio emission
Diffuse radio emission has been found in many galaxy clusters, predominantly in massive systems which are in the state of merging. The radio emission can usually be classified as relic or halo emission, which are believed to be related to merger shocks or volume-filling turbulence, respectively. Recent observations have revealed radio bridges for some pairs of very close galaxy clusters. The mechanisms that may allow one to explain the high specific density of relativistic electrons, which are necessary to explain the radio luminosity of these bridge regions, have been poorly explored until now. When inspecting the first data release of the LOFAR Two-Metre Sky Survey (LoTSS), we discovered diffuse radio emission in the galaxy cluster Abell 1430. Here, for this work, we aim to determine the dynamical state of the cluster and characterise the diffuse radio emission. We analysed the LoTSS data in detail and complemented them with recent Karl G. Jansky Very Large Array observations in the L-band. To study the dynamical state of the cluster, we analysed XMM-Newton data, Chandra data, and Sloan Digital Sky Survey data. Moreover, we compared our results to clusters extracted from THE THREE HUNDRED PROJECT cosmological simulation. We find that Abell 1430 consists of two components, namely A1430-A and A1430-B, with a mass ratio of about 2:1. The massive component shows diffuse radio emission which can be classified as radio halo which shows a low radio power at 1.4 GHz with respect to the mass of the cluster. Most interestingly, there is extended diffuse radio emission in the following dubbed as the ‘Pillow’ according to its morphology, which is apparently related to A1430-B and which is neither typical halo nor typical relic emission. The origin of this emission is puzzling. We speculate that the two components of Abell 1430 undergo an off-axis merger. In this scenario, A1430-B is moving towards the main cluster component and may have compressed and stirred the medium in the filament between the two cluster components. We have discovered evidence for diffuse radio emission related to the low-density intracluster or intergalactic medium in Abell 1430. To date, only a few examples of emission originating from such regions are known. These discoveries are crucial to constrain possible acceleration mechanisms which may allow us to explain the presence of relativistic electrons in these regions. In particular, our results indicate a spectral index of α 144 MHz 1.5 GHz = -1.4±0.5 for the Pillow. If upcoming observations confirm a slope as flat as -1.4 or even flatter, this would pose a challenge for the electron acceleration scenarios.
79 ASTRONOMY AND ASTROPHYSICS↗