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Vibrational and electronic properties of Np 2 O 5 from experimental spectroscopy and first principles calculations

High-valence actinide oxides are critical to understanding the behavior of 5f-electrons, yet their structural and electronic properties remain poorly understood due to challenges in synthesis and handling. We report the first Raman spectroscopic study of single-crystalline Np 2 O 5 and the first scanning tunneling spectroscopy (STS) measurement on any neptunium-containing material. Hydrothermally synthesized crystals were structurally verified by X-ray diffraction. Raman spectra revealed sharply resolved vibrational features, including previously unreported low-frequency modes. STS measurements revealed a band gap of 1.5 eV. Density functional theory (DFT) enables vibrational mode assignments, reveals neptunium-dominated low-frequency phonons, oxygen-dominated high-frequency modes, and predicts an indirect band gap of 1.68 eV. This predicted value is in excellent agreement with the experimentally measured STS gap. This combined Raman, DFT, and STS approach provides a robust framework for correlating lattice dynamics and electronic structure in actinide materials, providing benchmark data for Np 2 O 5 , and opening new avenues for probing structure–property relationships in complex f-electron materials.

36 - MATERIALS SCIENCE↗

Synthesis of PHI-type zeolite harmotome using barium as an inorganic structure-directing agent inspired from natural mineral compositions

Zeolites are nanoporous aluminosilicates widely used as commercial adsorbents, heterogeneous catalysts, and ion-exchange materials due to their unique porosity, acidity, and thermal stability. The vast majority of synthetically-realized zeolite structures are prepared under hydrothermal conditions in alkaline media, and often in the presence of an organic structure-directing agent that facilitates the crystallization of diverse porous networks. Due to economic and environmental disadvantages of organic-based syntheses, it is often desirable to produce zeolites in organic-free media using alkali metal ions as the most commonly employed inorganic structure-directing agents (ISDAs). Here, in this study, we were inspired by the elemental compositions of natural zeolite minerals to examine the use of an alkaline earth metal ion as the ISDA to prepare zeolites with the PHI framework type. Two natural minerals exhibiting this crystal structure are phillipsite and harmotome. Both structures contain sodium and potassium as extra-framework cations, but only harmotome contains barium cations. Here we examined how the combination of alkali and alkaline earth ISDAs promote the formation of PHI-type zeolites. Our findings reveal that each isostructure is prepared under different synthesis conditions where simply adding barium to a growth mixture does not always lead to harmotome formation. Harmotome is formed in more dilute and alkaline growth media; however, time-resolved analyses of zeolite crystallization reveal that harmotome can be synthesized at low temperatures (ca. 65 °C) with rates that are 5-times faster than syntheses of phillipsite. This seemingly indicates that barium reduces the energetic barrier for PHI-type zeolite nucleation in ways that are not fully understood. Moreover, harmotome crystals exhibit an average particle size of ca. 60 nm, which is nearly 40-fold smaller than phillipsite crystals prepared under similar conditions. Collectively, these findings identify routes to control crystallization of PHI-type zeolites and may provide a broader strategy for using the composition of natural zeolite minerals to optimize the preparation of synthetic analogues.

36 MATERIALS SCIENCE↗

Low Thermal Conductivity in Heteroanionic Materials with Layers of Homoleptic Polyhedra

Although BiAgOSe, an analogue of a well-studied thermoelectric material BiCuOSe, is thermodynamically stable, its synthesis is complicated by the low driving force of formation from the stable binary and ternary intermediates. Here we have developed a “subtraction strategy” to suppress byproducts and produce pure phase BiAgOSe using hydrothermal methods. Electronic structure calculations and optical characterization show that BiAgOSe is an indirect bandgap semiconductor with a bandgap of 0.95 eV. The prepared sample exhibits lower lattice thermal conductivities (0.61 W·m –1 ·K –1 at room temperature and 0.35 W·m –1 ·K –1 at 650 K) than BiCuOSe. Further, lattice dynamical simulations and variable temperature diffraction measurements demonstrate that the low lattice thermal conductivity arises from both the low sound velocity and high phonon–phonon scattering rates in BiAgOSe. These in turn result primarily from the soft Ag–Se bonds in the edge-sharing AgSe 4 tetrahedra and large sublattice mismatch between the quasi-two-dimensional [Bi 2 O 2 ] 2+ and [Ag 2 Se 2 ] 2– layers. These results highlight the advantages of manipulating the chemistry of homoleptic polyhedra in heteroanionic compounds for electronic structure and phonon transport control.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Growth mechanism of glucose-based hydrochar under the effects of acid and temperature regulation

Improving the tailorability of hydrochar synthesis is an effective way to enhance its performance and utilization efficiency. In this study, the growth rate, morphology, and molecular structure of hydrochar were controlled by regulating the pH and temperature of the hydrothermal carbonization process. Growth process analysis indicates that hydrochar has three growth periods: induction, rapid, and stable growth periods. It is mainly controlled by 5-hydroxymethylfurfural (HMF), which is formed by converting glucose and its transformation products. Further, the regulation of acid can significantly shorten the induction period of hydrochar, even under low-temperature conditions (<180 °C), and increase the growth rate of hydrochar. However, the degree of hydrochar adhesion varies: the lower the temperature, the greater the degree of its adhesion. Molecular structural analysis demonstrates that hydrochar mainly consists of furan structural domains and aromatic clusters, and its surface is rich in oxygen-containing functional groups. The degree at which hydrochar was aromatized was improved by increasing the reaction temperature (160–220 °C); whereas the regulation of acid reduced it and increased the content of oxygen-containing functional groups on the hydrochar surface. Based on these results, it is proposed that hydrochar formation has five stages and three growth periods with or without acid regulation.

59 BASIC BIOLOGICAL SCIENCES↗

Chemical preintercalation of magnesium ions into ⍺-MoO 3 structure for improved electrochemical stability in Li-ion cells

Chemical preintercalation of layered materials, used as electrodes in intercalation-based energy storage devices, represents a promising strategy to enhance electrochemical stability and extend cycle life. However, standardized synthesis approaches for the chemical preintercalation of diverse ions into various layered materials are lacking, necessitating the development of specific synthesis routes for each ion and layered phase combination. In this study, we present the first successful demonstration of Mg 2+ ion chemical preintercalation into the interlayer region of α-MoO 3 , revealing its stabilizing effect during cycling in non-aqueous Li-ion cells. Using ethanol during hydrothermal treatment facilitated molybdenum reduction, which was critical for Mg 2+ ion preintercalation. Interestingly, we found that Mg preintercalation was accompanied by the incorporation of water. Mg-preintercalated α-MoO 3 exhibited enhanced charge storage capacity, electrochemical stability, and power capability compared to pristine α-MoO 3 electrodes. This improved performance is attributed to the structural stabilization provided by Mg 2+ pillars, which prevent undesirable phase transformations during repeated Li intercalation/deintercalation, and increased Li + ion diffusion due to the shielding of electrostatic interactions between electrochemically cycled ions and the α-MoO 3 lattice, enabled by structural water. In conclusion, our study offers new insights into developing chemical preintercalation synthesis approaches that can be broadly applied to a wide range of pillaring ions and layered material hosts.

25 ENERGY STORAGE↗

Waste to worth: A high-temperature water-gas shift magnetite catalyst with encapsulated core-shell structure from coal fly ash

In this paper, we demonstrate the synthesis of magnetite-based, encapsulated catalyst with a core-shell structure from coal fly ash, an industrial solid waste, and its application to industrially important high temperature water-gas shift reaction (HT-WGSR). The catalyst precursor was first synthesized through a leaching-precipitation-hydrothermal process, leading to the formation of a nanosheet-like hematite precursor consisting of Fe 3+ as primary element and minor cations including Al 3+ , Mg 2+ and other cations (e.g. Ca 2+ and Ti 4+ ). During the WGSR, the nanosheets broke into smaller particles with a core of magnetite with a diameter of ~20 nm, whereas the inherent impurity elements were activated and migrated to the outer surface forming a shell with a thickness of ~4 nm. Due to the protection of shell, the as-synthesized catalyst exhibited improved activity, thermal stability and long-term durability for HT-WGSR at 400 °C and 450 °C. Compared to the pure hematite, this catalyst exhibited much higher activity and stability, i.e., increased CO conversion and decreased deactivation rate constant, by a factor of four and three, respectively. Additionally, through a bottom-up reverse synthesis, we have confirmed that Al 3+ functioned as a textual promoter enhancing the interfacial area of the catalyst. On the other hand, the presence of minor impurity elements, in particular 2.58 wt% Mg 2+ and 0.18 wt% Ti 4+ , were found to increase the basicity, and promote the adsorption rate of CO, the redox of catalysts, and the alteration of the reaction mechanism from regenerative to associative with the formation of a strong intermediate formate. Finally, this study not only opens a new direction on the valorization of solid waste into high-value catalysts, promoting the sustainability of solid waste management, but also provides an alternative, cost-effective and scalable approach for the design and fine-tuning of encapsulated catalysts.

01 COAL, LIGNITE, AND PEAT↗

The Dopamine Assisted Synthesis of MoO3/Carbon Electrodes With Enhanced Capacitance in Aqueous Electrolyte

A capacitance increase phenomenon is observed for MoO 3 electrodes synthesized via a sol-gel process in the presence of dopamine hydrochloride (Dopa HCl) as compared to α-MoO 3 electrodes in 5M ZnCl 2 aqueous electrolyte. The synthesis approach is based on a hydrogen peroxide-initiated sol-gel reaction to which the Dopa HCl is added. The powder precursor (Dopa) x MoO y , is isolated from the metastable gel using freeze-drying. Hydrothermal treatment (HT) of the precursor results in the formation of MoO 3 accompanied by carbonization of the organic molecules; designated as HT-MoO 3 /C. HT of the precipitate formed in the absence of dopamine in the reaction produced α-MoO 3 , which was used as a reference material in this study (α-MoO 3 -ref). Scanning electron microscopy (SEM) images show a nanobelt morphology for both HT-MoO 3 /C and α-MoO 3 -ref powders, but with distinct differences in the shape of the nanobelts. The presence of carbonaceous content in the structure of HT-MoO 3 /C is confirmed by FTIR and Raman spectroscopy measurements. X-ray diffraction (XRD) and Rietveld refinement analysis demonstrate the presence of α-MoO 3 and h-MoO 3 phases in the structure of HT-MoO 3 /C. The increased specific capacitance delivered by the HT-MoO 3 /C electrode as compared to the α-MoO 3 -ref electrode in 5M ZnCl 2 electrolyte in a −0.25–0.70 V vs. Ag/AgCl potential window triggered a more detailed study in an expanded potential window. In the 5M ZnCl 2 electrolyte at a scan rate of 2 mV s −1 , the HT-MoO 3 /C electrode shows a second cycle capacitance of 347.6 F g −1 . The higher electrochemical performance of the HT-MoO 3 /C electrode can be attributed to the presence of carbon in its structure, which can facilitate electron transport. Our study provides a new route for further development of metal oxides for energy storage applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Aqueous organic geochemistry at high temperature/high pressure

A description of the fate and chemical alterations of organic matter under hydrothermal conditions is given, with a brief overview of the geographic localities where these processes have been investigated to date. Two major aspects are examined: (1) alteration and degradation processes and reactions, both reductive and oxidative; and (2) synthesis processes and reactions which are primarily reductive. Examples of industrial applications of the related supercritical fluid technology are discussed.

Simoneit, Bernd R. T.↗

From cellulose to 1,2,4-benzenetriol via catalytic degradation over a wood-based activated carbon catalyst

In this study, spherical P-doped activated carbon (CSP) was obtained from poplar bark by microwave carbonization with phosphoric acid as the dopant and activating agent. Phosphorus bonded with four oxygen atoms to form a phosphate-like structure rather than directly bonding with C atoms in CSP; such groups can provide Lewis acid active sites with moderately strong acidity. The Lewis acid and total acid content increased with increasing phosphoric acid doping ratio. The use of phosphoric acid as an activating agent promotes the formation of a developed porous structure. CSP 1 (mass ratio of raw material to acid = 1 : 1) had a specific surface area of 1115 m 2 g –1 with developed micro–mesoporous structures, mainly micropores. Investigation of the activity of CSP in catalytic cellulose hydrolysis during hydrothermal degradation showed that Brønsted acid sites promote hydrolysis and dehydration of cellulose, Lewis acid sites promote subsequent reactions such as isomerization, rearrangement, and oligomerization, and the developed pores can provide reaction sites and facilitate reactant transportation. The optimal reaction conditions, i.e. , 1 h at 230 °C and 1 MPa with CSP 1 (0.4 g) as the catalyst, gave a cellulose conversion of >99.9%, with 42.30% selectivity for 1,2,4-benzenetriol. This study provides an effective method for preparing 1,2,4-benzenetriol from cellulose with biomass-based activated carbon as the catalyst, which enables green synthesis of 1,2,4-benzenetriol and promotes the use of biomass waste resources.

1,2,4-benzenetriol↗

Atomic Layer Deposition with TiO2 for Enhanced Reactivity and Stability of Aromatic Hydrogenation Catalysts

Hydrogenation of aromatic molecules in fossil- and bio-derived fuels is essential for decreasing emissions of harmful combustion products and addressing growing concerns around urban air pollution. In this work, we used atomic layer deposition to significantly enhance the hydrogenation performance of a conventional supported Pd catalyst by applying an ultrathin coating of TiO2 in a scalable powder coating process. The TiO2-coated catalyst showed substantial gains in the conversion of multiple aromatic molecules, including a 5-fold improvement in turnover frequency versus the uncoated catalyst in the hydrogenation of naphthalene. This activity enhancement was maintained upon scaling the coating synthesis process from 3 to 100 g. Based on the results from Xray photoelectron spectroscopy, X-ray absorption spectroscopy, and computational modeling, the activity enhancement was attributed to ensemble effects resulting from partial TiO2 coverage of the Pd surface rather than fundamental changes to the Pd electronic structure. Additional durability testing confirmed that the TiO2 coating improved the thermal and hydrothermal stability of the catalyst as well as tolerance toward sulfur impurities in the reactant stream. Using an economic model of an industrial deep hydrogenation process, we found that an increase in catalyst activity or lifetime of 2× would justify even a relatively high estimate for the cost of TiO2 atomic layer deposition coatings at scale

atomic layer↗

Improving charge transport in integrated MoO 3 /C electrode materials for water-in-salt energy storage systems by incorporating oxygen vacancies

Improvements in the charge storage properties of α-MoO 3 used as an electrode with a 30m ZnCl 2 water-in-salt electrolyte have been achieved by enhancements in electron and ion transport enabled by an inventive synthesis route. Electron transport was improved through the integration of MoO 3 with dopamine-derived carbon via a chemical preintercalation route, and enhanced ion transport was achieved by incorporating oxygen vacancies in MoO 3 structure through ethanol 2 reduction under hydrothermal conditions. Here, the presence of carbon was confirmed by corresponding D and G bands observed in Raman spectroscopy measurements. The presence of oxygen vacancies was proven through correlated XPS, TGA, Raman spectroscopy and XRD analyses, with the introduction of oxygen vacancies leading to an expanded interlayer region. Four-point probe measurements provided evidence of increased electronic conductivity due to the incorporation of carbon, and cyclic voltammetry-based charge storage mechanism analyses revealed increases in ion transport kinetics due to oxygen vacancy formation. Tuning the oxygen vacancy concentration is critical, as excessive concentrations of these point defects leads to structural instability and poor capacity retention. This work demonstrates the combined potential of carbon and oxygen vacancies in moderate concentrations to enhance the charge storage properties of transition metal oxides. The strategies developed in this study offer a path to the development of promising materials for high-rate, high-capacity, and long-duration electrochemical energy storage technologies.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

NaCo 2 (SeO 3 ) 2 (OH): competing magnetic ground states of a new sawtooth structure with 3d 7 Co 2+ ions

While certain magnetic sublattices have long been known theoretically to give rise to emergent physics via competing magnetic interactions and quantum effects, finding such configurations in real materials is often deeply challenging. Here we report the synthesis and characterization of a new such material, NaCo 2 (SeO 3 ) 2 (OH) which crystallizes with a highly frustrated sublattice of sawtooth Co 2+ chains. Single crystals of NaCo 2 (SeO 3 ) 2 (OH) were synthesized using a low-temperature hydrothermal method. X-ray single crystal structure analysis reveals that the material crystallizes in orthorhombic space group of Pnma (no. 62). Its crystal structure exhibits one-dimensional chains of corner-sharing isosceles triangles that are made of two crystallographically distinct 3d 7 Co 2+ sites (Co(1) and Co(2)). The chains run along the b-axis and are interconnected via [SeO 3 ] groups to form a three-dimensional structure mediating super-exchange interactions. The temperature dependent magnetization data show a ferromagnetic-like (FM) transition at 11 K (T 1 ) followed by an antiferromagnetic (AFM) transition at about 6 K (T 2 ). Neutron-powder diffraction measurements reveal that at T 1 = 11 K only the Co(2) site orders magnetically, forming ferromagnetic zigzag chains along the b-axis. Below T 2 = 6 K, both Co(1) and Co(2) sites order in a nearly orthogonal configuration, with Co(1) moments lying inside the plane of the sawtooth chain while Co(2) moments cant out of the plane. The canting of the magnetic moments leads to a net ferromagnetic component along b-axis, parallel to the chain direction. The ordered moments are fully compensated in the ac-plane. Inelastic neutron scattering measurements reveal crystal field excitations that are consistent with the presence of a spin–orbital entangled pseudo-spin state J eff = 1/2 for the Co 2+ ions. Low-energy spin-wave excitations are observed below the second magnetic transition. The analysis of powder excitation spectrum suggests complex exchange interactions that go beyond a Heisenberg Hamiltonian model with nearest neighbor couplings. Our results demonstrate the richness of the magnetic properties of sawtooth-type structures and encourage the study of similar structures with different oxyanion groups.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ni/CeO 2 Nanocatalysts with Optimized CeO 2 Support Morphologies for CH 4 Oxidation

Catalytic oxidation of CH 4 over nonprecious Ni/CeO 2 catalysts has attracted wide attention. Controlling the morphology of a CeO 2 support can enhance the CH 4 oxidation activity without changing the catalyst composition. Here, in this paper, a series of 2 wt % Ni/CeO 2 nanocatalysts with different CeO 2 support morphologies (nanoparticles (P), rods (R), cubes (C)) and synthetic procedures (precipitation, sol-gel (SG)) were evaluated for their CH 4 oxidation performance. The redox properties of CeO 2 supports and corresponding Ni loaded catalysts were characterized by H 2 -temperature-programmed reduction and oxygen storage capacity (OSC) measurements. The relationship among the CeO 2 morphologies, surface areas, redox properties, and CH4 oxidation activity for both CeO 2 supports and Ni/CeO 2 catalysts was established. The findings suggest that CeO 2 -R has a greater amount of surface oxygen vacancies as well as an improved OSC and CH4 oxidation activity compared to CeO 2 -P and CeO 2 -C supports. The same CH 4 oxidation activity pattern was observed for the Ni containing catalysts (Ni/CeO 2 -R > Ni/CeO 2 -P > Ni/CeO 2 -C). Increasing the CeO 2 surface area by using a sol-gel synthesis method (CeO 2 -SG) improved the amount of surface oxygen vacancies and CH 4 oxidation performance of CeO 2 -SG and Ni/CeO 2 -SG compared to CeO 2 -R and Ni/CeO 2 -R, respectively. Finally, all studied Ni/CeO 2 nanocatalysts showed improved hydrothermal stability compared to conventional Pd/Al 2 O 3 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A "Warm Formamide" Scenario for the Origins of Life Might not be so Hot: Comment on "Formamide and the Origin of Life"

In this review, Saladino et al. present an intriguing hypothesis surrounding the role of formamide in the origins of life on Earth, backed by experimental results supporting each step from formamide to RNA polymers. The overall premise is that, from formamide and inorganic phosphate, RNA molecules over 100 nucleotides in length can be produced. In addition, many carboxylic acids likely relevant to prebiotic metabolism, are formed along the way. Thus, from a rather simple organic molecule that has been observed in outer space (formamide), you can generate many of the compounds necessary for the origins of life. However, because high temperatures (160 C) are required for the formamide reactions, it remains unclear where the "warm formamide" scenario could have occurred. Low-temperature, aqueous hydrogen cyanide-based prebiotic chemistry that we know actually happened has been shown to produce many of the molecules invoked in the formamide hypothesis: amino acids, carboxylic acids, sugar acids, and nucleobases have all been found in meteorites recovered on Earth, providing a plausible route for their synthesis and delivery. In contrast, a large portion of the formamide hypothesis is based on relatively hightemperature reactions, A plausible milieu for high-temperature reactions with concentrated formamide is yet to be described, and is critical for this hypothesis to be validated. Hydrothermal vents are attractive heat sources, and the higher boiling point of formamide has been invoked as a mechanism to concentrate it from an aqueous solution, Unless the water can actually evaporate, however, there would be no net enrichment. For example, in the context of a deep-sea vent, any water "removed" by heating would be quickly replaced. Some of the individual reactions underpinning the present hypothesis have been met with skepticism because they go against conventional wisdom, To name a few of the surprising results: the observation that nucleosides can be converted to cyclic phosphates when heated in the presence of minerals and inorganie phosphate; that 3'-5' cGMP and cAMP nucleotides polymerize rapidly into RNA oligomers, even in the absence of monovalent counterions and that end-to-end ligation reactions between RNA oligomers occur in essentially pure water, without requiring any activating groups or counterions. Because the polymerization reactions are simply transesterification reactions, that they readily occur in the absence of cations makes one wonder why nearly all ribozyme-catalyzed transesterification reactions are metal-ion dependent; similarly, that the end-to-end ligation reactions do not require activation runs counter to the observation that all protein-catalyzed ligation and polymerization reactions of RNA and DNA require activated substrates. Detailed mechanistic studies of the reported reactions are warranted and could provide important insights for understanding the chemistry behind the origins of life. Because the authors have produced many of the experimental results supporting their hypothesis, they could demonstrate the validity of their hypothesis by converting formamide into approx 100 nucleotide RNA oligomers, using the products of one reaction as the reactants for the next reaction, under specific conditions plausible on the pre-biotic Earth. Such a demonstration would represent a milestone for our understanding of the origins of life.

Burton, Aaron S.↗

A 'Warm Formamide' Scenario for the Origins of Life Might Not Be so Hot Comment on 'Formamide and the Origin of Life' by E. Di Mauro Et Al.

In this review, Saladino et al. present an intriguing hypothesis surrounding the role of formamide in the originsof life on Earth, backed by experimental results supporting each step from formamide to RNA polymers [1]. The overall premise is that, from formamide and inorganic phosphate, RNA molecules over 100 nucleotides in length canbe produced. In addition, many carboxylic acids likely relevant to prebiotic metabolism are formed along the way. Thus, from a rather simple organic molecule that has been observed in outer space (formamide), you can generatemany of the compounds necessary for the origins of life. However, because high temperatures (160 C) are requiredfor the formamide reactions, it remains unclear where the warm formamide scenario could have occurred.Low-temperature, aqueous hydrogen counter to the observation that all protein-catalyzed ligation and polymerization reactions of RNA and DNA requireactivated substrates. Detailed mechanistic studies of the reported reactions are warranted and could provide important insights for understanding the chemistry behind the origins of life.Because the authors have produced many of the experimental results supporting their hypothesis, they coulddemonstrate the validity of their hypothesis by converting formamide into 100 nucleotide RNA oligomers, usingthe products of one reaction as the reactants for the next reaction, under specific conditions plausible on the pre-bioticEarth. Such a demonstration would represent a milestone for our understanding of the origins of life.cyanide-based prebiotic chemistry that we know actually happened has beenshown to produce many of the molecules invoked in the formamide hypothesis: amino acids, carboxylic acids, sugaracids, and nucleobases have all been found in meteorites recovered on Earth [e.g. [24]], providing a plausible routefor their synthesis and delivery. In contrast, a large portion of the formamide hypothesis is based on relatively high-temperature reactions. A plausible milieu for high-temperature reactions with concentrated formamide is yet to bedescribed, and is critical for this hypothesis to be validated. Hydrothermal vents are attractive heat sources, and the higher boiling point of formamide has been invoked as a mechanism to concentrate it from an aqueous solution.Unless the water can actually evaporate, however, there would be no net enrichment. For example, in the context of a deep-sea vent, any water removed by heating would be quickly replaced.Some of the individual reactions underpinning the present hypothesis [1] have been met with skepticism becausethey go against conventional wisdom. To name a few of the surprising results: the observation that nucleosides can beconverted to cyclic phosphates when heated in the presence of minerals and inorganic phosphate [5]; that 35 cGMPand cAMP nucleotides polymerize rapidly into RNA oligomers, even in the absence of monovalent counterions [6];and that end-to-end ligation reactions between RNA oligomers occur in essentially pure water, without requiring any activating groups or counterions [7,8]. Because the polymerization reactions are simply transesterification reactions,that they readily occur in the absence of cations makes one wonder why nearly all ribozyme-catalyzed transesterification reactions are metal-ion dependent; similarly, that the end-to-end ligation reactions do not require activation runs.

life↗

Synthesis and characterization of UiO-66-NH 2 incorporated graphene aerogel composites and their utilization for absorption of organic liquids

This work details the synthesis, materials characterization and absorption capacity of graphene aerogel (GA) loaded with UiO-66-NH 2 metal organic framework (MOF). Throughout the study, a series of density-tunable MOF/GA composites were synthesized by adjusting the MOF/graphene oxide (GO) mass ratio of the precursors before hydrothermal reduction and subsequent critical point drying to achieve MOF-x%/GA composites, with x, ranging from 0 to 100, denoting the weight percent ratio of MOF to GO in the starting solution. Scanning electron microscopy (SEM) images and Barrett-Joyner-Halenda (BJH) pore size calculations supported that MOF loading enlarged the macroporous (>50 nm) structure of the GA framework but had no influence on the mesoporous (2–50 nm) structure of GA. The degree of MOF loading first decreased and then increased the density of resulting composites, exhibiting a minimum for the 10–30% samples. Such behavior with respect to MOF loading has not been reported previously. MOF-x%/GA samples were further investigated for absorption capacity using various organic liquids. MOF-30%/GA proved to be the best absorbent sample for all solvents tested, achieving the highest capacity for chloroform at 147.0 ± 10.0 mg/mg. The behavior is attributed to the structural changes induced by the MOF incorporation as well as the interactions between the organic molecules and the MOF.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mechanochemically Assisted Synthesis of High-Entropy Layer-Structured Dittmarite Analogues

High-entropy solid-solution materials, especially layered ones incorporating five or more near-equimolar components into single-phase crystal structures, may spark functional synergism toward the electrochemistry area because of their unique antisite disordering structures and the synergistic effect of multiple active sites. Herein, high-entropy dittmarite analogues (HEDAs) were synthesized via a mechanochemistry-assisted hydrothermal method. Furthermore, the as-prepared HEDAs have single dittmarite phases with five homogeneously distributed metal elements, exhibiting enhanced activities in oxygen evolution catalysis compared to the single metal counterparts.

36 MATERIALS SCIENCE↗

Magnetosynthesis Effect on the Structure and Ground State of Cu 2+ -Based Antiferromagnets

Synthetic variables can have an outsized influence on the crystal structure and magnetic properties of a material, particularly those of quantum materials. In this work, we investigate the impact of synthesis under a magnetic field (magnetosynthesis) on the crystal structure and magnetic properties of several Cu 2+ (S = 1/2)-based materials with antiferromagnetic interactions and varying levels of magnetic frustration, from simple antiferromagnets to a quantum spin liquid. Here, we develop methods to apply small (0.09–0.37 T) magnetic fields during low-temperature hydrothermal, evaporative, and rehydration syntheses of the simple antiferromagnet CuCl 2 ·2H 2 O, the canted antiferromagnet (Cu,Zn) 3 Cl 4 (OH) 2 ·2H 2 O, the frustrated and canted antiferromagnet atacamite Cu 2 (OH) 3 Cl, and the highly frustrated quantum spin liquid herbertsmithite Cu 3 Zn(OH) 6 Cl 2 . We report the first single-crystal X-ray structural determination of the Cu 3 Cl 4 (OH) 2 ·2H 2 O structure type and probe the stability of this phase both experimentally and computationally. Atacamite Cu 2 (OH) 3 Cl synthesized under a 0.19 T field experiences a 0.15 K (∼3%) decrease in its Néel transition temperature. This result suggests that magnetosynthesis with small applied fields may have a very subtle influence upon the magnetic properties of moderately magnetically frustrated 3 d materials.

36 MATERIALS SCIENCE↗