Chemical Differences in Environmental Films Collected on Surfaces with Different Hydrophilicity.

Environmental films form when airborne particles and molecular species adsorb on solid surfaces. Recent studies have characterized these films but overlook how collection methods and host-surface character (orientation, chemical functionality, or height) change the deposition process. In this work, environmental films are collected at a rural location on gold and silicon surfaces (water contact angles of ca.

Contrasting Effects of Catecholate and Hydroxamate Siderophores on Molybdenite Dissolution.

Molybdenum (Mo) is essential for many enzymes but is often sequestered within minerals, rendering it not readily bioavailable. Metallophores, metabolites secreted by microorganisms and plants, promote mineral dissolution to increase the metal bioavailability. However, interactions between metallophores and Mo-bearing minerals remain unclear.

Understanding Trace Iron and Chromium Incorporation During Gibbsite Crystallization and Effects on Mineral Dissolution.

Incorporation of pollutants, e.g., heavy metals, or critical elements, e.

Solvent-mediated oxide hydrogenation in layered cathodes.

Self-discharge and chemically induced mechanical effects degrade calendar and cycle life in intercalation-based electrochromic and electrochemical energy storage devices. In rechargeable lithium-ion batteries, self-discharge in cathodes causes voltage and capacity loss over time. The prevailing self-discharge model centers on the diffusion of lithium ions from the electrolyte into the cathode.

Guided anisotropic oxygen transport in vacancy ordered oxides.

Anisotropic and efficient transport of ions under external stimuli governs the operation and failure mechanisms of energy-conversion systems and microelectronics devices. However, fundamental understanding of ion hopping processes is impeded by the lack of atomically precise materials and probes that allow for the monitoring and control at the appropriate time- and length- scales. In this work, using in-situ transmission electron microscopy, we directly show that oxygen ion migration in vacancy ordered, semiconducting SrFeO epitaxial thin films can be guided to proceed through two distinctly different diffusion pathways, each resulting in different polymorphs of SrFeO with different ground electronic properties before reaching a fully oxidized, metallic SrFeO phase.

Dynamic Molecular Investigation of the Solid-Electrolyte Interphase of an Anode-Free Lithium Metal Battery Using Liquid SIMS and Cryo-TEM.

We use liquid secondary ion mass spectroscopy, cryogenic transmission electron microscopy, and density functional theory calculation to delineate the molecular process in the formation of the solid-electrolyte interphase (SEI) layer under the dynamic operating conditions. We discover that the onset potential for SEI layer formation and the thickness of the SEI show dependence on the solvation shell structure. On a Cu film anode, the SEI is noticed to start to form at around 2.

Molecular Imaging Reveals Two Distinct Mixing States of PM Particles Sampled in a Typical Beijing Winter Pollution Case.

Mixing states of aerosol particles are crucial for understanding the role of aerosols in influencing air quality and climate. However, a fundamental understanding of the complex mixing states is still lacking because most traditional analysis techniques only reveal bulk chemical and physical properties with limited surface and 3-D information. In this research, 3-D molecular imaging enabled by ToF-SIMS was used to elucidate the mixing states of PM samples obtained from a typical Beijing winter haze event.

Molecular identification of wines using liquid SIMS and PCA analysis.

Composition analysis in wine is gaining increasing attention because it can provide information about the wine quality, source, and nutrition. In this work, liquid secondary ion mass spectrometry (SIMS) was applied to 14 representative wines, including six wines manufactured by a manufacturer in Washington State, United States, four Cabernet Sauvignon wines, and four Chardonnay wines from other different manufacturers and locations. liquid SIMS has the unique advantage of simultaneously examining both organic and inorganic compositions from liquid samples.

A Mineral-Doped Micromodel Platform Demonstrates Fungal Bridging of Carbon Hot Spots and Hyphal Transport of Mineral-Derived Nutrients.

Soil fungi facilitate the translocation of inorganic nutrients from soil minerals to other microorganisms and plants. This ability is particularly advantageous in impoverished soils because fungal mycelial networks can bridge otherwise spatially disconnected and inaccessible nutrient hot spots. However, the molecular mechanisms underlying fungal mineral weathering and transport through soil remains poorly understood primarily due to the lack of a platform for spatially resolved analysis of biotic-driven mineral weathering.

Manipulating the insulator-metal transition through tip-induced hydrogenation.

Manipulating the insulator-metal transition in strongly correlated materials has attracted a broad range of research activity due to its promising applications in, for example, memories, electrochromic windows and optical modulators. Electric-field-controlled hydrogenation using ionic liquids and solid electrolytes is a useful strategy to obtain the insulator-metal transition with corresponding electron filling, but faces technical challenges for miniaturization due to the complicated device architecture. Here we demonstrate reversible electric-field control of nanoscale hydrogenation into VO with a tunable insulator-metal transition using a scanning probe.

Spontaneous Lithiation of Binary Oxides during Epitaxial Growth on LiCoO.

Epitaxial growth is a powerful tool for synthesizing heterostructures and integrating multiple functionalities. However, interfacial mixing can readily occur and significantly modify the properties of layered structures, particularly for those containing energy storage materials with smaller cations. Here, we show a two-step sequence involving the growth of an epitaxial LiCoO cathode layer followed by the deposition of a binary transition metal oxide.

Mass spectral imaging showing the plant growth-promoting rhizobacteria's effect on the Brachypodium awn.

The plant growth-promoting rhizobacteria (PGPR) on the host plant surface play a key role in biological control and pathogenic response in plant functions and growth. However, it is difficult to elucidate the PGPR effect on plants. Such information is important in biomass production and conversion.

Electrochemically induced amorphous-to-rock-salt phase transformation in niobium oxide electrode for Li-ion batteries.

Intercalation-type metal oxides are promising negative electrode materials for safe rechargeable lithium-ion batteries due to the reduced risk of Li plating at low voltages. Nevertheless, their lower energy and power density along with cycling instability remain bottlenecks for their implementation, especially for fast-charging applications. Here, we report a nanostructured rock-salt NbO electrode formed through an amorphous-to-crystalline transformation during repeated electrochemical cycling with Li.

The behavior of iodine in stabilized granular activated carbon and silver mordenite in cementitious waste forms.

Both granular activated carbon (GAC) and silver mordenite (AgM) are utilized for the removal of contaminants and radionuclides (e.g., radioiodine) from off-gas streams in nuclear fuel reprocessing and high temperature immobilization of nuclear waste.

Molecular imaging of plant-microbe interactions on the seed surface.

Plant growth-promoting rhizobacteria (PGPR) play a crucial role in biological control and pathogenic defense on and within plant tissues, however the mechanisms by which plants associate with PGPR to elicit such beneficial effects need further study. Here, we present time-of-flight secondary ion mass spectrometry (ToF-SIMS) imaging of (Brachypodium) seeds with and without exposure to two model PGPR, , Gram-negative () and Gram-positive A6 (). Delayed image extraction was used to image PGPR-treated seed sections to reveal morphological changes.

Real-Time Characterization of the Fine Structure and Dynamics of an Electrical Double Layer at Electrode-Electrolyte Interfaces.

The chemisorption of an electrolyte species on electrode surfaces is ubiquitous and affects the dynamics and mechanism of various electrochemical reactions. Understanding of the chemical structure and property of the resulting electrical double layer is vital but limited. Herein, we operando probed the electrochemical interface between a gold electrode surface and a common electrolyte, phosphate buffer, using our newly developed in situ liquid secondary ion mass spectrometry.

Molecular Determination of Organic Adsorption Sites on Smectite during Fe Redox Processes Using ToF-SIMS Analysis.

Turnover of soil organic carbon (SOC) is strongly affected by a balance between mineral protection and microbial degradation. However, the mechanisms controlling the heterogeneous and preferential adsorption of different types of SOC remain elusive. In this work, the heterogeneous adsorption of humic substances (HSs) and microbial carbon (MC) on a clay mineral (nontronite NAu-2) during microbial-mediated Fe redox cycling was determined using time-of-flight secondary ion mass spectrometry (ToF-SIMS).

Environment of Metal-O-Fe Bonds Enabling High Activity in CO Reduction on Single Metal Atoms and on Supported Nanoparticles.

Single-atom catalysts are often reported to have catalytic properties that surpass those of nanoparticles, while a direct comparison of sites common and different for both is lacking. Here we show that single atoms of Pt-group metals embedded into the surface of FeO have a greatly enhanced interaction strength with CO compared with the FeO surface. The strong CO adsorption on single Rh atoms and corresponding low activation energies lead to 2 orders of magnitude higher conversion rates of CO compared to Rh nanoparticles.

Anion Exchange of Ruddlesden-Popper Lead Halide Perovskites Produces Stable Lateral Heterostructures.

Heterostructures of three-dimensional (3D) halide perovskites are unstable because of facile anion interdiffusion at halide interfaces. Two-dimensional (2D) Ruddlesden-Popper halide perovskites (RPPs) show suppressed and anisotropic ion diffusion that could enable stable RPP heterostructures, yet the direct and general growth of lateral RPP heterostructures remains challenging. Here, we show that halide miscibility in RPPs decreases with perovskite layer thickness (), enabling the formation of sharp halide lateral heterostructures from = 1 and 2 RP lead iodide microplates via anion exchange with hydrogen bromide vapor.

Molecular Examination of Ion-Pair Competition in Alkaline Aluminate Solutions Using In Situ Liquid SIMS.

Understanding the structure and composition of aluminate complexes in extremely alkaline systems such as Bayer liquors has received enormous attention due to their fundamental and industrial importance. However, obtaining direct molecular information of the underlying ion-ion interactions using traditional approaches such as NMR spectroscopy or Raman spectroscopy is challenging due to the weakness of these interactions and/or their complex overlapping spectral signatures. Here, we exploit in situ liquid secondary-ion mass spectrometry (SIMS) as a new approach and show how it enables new insights.

Onshore soil microbes and endophytes respond differently to geochemical and mineralogical changes in the Aral Sea.

There is limited knowledge about how microbiome develops along the geochemical and mineralogical change in onshore soils derived from continuous desiccation of lakes. In this study, geochemistry and mineralogy were studied in the Aral Sea onshore soils exposed in different periods (from the 1970s to 2018), followed by microbial analyses on the studied soils and the aboveground organs of dominant plants. The soils exhibited an increasing gradient of total soluble salts (TSS: 0.

Three-Dimensional Mass Spectrometric Imaging of Biological Structures Using a Vacuum-Compatible Microfluidic Device.

Three-dimensional (3D) molecular imaging of biological structures is important for a wide range of research. In recent decades, secondary-ion mass spectrometry (SIMS) has been recognized as a powerful technique for both two-dimensional and 3D molecular imaging. Sample fixations (e.

In Vivo Molecular Insights into Syntrophic Aggregates.

Direct interspecies electron transfer (DIET) has been considered as a novel and highly efficient strategy in both natural anaerobic environments and artificial microbial fuel cells. A syntrophic model consisting of and was studied in this work. We conducted in vivo molecular mapping of the outer surface of the syntrophic community as the interface of nutrients and energy exchange.

Role of clay-associated humic substances in catalyzing bioreduction of structural Fe(III) in nontronite by Shewanella putrefaciens CN32.

Previous studies have shown that humic substances can serve as electron shuttle to catalyze bioreduction of structural Fe(III) in clay minerals, but it is unclear if clay-sorbed humic substances can serve the same function. It is unknown if the electron shuttling function is dependent on electron donor type and if humic substances undergo change as a result. In this study, humic acid (HA) and fulvic acid (FA) were sorbed onto nontronite (NAu-2) surface.