Quantitative Description of Metal Center Organization and Interactions in Single-Atom Catalysts.

Ultra-high-density single-atom catalysts (UHD-SACs) present unique opportunities for harnessing cooperative effects between neighboring metal centers. However, the lack of tools to establish correlations between the density, types, and arrangements of isolated metal atoms and the support surface properties hinders efforts to engineer advanced material architectures. Here, this work precisely describes the metal center organization in various mono- and multimetallic UHD-SACs based on nitrogen-doped carbon (NC) supports by coupling transmission electron microscopy with tailored machine-learning methods (released as a user-friendly web app) and density functional theory simulations.

Development and evaluation of PlasmoPod: A cartridge-based nucleic acid amplification test for rapid malaria diagnosis and surveillance.

Malaria surveillance is hampered by the widespread use of diagnostic tests with low sensitivity. Adequate molecular malaria diagnostics are often only available in centralized laboratories. PlasmoPod is a novel cartridge-based nucleic acid amplification test for rapid, sensitive, and quantitative detection of malaria parasites.

Rapid Electrochemical Flow Analysis of Urinary Creatinine on Paper: Unleashing the Potential of Two-Electrode Detection.

The development of low-cost, disposable electrochemical sensors is an essential step in moving traditionally inaccessible quantitative diagnostic assays toward the point of need. However, a major remaining limitation of current technologies is the reliance on standardized reference electrode materials. Integrating these reference electrodes considerably restricts the choice of the electrode substrate and drastically increases the fabrication costs.

The interface of condensates of the hnRNPA1 low-complexity domain promotes formation of amyloid fibrils.

The maturation of liquid-like protein condensates into amyloid fibrils has been associated with several neurodegenerative diseases. However, the molecular mechanisms underlying this liquid-to-solid transition have remained largely unclear. Here we analyse the amyloid formation mediated by condensation of the low-complexity domain of hnRNPA1, a protein involved in amyotrophic lateral sclerosis.

Rapid droplet-based mixing for single-molecule spectroscopy.

Probing non-equilibrium dynamics with single-molecule spectroscopy is important for dissecting biomolecular mechanisms. However, existing microfluidic rapid-mixing systems for this purpose are incompatible with surface-adhesive biomolecules, exhibit undesirable flow dispersion and are often demanding to fabricate. Here we introduce droplet-based microfluidic mixing for single-molecule spectroscopy to overcome these limitations in a wide range of applications.

Smartphone Imaging Flow Cytometry for High-Throughput Single-Cell Analysis.

We present a portable imaging flow cytometer comprising a smartphone, a small-footprint optical framework, and a PDMS-based microfluidic device. Flow cytometric analysis is performed in a sheathless manner via elasto-inertial focusing with a custom-written Android program, integrating a graphical user interface (GUI) that provides a high degree of user control over image acquisition. The proposed system offers two different operational modes.

Geminal-atom catalysis for cross-coupling.

Single-atom catalysts (SACs) have well-defined active sites, making them of potential interest for organic synthesis. However, the architecture of these mononuclear metal species stabilized on solid supports may not be optimal for catalysing complex molecular transformations owing to restricted spatial environment and electronic quantum states. Here we report a class of heterogeneous geminal-atom catalysts (GACs), which pair single-atom sites in specific coordination and spatial proximity.

Hydrogen Transport and Evolution in Ni-MH Batteries by Neutron Imaging.

Efficiency losses due to side reactions are one of the main challenges in battery development. Despite providing valuable insights, the results of standard analysis on the individual components cannot be simply extrapolated to the full operating system. Therefore, non-destructive, and high resolution approaches that allow the investigation of the full system are desired.

Evidence of bifunctionality of carbons and metal atoms in catalyzed acetylene hydrochlorination.

Carbon supports are ubiquitous components of heterogeneous catalysts for acetylene hydrochlorination to vinyl chloride, from commercial mercury-based systems to more sustainable metal single-atom alternatives. Their potential co-catalytic role has long been postulated but never unequivocally demonstrated. Herein, we evidence the bifunctionality of carbons and metal sites in the acetylene hydrochlorination catalytic cycle.

A re-evaluation of the role of coumarin C460 as a fluorescent Pd(II) sensor.

In 2018, Ashwin and co-workers presented a method for the selective and sensitive detection of Pd based on variations in the fluorescence of coumarin (C460). Herein, we re-evaluate the ability of C460 to probe Pd concentration via a systematic reproduction of the experiments reported in the original publication and the performance of additional control experiments. Our analysis indicates that C460 is in fact not a fluorescence sensor for Pd, but rather can act as a pH sensor over a restricted pH range.

Economic and Environmental Competitiveness of Ethane-Based Technologies for Vinyl Chloride Synthesis.

The synthesis of the vinyl chloride monomer (VCM), employed to manufacture poly(vinyl chloride) (PVC) plastic, primarily relies on oil-derived ethylene, resulting in high costs and carbon footprint. Natural gas-derived ethane in VCM synthesis has long been considered a transformative feedstock to lower emissions and expenses. In this work, we evaluate the environmental potential and economics of recently developed catalytic ethane chlorination technologies for VCM synthesis.

Indoor Self-Powered Perovskite Optoelectronics with Ultraflexible Monochromatic Light Source.

Self-powered skin optoelectronics fabricated on ultrathin polymer films is emerging as one of the most promising components for the next-generation Internet of Things (IoT) technology. However, a longstanding challenge is the device underperformance owing to the low process temperature of polymer substrates. In addition, broadband electroluminescence (EL) based on organic or polymer semiconductors inevitably suffers from periodic spectral distortion due to Fabry-Pérot (FP) interference upon substrate bending, preventing advanced applications.

Integrative modeling of hemodynamic changes and perfusion impairment in coronary microvascular disease.

Coronary microvascular disease is one of the responsible factors for cardiac perfusion impairment. Due to diagnostic and treatment challenges, this pathology (characterized by alterations to microvasculature local hemodynamics) represents a significant yet unsolved clinical problem. Due to the poor understanding of the onset and progression of this disease, we propose a new and noninvasive strategy to quantify hemodynamic changes occurring in the microvasculature.

α-Synuclein Aggregation Is Triggered by Oligomeric Amyloid-β 42 via Heterogeneous Primary Nucleation.

An increasing number of cases where amyloids of different proteins are found in the same patient are being reported. This observation complicates diagnosis and clinical intervention. Amyloids of the amyloid-β peptide or the protein α-synuclein are traditionally considered hallmarks of Alzheimer's and Parkinson's diseases, respectively.

Single-cell transcriptional uncertainty landscape of cell differentiation.

Single-cell studies have demonstrated the presence of significant cell-to-cell heterogeneity in gene expression. Whether such heterogeneity is only a bystander or has a functional role in the cell differentiation process is still hotly debated. In this study, we quantified and followed single-cell transcriptional uncertainty - a measure of gene transcriptional stochasticity in single cells - in 10 cell differentiation systems of varying cell lineage progressions, from single to multi-branching trajectories, using the stochastic two-state gene transcription model.

An image-guided microfluidic system for single-cell lineage tracking.

Cell lineage tracking is a long-standing and unresolved problem in biology. Microfluidic technologies have the potential to address this problem, by virtue of their ability to manipulate and process single-cells in a rapid, controllable and efficient manner. Indeed, when coupled with traditional imaging approaches, microfluidic systems allow the experimentalist to follow single-cell divisions over time.

Tuning the zeolite acidity enables selectivity control by suppressing ketene formation in lignin catalytic pyrolysis.

Unveiling catalytic mechanisms at a molecular level aids rational catalyst design and selectivity control for process optimization. In this study, we find that the Brønsted acid site density of the zeolite catalyst efficiently controls the guaiacol catalytic pyrolysis mechanism. Guaiacol demethylation to catechol initiates the reaction, as evidenced by the detected methyl radicals.

Improving time-resolution and sensitivity of X-ray photoelectron spectroscopy of a powder catalyst by modulated excitation.

Ambient pressure X-ray photoelectron spectroscopy (APXPS) is a powerful tool to characterize the surface structure of heterogeneous catalysts . In order to improve the time resolution and the signal-to-noise (S/N) ratio of photoemission spectra, we collected consecutive APXP spectra during the periodic perturbation of a powder Pd/AlO catalyst away from its equilibrium state according to the modulated excitation approach (ME). Averaging of the spectra along the alternate pulses of O and CO improved the S/N ratio demonstrating that the time resolution of the measurement can be limited solely to the acquisition time of one spectrum.

Microalgae Biofuel for a Heavy-Duty Transport Sector within Planetary Boundaries.

In this contribution, we study the extent to which 68 scenarios for microalgae biofuels could help the heavy-duty transport sector operate within planetary boundaries. The proposed scenarios are built considering a range of alternative configurations based on three types of fuel production processes (i.e.

Methane Oxidation over Cu /[CuOH] Pairs and Site-Specific Kinetics in Copper Mordenite Revealed by Operando Electron Paramagnetic Resonance and UV/Visible Spectroscopy.

Cu-exchanged mordenite (MOR) is a promising material for partial CH oxidation. The structural diversity of Cu species within MOR makes it difficult to identify the active Cu sites and to determine their redox and kinetic properties. In this study, the Cu speciation in Cu-MOR materials with different Cu loadings has been determined using operando electron paramagnetic resonance (EPR) and operando ultraviolet-visible (UV/Vis) spectroscopy as well as in situ photoluminescence (PL) and Fourier-transform infrared (FTIR) spectroscopy.

Dynamical Equilibrium between Brønsted and Lewis Sites in Zeolites: Framework-Associated Octahedral Aluminum.

While the structures of Brønsted acid sites (BAS) in zeolites are well understood, those of Lewis acid sites (LAS) remain an active area of investigation. Under hydrated conditions, the reversible formation of framework-associated octahedral aluminum has been observed in zeolites in the acidic form. However, the structure and formation mechanisms are currently unknown.

Paper-Based Laser-Pyrolyzed Electrofluidics: An Electrochemical Platform for Capillary-Driven Diagnostic Bioassays.

Microfluidic paper-based analytical devices (µPADs) are indispensable tools for disease diagnostics. The integration of electronic components into µPADs enables new device functionalities and facilitates the development of complex quantitative assays. Unfortunately, current electrode fabrication methods often hinder capillary flow, considerably restricting µPAD design architectures.

exRNA-eCLIP intersection analysis reveals a map of extracellular RNA binding proteins and associated RNAs across major human biofluids and carriers.

Although the role of RNA binding proteins (RBPs) in extracellular RNA (exRNA) biology is well established, their exRNA cargo and distribution across biofluids are largely unknown. To address this gap, we extend the exRNA Atlas resource by mapping exRNAs carried by extracellular RBPs (exRBPs). This map was developed through an integrative analysis of ENCODE enhanced crosslinking and immunoprecipitation (eCLIP) data (150 RBPs) and human exRNA profiles (6,930 samples).

Low-carbon diets can reduce global ecological and health costs.

Potential external cost savings associated with the reduction of animal-sourced foods remain poorly understood. Here we combine life cycle assessment principles and monetarization factors to estimate the monetary worth of damage to human health and ecosystems caused by the environmental impacts of food production. We find that, globally, approximately US$2 of production-related external costs were embedded in every dollar of food expenditure in 2018-corresponding to US$14.

Global Sensitivity Analysis in Life-Cycle Assessment of Early-Stage Technology using Detailed Process Simulation: Application to Dialkylimidazolium Ionic Liquid Production.

The ability to assess the environmental performance of early-stage technologies at production scale is critical for sustainable process development. This paper presents a systematic methodology for uncertainty quantification in life-cycle assessment (LCA) of such technologies using global sensitivity analysis (GSA) coupled with a detailed process simulator and LCA database. This methodology accounts for uncertainty in both the background and foreground life-cycle inventories, and is enabled by lumping multiple background flows, either downstream or upstream of the foreground processes, in order to reduce the number of factors in the sensitivity analysis.