Rational design of a methanation reactor by neutron imaging.

The reaction conditions in industrial scale chemical reactors can differ markedly from the ones in a small laboratory scale reactor. The differences are both conceptual and practical, and can at best be analysed by studying a full reactor, which requires an analytical method capable of quantifying the distribution of reactants and products in a running reactor. For this, we introduce non-destructive neutron imaging in combination with modelling.

Direct nanopatterning of complex 3D surfaces and self-aligned superlattices via molecular-beam holographic lithography.

Conventional lithography methods involving pattern transfer through resist templating face challenges of material compatibility with various process solvents. Other approaches of direct material writing often compromise pattern complexity and overlay accuracy. Here we explore a concept based on the Moiré interference of molecular beams to directly pattern complex three-dimensional (3D) surfaces made by any evaporable materials, such as metals, oxides and organic semiconductors.

Efficient Blade-Coated Wide-Bandgap Perovskite Solar Cells via Interface Engineering.

Most high-efficiency all-perovskite tandem solar cells use a "superstrate" configuration, integrating a wide-bandgap (WBG) top subcell and a narrow bandgap (NBG) bottom subcell. However, this structure suffers oxidative degradation due to easily air-exposable bottom NBG subcells. A "substrate" structure offers improved stability for tandems by encapsulating the NBG top subcell with the air-stable WBG bottom subcell.

Machine learning and statistical classification in CRISPR-Cas12a diagnostic assays.

CRISPR-based diagnostics have gained increasing attention as biosensing tools able to address limitations in contemporary molecular diagnostic tests. To maximize the performance of CRISPR-based assays, much effort has focused on optimizing the chemistry and biology of the biosensing reaction. However, less attention has been paid to improving the techniques used to analyze CRISPR-based diagnostic data.

Adding a Twist to Lateral Flow Immunoassays: A Direct Replacement of Antibodies with Helical Affibodies, from Selection to Application.

Immunoreagents, most commonly antibodies, are integral components of lateral flow immunoassays. However, the use of antibodies comes with limitations, particularly relating to their reproducible production, and poor thermal and chemical stability. Here, we employ phage display to develop affibodies, a class of nonimmunoglobulin affinity proteins based on a small three-helix bundle scaffold, against SARS-CoV-2 Spike protein.

Microfluidic mimicry of the Golgi-linked -glycosylation machinery.

The complexity of the eukaryotic glycosylation machinery hinders the development of cell-free protein glycosylation since methods struggle to simulate the natural environment of the glycosylation machinery. Microfluidic technologies have the potential to address this limitation due to their ability to control glycosylation parameters, such as enzyme/substrate concentrations and fluxes, in a rapid and precise manner. However, due to the complexity and sensitivity of the numerous components of the glycosylation machinery, very few "glycobiology-on-a-chip" systems have been proposed or reported in the literature.

Tracking Dynamics of Supported Indium Oxide Catalysts in CO Hydrogenation to Methanol by In Situ TEM.

Supported reducible oxides, such as indium oxide on monoclinic zirconia (InO/m-ZrO), are promising catalysts for green methanol synthesis via CO hydrogenation. Growing evidence suggests that dynamic restructuring under reaction conditions plays a crucial but poorly understood role in catalytic performance. To address this, the direct visualization of the state-of-the-art InO/m-ZrO catalyst under CO hydrogenation conditions (T  =  553 K, P  =  1.

Onboard Carbon Capture for Circular Marine Fuels.

The transition to low- and zero-carbon fuels is the primary driver for reducing emissions in the maritime industry, with methanol and natural gas emerging as the most promising options. However, carbon-based fuels will continue to emit considerable amounts of pollutants during their use phase. This work explores the application of circular economy principles in the shipping industry by integrating carbon capture and utilization technologies.

On Paper Diagnostics: A Brief History and Future Perspectives.

For centuries, diagnostic technologies have played a key role in medicine. Effective diagnostics can help clinicians identify the presence and extent of disease in their patients, as well as their general health. Precipitated by advances in biochemistry, chemistry, and engineering, the 20th and 21st centuries have witnessed rapid advancement in diagnostic technologies.

Tracking Active Site Formation during Oxidative Activation of Copper-Exchanged Zeolites for Methane-to-Methanol Conversion.

The evolution of active sites in Cu-zeolites for the CH-to-CHOH conversion has been investigated during oxidative treatment in O. Three samples with different frameworks but comparable Cu loadings and Si/Al ratios have been prepared to assess the influence of topology on material oxidizability and the nature of the generated Cu(II) species. Complementary spectroscopic studies highlight that isomeric Cu(II) centers hosted within different topologies are characterized by distinct formation rates.

Sustainable Development Goals-Based Prospective Process Design Using Hybrid Modeling.

Replacing fossil technologies with renewable carbon-based technologies is of vital importance for the development of sustainable chemical processes in the future. However, impacts beyond climate change should be carefully evaluated to ensure that this transition to defossilized chemicals is truly sustainable. Here, we develop a framework for sustainable process design that explicitly accounts for the performance attained in the Sustainable Development Goals (SDGs), which is computed using standard life cycle assessment (LCA) metrics alongside the planetary boundaries (PBs) concept.

Multi-Objective Optimization of a Hybrid Fossil/Renewable Carbon Methanol Cluster.

Replacing fossil carbon- with renewable carbon-based technologies is imperative for transitioning to sustainable chemical production. However, most production pathways based on renewable carbon are currently economically unappealing. Here, we show that hybrid clusters exploiting synergies between different fossil and renewable carbon-based processes in terms of heat, mass, and power integration could make defossilized chemical technologies more competitive.

Win-Win More Sustainable Routes for Acetic Acid Synthesis.

Current efforts to decarbonize the chemical sector by using captured CO and electrolytic H typically lead to high production costs and environmental collateral damage. Hence, there is a clear need to look for alternative, more efficient synthesis routes that could pave the way for a fully sustainable chemical industry. Bearing this in mind, here, we evaluate the economic and environmental implications of two low technology readiness level (TRL) novel single-step synthesis routes for acetic acid production using CO as a raw material: gas-to-acid methane carboxylation and semiartificial photosynthesis.

Environmental impacts of restructuring the EU's natural gas supply and consumption: Learnings from the 2022 energy crisis.

In 2022, the European Union put forward the REPowerEU plan in response to Russia's invasion of Ukraine, aiming at enhancing short-term energy security by diversifying imports and reducing natural gas demand while accelerating the deployment of renewable alternatives in the long term. Here, we quantify the life cycle environmental impacts of both REPowerEU's short-term measures, including the controversial extended coal-fired power plant operations, and how the first year of the crisis was managed in practice. We find that the policy measures' impact on greenhouse gas (GHG) emissions would be negligible, although they could have detrimental effects on other environmental categories.

C-Based Route for Vinyl Chloride Synthesis with Environmental and Economic Benefits.

Selective coupling of C platform molecules to C olefins is a cornerstone for establishing a sustainable chemical industry based on nonpetroleum sources. Vinyl chloride (CHCl), one of the top commodity petrochemicals, is commercially produced from coal- or oil-derived C hydrocarbon (acetylene and ethylene) feedstocks with a high carbon footprint. Here, we report a C-based route for vinyl chloride synthesis via the selective oxidative coupling of methyl chloride.

Influence of zinc oxide nanoparticles on the carbon accumulation on silver exposed to carbon dioxide hydrogenation reaction conditions.

The strong influence of surface adsorbates on the morphology of a catalyst is exemplified by studying a silver surface with and without deposited zinc oxide nanoparticles upon exposure to reaction gases used for carbon dioxide hydrogenation. Ambient pressure X-ray photoelectron spectroscopy and scanning tunneling microscopy measurements indicate accumulation of carbon deposits on the catalyst surface at 200 °C. While oxygen-free carbon species observed on pure silver show a strong interaction and decorate the atomic steps on the catalyst surface, this decoration is not observed for the oxygen-containing species observed on the silver surface with additional zinc oxide nanoparticles.

Ligand-Induced Activation of Single-Atom Palladium Heterogeneous Catalysts for Cross-Coupling Reactions.

Single-atom heterogeneous catalysts (SACs) are potential, recoverable alternatives to soluble organometallic complexes for cross-coupling reactions in fine-chemical synthesis. When developing SACs for these applications, it is often expected that the need for ligands, which are essential for organometallic catalysts, can be bypassed. Contrary to that, ligands remain almost always required for palladium atoms stabilized on commonly used functionalized carbon and carbon nitride supports, as the catalysts otherwise show limited activity.

PULPO: A framework for efficient integration of life cycle inventory models into life cycle product optimization.

This work presents the PULPO (ython-based ser-defined ifecycle roduct ptimization) framework, developed to efficiently integrate life cycle inventory (LCI) models into life cycle product optimization. Life cycle optimization (LCO), which has found interest in both the process systems engineering and life cycle assessment (LCA) communities, leverages LCA data to go beyond simple assessments of a limited number of alternatives and identify the best possible product systems configuration subject to a manifold of choices, constraints, and objectives. However, typically, aggregated inventories are used to build the optimization problems.

Microfluidics-Driven Manufacturing and Multiscale Analytical Characterization of Nanoparticle-Vesicle Hybrids.

Coating synthetic nanoparticles (NPs) with lipid membranes is a promising approach to enhance the performance of nanomaterials in various biological applications, including therapeutic delivery to target organs. Current methods for achieving this coating often rely on bulk approaches which can result in low efficiency and poor reproducibility. Continuous processes coupled with quality control represent an attractive strategy to manufacture products with consistent attributes and high yields.

Reaction Intermediates Involved in the Epoxidation of Ethylene Over Silver Revealed by In Situ Photoelectron Spectroscopy.

Ethylene oxide (EO) is a crucial building block in the chemical industry, and its production via ethylene epoxidation (EPO) is a pivotal process. Silver-based catalysts are known for their high selectivity and are currently largely used in the industrial process. Extensive research over the past 20 years has assumed the oxametallacycle (OMC) as a reaction intermediate, implying that ethylene reacts with adsorbed oxygen on the surface of silver.

Strategies for Controlling Emission Anisotropy in Lead Halide Perovskite Emitters for LED Outcoupling Enhancement.

In the last decade, momentous progress in lead halide perovskite (LHP) light-emitting diodes (LEDs) is witnessed as their external quantum efficiency (η) has increased from 0.1 to more than 30%. Indeed, perovskite LEDs (PeLEDs), which can in principle reach 100% internal quantum efficiency as they are not limited by the spin-statistics, are reaching their full potential and approaching the theoretical limit in terms of device efficiency.

Evidence of Preferential Aluminum Site Loss during Reaction-Induced Dealumination.

Understanding the mechanism of steam-induced dealumination of zeolite catalysts is of high relevance for tuning their performance and stability in multiple industrial processes. A combination of Al and H-H double-quantum single-quantum magic angle spinning nuclear magnetic resonance and diffuse-reflectance ultraviolet-visible spectroscopies identified a preferential dealumination of tetrahedral aluminum sites in H-ZSM-5 zeolites. Framework aluminum atoms facing channels display reactivity toward steam higher than that of those in their intersections.

Mitigation Strategies against Antibody Aggregation Induced by Oleic Acid in Liquid Formulations.

Polysorbates 20 and 80 (PS20 and PS80) are commonly used in the formulations of biologics to protect against interfacial stresses. However, these surfactants can degrade over time, releasing free fatty acids, which assemble into solid particles or liquid droplets. Here, we apply a droplet microfluidic platform to analyze the interactions between antibodies and oleic acid, the primary free fatty acid resulting from the hydrolysis of PS80.