Ammonia (NH) production in 2023 reached 150 million tons and is associated with potential concomitant production of up to 500 million tons of CO each year. Efforts to produce green NH are compromised since it is difficult to separate using conventional condensation chillers, but in situ separation with minimal cooling is challenging. While metal-organic framework materials offer some potential, they are often unstable and decompose in the presence of caustic and corrosive NH.
View Article and Find Full Text PDFUnderstanding the nature of intermediates/active species in reactions is a major challenge in chemistry. This is because spectator species typically dominate the experimentally derived data and consequently active phase contributions are masked. Transient methods offer a means to bypass this difficulty.
View Article and Find Full Text PDFModifying traditional Co/TiO-based Fischer-Tropsch (FT) catalysts with Mn promoters induces a selectivity shift from long-chain paraffins toward commercially desirable alcohols and olefins. In this work, we use gas cell scanning transmission electron microscopy (STEM) with energy-dispersive X-ray spectroscopy (EDS) elemental mapping, and near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) to demonstrate how the elemental dispersion and chemical structure of the as-calcined materials evolve during the H activation heat treatment required for industrial CoMn/TiO FT catalysts. We find that Mn additions reduce both the mean Co particle diameter and the size distribution but that the Mn remains dispersed on the support after the activation step.
View Article and Find Full Text PDFDecubitus ulcers, also known as bed ulcers or pressure ulcers, result from prolonged pressure on the skin, with contributing factors such as shear forces, friction and excessive moisture. Pressure ulcers have significant physical, social and psychological consequences for patients and impose a substantial financial burden on healthcare providers. Patient and caregiver education has been suggested as a potential approach for preventing pressure ulcers.
View Article and Find Full Text PDFPhotoreforming of lignocellulose biomass is widely recognised as a challenging but key technology for producing value-added chemicals and renewable hydrogen (H ). In this study, H production from photoreforming of organosolv lignin in a neutral aqueous solution was studied over a 0.1 wt % Pt/TiO (P25) catalyst with ultraviolet A (UVA) light.
View Article and Find Full Text PDFConversion of methane (CH) to ethylene (CH) and/or acetylene (CH) enables routes to a wide range of products directly from natural gas. However, high reaction temperatures and pressures are often required to activate and convert CH controllably, and separating C products from unreacted CH can be challenging. Here, we report the direct conversion of CH to CH and CH driven by non-thermal plasma under ambient (25 °C and 1 atm) and flow conditions over a metal-organic framework material, MFM-300(Fe).
View Article and Find Full Text PDFHeterogenisation of homogeneous catalysts onto solid supports represents a potential strategy to make the homogeneous catalytic function recyclable and reuseable. Yet, it is usually the case that immobilised catalysts have much lower catalytic activity than their homogeneous counterpart. In addition, the presence of a solid interface introduces a higher degree of complexity by modulating solid/fluid interactions, which can often influence adsorption properties of solvents and reactive species and, ultimately, catalytic activity.
View Article and Find Full Text PDFFor industrial applications of self-assembled wormlike micelles, measurement and characterization of a micellar material's microstructure and rheology are paramount for the development and deployment of new high-performing and cost-effective formulations. Within this workflow, there are significant bottlenecks associated with experimental delays and a lack of transferability of results from one chemistry to another. In this work, we outline a process to predict microscopic and thermodynamic characteristics of wormlike micelles directly from rheological data by combining a more robust and efficient fitting algorithm with a recently published constitutive model called the Toy Shuffling model [J.
View Article and Find Full Text PDFGlucose is a key intermediate in cellulose photoreforming for H production. This work presents a mechanistic investigation of glucose photoreforming over TiO and Pt/m-TiO catalysts. Analysis of the intermediates formed in the process confirmed the α-scission mechanism of glucose oxidation forming arabinose (C sugar) and formic acid in the initial oxidation step.
View Article and Find Full Text PDFWaste PVC is scarcely recycled due to its high chlorine content and its use in composite materials, which reduces the applicability of conventional waste treatment methods, including thermal, mechanical and chemical recycling. For this reason, alternative treatment options are being developed to increase the recyclability of waste PVC. This paper focuses on one such option which utilises ionic liquids (ILs) for material separation and dehydrochlorination of PVC contained in composite materials.
View Article and Find Full Text PDFObjectives: There is emerging use of artificial intelligence (AI) models to aid diagnostic imaging. This review examined and critically appraised the application of AI models to identify surgical pathology from radiological images of the abdominopelvic cavity, to identify current limitations and inform future research.
Design: Systematic review.
Water scarcity and the consequent increase of freshwater prices are a cause for concern in regions where shale gas is being extracted via hydraulic fracturing. Wastewater treatment methods aimed at reuse/recycle of fracking wastewater can help reduce water stress of the fracking process. Accordingly, this study assessed the catalytic performance and life cycle environmental impacts of cerium-based mixed oxide catalysts for catalytic wet oxidation (CWO) of organic contaminants, in order to investigate their potential as catalysts for fracking wastewater treatment.
View Article and Find Full Text PDFSuperbase ionic liquids (ILs) with a trihexyltetradecylphosphonium cation and a benzimidazolide ([P][Benzim]) or tetrazolide ([P][Tetz]) anion were investigated in a dual-IL system allowing the selective capture and separation of CO and SO, respectively, under realistic gas concentrations. The results show that [P][Tetz] is capable of efficiently capturing SO in preference to CO and thus, in a stepwise separation process, protects [P][Benzim] from the negative effects of the highly acidic contaminant. This results in [P][Benzim] maintaining >53% of its original CO uptake capacity after 30 absorption/desorption cycles in comparison to the 89% decrease observed after 11 cycles when [P][Tetz] was not present.
View Article and Find Full Text PDFCatalytic wastewater treatment has rarely been applied to treat high-ionic-strength wastewater (HISWW) as it contains large amounts of catalyst poisons (e.g., Cl).
View Article and Find Full Text PDFPlasma catalysis is a promising technology for decentralized small-scale ammonia (NH) synthesis under mild conditions using renewable energy, and it shows great potential as an alternative to the conventional Haber-Bosch process. To date, this emerging process still suffers from a low NH yield due to a lack of knowledge in the design of highly efficient catalysts and the in situ plasma-induced reverse reaction (i.e.
View Article and Find Full Text PDFPhotocatalytic reforming of biomass has emerged as an area of significant interest within the last decade. The number of papers published in the literature has been steadily increasing with keywords such as 'hydrogen' and 'visible' becoming prominent research topics. There are likely two primary drivers behind this, the first of which is that biomass represents a more sustainable photocatalytic feedstock for reforming to value-added products and energy.
View Article and Find Full Text PDFACS Sustain Chem Eng
April 2022
Photoreforming of cellulose is a promising route for sustainable H production. Herein, ball-milling (BM, with varied treatment times of 0.5-24 h) was employed to pretreat microcrystalline cellulose (MCC) to improve its activity in photoreforming over a Pt/TiO catalyst.
View Article and Find Full Text PDFSpiky/hollow metal nanoparticles have applications across a broad range of fields. However, the current bottom-up methods for producing spiky/hollow metal nanoparticles rely heavily on the use of strongly adsorbing surfactant molecules, which is undesirable because these passivate the product particles' surfaces. Here we report a high-yield surfactant-free synthesis of spiky hollow Au-Ag nanostars (SHAANs).
View Article and Find Full Text PDFIntroduction: The application of artificial intelligence (AI) technologies as a diagnostic aid in healthcare is increasing. Benefits include applications to improve health systems, such as rapid and accurate interpretation of medical images. This may improve the performance of diagnostic, prognostic and management decisions.
View Article and Find Full Text PDFA superbase ionic liquid (IL), trihexyltetradecylphosphonium benzimidazolide ([P][Benzim]), is investigated for the capture of CO in the presence of NO impurities. The effect of the waste gas stream contaminant on the ability of the IL to absorb simultaneously CO is demonstrated using novel measurement techniques, including a mass spectrometry breakthrough method and infrared spectroscopy. The findings show that the presence of an industrially relevant concentration of NO in a combined feed with CO has the effect of reducing the capacity of the IL to absorb CO efficiently by ∼60% after 10 absorption-desorption cycles.
View Article and Find Full Text PDFMetal-organic framework (MOF) materials provide an excellent platform to fabricate single-atom catalysts due to their structural diversity, intrinsic porosity, and designable functionality. However, the unambiguous identification of atomically dispersed metal sites and the elucidation of their role in catalysis are challenging due to limited methods of characterization and lack of direct structural information. Here, we report a comprehensive investigation of the structure and the role of atomically dispersed copper sites in UiO-66 for the catalytic reduction of NO at ambient temperature.
View Article and Find Full Text PDFA little-studied p-type ternary oxide semiconductor, copper(I) tungstate (CuWO), was assessed by a combined theoretical/experimental approach. A detailed computational study was performed to solve the long-standing debate on the space group of CuWO, which was determined to be triclinic 1. CuWO was synthesized by a time-efficient, arc-melting method, and the crystalline reddish particulate product showed broad-band absorption in the UV-visible spectral region, thermal stability up to ∼260 °C, and cathodic photoelectrochemical activity.
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