Publications by authors named "Tewodros Asefa"

Bis-porphyrin nanocages (MBiCage, M = FeCl, Co, Zn) and their host-guest complexes with C and C were used to examine how molecular porosity and interactions with carbon nanomaterials affect the CO reduction activity of metalloporphyrin electrocatalysts. The cages were found to adsorb on carbon black to provide electrocatalytic inks with excellent accessibilities of the metal sites (≈50%) even at high metal loadings (2500 nmol cm), enabling good activity for reducing CO to CO. A complex of C bound inside (FeCl)BiCage achieves high current densities for CO formation at low overpotentials (|j| >7 mA cm, η = 320 mV; >13.

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Developing highly efficient, cost-effective, and robust electrocatalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is paramount for the large-scale commercialization of renewable fuel cells and rechargeable metal-air batteries. Herein, a new ternary-atom catalyst that is composed of paired Fe sites and single Ni sites (as Fe-N and Ni-N) coordinated onto hollow nitrogen-doped carbon microspheres is developed. The as-synthesized catalyst exhibits remarkable activities toward both the ORR and OER in alkaline media, with superior performances to those of the control materials that contain only Fe-N or Ni-N sites.

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Nanostructured materials continue to find applications in various electronic and sensing devices, chromatography, separations, drug delivery, renewable energy, and catalysis. While major advancements on the synthesis and characterization of these materials have already been made, getting information about their structures at sub-nanometer resolution remains challenging. It is also unfortunate to find that many emerging or already available powerful analytical methods take time to be fully adopted for characterization of various nanomaterials.

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Non-free radical photocatalysis with metal oxide catalysts is an important advanced oxidation process that enables the removal of various emerging environmental pollutants, such as tetracycline. Here, four hexagonal LaO photocatalysts with different densities of oxygen vacancy and crystalline features are synthesized and then further treated by ball milling. Ball milling of these LaO photocatalysts is found to increase the amount of oxygen vacancies on their surfaces and thereby the amount of O species produced by them.

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Chlorhexidine dodecyl sulfate (CHX-DS) was synthesized and characterized single-crystal X-ray diffraction (SC-XRD), H nuclear magnetic resonance (NMR) spectroscopy, H nuclear Overhauser effect spectroscopy (NOESY), and attenuated total reflectance Fourier-transform infrared spectroscopy (ATR-FTIR). The solid-state structure, comprising a 1 : 2 stoichiometric ratio of chlorhexidine cations [CHClN] to dodecyl sulfate anions [CHSO], is the first report of chlorhexidine isolated with a surfactant. CHX-DS exhibits broad-spectrum antibacterial activity and demonstrates superior efficacy for reducing bacteria-generated volatile sulfur compounds (VSCs) as compared to chlorhexidine gluconate (CHG).

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Controlling the ratio of metals in bimetallic organic frameworks (MOFs) can not only alter the structures but also tailor the properties of MOFs. Herein, we report a series of electrocatalytically active CoNi-based bimetallic MOFs that are synthesized with the 3,5-pyridinedicarboxylic acid (3,5-Hpdc) ligand (where  :  = 20 : 1, 15 : 1, 10 : 1, 5 : 1, 1 : 1, and 1 : 20) and a facile, scalable, low temperature synthetic route. The materials have one-dimensional (1D), rod-like microstructures with different aspect ratios.

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Environmental pollution remains one of the most challenging problems facing society worldwide. Much of the problem has been caused by human activities and increased usage of various useful chemical agents that inadvertently find their way into the environment. Triclosan (TCS) and related phenolic compounds and derivatives belong to one class of such chemical agents.

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Article Synopsis
  • Developing efficient, noble metal-free electrocatalysts for the oxygen reduction reaction (ORR) is a significant challenge in renewable energy systems.
  • A newly synthesized catalyst made of N-doped mesoporous carbon with 4.05 wt% single iron atoms shows high electrocatalytic activity in both acidic and alkaline environments, rivaling platinum-based catalysts.
  • The catalyst demonstrates durability, effective methanol tolerance, and powers fuel cells and batteries with impressive maximum power densities of 320 and 91 mW cm², attributed to its unique Fe-N atomic structure.
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The development of materials that can more efficiently administer antimicrobial agents in a controlled manner is urgently needed due to the rise in microbial resistance to traditional antibiotics. While new classes of antibiotics are developed and put into widespread usage, existing, inexpensive compounds can be repurposed to fight bacterial infections. Here, we present the synthesis of amine-functionalized SBA-15 mesoporous silica nanomaterials with physisorbed rafoxanide (RFX), a commonly used salicylanilide anthelmintic, and anchored Cu(II) ions that exhibit enhanced antimicrobial efficacy against the pathogenic bacterium .

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The development of durable and efficient electrocatalysts composed of low-cost, earth-abundant metals for the oxygen evolution reaction (OER) is crucial for industrial-scale water splitting to produce green hydrogen on a large scale. Transition metal borates are considered good candidate electrocatalysts for OER due to their low cost, ease of synthesis, and good catalytic activity. In this work, we demonstrate that the incorporation of an oxophilic main group metal, bismuth (Bi), into cobalt borates produces highly effective electrocatalysts for OER.

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A hierarchically ordered porous carbon electrocatalyst with exclusively surface-anchored cobalt species, dubbed Co@HOPC, is synthesized from polyaniline and cobalt-functionalized silica microparticles templates, and its high electrocatalytic activity for the oxygen evolution reaction (OER) is demonstrated. The material requires a small potential (320 mV) to drive the reaction with a current density of 10 mA cm and a small Tafel slope of 31.2 mV dec .

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Conductive polymer hydrogels have large surface areas and electrical conductivities. Their properties can be further tailored by functionalizing them with metals and nonmetals. However, the potential applications of metal-functionalized hydrogels for electrocatalysis have rarely been investigated.

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Cetylpyridinium trichlorostannate (CPC-Sn), comprising cetylpyridinium chloride (CPC) and stannous chloride, was synthesized and characterized via single-crystal X-ray diffraction measurements indicating stoichiometry of CHNSnCl where the molecules are arranged in a 1:1 ratio with a cetylpyridinium cation and a [SnCl] anion. CPC-Sn has shown potential for application as a broad-spectrum antimicrobial agent, to reduce bacteria-generated volatile sulfur compounds and to produce advanced functional materials. In order to investigate its controlled-release properties, electrical resistance tomography was implemented.

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The production of hydrogen via electrochemical water splitting has the potential to enable the utilization of hydrogen-powered fuel cells on a large scale. However, to realize this technology, inexpensive, noble metal-free electrocatalysts possessing high performances for the hydrogen evolution reaction (HER) are needed. Mo C nanoparticles recently receive much attention as alternative noble metal-free electrocatalysts because their electronic structures are akin to that of Pt.

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Bacterial infections are nowadays among the major threats to public health worldwide. Thus, there is an urgent and increased need for new antimicrobial agents. As a result, the exploration of the antimicrobial properties of different substances including ionic liquids (ILs) has recently attracted great attention.

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Article Synopsis
  • The study discusses a new material made from a 1:2 ratio of chlorhexidine and N-cyclohexylsulfamate (cyclamate), detailing its synthesis, crystal structure, and antimicrobial properties.
  • The combination of various advanced techniques, including X-ray diffraction and mass spectrometry, confirms its unique chemical structure and demonstrates its efficacy.
  • This material not only shows significant antimicrobial activity at low concentrations but also potentially enhances the taste of chlorhexidine by using cyclamate instead of inactive gluconate.
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The growing energy demand worldwide has led to increased use of fossil fuels. This, in turn, is making fossil fuels dwindle faster and cause more negative environmental impacts. Thus, alternative, environmentally friendly energy sources such as fuel cells and electrolyzers are being developed.

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Single-atom catalysts (SACs) have aroused great attention due to their high atom efficiency and unprecedented catalytic properties. A remaining challenge is to anchor the single atoms individually on support materials via strong interactions. Herein, single atom Co sites have been developed on functionalized graphene by taking advantage of the strong interaction between Co ions and the nitrile group of cyanographene.

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Developing efficient, inexpensive, and durable electrocatalysts for the oxygen reduction reaction (ORR) is important for the large-scale commercialization of fuel cells and metal-air batteries. Herein, a hierarchically porous bimetallic Fe/Co single-atom-coordinated N-doped carbon (Fe/Co-N -C) electrocatalyst for ORR is synthesized from Fe/Co-coordinated polyporphyrin using silica template-assisted and silica-protection synthetic strategies. In the synthesis, first silica nanoparticles-embedded, silica-protected Fe/Co-polyporphyrin is prepared.

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Article Synopsis
  • Electrocatalysis is crucial for sustainable energy technologies, helping to decrease reliance on fossil fuels through advancements in diverse electrochemical reactions.
  • Recent studies focus on porous electrocatalysts for key reactions like hydrogen evolution, oxygen reduction, CO reduction, nitrogen reduction, and oxygen evolution, emphasizing their benefits for optimizing active sites.
  • The review covers current knowledge, challenges, and future directions for research on porous electrocatalysts, including strategies for synthesis and performance testing.
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Reducing the amount of iridium in oxygen evolution electrocatalysts without compromising their catalytic performances is one of the major requirements in proton-exchange-membrane water electrolyzers. Herein, with the help of theoretical studies, we show that anatase-type TiO -IrO solid solutions possess more active iridium catalytic sites for the oxygen evolution reaction (OER) than IrO , the benchmark OER catalyst. Note that the same is not observed for their rutile-type counterparts.

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A mesoporous TiO material comprised of small, crystalline, vacancy-rich anatase nanoparticles (NPs) shows unique optical, thermal, and electronic properties. It is synthesized using polymer-derived mesoporous carbon (PDMC) as a template. The PDMC pores serve as physical barriers during the condensation and pyrolysis of a titania precursor, preventing the titania NPs from growing beyond 10 nm in size.

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Article Synopsis
  • Cetylpyridinium tetrachlorozincate ((CP)ZnCl) was synthesized and its structure analyzed through single-crystal X-ray diffraction, revealing a unique arrangement with two cetylpyridinium cations for every zinc chloride tetrahedron.
  • The crystal structures showed a zig-zag pattern at different temperatures and indicated that the compound might be used as a broad-spectrum antimicrobial to reduce sulfur compounds produced by bacteria and for creating advanced materials.
  • The minimum inhibitory concentration (MIC) of (CP)ZnCl against specific bacteria was determined to be 60, 6, and 6 μg/mL, demonstrating effectiveness similar to pure cetylpyridinium chloride, even though it contains a portion
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The surface functionalization of nanoporous silica materials with chemical agents opens up numerous possibilities, including improvement in the materials' ability to carry high payloads of drugs. In this study, KCC-1 nanofibrous silica microparticles are functionalized with methyl groups and then combined with poly(vinyl alcohol) (PVA) and poly(acrylic acid) (PAA) to produce hybrid aerogels that can deliver a poorly water-soluble anticancer drug. The synthetic steps involve freeze-drying a polymer solution of PVA and PAA that contains methyl-modified KCC-1 microparticles and then cross-linking the two polymers via a solid-state reaction.

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Cyclohexane can serve as a good dihydrogen (H) carrier and a safer medium to store and transport H, as it is liquid under ambient conditions and it has a relatively high hydrogen density per unit volume (0.056 g(H)/cm(Cy)). However, cyclohexane can release H only with efficient cyclohexane dehydrogenation catalysts.

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