In this study, heterostructures based on Bismuth molybdite/iron oxide (BiMoO/FeO) thin films were fabricated by a dip-coating technique using precursor solutions. The heterostructures were deposited on fluorine-doped tin oxide glass substrates. From a detailed characterization using X-ray diffraction and X-ray photoelectron spectroscopy, the formation of the orthorhombic phase for BiMoO and the co-existence of hematite and maghemite in FeO was demonstrated.
View Article and Find Full Text PDFMg-S batteries hold great promise as a potential alternative to Li-based technologies. Their further development hinges on solving a few key challenges, including the lower capacity and poorer cycling performance when compared to Li counterparts. At the heart of the issues is the lack of knowledge on polysulfide chemical behaviors in the Mg-S battery environment.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2023
The use of molecularly modified electrodes in catalysis heralds a new paradigm in designing chemical transformations by allowing control of catalytic activity. Herein, we provide an overview of reported methods to develop electrodes functionalized with organometallic complexes and a summary of commonly used techniques for characterizing the electrode surface after immobilization. In addition, we highlight the implications of surface functionalization in catalysis to emphasize the key aspects that should be considered during the development and optimization of functionalized electrodes.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2023
Direct synthesis of CH COOH from CH and CO is an appealing approach for the utilization of two potent greenhouse gases that are notoriously difficult to activate. In this Communication, we report an integrated route to enable this reaction. Recognizing the thermodynamic stability of CO , our strategy sought to first activate CO to produce CO (through electrochemical CO reduction) and O (through water oxidation), followed by oxidative CH carbonylation catalyzed by Rh single atom catalysts supported on zeolite.
View Article and Find Full Text PDFACS Appl Mater Interfaces
May 2023
Next-generation materials for fast ion conduction have the potential to revolutionize battery technology. Metal-organic frameworks (MOFs) are promising candidates for achieving this goal. Given their structural diversity, the design of efficient MOF-based conductors can be accelerated by a detailed understanding and accurate prediction of ion conductivity.
View Article and Find Full Text PDFInvited for this month's cover is the group of Dunwei Wang from Boston College and Serhiy Cherevko from the Helmholtz Institute Erlangen-Nürnberg for Renewable Energy. The image illustrates the impact of different electrolyte environments on the stability of hematite decorated with an iridium molecular catalyst used for solar water splitting. The Research Article itself is available at 10.
View Article and Find Full Text PDFAs an inedible component of biomass, lignin features rich functional groups that are desired for chemical syntheses. How to effectively depolymerize lignin without compromising the more valuable cellulose and hemicellulose has been a significant challenge. Existing biomass processing procedures either induce extensive condensation in lignin that greatly hinders its chemical utilization or focus on fully depolymerizing lignin to produce monomers that are difficult to separate for subsequent chemical synthesis.
View Article and Find Full Text PDFMolecular catalysts are promising oxygen evolution promoters in conjunction with photoanodes for solar water splitting. Maintaining the stability of both photoabsorber and cocatalyst is still a prime challenge, with many efforts tackling this issue through sophisticated material designs. Such approaches often mask the importance of the electrode-electrolyte interface and overlook easily tunable system parameters, such as the electrolyte environment, to improve efficiency.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2023
Atomically dispersed catalysts have been shown highly active for preferential oxidation of carbon monoxide in the presence of excess hydrogen (PROX). However, their stability has been less than ideal. We show here that the introduction of a structural component to minimize diffusion of the active metal center can greatly improve the stability without compromising the activity.
View Article and Find Full Text PDFWater oxidation is the step limiting the efficiency of electrocatalytic hydrogen production from water. Spectroelectrochemical analyses are employed to make a direct comparison of water oxidation reaction kinetics between a molecular catalyst, the dimeric iridium catalyst [Ir(pyalc)(HO)-(μ-O)] (, pyalc = 2-(2'pyridinyl)-2-propanolate) immobilized on a mesoporous indium tin oxide (ITO) substrate, with that of an heterogeneous electrocatalyst, an amorphous hydrous iridium () film. For both systems, four analogous redox states were detected, with the formation of Ir(4+)-Ir(5+) being the potential-determining step in both cases.
View Article and Find Full Text PDFMulti-elemental alloy (MEA) nanoparticles have recently received notable attention owing to their high activity and superior phase stability. Previous syntheses of MEA nanoparticles mainly used carbon as the support, owing to its high surface area, good electrical conductivity, and tunable defective sites. However, the interfacial stability issue, such as nanoparticle agglomeration, remains outstanding due to poor interfacial binding between MEA and carbon.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2021
Metal-organic frameworks (MOF) are promising media for achieving solid-state Mg conduction and developing a magnesium-based battery. To this end, the chemical behavior and transport properties of an Mg(TFSI)/DME electrolyte system inside Mg-MOF-74 were studied by density functional theory (DFT). We found that inside the MOF chemical environment, solvent and anion molecules occupy the coordinatively unsaturated open metal sites of Mg-MOF-74, while Mg ions adsorb directly onto the carboxylate group of the MOF organic linker.
View Article and Find Full Text PDFRedox-switchable polymerizations of lactide and epoxides were extended to the solid state by anchoring an iron-based polymerization catalyst to TiO nanoparticles. The reactivity of the molecular complexes and their redox-switching characteristics were maintained in the solid-state. These properties resulted in surface-initiated polymerization reactions that produced polymer brushes whose chemical composition is dictated by the oxidation state of the iron-based complex.
View Article and Find Full Text PDFLithium metal anode holds great promises for next-generation battery technologies but is notoriously difficult to work with. The key to solving this challenge is believed to lie in the ability of forming stable solid-electrolyte interphase (SEI) layers. To further address potential safety issues, it is critical to achieve this goal in nonflammable electrolytes.
View Article and Find Full Text PDFOsteosarcoma is a bone tumor frequently diagnosed in children and young adults. Despite advances in chemotherapy and surgical resection, tumors metastasize in 30% of osteosarcoma patients. In addition, side effects caused by chemotherapeutic drugs, as well as the development of chemoresistance, highlight the need to identify the molecular mechanisms involved in the pathogenesis of osteosarcoma.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2021
In this work, we present an in situ method to probe the evolution of photoelectrochemically driven surface oxidation on photoanodes during active operation in aqueous solutions. A standard solution of KFe(CN)-KPi was utilized to benchmark the photocurrent and assess progressive surface oxidation on TaN in various oxidizing solutions. In this manner, a proportional increase in the surface oxygen concentration was detected with respect to oxidation time and further correlated with a continuous decline in the photocurrent.
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