Publications by authors named "Dunwei Wang"

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.

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  • - Rechargeable magnesium (Mg) batteries show potential as an alternative to lithium-ion batteries, but a major hurdle is finding effective cathode materials.
  • - The study presents a new cathode design using two-dimensional metal-organic frameworks (2D-MOFs) that incorporates sulfur (S) functionality, providing good Mg storage capacity and excellent cycling performance.
  • - Although the initial Mg insertion causes structural changes, the 2D structure remains intact during charging and discharging, which is crucial for maintaining the high reversibility of the cathode material.
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  • The Baeyer-Villiger oxidation is an important process for converting ketones into esters, typically done with hard-to-handle peroxides.
  • Researchers have developed an electrochemical method that uses water as the oxygen source, overcoming previous low selectivity issues by employing the FeO catalyst to enhance reaction selectivity.
  • By confining the reactions to the catalyst surfaces, unwanted side reactions are minimized, leading to a more efficient and selective nucleophilic oxidation process in electrochemical organic synthesis.
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  • - Molecular Ir catalysts are key for studying water oxidation, crucial for making renewable fuels, and previous research focused primarily on how active species emerge from their precursors.
  • - This study investigates the catalytic cycle of a specific Ir catalyst known as the "blue dimer" using advanced techniques like SEIRAS and PSD to analyze its behavior at an electrode/electrolyte interface.
  • - Findings reveal that two important intermediates, oxo (Ir═O) and superoxo (Ir-OO), can be identified and their relative abundance can be manipulated based on the reaction's thermodynamic conditions.
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Mg-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.

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  • Solar water oxidation is essential for artificial photosynthesis and involves a process that requires four holes and releases four protons.
  • Research indicates that the density of catalysts used affects the reaction rates, particularly in how they interact with surface hole concentrations on photoelectrodes.
  • The study finds that low-density catalysts enhance charge transfer at low photon flux, but can slow down charge recombination at high photon flux, suggesting that optimizing catalyst density is crucial for improving the performance of solar water splitting devices.
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  • * This research compares dinuclear iridium catalysts (Ir-DHC) on two different supports, indium tin oxide (ITO) and cerium oxide (CeO), to isolate the effects of the support on catalytic activity during water oxidation.
  • * Results showed that at higher temperatures (310-323 K), Ir-DHC on ITO performed significantly better than on CeO due to varying abilities of the supports to redistribute holes, emphasizing the support's role in catalytic efficiency.
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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.

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  • Atomically dispersed catalysts, particularly single-atom catalysts, are promising for oxidizing methane to produce valuable compounds like acetic acid and methanol, but they usually have low active site loading, resulting in low product yield.
  • The study introduces a method using metal-organic frameworks with porphyrin linkers to enhance rhodium concentrations, achieving a high loading of 5 wt% with excellent dispersity.
  • When tested for acetic acid production, this new catalyst reached a performance benchmark of 23.62 mmol·g·h and demonstrated sensitivity to light, allowing for different selectivity between acetic acid and methanol based on illumination conditions.
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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.

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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.

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Invited 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.

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As 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.

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Molecular 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.

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  • Oxidative methane carbonylation is a method for creating valuable compounds like acetic acid (CHCOOH) using methane as a starting material.
  • The researchers developed a catalyst using immobilized iridium (Ir) complexes on an oxide support, allowing for efficient methane activation and easy recycling.
  • The study found that the migration of methyl groups, crucial for forming carbon-carbon bonds, is influenced by the oxidation state of the iridium, with Ir(IV) favoring acetic acid production and Ir(III) favoring alcohol production (CHOH).
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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.

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Water 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.

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Multi-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.

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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.

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Redox-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.

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Lithium 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.

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Osteosarcoma 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.

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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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