In the Fenton-like reaction, revealing the dynamic evolution of the active sites is crucial to achieve the activity improvement and stability of the catalyst. This study reports a perovskite oxide in which atomic (Co) in situ embedded exsolution occurs during the high-temperature phase transition. This unique anchoring strategy significantly improves the Co/Co cycling efficiency at the interface and inhibits metal leaching during peroxymonosulfate (PMS) activation.
View Article and Find Full Text PDFOngoing research to develop advanced electrocatalysts for the oxygen evolution reaction (OER) is needed to address demand for efficient energy conversion and carbon-free energy sources. In the OER process, acidic electrolytes have higher proton concentration and faster response than alkaline ones, but their harsh strongly acidic environment requires catalysts with greater corrosion and oxidation resistance. At present, iridium oxide (IrO) with its strong stability and excellent catalytic performance is the catalyst of choice for the anode side of commercial PEM electrolysis cells.
View Article and Find Full Text PDFTransition metal oxides are promising electrocatalysts for zinc-air batteries, yet surface reconstruction caused by the adsorbate evolution mechanism, which induces zinc-ion battery behavior in the oxygen evolution reaction, leads to poor cycling performance. In this study, we propose a lattice oxygen mechanism involving proton acceptors to overcome the poor performance of the battery in the OER process. We introduce a stable solid base, hydroxy BaCaSiO, onto the surfaces of PrBaCaCoO perovskite nanofibers with a one-step exsolution strategy.
View Article and Find Full Text PDFACS Appl Mater Interfaces
May 2023
Rapid and full recovery is the major challenge for the commercialization and further growth of textile-based wearable supercapacitors. Herein, reversibly stretchable and rapidly reboundable textile supercapacitors (TSCs) are developed via the utilization of NiCuSe/Cu-Ni alloy-plated cotton cloth (CNAPCC) textile as the cathode and FeCuSe/CNAPCC textile as the anode. Both NiCuSe/CNAPCC and FeCuSe/CNAPCC are obtained by a simple in situ oxidation reaction, followed by an ion exchange strategy.
View Article and Find Full Text PDFElectrochemical reduction of CO into high energy density multi-carbon chemicals or fuels (e. g., ethylene) via new renewable energy storage has extraordinary implications for carbon neutrality.
View Article and Find Full Text PDFThe oxygen reduction reaction is essential for fuel cells and metal-air batteries in renewable energy technologies. Developing platinum-group-metal (PGM)-free catalysts with comparable catalytic performance is highly desired for cost efficiency. Here, we report a tin (Sn) nanocluster confined catalyst for the electrochemical oxygen reduction.
View Article and Find Full Text PDFSearching for bifunctional noble-free electrocatalysts with high activity and stability are urgently demanded for the commercial application of zinc-air batteries (ZABs). Herein, the authors propose a controllable dual interface engineering concept to design a noble-metal-free bifunctional catalyst with two well-designed interfaces (Ni FeN|MnO and MnO|CNTs) via a simple etching and wet chemical route. The heterointerface between MnO and Ni FeN facilitates the charge transfer rate during surface reaction, and heterointerface between MnO and carbon nanotubes (CNTs) support provides effective electron transfer path, while the CNTs matrix builds free diffusion channels for gas and electrolyte.
View Article and Find Full Text PDFHydrogen peroxide (H O ) is an environment-friendly and efficient oxidant with a wide range of applications in different industries. Recently, the production of hydrogen peroxide through direct electrosynthesis has attracted widespread research attention, and has emerged as the most promising method to replace the traditional energy-intensive multi-step anthraquinone process. In ongoing efforts to achieve highly efficient large-scale electrosynthesis of H O , carbon-based materials have been developed as 2e oxygen reduction reaction catalysts, with the benefits of low cost, abundant availability, and optimal performance.
View Article and Find Full Text PDFACS Appl Mater Interfaces
June 2021
Low-cost transition-metal oxide is regarded as a promising electrocatalyst family for an oxygen evolution reaction (OER). The classic design principle for an oxide electrocatalyst believes that point defect engineering, such as oxygen vacancies (V) or heteroatom doping, offers the opportunities to manipulate the electronic structure of material toward optimal OER activity. Oppositely, in this work, we discover a counterintuitive phenomenon that both V and an aliovalent dopant (i.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2020
Single atom catalysts (SACs) are of great importance for oxygen reduction, a critical process in renewable energy technologies. The catalytic performance of SACs largely depends on the structure of their active sites, but explorations of highly active structures for SAC active sites are still limited. Herein, we demonstrate a combined experimental and theoretical study of oxygen reduction catalysis on SACs, which incorporate M-N C site structure, composed of atomically dispersed transition metals (e.
View Article and Find Full Text PDFHerein we present a new viologen-based radical-containing metal-organic framework (RMOF) Gd-IHEP-7, which upon heating in air undergoes a single-crystal-to-single-crystal transformation to generate Gd-IHEP-8. Both RMOFs exhibit excellent air and water stability as a result of favorable radical-radical interactions, and their long-lifetime radicals result in wide spectral absorption in the range 200-2500 nm. Gd-IHEP-7 and Gd-IHEP-8 show excellent activity toward solar-driven nitrogen fixation, with ammonia production rates of 128 and 220 μmol h g , respectively.
View Article and Find Full Text PDFThe one-step electrochemical synthesis of HO is an on-site method that reduces dependence on the energy-intensive anthraquinone process. Oxidized carbon materials have proven to be promising catalysts due to their low cost and facile synthetic procedures. However, the nature of the active sites is still controversial, and direct experimental evidence is presently lacking.
View Article and Find Full Text PDFJ Colloid Interface Sci
August 2020
The supercapacitive performance of high-rate capacity and long-term cycling stability is still a big challenge for electroactive materials. Herein, Ni and Zn co-substituted Co carbonate hydroxide (NiZn-CoCH) flowers array is self-assembled on nickel foams (NFs) using l-ascorbic acid as a nanostructure inducer. The NiZn-CoCH flowers, consisting of silk-like nanosheets, are deservedly large electrode-electrolyte contact area and suitable ion-diffusion channel.
View Article and Find Full Text PDFInsect Biochem Mol Biol
April 2020
The antifungal activity of insect chitinase has rarely been studied. Here, we show that chitinase ChtIV, which is specifically expressed in the midgut of Asian corn borer (Ostrinia furnacalis), has antifungal activity toward phytopathogenic fungi. ChtIV exhibited high stability and mycelial hydrolytic activity in the extreme midgut environment, which has a pH of 10 and is rich in proteases.
View Article and Find Full Text PDFSubstantial consumption of fossil fuels causes an increase in CO emissions and intensifies global pollution problems, such as the greenhouse effect. Recently, a new type of ultra-low-density porous material, metal-organic frameworks (MOFs), has been developed for the photocatalytic conversion of CO. Herein, a composite photocatalytic catalyst based on NH-MIL-125(Ti) and reduced graphene oxide (rGO@NH-MIL-125) was fabricated through a facile "one-pot" process.
View Article and Find Full Text PDFHydrogen adsorption/desorption behavior plays a key role in hydrogen evolution reaction (HER) catalysis. The HER reaction rate is a trade-off between hydrogen adsorption and desorption on the catalyst surface. Herein, we report the rational balancing of hydrogen adsorption/desorption by orbital modulation using introduced environmental electronegative carbon/nitrogen (C/N) atoms.
View Article and Find Full Text PDFReasonably designing self-supported metal-organic framework (MOF) nanoarrays is profound for applications in energy storage and conversion. Herein, we construct a triangle-like nickel-cobalt bimetallic metal-organic framework nanosheet array on nickel foam (NiCo-MOF/NF) via facile one-step hydrothermal reaction, served as battery-like electrode material for hybrid supercapacitors. By adjusting the molar ratio of Ni and Co, the optimal NiCo-MOF/NF with Ni/Co = 3:2 (3-2 NiCo-MOF/NF) produces an impressive specific capacity of 1003.
View Article and Find Full Text PDFUniform ruthenium phosphide (Ru2P and RuP) nanocrystals grown in situ on N- and P-codoped graphene were obtained by pyrolyzing tris(triphenylphosphine) ruthenium(ii) chloride (TPP-Ru) with pyritic acid (PA). Interestingly, Ru2P and RuP can be controllably prepared by varying the molar ratio of PA to TPP-Ru. As an efficient electrocatalyst for the hydrogen evolution reaction (HER), Ru2P exhibited a better performance than RuP in alkaline medium.
View Article and Find Full Text PDFIdentification of active sites is one of the main obstacles to rational design of catalysts for diverse applications. Fundamental insight into the identification of the structure of active sites and structural contributions for catalytic performance are still lacking. Recently, X-ray absorption spectroscopy (XAS) and density functional theory (DFT) provide important tools to disclose the electronic, geometric and catalytic natures of active sites.
View Article and Find Full Text PDFThe fabrication of a perovskite oxide with a tunable pore-size was implemented by a general inorganic salt-template strategy. As a proof-of-concept, hierarchically porous PrBa0.5Sr0.
View Article and Find Full Text PDFAg-CeO plasmonic photocatalysts with multiple morphologies were synthesized a simple solvent-driven method. The phase compositions, morphologies and optical properties of the samples were systematically investigated. A combination of noble metal Ag and semiconductor CeO in certain solvents (such as methanol and ethylene glycol) enhanced surface plasmon resonance (SPR), which was attributed to the good dispersion of Ag particles on CeO and high Ag ratios on the surface.
View Article and Find Full Text PDFCarbon capture, utilization, and sequestration technologies have been extensively studied to utilize carbon dioxide (CO), a greenhouse gas, as a resource. So far, however, effective technologies have not been proposed owing to the low efficiency conversion rate and high energy requirements. Here, we present a hybrid Na-CO cell that can continuously produce electrical energy and hydrogen through efficient CO conversion with stable operation for over 1,000 hr from spontaneous CO dissolution in aqueous solution.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2018
A novel synthesis strategy is demonstrated to prepare Mo P/Mo nanobelts with porous structure for the first time. The growth and formation mechanism of the porous Mo P/Mo nanobelt structure was disclosed by varying the contents of H /PH and the reaction temperature. During the hydrogen evolution reaction (HER) catalysis, the optimized porous Mo P/Mo nanobelts exhibited a small overpotential of 78 mV at a current density of 10 mA cm and a low Tafel slope of 43 mV dec , as well as long-term stability in alkaline media, surpassing Pt wire.
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