γ-FeO with the intrinsic cation vacancies is an ideal substrate for heteroatom doping into the highly active octahedral sites in spinel oxide catalysts. However, it is still a challenge to confirm the vacancy location of γ-FeO through experiments and obtain enhanced catalytic performance by preferential occupation of octahedral sites for heteroatom doping. Here, a Mn-doped γ-FeO incorporated with carbon nanotubes catalyst was developed to successfully achieve preferential doping into highly active octahedral sites by employing γ-FeO as the precursor.
View Article and Find Full Text PDFJ Colloid Interface Sci
November 2024
Investigating efficient non-precious metal-based catalysts for water electrolysis to produce hydrogen is a significant and urgent need in the field of clean energy technologies. Moreover, utilizing transition metal dichalcogenides (TMDs) to replace the oxygen evolution reaction (OER) with the urea oxidation reaction (UOR), coupled with the hydrogen evolution reaction (HER), is an effective energy-saving hydrogen production method. A heterostructure NiS/MoO catalyst was prepared by a simple method, which exhibits excellent activity for UOR, requiring only 1.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2024
Strain engineering is an effective strategy to improve the activity of catalysts, especially for flexible carbon-based materials. Nitrogen-coordinated single atomic metals on a carbon skeleton (M-N/C) are of interest in catalytic electroreduction reactions due to their high activity and atomic utilization. However, the effect of strain on the structure-activity relationship between the electrochemical activity and the electronic and geometric structures of Ni-N/C remains unclear.
View Article and Find Full Text PDFAs a novel electrochemical energy conversion device, direct ethanol fuel cells are currently encountering two significant challenges: CO poisoning and the difficulty of C-C bond cleavage in ethanol. In this work, an amorphous PdS nanowires/ultrafine IrMnO bimetallic oxides (denoted as a-PdS/IrMnO NWs) catalyst with abundant oxide/metal (crystalline/amorphous) inverse heterogeneous interfaces was synthesized via a hydrothermal process succeeded by a nonthermal air-plasma treatment. This unique interfacial electronic structure along with the incorporation of oxyphilic metal has resulted in a significant enhancement in the electrocatalytic performance of a-PdS/IrMnO NWs toward the ethanol oxidation reaction, achieving current densities of 12.
View Article and Find Full Text PDFThe catalyst-reconstruction makes it challenging to clarify the practical active sites and unveil the actual reaction mechanism during the CO electroreduction reaction (CO RR). However, currently the impact of the electrolyte microenvironment in which the electrolyte is in contact with the catalyst is overlooked and might induce a chemical evolution, thus confusing the reconstruction process and mechanism. In this work, the carbonate adsorption properties of metal oxides were investigated, and the mechanism of how the electrolyte carbonate affect the chemical evolution of catalysts were discussed.
View Article and Find Full Text PDFCarbon dioxide electroreduction reaction (CORR) can take full advantage of sustainable power to reduce the continuously increasing carbon emissions. Recycling CO to produce formic acid or formate is a technologically and economically viable route to accomplish CO cyclic utilization. Developing efficient and cost-effective electrocatalysts with high selectivity towards formate is prioritized for the industrialized applications of CORR electrolysis.
View Article and Find Full Text PDFACS Appl Mater Interfaces
August 2023
The main obstacle to the development of large-scale electrochemical hydrogen production based on water splitting is the slow four-electron kinetics of OER (oxygen evolution reaction). The most efficient method is to create sophisticated and effective OER catalysts. Here, we proposed the controlled synthesis of high-entropy layered double hydroxides (HELDH) for wide component regulation and the component design of high OER activity to make up for the restricted component regulation in conventional catalysts.
View Article and Find Full Text PDFJ Colloid Interface Sci
November 2023
Photoelectrocatalyzing water reduction is a potential approach to building a green and sustainable society. As a benchmark photocathode, CuO receives much attention but faces serious charge recombination and photocorrosion. This work prepared an excellent CuO/MoO photocathode via in situ electrodeposition.
View Article and Find Full Text PDFThe sluggish kinetics and mutual interference of oxygen evolution and reduction reactions in the air electrode resulted in large charge/discharge overpotential and low energy efficiency of Zn-air batteries. In this work, we designed a breathing air-electrode configuration in the battery using P-type Ca Co O and N-type CaMnO as charge and discharge thermoelectrocatalysts, respectively. The Seebeck voltages generated from thermoelectric effect of Ca Co O and CaMnO synergistically compensated the charge and discharge overpotentials.
View Article and Find Full Text PDFPhys Chem Chem Phys
February 2023
The recent development of some special oxygen evolution reaction (OER) electrocatalysts shows that the lattice oxygen could participate in the catalysis process the lattice oxygen oxidation mechanism (LOM), which the provides good possibility of exploring advanced electrocatalysts that could overcome the scaling relationship in conventional catalysis processes through a traditional adsorbate evolution mechanism. In this work, we theoretically predict that, benefiting from the unhybridized O-Li orbitals and the resulting metastable Li-O-Li ligands, the lattice oxygen could be easily activated and oxidized at relatively high oxidation voltages. Thus, lithium-excess disordered rocksalts (DRX) should possess the potential for acting as active OER electrocatalysts, which catalyze through the LOM pathway.
View Article and Find Full Text PDFThe state-of-the-art active hydrogen evolution reaction (HER) catalysts in acid electrolytes generally lose considerable catalytic performance in alkaline electrolytes mainly due to the additional water dissociation step. Designing composite materials is an effective strategy to accelerate alkaline water electrolysis by optimizing the electronic structure of materials. Here, different phases of Co(OH) -supported Ru clusters (α/β-Co(OH) @Ru) are prepared for enabling a highly efficient electrocatalytic HER performance in alkaline solution.
View Article and Find Full Text PDFHigh-entropy compounds with extraordinary properties due to the synergistic effect of multiple components have exhibited great potential and attracted extensive attention in various fields, including physics, mechanical property analysis, and energy storage. Achieving universal stability and synthesis of high-entropy compounds with a wide range of components and structures continues to be difficult due to the high complexity of multicomponent mixing. Here, we propose a design strategy with high generality for realizing the stability and synthesis of high-entropy compounds that one metal site like the framework in the compound structures with bimetallic sites stabilizes another site to accommodate different elements.
View Article and Find Full Text PDFThe rapid development of portable, flexible, and wearable devices motivates the requirement for flexible zinc-air batteries (FZABs) not only to provide high energy density but also to have sufficient deformability for wearer comfort. The gel polymer electrolyte (GPE) serves as the core part of the FZABs, playing a key function in the battery's practical output performance such as discharge voltage, energy density, and cycling life. Unfortunately, ascribed to its high water absorption, the GPE regularly shows comparatively poor mechanical strength, which is difficult to offer sufficient physical support between electrodes.
View Article and Find Full Text PDFThe ever-increasing demand for flexible and portable electronics has stimulated research and development in building advanced electrochemical energy devices which are lightweight, ultrathin, small in size, bendable, foldable, knittable, wearable, and/or stretchable. In such flexible and portable devices, semi-solid/solid electrolytes besides anodes and cathodes are the necessary components determining the energy/power performances. By serving as the ion transport channels, such semi-solid/solid electrolytes may be beneficial to resolving the issues of leakage, electrode corrosion, and metal electrode dendrite growth.
View Article and Find Full Text PDFMetal-organic framework (MOF) derivatives promise great potential in energy storage and conversion because of their excellent tunability in both the active metal sites, organic links, and the overall structures down to atomic and up to mesoscale. Nevertheless, a big challenge is to precisely control and thoroughly understand the actual MOF-to-derivative conversion process to realize the template-free synthesis of the MOF-derived ordered mesoporous materials. Here, a class of ordered mesoporous N-doped carbon nanoflakes is presented with slit-shaped pores synthesized by one-step pyrolysis of Zn Cu -MOF, where the Cu doping plays a critically important direction-inducing function on the dissociation of organic ligands during the pyrolysis.
View Article and Find Full Text PDFACS Appl Mater Interfaces
August 2022
Converting CO into value-added chemicals and fuels is one of the promising approaches to alleviate CO emissions, reduce the dependence on nonrenewable energy resources, and minimize the negative environmental effect of fossil fuels. This work used density functional theory (DFT) calculations combined with microkinetic modeling to provide fundamental insight into the mechanisms of CO hydrogenation to hydrocarbons over the iron carbide catalyst, with a focus on understanding the energetically favorable pathways and kinetic controlling factors for selective hydrocarbon production. The crystal orbital Hamiltonian population analysis demonstrated that the transition states associated with O-H bond formation steps within the path are less stable than those of C-H bond formation, accounting for the observed higher barriers in O-H bond formation from DFT.
View Article and Find Full Text PDFHigh-entropy oxide (HEO) including multiple principal elements possesses great potential for various fields such as basic physics, mechanical properties, energy storage, and catalysis. However, the synthesis method of high-entropy compounds through the traditional heating approach is not conducive to the rapid properties screening, and the current elemental combinations of HEO are also highly limited. Herein, we report a rapid synthesis method for HEO through the Joule-heating of nickel foil with dozens of seconds.
View Article and Find Full Text PDFHere, we report the synthesis of activated NiCo LDH to immobilize Pt, Ir and Rh single atoms for hydrogen evolution reaction. The Pt/A-NiCo LDH electrocatalyst exhibits the highest catalytic ability with a low overpotential of 16 mV to achieve a current density of 10 mA cm and a mass activity about 24.8-fold that of commercial Pt/C.
View Article and Find Full Text PDFConstructing structure-function relationships is critical for the rational design and development of efficient catalysts for CO electroreduction reaction (CORR). InO is well-known for its specific ability to produce formic acid. However, how the crystal phase and surface affect the CORR activity is still unclear, making it difficult to further improve the intrinsic activity and screen for the most active structure.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2022
Facilitating the efficient activation of N molecules and inhibiting the competing hydrogen evolution reaction remain a challenge in the nitrogen reduction reaction (NRR). A heteroatom doping strategy is an effective way to optimize the energy barrier during the NRR process to improve the catalytic efficiency. Herein, we report Ni-doped MoC anchored on graphitized porous conductive carbon for regulating the electronic structure and catalytic properties of electrocatalysts toward NRR.
View Article and Find Full Text PDFIon exchange membranes (IEMs) play important roles in energy generation and storage field, such as fuel cell, flow battery, however, a major barrier in the way of large-scale application is the high cost of membranes (e.g., Nafion membranes price generally exceeds USD$ 200 m ).
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