Repulsing Cl to reduce its negative effects during seawater electrolysis is a promising strategy to guard against the corrosion of high-valence metal sites. Herein, we synthesized FeP/NiP by a facile Br-induced partial phase transition strategy. This FeP/NiP possessed intensified built-in electric field (BEF) due to large work function difference (Δ), demonstrating outstanding OER and HER activity in alkaline freshwater/seawater solution and exhibiting a low cell voltage for an anion exchange membrane water electrolyzer (AEMWE) system.
View Article and Find Full Text PDFPrecisely designing asymmetric active centers and exploring their electronic regulation effects to prepare efficient bifunctional single-atom catalysts (SACs) is important for boosting the practical applications of zinc-air batteries (ZABs). Herein, an effective strategy has been developed by introducing an axial S atom to the FeN active center, simultaneously assisted by pyrolyzing the graphene oxide (GO) sheathed zeolitic-imidazolate framework-8 (ZIF8) composite and constructing a three-dimensional (3D) porous framework with abundant FeNS moieties. This structure can accelerate the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) kinetics owing to the modulated electronic redistribution and -band center with a reduced energy barrier.
View Article and Find Full Text PDFIt offers bright prospects to develop non-Pt group metal (non-PGM) electrocatalysts in the area of energy storage and conversion. Herein, we reported a simple spatial isolation strategy to synthesize Co-based electrocatalysts, using partially substituted Zn atoms in a ZnCo-ZIF precursor. The "fence" effect that originated from the partially substituted Zn atoms can yield a better isolation of Co atoms, achieving selective loading of Co species on nitrogen-doped porous carbon varying from nanoparticles to single atoms.
View Article and Find Full Text PDFRegulating the asymmetric active center of a single-atom catalyst to optimize the binding energy is critical but challenging to improve the overall efficiency of the electrocatalysts. Herein, an effective strategy is developed by introducing an axial hydroxyl (OH) group to the Fe─N center, simultaneously assisting with the further construction of asymmetric configurations by replacing one N atom with one S atom, forming FeNS─OH configuration. This novel structure can optimize the electronic structure and d-band center shift to reduce the reaction energy barrier, thereby promoting oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalytic activities.
View Article and Find Full Text PDFThe coordination of the electronic structure and charge transfer through heteroatomic doping and sulfur vacancies is one of the most vital strategies for enhancing the electrocatalytic performance of the oxygen and hydrogen evolution reactions (OER, HER) through water splitting. Se-doped CuCoS nanosheets (CuCoSSe) with abundant sulfur vacancies were synthesized a simple hydrothermal method to achieve remarkably efficient electrocatalytic water splitting. Importantly, incorporating Se in three-dimensional nanosheet structures effectively fine-tunes the electronic structure, ensuring ample accessibility of active sites for swift charge carrier transfer and improved reaction kinetics.
View Article and Find Full Text PDFExploring efficient, easy-to-manufacture, and inexpensive bifunctional electrocatalysts with abundant accessible active sites is crucial for rechargeable zinc-air batteries (ZABs). Herein, we report the strategy consisting of the space confinement and pore-making engineering to fabricate single-atom catalyst enriched with Fe-N sites anchored on N-doped hierarchically porous carbon (Fe-NC-CN). The optimized Fe-NC-CN exhibits excellent oxygen reduction/evolution reaction (ORR/OER) activities with a half-wave potential (E) of 0.
View Article and Find Full Text PDFThe development of innovative and efficient Fe-N-C catalysts is crucial for the widespread application of zinc-air batteries (ZABs), where the inherent oxygen reduction reaction (ORR) activity of Fe single-atom sites needs to be optimized to meet the practical application. Herein, a three-dimensional (3D) hollow hierarchical porous electrocatalyst (ZIF8@FePMPDA-920) rich in asymmetric Fe-N -OH moieties as the single atomic sites is reported. The Fe center is in a penta-coordinated geometry with four N atoms and one O atom to form Fe-N -OH configuration.
View Article and Find Full Text PDFExosomes are focused as natural drug delivery vehicles with the advantages of biocompatible, biodegradable and non-immunogenic. However, the low yield of exosomes is one of the challenges that constrain its application. Mimetic exosomes (m-Exo) are the novel cell-derived nano-carriers with similar properties to exosomes and the substantially greater yield is attractive.
View Article and Find Full Text PDFRational hybridization of two-dimensional (2D) nanomaterials with extrinsic species has shown great promise for boosting the electrocatalytic oxygen evolution reaction (OER). To date, the rational design and engineering of heterojunctions based on three or more components has been rather limited. Herein, by taking advantage of the high intrinsic activity of NiFe layered double hydroxide (LDH), strong synergistic effects between different components, and good electronic conductivity of reduced graphene oxide (rGO), we demonstrate the successful synthesis of NiMoO/NiFe LDH/rGO nanosheets.
View Article and Find Full Text PDFHollow CuCoS nanorods (H-CCS-Ns) have been successfully developed via a facile successive anion/cation-exchange method. The outstanding electrocatalytic performance of H-CCS-Ns is mainly attributed to its distinctive hollow structure, which accelerates the electron transfer rate and provides abundant active sites. Moreover, a mechanism study indicates that H-CCS-Ns has highly active octahedral Co, and the existence of Co cations optimizes the adsorption of oxygen-involved intermediates, making H-CCS-Ns a promising OER electrocatalyst.
View Article and Find Full Text PDFIridium (Ir)-based electrocatalysts are widely explored as benchmarks for acidic oxygen evolution reactions (OERs). However, further enhancing their catalytic activity remains challenging due to the difficulty in identifying active species and unfavorable architectures. In this work, we synthesized ultrathin Ir-IrO/C nanosheets with ordered interlayer space for enhanced OER by a nanoconfined self-assembly strategy, employing block copolymer formed stable end-merged lamellar micelles.
View Article and Find Full Text PDFRestacking of 2D nanomaterials is often deemed to be detrimental to their applications. In contrast to this common notion, here we demonstrate that tightly packed stacked MoS2 exhibits a higher electrocatalytic activity for hydrogen evolution than the more loosely stacked ones.
View Article and Find Full Text PDFACS Appl Mater Interfaces
July 2019
Graphitic carbon nitride (g-CN), characterized with a suitable bandgap, has aroused great interest as a robust and efficient catalyst for solar energy utilization. Herein, we introduce a new strategy to fabricate a three-dimensional (3D) porous g-CN by a facile NaCl-assisted ball-milling strategy. The porous structure-induced advantages, such as a higher specific surface area, more efficient charge separation, and faster electron-transfer efficiency, enable the 3D porous g-CN to achieve impressive properties as a bifunctional catalyst for both photocatalytic hydrogen evolution and electrocatalytic oxygen evolution reaction (OER).
View Article and Find Full Text PDFThe exploration of highly active catalysts for hydrogen evolution reaction (HER) is beneficial to realize high catalytic activity and enhance kinetics for water splitting. Herein, flower-like molybdenum disulfide/carbon nitride (MoS/CN) nanosheets with thickness of 4.6 nm and enlarged interlayer spacing of 0.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2017
Hierarchical nanostructures with heteroatom doping have been considered as an important component in electrode materials for advanced supercapacitors. Herein, with the aid of C, N, and S codoped NiCo(CO)(OH)/C (NSH) with a hierarchical structure was synthesized through a facile one-step hydrothermal method. Notably, it is the first report on a carbon precursor as a structure inducer for designing a three-dimensional (3D) carnation-like hierarchical structure.
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