The development of efficient nonprecious metal electrocatalysts for industrial anion exchange membrane water electrolysis (AEM-WE) remains challenging, primarily due to sluggish OH transfer from the anion exchange membrane (AEM) to catalytic sites, causing H accumulation and performance degradation. Herein, we developed a zwitterion-modified NiFe catalyst (z-NiFe) through gradient soaking, facilitates rapid OH transfer across the AEM-electrocatalyst interface, effectively neutralizing the generated H and enhancing catalytic performance. In-situ Raman spectroscopy and OH conductivity measurements reveal an alkaline-enriched surface environment, which inhibits H accumulation-induced chemical corrosion and enhances water oxidation performances.
View Article and Find Full Text PDFThe mechanical stability of the catalytic electrodes used for hydrogen evolution reactions (HER) is crucial for their industrial applications in anion exchange membrane water electrolysis (AEM-WE). This study develops a corrosion strategy to construct a self-supported electrocatalyst (Int-Ni/MoO) with high mechanical stability by anchoring the Ni/MoO catalytic layer with a dense interlayer of MoO nanoparticles. The Int-Ni/MoO exhibits a strengthened homostructural interface between the interlayer and catalytic layer, preventing the detachment of the catalyst during ultrasonic treatment.
View Article and Find Full Text PDFNoble metal-free electrodes for anion exchange membrane water electrolysis (AEM-WE) operating at high current densities are critical for sustainable hydrogen production. However, the massive amount of bubbles resulted in insufficient mass transfer and unevenly distributed local stress, which poses a major challenge in designing an efficient and robust hydrogen evolution catalyst. Herein, a facile chemical corrosion method is developed to synthesize an interlayer-anchored NiMo/MoO catalyst on a nickel foam (NF) substrate (NiMo/Int/NF) with high hydrogen evolution activity (overpotential of 80.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2023
Electricity-driven organo-oxidations have shown an increasing potential recently. However, oxygen evolution reaction (OER) is the primary competitive reaction, especially under high current densities, which leads to low Faradaic efficiency (FE) of the product and catalyst detachment from the electrode. Here, we report a bimetallic Ni-Cu electrocatalyst supported on Ni foam (Ni-Cu/NF) to passivate the OER process while the oxidation of 5-hydroxymethylfurfural (HMF) is significantly enhanced.
View Article and Find Full Text PDFSelf-reconstruction has been considered an efficient means to prepare efficient electrocatalysts in various energy transformation process for bond activation and breaking. However, developing nano-sized electrocatalysts through complete in-situ reconstruction with improved activity remains challenging. Herein, we report a bottom-up evolution route of electrochemically reducing CsRhI halide-perovskite clusters on N-doped carbon to prepare ultrafine Rh nanoparticles (~2.
View Article and Find Full Text PDFDefect engineering provides a promising approach for optimizing the trade-off between support structures and active nanoparticles in heterojunction nanostructures, manifesting efficient synergy in advanced catalysis. Herein, a high density of distorted lattices and defects are successfully formed in bronze TiO through caging alkali-metal Na cations in open voids (Na-TiO(B)), which could efficiently cohere nanoparticulate electrocatalysts toward alkaline hydrogen evolution reaction (HER). The RuMo bimetallic nanoparticles could directionally anchor on Na-TiO(B) with a certain angle of ∼22° due to elimination of the lattice mismatch, thus promoting uniform dispersion and small sizing of supported nanoparticles.
View Article and Find Full Text PDFInorg Chem
November 2021
Exploring new excellent electrocatalysts for the hydrogen evolution reaction (HER) is of significance for the development of hydrogen energy. Herein, a ternary chalcogenide (PtPbS) is successfully designed and synthesized using layered PtS as a matrix. The energy level of the Pt 5d orbital is upshifted to the Fermi surface after replacing S atoms by Pb atoms, which results in the high conductivity of PtPbS.
View Article and Find Full Text PDFChem Commun (Camb)
August 2021
The exploration of efficient electrocatalysts for the hydrogen evolution reaction (HER) is beneficial to obtain renewable clean energy. Herein, a new parkerite-type compound Pt3Bi2S2 was synthesized, constructed by [PtBi4S2] octahedra. The Bi 6p orbital electrons upshift the Pt 5d band to promote hydrogen adsorption.
View Article and Find Full Text PDFThe advancement of efficient electrocatalysts toward the nitrogen reduction reaction (NRR) is critical in sustainable ammonia synthesis under ambient pressure and temperature. Manipulating the electronic configuration of electrocatalysts is particularly vital to form metal-nitrogen (MN) bonds during the NRR through regulating the active electronic states of sites. Here, in sharp contrast to stable 2H MoS without metal chains, MoMo bonding in metastable polymorphs of MoS bulk (zigzag chain in the 1T' phase and diamond chain in the 1T″' phase) is discovered to significantly increase intrinsic electron localization around the metal chains.
View Article and Find Full Text PDFTo work against the volume expansion (∼300%) of SnO during lithiation, here a sub-micro sized, interconnected, and porous SnO cube with rationally designed reserved space (∼375%) is synthesized via an artful topochemistry route (CaSn(OH)-CaSnO-SnO). Owing to its microstructure, this novel material harvests enhanced lithium-storage performance.
View Article and Find Full Text PDFElectrocatalytic water splitting, as one of the most promising methods to store renewable energy generated by intermittent sources, such as solar and wind energy, has attracted tremendous attention in recent years. Developing efficient, robust, and green catalysts for the hydrogen and oxygen evolution reactions (HER and OER) is of great interest. This study concerns a facile and green approach for producing RuNi/RuNi oxide nanoheterostructures by controllable partial oxidation of RuNi nanoalloy, which is characterized and confirmed by various techniques, including high-resolution transmission electron microscopy and synchrotron-based X-ray absorption spectroscopy.
View Article and Find Full Text PDFIn this paper, a series of nitrogen-doped mesoporous carbons (NMCs) with three-dimensional (3D) interconnected mesopores have been prepared using flour as carbon source, dicyanamide as nitrogen source and colloidal silica as hard template. The optimized material (NMC-4) prepared with the colloidal silica/flour mass ratio of 4 has a high nitrogen doping level of 5.69 at.
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