Angew Chem Int Ed Engl
February 2025
Electrochemical treatment of urea wastewater purification significantly aids in environmental protection, but it remains a considerable challenge in designing high performance anode urea oxidation electrocatalysts. Herein, we report a La-induced three-dimensional ordered macroporous (3DOM) NiO heterostructure to improve Ni sites electron density for urea electrooxidation by activating the La-O-Ni bridge. This material demonstrated exceptional performance in a membrane electrode assembly (MEA) device, characterized by a low cell voltage (1.
View Article and Find Full Text PDFThe utilization of rare earth elements to regulate the interaction between catalysts and oxygen-containing species holds promising prospects in the field of oxygen electrocatalysis. Through structural engineering and adsorption regulation, it is possible to achieve high-performance catalytic sites with a broken activity-stability tradeoff. Herein, this work fabricates a hierarchical CeO/NiCo hydroxide for electrocatalytic oxygen evolution reaction (OER).
View Article and Find Full Text PDFThe electronic structure and geometric configuration of catalysts play a crucial role to design novel perovskite-type catalysts for oxygen reduction reaction (ORR). Nowadays, many studies are more concerned with the influence of electronic structure and ignore the geometric effect, which plays a nonnegligible role in enhancing catalytic performances. Herein, this work regulates the MnO octahedral tilting degree of LaMnO by modulating the concentration of Y, excluding the electronic effect from the valence state of manganese.
View Article and Find Full Text PDFTo master the activation law and mechanism of surface lattice oxygen for the oxygen evolution reaction (OER) is critical for the development of efficient water electrolysis. Herein, we propose a strategy for triggering lattice-oxygen oxidation and enabling non-concerted proton-electron transfers during OER conditions by substituting Al in LaSrCoO. According to our experimental data and density functional theory calculations, the substitution of Al can have a dual effect of promoting surface reconstruction into active Co oxyhydroxides and activating deprotonation on the reconstructed oxyhydroxide, inducing negatively charged oxygen as an active site.
View Article and Find Full Text PDFOriented synthesis of transition metal sulfides (TMSs) with controlled compositions and crystal structures has long been promising for electronic devices and energy applications. Liquid-phase cation exchange (LCE) is a well-studied route by varying the compositions. However, achieving crystal structure selectivity is still a great challenge.
View Article and Find Full Text PDFFormate is identified as economically viable chemical fuel from electrochemical carbon dioxide reduction. However, the selectivity of current catalysts toward formate is limited by the competitive reaction such as HER. Herein, we propose a CeO modification strategy to improve the selectivity of catalysts for formate through tuning of the *OCHO intermediate, which is important for formate production.
View Article and Find Full Text PDFPerovskite oxides are an important class of oxygen evolution reaction (OER) catalysts offering an ordered atomic arrangement and a highly flexible electronic structure. Currently, understanding and adjusting the dynamic reconstruction of perovskite during the OER process remains a formidable challenge. Here, we report the artificial construction of a heterostructure by the cation exsolution of perovskite to control the active site formation and reconstruction.
View Article and Find Full Text PDFRealizing the rational design of perovskite oxides with controllable compositions and nanostructures remains a tremendous challenge for the development of efficient electrocatalysts. Herein, a ligand-assisted synthetic strategy to fabricate perovskite oxides LaCo Fe O with yolk-shell nanostructures is developed. Benefiting from the unique structural and compositional merits, LaCo Fe O exhibits an overpotential of 310 mV at a current density of 10 mA cm and long-term stability of 100 h for the oxygen evolution reaction.
View Article and Find Full Text PDFThe oxygen-related electrochemical process, including the oxygen evolution reaction and oxygen reduction reaction, is usually a kinetically sluggish reaction and thus dominates the whole efficiency of energy storage and conversion devices. Owing to the dominant role of the oxygen-related electrochemical process in the development of electrochemical energy, an abundance of oxygen-related electrocatalysts is discovered. Among them, perovskite-type materials with flexible crystal and electronic structures have been researched for a long time.
View Article and Find Full Text PDFStructural engineering and compositional controlling are extensively applied in rationally designing and fabricating advanced freestanding electrocatalysts. The key relationship between the spatial distribution of components and enhanced electrocatalysis performance still needs further elaborate elucidation. Here, CeO substrate supported CoS (CeO -CoS ) and CoS with CeO surface decorated (CoS -CeO ) materials are constructed to comprehensively investigate the origin of spatial architectures for the oxygen evolution reaction (OER).
View Article and Find Full Text PDFZinc-air batteries offer a possible solution for large-scale energy storage due to their superhigh theoretical energy density, reliable safety, low cost, and long durability. However, their widespread application is hindered by low power density. Herein, a multiscale structural engineering of Ni-doped CoO nanosheets (NSs) for zinc-air batteries with superior high power density/energy density and durability is reported for the first time.
View Article and Find Full Text PDFAtomic-level structure engineering can substantially change the chemical and physical properties of materials. However, the effects of structure engineering on the capacitive properties of electrode materials at the atomic scale are poorly understood. Fast transport of ions and electrons to all active sites of electrode materials remains a grand challenge.
View Article and Find Full Text PDFACS Appl Mater Interfaces
May 2018
Transition-metal phosphides (TMPs) have lately drawn intensive attention because of their noble metal-free properties and high catalytic activities for the hydrogen evolution reaction (HER). The current research mainly focuses on the development of TMPs toward the HER in acidic solutions; however, less efforts have been directed to specifically design TMPs for alkaline HER. Here, we design a new bi-functional metal phosphide-oxide catalyst to facilitate the overall multistep HER process in alkaline environments.
View Article and Find Full Text PDF