Authors: Ping Li, Wenqin Li, Yuqi Huang, Quhua Huang, Shuanghong Tian
Published: 2023-04-10
Source: Full article
AbstractExploring active and durable Ni‐based materials with optimized electronic and architectural engineering to promote the urea oxidation reaction (UOR) is pivotal for the urea‐related technologies. Herein a 3D self‐supported hierarchical‐architectured nanoarray electrode (CC/MnNi@NC) is proposed in which 1D N‐doped carbon nanotubes (N‐CNTs) with 0D MnNi nanoparticles (NPs) encapsulation are intertwined into 2D nanosheet aligned on the carbon cloth for prominently boosted and sustained UOR electrocatalysis. From combined experimental and theoretical investigations, Mn‐alloying can regulate Ni electronic state with downshift of the d‐band center, facilitating active Ni3+ species generation and prompting the rate‐determining step (*COO intermediate desorption). Meanwhile, the micro/nano‐hierarchical nanoarray configuration with N‐CNTs encapsulating MnNi NPs can not only endow strong operational durability against metal corrosion/agglomeration and enrich the density of active sites, but also accelerate electron transfer, and more intriguingly, promote mass transfer as a result of desirable superhydrophilic and quasi‐superaerophobic characteristics. Therefore, with such elegant integration of 0D, 1D and 2D motifs into 3D micro/nano‐hierarchical architecture, the resulting CC/MnNi@NC can deliver admirable UOR performance, favorably comparable to the best‐performing UOR electrocatalysts reported thus far. This work opens a fresh prospect in developing advanced electrocatalysts via electronic manipulation coupled with architectural engineering for various energy conversion technologies.