3D Hierarchical-Architectured Nanoarray Electrode for Boosted and Sustained Urea Electro-Oxidation,Small

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3D Hierarchical-Architectured Nanoarray Electrode for Boosted and Sustained Urea Electro-Oxidation
Small ( IF 13.0 ) Pub Date : 2023-04-10 , DOI: 10.1002/smll.202300725
Ping Li _{1,

2} , Wenqin Li _{1,

2} , Yuqi Huang _{1,

2} , Quhua Huang _{1,

2} , Shuanghong Tian _{1,

2}

Affiliation

Exploring 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.

中文翻译：

用于增强和持续尿素电氧化的 3D 分层结构纳米阵列电极

通过优化电子和建筑工程探索活性和耐用的镍基材料以促进尿素氧化反应（UOR）是尿素相关技术的关键。本文提出了一种 3D 自支撑分层结构纳米阵列电极（CC/MnNi@NC），其中 1D N 掺杂碳纳米管（N-CNT）与 0D MnNi 纳米颗粒（NP）封装交织成在碳上排列的 2D 纳米片用于显着增强和持续 UOR 电催化的布。结合实验和理论研究，Mn合金化可以通过d带中心下移来调节Ni电子态，促进活性Ni ³⁺物种的生成并促进速率决定步骤（*COO中间解吸）。同时，N-CNTs封装MnNi NPs的微/纳米分级纳米阵列结构不仅可以赋予强大的抗金属腐蚀/团聚的操作耐久性并丰富活性位点的密度，而且可以加速电子传递，更有趣的是，可以促进传质由于具有理想的超亲水性和准超疏气特性。因此，通过将 0D、1D 和 2D 图案优雅地集成到 3D 微/纳米分层结构中，所得的 CC/MnNi@NC 可以提供令人钦佩的 UOR 性能，可与迄今为止报道的性能最佳的 UOR 电催化剂相媲美。这项工作为通过电子操纵与各种能量转换技术的建筑工程开发先进电催化剂开辟了新的前景。

更新日期：2023-04-10

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