内置氮转移通道的不对称电极设计实现电化学氨合成三相反应区的最大化

Electron Pub Date : 2023-08-11 DOI:10.1002/elt2.2
Chao Wang, Qiyang Cheng, Mengfan Wang, Sisi Liu, Yanzheng He, Chengwei Deng, Yi Sun, Tao Qian, Na Xu, Federico Rosei, Chenglin Yan
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引用次数: 0

摘要

无碳电化学氮还原反应(NRR)是一种很有吸引力的绿色氨合成策略,但仍存在显著的性能瓶颈。在NRR测试过程中,传统的工作电极通常被电解质淹没,只有表面材料才能接触到氮气,这不可避免地导致反应速率缓慢。在此,提出了一种不对称电极设计来应对这一挑战。在负载电催化剂的电极的一面上构建了亲气层,而另一面保持其原始结构,旨在同时实现导电骨架内促进的氮转移和电解质渗透。这种不对称结构在电极内提供了广泛的三相反应区,如理论模拟和实验测量的结合所证明的,这充分发挥了负载的电催化剂。正如预期的那样,与可逆氢电极相比,概念验证不对称电极在−0.3 V下的NH3产率为40.81μg h−1 mg−1,法拉第效率为71.71%,分别是传统电极的4倍和7倍以上。这项工作提出了一种增强界面反应动力学的通用策略,并对涉及气体的电化学反应的电极设计具有指导意义。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Asymmetric electrode design with built-in nitrogen transfer channel achieving maximized three-phase reaction region for electrochemical ammonia synthesis

Asymmetric electrode design with built-in nitrogen transfer channel achieving maximized three-phase reaction region for electrochemical ammonia synthesis

Carbon-free electrochemical nitrogen reduction reaction (NRR) is an appealing strategy for green ammonia synthesis, but there is still a significant performance bottleneck. Conventional working electrode is usually flooded by the electrolyte during the NRR test, and only the surface material could get access to the nitrogen, which inevitably gives rise to sluggish reaction rate. Herein, an asymmetric electrode design is proposed to tackle this challenge. An aerophilic layer is constructed on one face of the electrocatalyst-loaded electrode, while the other side maintains its original structure, aiming to achieve facilitated nitrogen transfer and electrolyte permeation within the conductive skeleton simultaneously. This asymmetric architecture affords extensive three-phase reaction region within the electrode as demonstrated by the combination of theoretical simulations and experimental measurements, which gives full play to the loaded electrocatalyst. As expected, the proof-of-concept asymmetric electrode delivers an NH3 yield rate of 40.81 μg h−1 mg−1 and a Faradaic efficiency of 71.71% at −0.3 V versus the reversible hydrogen electrode, which are more than 4 and 7 times that of conventional electrode, respectively. This work presents a versatile strategy for enhancing the interfacial reaction kinetics and is instructive to electrode design for gas-involved electrochemical reactions.

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