电催化剂
电解质
电极
大规模运输
阴极
化学
氧化还原
扩散
还原(数学)
选择性
大众运输
动力学
纳米技术
化学工程
作者
Haolan Tao,Cheng Lian,Haibo Jiang,Chunzhong Li,Honglai Liu,René Roij
摘要
The electrocatalytic nitrogen reduction reaction (NRR) for NH3 synthesis is still far from being practical and competitive with the common Haber–Bosch process. The rational design of highly selective NRR electrocatalyst is therefore urgently needed, which requires a deep understanding of both the electrode–electrolyte interface and the mass transport of reactants. Here, we develop a theoretical framework that includes electric double layer (EDL), mass transport, and the NRR kinetics. This allows us to evaluate the roles of near-electrode environment and N2 diffusion on the NRR selectivity and activity. The EDL, as the immediate reaction environment, remarkably impedes the diffusion of N2 to the cathode surface at high electrode potentials, which explains experimental observations. This article also gives microscopic insights into the interplay between N2 diffusion and reaction activity under the nano-confinement, providing theoretical guidance for future design of advanced NRR electrocatalytic systems.
科研通智能强力驱动
Strongly Powered by AbleSci AI