Anion/cation-induced strong electronic polarization of N,Fe-CoS2 electrocatalyst to boost efficient oxygen evolution

• Published in: Journal of colloid and interface science 2024-01, Vol.654 (Pt B), p.1089-1097
• Main Authors: Li, Sijun, Ma, Zemian, Fu, Mimi, Luo, Wei, Yu, Yanli, Jiang, Yimin, Shen, Wei, He, Rongxing, Li, Ming
• Format: Article
• Language: English
• Subjects: Anion/cation-codoping; catalysts; catalytic activity; cations; durability; electroplating; N,Fe-CoS2; OER; oxidation; oxygen production; Strong electronic polarization; Ultra-low overpotential
• ISSN: 0021-9797; 1095-7103; 1095-7103
• DOI: 10.1016/j.jcis.2023.10.104

[Display omitted] •A high-performance anion/cation-codoped Co-based catalyst for OER was constructed.•Anion and cation induced synergistically a strong surface electronic polarization.•N,Fe-CoS2 acquired an ultra-low OER overpotential of 261 mV at 300 mA∙cm−2. Designing and developing the high activity and long-term durability electrocatalysts for oxygen evolution reaction (OER) has primary significance for breaking the bottleneck of water electrolysis. Herein, an anion/cation-codoped CoS2 based electrocatalyst, N,Fe-CoS2, for the efficient OER was constructed via two-step electrodeposition and low-temperature calcination. The anion and cation optimized significantly the surface electronic structure of N,Fe-CoS2 and induced synergistically a strong surface electronic polarization along with the generation of abundant Co3+ active sites, which improved considerably the intrinsic catalytic activity. The doping N anion also hindered effectively the catalyst surface oxidation and enhanced the catalytic durability. Benefiting from these, N,Fe-CoS2 exhibited the outstanding OER activity and catalytic durability, and especially at a high current density, acquired its ultra-low OER overpotential of 261 mV at 300 mA∙cm−2 and maintained continuously a stable current density for 80 h without visible attenuation at 100 mA∙cm−2. DFT calculations confirmed the cooperative effect of N anions and Fe cations on improving catalytic activity and unveiled that Fe cations in N,Fe-CoS2 acted a key role in modulating electron densities instead of acting as catalytic sites. This work has an important implication for realizing the synergistic regulation of electron densities of catalytic materials by anions and cations.