Atomically Dispersed Selenium Sites on Nitrogen‐Doped Carbon for Efficient Electrocatalytic Oxygen Reduction

Abstract

Owing to their unique electronic structure and maximum atom utilization efficiency, single‐atom catalysts have received widespread attention and exhibited efficient activity. Herein, we report the preparation of non‐metal Se single atoms embedded in nitrogen‐doped carbon (NC) via a high‐temperature reduction strategy for electrocatalytic oxygen reduction reaction (ORR). Selenium dioxide is reduced to selenium by NC at high temperature and partially anchored to form C−Se−C bond. Impressively, the obtained single‐atom catalyst exhibits outstanding ORR activity and stability that even surpasses state‐of‐the‐art noble metal catalysts and many previously reported nanocatalysts. Experimental and theoretical calculations reveal that the Se single atoms can serve as the ORR active sites and contribute to lowering the reaction barrier. Our discoveries demonstrate the promising prospects for utilizing metal‐free single‐atom‐based materials for efficient electrocatalysis.

Pt3Co/Co Composite Catalysts on Porous N-Doped Carbon Support Derived from ZIF-67 with Enhanced HER and ORR Activities

“…This would improve the conductivity of the material , reduce the charge transfer resistance of the electrochemical reaction, and is beneficial to the electrochemical reaction. 34 X-ray photoelectron spectroscopy (XPS) was performed to examine the valence distribution of each element of the catalyst. The Pt 4f spectra of Pt 3 Co/Co@C catalysts at different heat treatment temperatures are shown in Figure 2d, where Pt 4f was found to be decomposed into two peaks, Pt 4f 7/2 and 4f 5/2 .…”

“…As the temperature increases, the I D / I G values shrink and the degree of graphitization of the carbon support increases, resulting in less structural defects and disorder of the support. This would improve the conductivity of the material , reduce the charge transfer resistance of the electrochemical reaction, and is beneficial to the electrochemical reaction …”

Pyridinic nitrogen dominated doping on Pd/carbon catalysts for enhanced hydrogenation performance

“…However, NC as the supports of Pd nanoparticles exhibited well dispersed with D Pd higher than 25%. Previous studies indicated that carbon materials with N doping favored well dispersion of metal nanoparticles compared to the un-doped ones ( Shen et al, 2019 ; Hu et al, 2022 ). For example, Warczinski et al has confirmed that loading of Pd on N-doped mesoporous carbon leaded to a better dispersion of Pd compared to those for Pd supported on N-free mesoporous carbon ( Warczinski et al, 2020 ).…”

Metal-Free SeBN Ternary-Doped Porous Carbon as Efficient Electrocatalysts for CO2 Reduction Reaction

“… 19 Furthermore, some promising but very preliminary studies showed that Se-doped carbon materials are electrochemically active, e.g., in water splitting and hydrogen production, 20 , 21 where the study of CO 2 RR is scarce. 22 It is noteworthy that the introduction of Se atoms together with other heteroatoms (e.g., N) simultaneously into the carbon skeleton may adjust the charge distribution both on the pristine carbon surface and in the bulk in a broad scope, as the large-sized Se atoms are believed to be bonded preferentially on the rim of the carbon matrix to modulate the surface properties of carbon frameworks, and the N is more effective in changing the bulk properties of carbon due to its similar atomic size to carbon. Thereby, simultaneous doping of carbons with Se and other elements may open up more structural possibilities for electrocatalysis.…”

“…In addition, Se doping can introduce extra catalytically active centers to tune the charge redistribution among carbon atoms, which are beneficial to tailor the electrical transport property of a carbon skeleton . Furthermore, some promising but very preliminary studies showed that Se-doped carbon materials are electrochemically active, e.g., in water splitting and hydrogen production, , where the study of CO 2 RR is scarce . It is noteworthy that the introduction of Se atoms together with other heteroatoms (e.g., N) simultaneously into the carbon skeleton may adjust the charge distribution both on the pristine carbon surface and in the bulk in a broad scope, as the large-sized Se atoms are believed to be bonded preferentially on the rim of the carbon matrix to modulate the surface properties of carbon frameworks, and the N is more effective in changing the bulk properties of carbon due to its similar atomic size to carbon.…”