S-Doping Promotes Pyridine Nitrogen Conversion and Lattice Defects of Carbon Nitride to Enhance the Performance of Zn–Air Batteries

Abstract

The efficient operation of Zn−air batteries (ZABs) requires highly active and stable reversible air catalysts. Studies have shown that heteroatom-doped carbonaceous nanomaterials are effective metal-free electrocatalysts for the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR). Herein, we design a facile and scalable catalyst doping scheme to manufacture S-doped carbon nitride (S-C 3 N 4 ). Surprisingly, this metal-free catalyst exhibits excellent OER and ORR electrocatalytic activities in alkaline electrolytes, being comparable to those of commercial Pt/C. For the first time, it is proved by experiments that S doping can not only effectively increase the lattice defects of C 3 N 4 but also promote the conversion of pyrrolic nitrogen to pyridine nitrogen, thereby enhancing the bifunctional catalytic activity (OER and ORR). When the catalyst is used as an air electrode for rechargeable ZABs, its performance is obviously better than that provided by commercial Pt/C. Our findings and material design strategies are expected to provide new ideas for the synthesis of various high-performance carbon-based electrocatalysts.

Modified graphene foam as a high-performance catalyst for oxygen reduction reaction

“…29 In another case, pyridinic-N enhances activity in the oxygen reduction reaction and, in combination with another heteroatom, may also effectively contribute to the use of materials as catalysts for additional application. 30–32…”

“…29 In another case, pyridinic-N enhances activity in the oxygen reduction reaction and, in combination with another heteroatom, may also effectively contribute to the use of materials as catalysts for additional application. [30][31][32] Electrochemical performance Catalytic activity is an extremely important parameter when evaluating electrocatalysts determined by cyclic voltammetry (CV) and linear sweep voltammetry (LSV). The potential application of the obtained electrocatalysts was investigated in relation to oxygen reduction reaction, which is a crucial reaction in metal-air batteries or fuel cells.…”

Bifunctional Single Atom Catalysts for Rechargeable Zinc–Air Batteries: From Dynamic Mechanism to Rational Design

“…[98,[209][210][211] Moreover, defective sites (e.g., vacancies, edge defects, topological defects) in carbon matrix were also verified as efficient active sites toward bifunctional oxygen electrocatalysis. [212,213] Thus, defective sites in carbon matrix could also behave as active sites, contributing to improved bifunctional activities.…”

(B, N)‐Rich B−C−N Nanosheet‐assembled Microwires as Effective Electrocatalysts for Oxygen Reduction Reaction

“…The authors have cited additional references within the Supporting Information. [27,28,[53][54][55][56][57][58][59][60][61][62][63][64][65][66][67][68][69]…”