A General Strategy Based on Hetero‐Charge Coupling Effect for Constructing Single‐Atom Sites

Abstract

AbstractSingle‐atom catalysts have emerged as cutting‐edge hotspots in the field of material science owing to their excellent catalytic performance brought about by well‐defined metal single‐atom sites (M SASs). However, huge challenges still lie in achieving the rational design and precise synthesis of M SASs. Herein, we report a novel synthesis strategy based on the hetero‐charge coupling effect (HCCE) to prepare M SASs loaded on N and S co‐doped porous carbon (M1/NSC). The proposed strategy was widely applied to prepare 17 types of M1/NSC composed of single or multi‐metal with the integrated regulation of the coordination environment and electronic structure, exhibiting good universality and flexible adjustability. Furthermore, this strategy provided a low‐cost method of efficiently synthesizing M1/NSC with high yields, that can produce more than 50 g catalyst at one time, which is key to large‐scale production. Among various as‐prepared unary M1/NSC (M can be Fe, Co, Ni, V, Cr, Mn, Mo, Pd, W, Re, Ir, Pt, or Bi) catalysts, Fe1/NSC delivered excellent performance for electrocatalytic nitrate reduction to NH3 with high NH3 Faradaic efficiency of 86.6 % and high NH3 yield rate of 1.50 mg h−1 mgcat.−1 at −0.6 V vs. RHE. Even using Fe1/NSC as a cathode in a Zn‐nitrate battery, it exhibited a high open circuit voltage of 1.756 V and high energy density of 4.42 mW cm−2 with good cycling stability.