An Adjacent Atomic Platinum Site Enables Single‐Atom Iron with High Oxygen Reduction Reaction Performance

Abstract

The modulation effect has been widely investigated to tune the electronic state of single‐atomic M‐N‐C catalysts to enhance the activity of oxygen reduction reaction (ORR). However, the in‐depth study of modulation effect is rarely reported for the isolated dual‐atomic metal sites. Now, the catalytic activities of Fe‐N4 moiety can be enhanced by the adjacent Pt‐N4 moiety through the modulation effect, in which the Pt‐N4 acts as the modulator to tune the 3d electronic orbitals of Fe‐N4 active site and optimize ORR activity. Inspired by this principle, we design and synthesize the electrocatalyst that comprises isolated Fe‐N4/Pt‐N4 moieties dispersed in the nitrogen‐doped carbon matrix (Fe‐N4/Pt‐N4@NC) and exhibits a half‐wave potential of 0.93 V vs. RHE and negligible activity degradation (ΔE1/2=8 mV) after 10000 cycles in 0.1 M KOH. We also demonstrate that the modulation effect is not effective for optimizing the ORR performances of Co‐N4/Pt‐N4 and Mn‐N4/Pt‐N4 systems.

Structural revolution of atomically dispersed Mn sites dictates oxygen reduction performance

“…For example, Li et al reported that Co single-atom catalyst can be tailored and optimized by regulating atomic configuration through the modulation of P coordination atoms. [30] Han et al described the modulation effect of Pt-N 4 moiety could bestow the Fe-N 4 on high ORR performance [31]. Research demonstrates the atomic level planar architecture of metal coordinated by four nitrogen atoms supplies as the real active sites [32].…”

Single-atom catalysts: stimulating electrochemical CO2 reduction reaction in the industrial era

“…Previous work showed that most carbon-supported SACs with abundant nitrogen-doped are stable activated single-metal ions to form the homogeneous microcosmic structure of M-N x -C y . The universal methods for synthesizing carbon-supported SACs include molecular skeleton encapsulation, [34][35][36][37][38] impregnation and pyrolysis, [39][40][41] coordination regulation, [42][43][44] and thermal dispersion.…”

Synergistically enhanced single-atomic site catalysts for clean energy conversion

“…4d. 57 They employed zeolite imidazole frameworks (ZIF8s) as N-rich carbon precursors to generate exclusive M-N 4 active sites. Fu et al constructed atomically dispersed Cu@N 4 and Zn@N 4 on a N-doped carbon support (Cu/Zn@NC) by directly pyrolyzing a CuZn-ZIF precursor.…”