Bimetallic diatomic nanoclusters with longitudinal Fe–O–Fe units and latitudinal Cu–S–Fe–S–Cu units as efficient ORR active sites

Abstract

In this work, Fe-Cu diatomic nanoclusters (Fe-Cu DA-NCs) with sizes of 0. 5 ~ 2.5 nm loaded in porous carbons (denoted as Fe-Cu DA-NC/C) were successfully prepared by virtue of...

Atomic‐Level Regulation of Cu‐Based Electrocatalyst for Enhancing Oxygen Reduction Reaction: From Single Atoms to Polymetallic Active Sites

“…[51] Copyright 2021, Elsevier; Reproduced with permission. [52] Copyright 2022, Royal Society of Chemistry; Reproduced with permission. [53] Copyright 2023, Wiley-VCH.…”

“…The coupling of N and S atoms with different electronegativities can modulate the electronic structure of Cu atoms, modulating the reaction free energy of intermediate adsorption and thus improving the catalytic efficiency of ORR. Li et al [52] modified the electronic structure of the active site in the Fe-CuDA-NC/C catalyst by doping with S and O heteroatoms to achieve a balance between O 2 adsorption and product desorption with d-band center optimization, which in turn improved the ORR catalytic activity. The E 1/2 of 0.95 V (vs RHE) for Fe-CuDA-NC/C in an O 2 -saturated 0.1 m KOH solution was superior to that of the commercial Pt/C catalyst (E 1/2 of 0.89 V (vs RHE)).…”

“…Copyright 2020, Wiley-VCH; Reproduced with permission [51]. Copyright 2021, Elsevier; Reproduced with permission [52]. Copyright 2022, Royal Society of Chemistry; Reproduced with permission [53].…”

Unified ORR mechanism criteria via charge–spin–coordination of Fe functional units

“…To put it bluntly, the high utilization efficiency of active Fe components is realized in an absolute sense. 51,[189][190][191] However, the following controversies still exist in the study of NCs: (1) as a metastable state, it is difficult to accurately regulate the atomic numbers and particle sizes of NCs in the carbonization process; (2) different types of NCs exhibit different synergistic catalytic mechanisms with FeN 4 sites due to structural differences; (3) inhibiting the dissolution of Fe-NCs under acidic conditions is the key to achieving the balance between enhanced activity and stability for the ORR. Therefore, elucidating the specific mechanism of NCs is particularly meaningful for realizing the efficient utilization of Febased components in catalysis.…”

Strengthening oxygen reduction activity based on the cooperation of pyridinic-N and graphitic-N for atomically dispersed Fe sites

“…1–3 However, the practical application of these devices has been limited by the oxygen reduction reaction (ORR) because of the slow reaction kinetics induced by the slow multi-electron transfer process. 4–6 In this regard, Pt-based catalysts are generally considered as efficient electrocatalysts for the ORR, but their expensive cost and inadequate stability are limitations to their widespread use. 7,8 Thus, a long-standing frontier problem has been the development of low-cost, highly active, and long-lasting non-precious metal catalysts for the ORR towards advancing the applicability of conversion devices.…”