Synergistic Promotion of Single-Atom Co Surrounding a PtCo Alloy Based On a g-C₃N₄ Nanosheet for Overall Water Splitting

Abstract

Atomically dispersed catalysts with maximum efficiencies for atom utilization have emerged as a frontier in the catalytic field. However, single-component monatomic catalysts are rarely reported for the overall photocatalytic water splitting reaction (OWS). Herein, a two-component synergistic photocatalyst was designed that contained a dispersion of single-atom Co (CoSAs) centers and PtCo alloy nanoparticles (Nps), which were supported over C3N4 nanosheets. Among these components, CoSAs centers act as highly active sites for the hydrogen evolution reaction (HER), and PtCo alloys act as highly active sites for the oxygen evolution reaction (OER). A synergistic effect between them occurs when the two different reactive centers are combined, indicating that there may be a spillover phenomenon of protons or hydroxyl groups between the CoSAs centers and PtCo alloy NPs. The synergistic promotion of CoSAs centers and PtCo alloys bridges the gap between achieving maximum atom utilization and optimal bifunctional activities for OWS reactions. This combination provides a promising model for the development of OWS by atomically dispersed catalysts.

An electron-hole rich dual-site nickel catalyst for efficient photocatalytic overall water splitting

“…As we all know, the ΔG H* of an ideal HER catalyst should be close to 0, which indicates that the catalysts are hard to poison. For Ni 2 P@PCOS, the high positive ΔG H* of the O site and PN sites (0.27 eV and 0.10 eV) suggest that the HER on the PCOS surface is nonspontaneous and needs to absorb a lot of energy to initiate 50 . However, it was discovered that the hydrogen-binding energies on the top of NiS site by −0.051 eV are much thermo-neutral and almost as efficient as Pt for the evolution of H 2 (in Fig.…”

Unraveling Structural Carboxyl Defects in g‐C3N4 for Improved Photocatalytic H2 Evolution via Alternating Hydrogen‐Oxygen‐Plasma Treatment

“…Distinguishing these issues in future work is a high priority. [ 38,39 ] Overall, the photocatalytic H 2 evolution results reveal a significantly boosted g‐C 3 N 4 photocatalytic performance over the carboxyl‐defective H 2 ‐O 2 ‐pCN photocatalyst produced by the two‐step plasma synthesis strategy.…”

Single-atom catalysts for energy conversion

“…Water splitting (H 2 O (l) / H 2 (g) + 1 2 O 2 (g), DG = +237.2 kJ mol −1 ) is considered to be the most promising and sustainable method for H 2 production. 58 This method is green given that only H 2 O is employed as the raw material, sunlight as the driving force, and no polluting gases are emitted. Photocatalytic H 2 O splitting involves two half-reactions, namely, the reduction reaction in the CB and the oxidation reaction in the VB of photocatalysts.…”