Polyethylenimine-Ethylenediamine-Induced Pd Metallene toward Alkaline Oxygen Reduction

Abstract

Designing two-dimensional (2D) materials functionalized with organic molecules is an effective tactic to enhance catalytic performances for the oxygen reduction reaction (ORR). Herein, we synthesize Pd metallene with in situ modification of polyethylenimine-ethylenediamine (Pd@PEI-EDA metallene), in which PEI-EDA serves as both the structure-directing agent and modifier. Pd@PEI-EDA metallene has ample active sites and tuneable electronic structures due to ultrathin nanosheets with abundant wrinkles and interfacial structure. In contrast with commercial Pd/C and Pt/C, Pd@PEI-EDA metallene displays preferable catalytic ORR performance under alkaline conditions. This work offers an in situ interface engineering tactic for the preparation of 2D polymer-metal electrocatalysts to boost the ORR performance.

Platinum Alloys for Methanol Oxidation Electrocatalysis: Reaction Mechanism and Rational Design of Catalysts with Exceptional Activity and Stability

“…In recent years, noble metal-based metallenes have emerged as a highly efficient class of two-dimensional electrocatalysts owing to their considerably high atomic utilization, specific surface area, and exposure to active sites [38][39][40][41][42][43][44][45][46][47][48]. The optimized contact of the electrocatalysts with supports is also guaranteed through the construction of such twodimensional materials.…”

“…On the other hand, their crimped structure, which is suggestive of electronic modulation and the inner strain effect, may play a crucial role in enhancing the tolerance toward poisoning species (such as CO ads ) due to weakened adsorption strength. Wu In recent years, noble metal-based metallenes have emerged as a highly efficient class of two-dimensional electrocatalysts owing to their considerably high atomic utilization, specific surface area, and exposure to active sites [38][39][40][41][42][43][44][45][46][47][48]. The optimized contact of the electrocatalysts with supports is also guaranteed through the construction of such twodimensional materials.…”

Crystalline–Amorphous Heterophase PdMoCrW Tetrametallene: Highly Efficient Oxygen Reduction Electrocatalysts for a Long-Term Zn–Air Battery

“…The introduction of high-valence metals is a well-established approach toward optimizing the adsorption on the catalyst surface and promoting the breaking of the H–OH bond from H 2 O molecules, thereby providing protons for the formation of OOH* or OH*. − Moreover, interface engineering is considered an effective strategy to enhance the ORR performance. The construction of crystalline–amorphous heterophase structures fully combines the advantages of crystalline (e.g., high conductivity and definite structure) and amorphous (e.g., abundant surface dangling bonds and highly unsaturated coordination) structures and induces a bandgap energy mismatch and spontaneous Fermi level equilibrium, which act as additional active sites to promote carrier transport and optimize interfacial polarization. − Recently, metallenes have attracted widespread attention as a result of their unique electronic structures and physical properties for the ORR. − The ultrathin two-dimensional (2D) structure of metallenes provides a high specific surface area and high atomic utilization. , Moreover, the quantum size effect caused by the curved structure effectively adjusts the d-band orbital overlap of the catalyst . Nevertheless, previous studies have predominantly concentrated on bi- and trimetallenes, whereas crystalline–amorphous heterophase tetrametallenes have not yet been reported.…”