Holey Pt Nanosheets on NiFe-Hydroxide Laminates: Synergistically Enhanced Electrocatalytic 2D Interface toward Hydrogen Evolution Reaction

Abstract

Next-generation electrocatalysts with smart integrated designs, maximizing the chemical cascade synergy for sustainable hydrogen production, are needed to address the urgent environmental threats, but scalable synthesis of precisely architectured nanohybrids rendering a few-nanometer interfacial controllability to augment the catalytic reactivity and operational stability is a major bottleneck. Herein, by inventing a surface-confined lateral growth of nanometer-thin and nanoporous two-dimensional (2D)-Pt on NiFe-LDH nanosheets, a highly reactive 2D−2D interfacially integrated nanoplatform is synthesized for an alkaline hydrogen evolution reaction (HER) which not only extracts high Pt-atomic utilization efficiency but also synergistically accelerates the water dissociation and hydrogen generation cascade on the colocalized Pt/M(OH) x active sites, endowing a 6.1-fold higher Pt mass activity than 20% Pt/C and also empowers a record-high HER operational stability for 50 h, due to the chemically enforced lamellar architecture. This work offers a gateway to produce active metal nanosheets tailored with a suitable active-template surface in order to invent and enforce futuristic catalysis technologies.

Ultrasmall Noble Metal Doped Ru2P@Ru/CNT as High-Performance Hydrogen Evolution Catalysts

“…The Nyquist plot (Figure S14) shows that Pt 0.095 –Ru 2 P@Ru/CNT has a much faster charge transfer rate than Ru 2 P@Ru/CNT, Ru 2 P/CNT, and Ru/CNT, implying that Pt 0.095 –Ru 2 P@Ru/CNT has stronger electron transmission ability . Previous studies have shown that metal centers with higher charge density are easier to adsorb H*, while ruthenium phosphide has stronger OH* adsorption energy. ,− Furthermore, Pt can be used as a proton acceptor for H* recombination to produce H 2 . , Therefore, the mechanism infers that water molecules are first decomposed into H* and OH* at the Ru 2 P@Ru interface. Ru 2 P is the adsorption site for OH*, and Ru with higher charge density is the adsorption site for H*, and then, H* transfers to the Pt site to generate and release H 2 .…”

“…40,49−51 Furthermore, Pt can be used as a proton acceptor for H* recombination to produce H 2 . 52,53 Therefore, the mechanism infers that water molecules are first decomposed into H* and OH* at the Ru 2 P@Ru interface. Ru 2 P is the adsorption site for OH*, and Ru with higher charge density is the adsorption site for H*, and then, H* transfers to the Pt site to generate and release H 2 .…”

2D/2D Heterostructures: Rational Design for Advanced Batteries and Electrocatalysis

“…Recently, a surface‐confined lateral growth of 2D porous Pt nanolayer was achieved on 2D NiFe‐LDH nanosheets to produce a highly integrated 2D/2D frame for alkaline HER. [ 174 ] This design considerably increased Pt‐atomic utilization efficiency and boosted the water dissociation for hydrogen generation, inducing an impressive 6.1‐fold mass activity compared to the commercial 20% Pt/C, together with a high HER operational stability for 50 h with only 19 mV potential drop. [ 174 ] The present work offers some hints on improving the stability of HER catalysts by the formation of intimate interfacial contact within 2D‐based heterostructures.…”

Network-Like Platinum Nanosheets Enabled by a Calorific-Effect-Induced-Fusion Strategy for Enhanced Catalytic Hydrogenation Performance

“…The superior catalytic performance endowed by the featuring structure aroused great research interest on the nanofoams ( Zhu et al, 2021 ). Strategies like templating ( Li et al, 2013 ; Tamaki et al, 2015 ; Jang et al, 2020 ) and selective dissolution ( Liu et al, 2009 ) have been successfully employed for the construction of Pt nanofoams. The advance up till now mainly focused on the 3D porous Pt structure, such as porous nanospheres ( Li et al, 2015 ; Jiang et al, 2016a ; Jiang et al, 2016b ), periodic porous structures ( Stein et al, 2008 ; Kim et al, 2013 ; Xu and Zhang, 2014 ), etc.…”