Single-Atom Au/NiFe Layered Double Hydroxide Electrocatalyst: Probing the Origin of Activity for Oxygen Evolution Reaction

Abstract

A fundamental understanding of the origin of oxygen evolution reaction (OER) activity of transition-metal-based electrocatalysts, especially for single precious metal atoms supported on layered double hydroxides (LDHs), is highly required for the design of efficient electrocatalysts toward further energy conversion technologies. Here, we aim toward single-atom Au supported on NiFe LDH (Au/NiFe LDH) to clarify the activity origin of LDHs system and a 6-fold OER activity enhancement by 0.4 wt % Au decoration. Combining with theoretical calculations, the active behavior of NiFe LDH results from the in situ generated NiFe oxyhydroxide from LDH during the OER process. With the presence ofAu, Au/NiFe LDH possesses an overpotential of 0.21 V in contrast to the calculated result (0.18 V). We ascribe the excellent OER activity ofAu/NiFe LDH to the charge redistribution of active Fe as well as its surrounding atoms causing by the neighboring Au on NiFe oxyhydroxide stabilized by interfacial CO and HO interfacing with LDH.

The Multifaceted Reactivity of Single‐Atom Heterogeneous Catalysts

“…[10] Aided by synthetic and analytical advancements,ahuge range of potential host materials has now been reported (Figure 2), which encompasses metal oxides, [11][12][13][14] metal hydroxides, [15,16] metals (also termed single-atom alloys (SAAs)), [17,18] micro/ mesoporous materials such as zeolites, [19,20] metal-organic frameworks (MOFs), [21,22] silicas, [23,24] carbon-based materials, [25][26][27][28] organopolymers, [29,30] nitrides, [31][32][33] and carbides. [10] Aided by synthetic and analytical advancements,ahuge range of potential host materials has now been reported (Figure 2), which encompasses metal oxides, [11][12][13][14] metal hydroxides, [15,16] metals (also termed single-atom alloys (SAAs)), [17,18] micro/ mesoporous materials such as zeolites, [19,20] metal-organic frameworks (MOFs), [21,22] silicas, [23,24] carbon-based materials, [25][26][27]…”

NiFe Alloy Nanoparticles with hcp Crystal Structure Stimulate Superior Oxygen Evolution Reaction Electrocatalytic Activity

“…Additionally,t he excellent OER catalytic activity is superior to most reported state-of-the-art catalysts (Table S3). [20] TheF aradaic efficiencyofhcp-NiFe@NC was tested in agastight electrochemical cell and derived up to % 90.6 % ( Figure S11). As shown in Figure S10, hcp-NiFe@NC doesntd isplay obvious redox peaks at corresponding potential under ascan rate of 10 mV s À1 ,which is different from the reference sample of NiFeN P. This observation suggested that there were no amorphous metallic oxides formed in OER with hcp-NiFe@NC as catalyst.…”

Mono‐/Multinuclear Water Oxidation Catalysts

“…[14] Am ixture of manganese chloride andg raphene oxide (GO) is annealed under an NH 3 atmosphere.T hen, the target product is successfully obtained after acid treatment. [37] In addition, Cao and coworkers used this methodt os ynthesize iron-based films, which exhibited high-efficiency OER performance under neutral conditions. Pan et al successfully synthesized at rifunctional catalystw ith the FeÀN 4 site, which had the ability to catalyze the OER.…”

“…Recently,t he Au/NiFe LDH, which shows ab etter OER performance than that of NiFe LDH, was introduced by Zhang et al [37] The potential (237 mV) of Au/NiFe LDH is smaller than that of NiFe LDH at 10 mA cm À2 in 1.0 m KOH. However,s ingleatom gold can improvea tomu tilization and reduce cost.…”