Key Takeaways & Executive Findings
- •• A unique catalyst surface where ultrathin Pt edges are modified by isolated Pd atoms and BiOx adatoms is rationally designed and achieved. • The Pd1/Pt-BiOx electrocatalyst exhibits an ultrahigh mass activity of 16.01 A mg−1 Pt+Pd toward ethanol oxidation and enables a direct ethanol fuel cell of peak power density of 56.7 mW cm−2. • The surrounding BiOx adatoms are critical for mitigating CO-poisoning on Pt surface, and the Pd1/Pt single-atom alloy further facilitates the electrooxidation of CH3CH2OH. • This work offers new insights into the rational design and construction of sophisticated catalyst surfaces at single-atomic sites for highly efficient electrocatalysis.
Abstract
Engineering nanomaterials at single-atomic sites could enable unprecedented catalytic properties for broad applications, yet it remains challenging to do so on the surface of multimetallic nanocrystals. Herein, we present the multifactorial engineering (size, shape, phase, and composition) of the fully ordered PtBi nanoplates at atomic level, achieving a unique catalyst surface where the face-centered cubic (fcc) Pt edges are modified by the isolated Pd atoms and BiOx adatoms. This Pd1/Pt-BiOx electrocatalyst exhibits an ultrahigh mass activity of 16.01 A mg−1 Pt+Pd toward ethanol oxidation in alkaline electrolyte and enables a direct ethanol fuel cell of peak power density of 56.7 mW cm−2. The surrounding BiOx adatoms are critical for mitigating CO-poisoning on the Pt surface, and the Pd1/Pt single-atom alloy further facilitates the electrooxidation of CH3CH2OH. This work offers new insights into the rational design and construction of sophisticated catalyst surface at single-atomic sites for highly efficient electrocatalysis.
1. Introduction
Direct alcohol fuel cells (DAFCs) represent attractive alternatives to hydrogen fuel cells for portable applications, due to their adoption of liquid alcohols (methanol, ethanol, etc.) as fuels, which are more convenient in production, storage, transportation, and refueling. However, the electrooxidations of alcohols are kinetically sluggish processes which suffer from the issues of high overpotentials, intermediates poisoning, and a large dosage of noble metals [1]. Pt is one of the most active monometallic electrocatalysts for alcohol oxidation reactions (AORs), yet commercial Pt catalysts still lack satisfactory catalytic performance for practical DAFCs [2–4].
Engineering multimetallic nanocrystals is one of the most effective strategies to boost AORs electrocatalysis [5–7]. As a notable example, the ternary Pt/Rh/SnO2 electrocatalyst combines the specific properties of its components, consequently enables the alcohol dehydrogenation, C–C bond breaking, and oxidation of dissociated CO, thus facilitating the oxidation of ethanol [8]. However, it remains challenging to control, at atomic-level, the multimetallic ensembles on the surface of catalysts, in order to maximize the multifunctional effects and minimize the usage of noble metals [9–23].
Great progress has been made in developing multimetallic electrocatalysts by tuning the size, shape, phase, composition, and surface of multimetallic nanocatalysts. In this regard, single-atom alloy emerges as a high-performance and low-cost electrocatalyst for broad applications, since it combines the multifunctional effects introduced by alloying with the ultrahigh atom utilization of single-atom catalysis [24]. On the other hand, it is well established that some oxyphilic adatoms (Bi, Pb, Sn, etc.) enable the formation of adsorbed hydroxyl species (–OHad) at lower potentials, which can mitigate the poisoning of CO species on Pt surface [25–31]. Different from the regulation of single structural parameters, i.e., size, shape, phase, composition, or surface, the multifactorial engineering strategy holds promise in developing unprecedented electrocatalysts via constructing well-defined multimetallic ensembles. However, the multifactorial engineering of structural parameters at atomic-level in a nanocrystal still remains as a challenging task [32–45].
In this work, starting from the hexagonal close packed (hcp) PtBi intermetallic nanoplates and via a rational design, we constructed a novel catalyst surface, namely, Pt edges modified by atomically dispersed noble metal atoms (M = Pd, Rh, or Ir) and BiOx adatoms (M/Pt-BiOx).
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Yujia Liao, Wen Chen, Yutian Ding, Lei Xie, Qi Yang, Qilong Wu, Xianglong Liu, Jinliang Zhu, Renfei Feng, Xian-Zhu Fu, Shuiping Luo, Jing-Li Luo (2025). Boosting Alcohol Oxidation Electrocatalysis with Multifactorial Engineered Pd1/Pt Single-Atom Alloy-BiOx Adatoms Surface. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01678-4
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Frequently Asked Questions
What is the main achievement of this research?
The research demonstrates a novel catalyst surface with Pd1/Pt single-atom alloy and BiOx adatoms, achieving ultrahigh mass activity for ethanol oxidation and enabling a direct ethanol fuel cell with high peak power density.
How does the Pd1/Pt-BiOx catalyst mitigate CO poisoning?
The surrounding BiOx adatoms are critical for mitigating CO-poisoning on the Pt surface by facilitating the formation of adsorbed hydroxyl species at lower potentials, which helps oxidize CO intermediates.
What is the significance of multifactorial engineering in this work?
Multifactorial engineering allows simultaneous control of size, shape, phase, and composition at the atomic level, leading to a well-defined catalyst surface that maximizes multifunctional effects and minimizes noble metal usage.
What are the potential applications of this catalyst?
The catalyst is promising for direct alcohol fuel cells, particularly for ethanol oxidation, offering high efficiency and reduced reliance on noble metals.
What is the mass activity reported for ethanol oxidation?
The Pd1/Pt-BiOx electrocatalyst exhibits an ultrahigh mass activity of 16.01 A mg−1 Pt+Pd toward ethanol oxidation in alkaline electrolyte.
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