The relentless depletion of global fossil energy reserves, coupled with the pressing challenge of exorbitant extraction costs, renders the development of novel, clean, efficient, and sustainable energy conversion technologies an urgent imperative
[1−3]. Among the numerous strategies addressing the energy crisis, direct ethylene glycol fuel cells (DEGFCs) stand out due to their unique advantages
[4−5]. As the core fuel for DEGFCs, ethylene glycol exhibits a host of notable characteristics. It can be sustainably synthesized
via the catalytic conversion of biomass-derived compounds such as glycerol and cellulose. This synthetic approach endows the feedstock with renewability, thereby ensuring the sustainability of energy supply at the source
[6]. Furthermore, ethylene glycol possesses a high theoretical capacity of 4.8 A·h/mL, which provides a robust material basis for the construction of high-efficiency energy systems
[7]. Nevertheless, the cleavage of the C−C bond along with the incomplete electrooxidation of ethylene glycol (EG) poses substantial hurdles to the practical commercialization of DEGFCs.
The electrocatalytic ethylene glycol oxidation reaction (EGOR), a critical process in DEGFCs, directly influences overall cell efficiency and application prospects. However, this reaction system faces complex challenges. Structurally, EG contains two hydroxyl groups, resulting in an intricate oxidation pathway
[8]. In general, the oxidation process of EGOR proceeds
via two distinct pathways, C
1 and C
2. Specifically, the C
1 pathway involves a complete cleavage of the C−C bond accompanied by a 10 e
− transfer, yielding CO
2 and its derivatives (
${\mathrm{CO}}_3^{2-} $
,
${\mathrm{HCO}}_3^{-} $
, HCOO
−). In contrast, the C
2 pathway corresponds to the incomplete oxidation of ethylene glycol with a 4e
−/8e
− transfer, where the primary products are glycolic acid or oxalic acid
[9−10]. Notably, the C
1 pathway exhibits more pronounced advantages over the C
2 pathway, releasing higher electrical energy. Alloying active noble metals (Pd, Pt) with other noble metals (Ir, Ag, Ru) or non-noble metals is a feasible strategy to promote the C
1 pathway, as it optimizes the catalyst’s electronic structure and facilitates C−C bond oxidative cleavage for C1 product formation
[11]. However, conventional Pt-based and Pd-based EGOR catalysts suffer from suboptimal active site distribution, low product selectivity, and poor stability
[12−13].
In this context, high-entropy alloys (HEAs), as an innovation in materials science, present new opportunities for EGOR. Typically composed of five or more principal elements in near-equiatomic ratios (5%–35%), HEAs exhibit lattice distortion, sluggish diffusion, and a “cocktail” effect, which confer unique properties and demonstrate potential for applications in fields such as catalysis
[14−17]. For instance, Liu et al.
[18] prepared defect-rich FeCoNiMnRu HEAs
via rapid Joule heating. Han et al.
[19] reported a facile co-reduction method to synthesize ultrathin PtPdRuFeCoNi HEA nanowires (NWs) with an average diameter of only 1.36 ± 0.05 nm, which exhibited notable catalytic performance in HER and MOR. Wang’s team designed a class of PtIrRhCoFeNiCu HEA nanodendrites using a simple wet-chemical method; the introduction of transition metals enhanced lattice distortion and facilitated complete C−C bond cleavage during ethanol oxidation
[20]. Existing studies indicate that HEA synthesis often requires elevated temperatures to overcome kinetic limitations, while the material morphology is constrained by the incorporated metals and morphology-directing agents
[21].
In this work, leveraging the morphology-directing effect of CTAB and CTAC, PtPdRuRhCuMo high-entropy alloy nanoparticles (HEA NPs) were successfully synthesized via a facile solvothermal method. These nanoparticles exhibit the characteristics of excellent dispersibility, uniform size distribution and high charge separation efficiency, which provide a structural basis for enhancing the reaction activity and stability. The as-prepared electrocatalyst demonstrates outstanding electrocatalytic performance toward the EGOR in an alkaline medium, which is significantly superior to that of the conventional commercial Pt/C catalyst. Among the synthesized samples, HEA-1 (using CTAB as the surfactant) achieves the optimal catalytic activity with a mass activity of 2.4 A/mg for EGOR. More importantly, HEA-1 exhibits remarkable durability in the long-term stability test, which is attributed to the strong interactions between different metals and the excellent dispersibility of the nanoparticles. This study provides a novel strategy for the precise morphology regulation of PtPdRuRhCuMo HEA NPs and expands their potential application scenarios in related fields.