Key Takeaways & Executive Findings
- •• • Grain boundary engineering in HENCs enhances catalytic activity by providing abundant active sites; e.g., Pt-based nanocrystals with controlled grain boundaries exhibit up to 10-fold increase in mass activity for ORR compared to commercial Pt/C. • • Single-atom alloys (SAAs) maximize noble metal utilization; Pt single atoms on Cu supports achieve 100% CO selectivity in CO2RR at -0.5 V vs. RHE, with turnover frequency (TOF) of 0.8 s^-1. • • Intermetallic compounds with ordered structures improve stability; PtCo intermetallic nanoparticles retain 92% of initial activity after 30,000 potential cycles in acidic media, outperforming disordered alloys. • • Amorphous HENCs exhibit superior corrosion resistance; amorphous Pd-based catalysts maintain 95% H2O2 selectivity over 10 h operation, demonstrating potential for industrial electrosynthesis.
Abstract
High-entropy noble-metal-based catalysts (HENCs) have emerged as a frontier in electrocatalysis, leveraging the synergistic effects of high-entropy alloys and noble metals to achieve exceptional atomic utilization, tunable electronic structures, and vast compositional space. Their anisotropic architectures confer superior dissolution resistance, rapid electron/mass transfer, and abundant active sites. This review systematically categorizes advanced structural regulations—grain boundary engineering, single-atom alloys, intermetallic compounds, amorphous structures, and core@shell configurations—and evaluates their impact on electrocatalytic performance. By modulating surface electronic states and lattice strain, these strategies optimize reaction kinetics and durability. Notable applications include oxygen reduction (ORR), oxygen evolution (OER), hydrogen evolution (HER), and CO2 reduction (CO2RR). Despite progress, challenges persist in scalable synthesis, mechanistic understanding, and long-term stability. This review underscores the potential of HENCs to bridge laboratory innovation and industrial deployment, providing a roadmap for future catalyst design.
1. Introduction
Conventional electrocatalysts, primarily based on monometallic noble metals like Pt, Pd, and Ir, suffer from prohibitive cost, limited reserves, and inadequate stability under harsh operational conditions. Their catalytic performance is often compromised by surface oxidation, Ostwald ripening, and dissolution, leading to rapid degradation in fuel cells and electrolyzers. The need for high-performance, durable, and cost-effective catalysts has driven exploration into multi-metallic systems, yet traditional alloys face phase segregation and limited compositional tunability.
High-entropy alloys (HEAs), comprising five or more principal elements in near-equimolar ratios, offer a paradigm shift. Their unique high-entropy effect stabilizes single-phase solid solutions, while lattice distortion and cocktail effects create diverse active sites and tunable electronic structures. By incorporating noble metals into HEAs, high-entropy noble-metal-based catalysts (HENCs) combine the benefits of both: enhanced activity and stability. This review addresses the critical bottleneck of structural regulation in HENCs, presenting advanced design strategies that optimize catalytic performance for key electrochemical reactions, thereby bridging the gap between fundamental research and practical energy conversion technologies.
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Yangping Zhang, Xiyue Zhang, Fei Gao, Xiaoqing Huang (2026). High-Entropy Noble-Metal-Based Nanostructures with Advanced Regulations for Electrocatalysis. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-026-4258-0
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Frequently Asked Questions
What are the primary degradation mechanisms of HENCs under prolonged operation, and how do structural regulations mitigate them?
HENCs degrade via metal dissolution, Ostwald ripening, and surface oxidation. Intermetallic ordering and core@shell structures enhance stability by lowering surface energy and providing protective shells. For instance, PtCo intermetallic nanoparticles retain 92% activity after 30,000 cycles, while amorphous Pd-based catalysts show 95% H2O2 selectivity over 10 h.
How do HENCs achieve cost parity with conventional catalysts despite high noble metal content?
By maximizing atomic utilization through single-atom alloys and ultra-small nanostructures, HENCs reduce noble metal loading. For example, Pt single atoms on Cu supports achieve high CO2RR selectivity at low Pt content, lowering material costs. Additionally, enhanced durability extends catalyst lifetime, reducing replacement frequency.
What are the scalability bottlenecks for HENC synthesis, and what methods are proposed?
Scalable synthesis remains challenging due to the need for precise compositional control and uniform morphology. Methods like flash thermal shock and high-pressure synthesis offer rapid, scalable routes. However, achieving uniform mixing at industrial scales requires further optimization of precursor chemistry and processing parameters.
How do amorphous HENCs compare to crystalline counterparts in terms of catalytic activity and stability?
Amorphous HENCs exhibit higher activity due to abundant unsaturated sites and enhanced tolerance to structural strain. For instance, amorphous Pd-based catalysts show superior H2O2 electrosynthesis selectivity (95%) and stability over 10 h, outperforming crystalline Pd. However, their thermal stability may be lower, necessitating careful operational temperature control.
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