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<p>Proton exchange membrane fuel cells (PEMFCs), as an efficient and clean energy conversion technology, face one of the core challenges to their commercial application: the sluggish kinetics of the cathodic oxygen reduction reaction (ORR), along with the high cost and limited stability of platinum (Pt)-based catalysts. Density functional theory (DFT) calculations serve as a bridge linking microscopic atomic structure to macroscopic catalytic performance, offering a powerful theoretical tool to deeply understand the ORR mechanism, uncover the origin of catalytic activity, and guide the rational design of high-performance Pt-based alloy catalysts.Based on a review of relevant domestic and international literature, this paper systematically summarizes the application and recent research progress of DFT calculations in the study of the oxygen reduction reaction on platinum-based alloys. It begins by elucidating key physicochemical descriptors derived from DFT calculations, including the adsorption energies of oxygen atoms and related intermediates (O*, OH*, OOH*), the d-band center theory as a core descriptor of electronic structure, surface vacancy formation energy, and the critical role of lattice strain effects in modulating catalytic activity. By synthesizing the current state of research, it also outlines design principles for optimizing catalyst electronic and geometric structures through strategies such as strain engineering. Furthermore, this review discusses the microscopic ORR mechanisms (e.g., dissociative and associative mechanisms) and analyzes the synergistic validation relationship between theoretical predictions and experimental synthesis and performance characterization. Finally, this review summarizes current challenges in the field, including the simplification of computational models and the need to account for solvation effects and dynamic behavior. Future research directions are also outlined, including the integration of high-throughput computing with machine learning, multiscale simulations, and the theoretical interpretation of advanced in-situ characterization techniques, aiming to provide theoretical guidance for designing novel, efficient, stable, and low-cost ORR electrocatalysts.</p>

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Research Progress on Density Functional Theory Calculations of the Oxygen Reduction Reaction on Platinum-Based Alloys

  • 期刊论文

  • 发表日期：

    2026年6月17日

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  • Pengda Dong,
  • Jieqiong Hu,
  • Fuxiang Guan,
  • Shu Ji,
  • Zhifeng Nie,
  • Xiujun Deng,
  • Jiheng Fang,
  • Yi Zhang,
  • Hongxing He

摘要

Proton exchange membrane fuel cells (PEMFCs), as an efficient and clean energy conversion technology, face one of the core challenges to their commercial application: the sluggish kinetics of the cathodic oxygen reduction reaction (ORR), along with the high cost and limited stability of platinum (Pt)-based catalysts. Density functional theory (DFT) calculations serve as a bridge linking microscopic atomic structure to macroscopic catalytic performance, offering a powerful theoretical tool to deeply understand the ORR mechanism, uncover the origin of catalytic activity, and guide the rational design of high-performance Pt-based alloy catalysts.Based on a review of relevant domestic and international literature, this paper systematically summarizes the application and recent research progress of DFT calculations in the study of the oxygen reduction reaction on platinum-based alloys. It begins by elucidating key physicochemical descriptors derived from DFT calculations, including the adsorption energies of oxygen atoms and related intermediates (O*, OH*, OOH*), the d-band center theory as a core descriptor of electronic structure, surface vacancy formation energy, and the critical role of lattice strain effects in modulating catalytic activity. By synthesizing the current state of research, it also outlines design principles for optimizing catalyst electronic and geometric structures through strategies such as strain engineering. Furthermore, this review discusses the microscopic ORR mechanisms (e.g., dissociative and associative mechanisms) and analyzes the synergistic validation relationship between theoretical predictions and experimental synthesis and performance characterization. Finally, this review summarizes current challenges in the field, including the simplification of computational models and the need to account for solvation effects and dynamic behavior. Future research directions are also outlined, including the integration of high-throughput computing with machine learning, multiscale simulations, and the theoretical interpretation of advanced in-situ characterization techniques, aiming to provide theoretical guidance for designing novel, efficient, stable, and low-cost ORR electrocatalysts.