Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans. However, their performance, cost, and durability are significantly related to Pt-based electrocatalysts, hampering their large-scale commercial application. Hence, considerable efforts have been devoted to improving the activity and durability of Pt-based electrocatalysts by controlled synthesis in recent years as an effective method for decreasing Pt use, and consequently, the cost. Therefore, this review article focuses on the synthesis processes of carbon-supported Pt-based electrocatalysts, which significantly affect the nanoparticle size, shape, and dispersion on supports and thus the activity and durability of the prepared electrocatalysts. The reviewed processes include (i) the functionalization of a commercial carbon support for enhanced catalyst–support interaction and additional catalytic effects, (ii) the methods for loading Pt-based electrocatalysts onto a carbon support that impact the manufacturing costs of electrocatalysts, (iii) the preparation of spherical and nonspherical Pt-based electrocatalysts (polyhedrons, nanocages, nanoframes, one- and two-dimensional nanostructures), and (iv) the postsynthesis treatments of supported electrocatalysts. The influences of the supports, key experimental parameters, and postsynthesis treatments on Pt-based electrocatalysts are scrutinized in detail. Future research directions are outlined, including (i) the full exploitation of the potential functionalization of commercial carbon supports, (ii) scaled-up one-pot synthesis of carbon-supported Pt-based electrocatalysts, and (iii) simplification of postsynthesis treatments. One-pot synthesis in aqueous instead of organic reaction systems and the minimal use of organic ligands are preferred to simplify the synthesis and postsynthesis treatment processes and to promote the mass production of commercial carbon-supported Pt-based electrocatalysts. Graphical Abstract This review focuses on the synthesis process of Pt-based electrocatalysts/C to develop aqueous one-pot synthesis at large-scale production for PEMFC stack application.

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Catalyst layer (CL) is the core component of proton exchange membrane (PEM) fuel cells, which determines the performance, durability, and cost. However, difficulties remain for a thorough understanding of the CLs’ inhomogeneous structure, and its impact on the physicochemical and electrochemical properties, operating performance, and durability. The inhomogeneous structure of the CLs is formed during the manufacturing process, which is sensitive to the associated materials, composition, fabrication methods, procedures, and conditions. The state-of-the-art visualization and characterization techniques are crucial to examine the CL structure. The structure-dependent physicochemical and electrochemical properties are then thoroughly scrutinized in terms of fundamental concepts, theories, and recent progress in advanced experimental techniques. The relation between the CL structure and the associated effective properties is also examined based on experimental and theoretical findings. Recent studies indicated that the CL inhomogeneous structure also strongly affects the performance and degradation of the whole fuel cell, and thus, the interconnection between the fuel cell performance, failure modes, and CL structure is comprehensively reviewed. An analytical model is established to understand the effect of the CL structure on the effective properties, performance, and durability of the PEM fuel cells. Finally, the challenges and prospects of the CL structure-associated studies are highlighted for the development of high-performing PEM fuel cells. Graphical abstract

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