Advanced Platinum-Based Oxygen Reduction Electrocatalysts for Fuel Cells.

ConspectusFuel cells are among the cutting-edge energy technologies. Their commercial development is still hindered by noble platinum (Pt) catalysts for the oxygen reduction reaction (ORR) at the cathode, which not only determine the energy conversion efficiency and service life but also are closely related to the cost and broad application of fuel cells. Given the bright and enormous future of fuel cells, ORR catalysts should possess highly efficient performance yet meet the acceptable Pt costs for large-scale application. Extensive efforts are concentrated on the optimization of Pt-based nanostructures and upgradation of functional carriers to achieve the low-cost and high-activity Pt-based catalysts. By improving the Pt utilization and accessible surface, reducing Pt consumption and catalyst costs, accelerating mass exchange and electron transfer, alleviating the corrosion and agglomeration of carriers and Pt, accompanying with the assistance of robust yet effective functional supports, the service level and life of Pt-based electrocatalysts would be significantly improved and fuel cells could get into commercial market covering broader applications.In this Account, we focus on the recent development of Pt-based catalysts to figure out the problems associated with ORR catalysts in fuel cells. Recent development of Pt-based catalysts is discussed in different stages: (1) multiscale development of Pt-based nanostructures; (2) multielement regulation over Pt-based alloy composition; (3) upgradation of carbon and noncarbon support architectures; (4) development of integrated Pt-based catalysts for fuel cells. Finally, we propose some future issues (such as reaction mechanism, dynamic evolutions, and structure-activity relationship) for Pt-based catalysts, which mainly involve the preparation strategy of Pt-integrated catalysts (combination of Pt nanostructures with nanocarbons), performance evaluation (standard measurement protocols, laboratory-level rotating disk electrode (RDE) measurements, application-level membrane electrode assembly (MEA) service test), advanced interpretation techniques (spectroscopy, electron microscopy, and in situ monitoring), and cutting-edge simulation/calculations and artificial intelligence (simulation, calculations, machine learning, big data screening). This Account calls for the comprehensive development of multiscale, multicomponent, and high-entropy Pt-based alloy nanostructures, and novel and stable carriers, which provide more available options for rational design of low-cost and high-performance Pt-integrated ORR catalysts. More importantly, it will give an in-depth understanding of the reaction mechanism, dynamic development, and structure-performance relationship for Pt-based catalysts in fuel cells and related energy technologies.