Proton exchange membrane fuel cells (PEMFCs) with high efficiency and nonpollution characteristics have attracted massive attention from both academic and industrial communities due to their irreplaceable roles in building the future sustainable energy system. However, the stability issue of Pt-based catalysts for oxygen reduction reaction (ORR) has become a central constraint to the widespread deployment of the devices relative to the catalytic activity. This review aims to provide comprehensive insights into how to improve the stability of Pt-based catalysts for ORR. First, the basic physical chemistry behind the catalyst degradation, including the fundamental understandings of carbon corrosion, catalyst dissolution, and particle sintering, is highlighted. After a discussion of advanced characterization techniques for the catalyst degradation, the design strategies for improving the stability of Pt-based catalysts are summarized. Finally, further insights into the remaining challenges and future research directions are also provided.

Stabilizing Pt-Based Electrocatalysts for Oxygen Reduction Reaction: Fundamental Understanding and Design Strategies.

The energy crisis and climate change are growing threats to human society. Fuel cells and electrolyzers using solar and wind as energy sources provide a promising carbon-free and sustainable energy future as an alternative to the present fossil fuels. Robust and efficient electrocatalysts constitute the cornerstone for practical applications of fuel cells and electrolyzers. However, their rational design is hindered by the lack of knowledge of the active site structures, the reaction pathways, and the degradation mechanisms. This calls for the operando characterization of the electrode–electrolyte–gas interface of electrocatalytic processes under working conditions. This review describes the understanding of various operando techniques for diverse nano-, molecular and single atom electrocatalysts. We highlight the progress achieved via operando techniques toward the elucidation of the structure–activity relationships of electrocatalysts.

Operando characterization techniques for electrocatalysis

Transition metal carbides and nitrides are interesting non-precious materials that have been shown to replace or reduce the loading of precious metals for catalyzing several important electrochemical reactions. The purpose of this review is to summarize density functional theory (DFT) studies, describe reaction pathways, identify activity and selectivity descriptors, and present a future outlook in designing carbide and nitride catalysts for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), nitrogen reduction reaction (N2RR), CO2 reduction reaction (CO2RR) and alcohol oxidation reactions. This topic is of high interest to scientific communities working in the field of electrocatalysis and this review should provide theoretical guidance for the rational design of improved carbide and nitride electrocatalysts.

Density functional theory studies of transition metal carbides and nitrides as electrocatalysts.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/ese3.833

Recent advances in graphene‐based materials for fuel cell applications

The electrocatalytic splitting of water holds great promise as a sustainable and environmentally friendly technology for hydrogen production. However, the sluggish kinetics of the oxygen evolution reaction (OER) at the...

Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices

Tuning the compositions and structures of Pd-based nanomaterials and their supports has shown great potentials in facilitating the sluggish ethanol oxidation reaction (EOR) in alkaline direct ethan...

Composition-Graded Cu–Pd Nanospheres with Ir-Doped Surfaces on N-Doped Porous Graphene for Highly Efficient Ethanol Electro-Oxidation in Alkaline Media

The activity degradation mechanism of Pt/C and PtCo/C electrocatalysts in proton-exchange membrane fuel cells during the accelerated degradation test (ADT) was directly investigated by the in situ ...

Comparative Investigation on the Activity Degradation Mechanism of Pt/C and PtCo/C Electrocatalysts in PEMFCs during the Accelerate Degradation Process Characterized by an in Situ X-ray Absorption Fine Structure

The development of highly active nitrogen-doped carbon-based transition metal (M-N-C) compounds for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) greatly helps reduce fuel cell cost, thus rapidly promoting their commercial applications. Among different M-N-C electro-catalysts, the series of Fe-N-C materials are highly favored because of their high ORR activity. However, there remains a debate on the effect of Fe, and rare investigations focus on the influence of Fe addition in the second heat treatment usually performed after acid leaching in the catalyst synthesis. It is thus very critical to explore the influences of Fe on the ORR electrocatalytic activity, which will, in turn, guide the design of Fe-N-C materials with enhanced performance. Herein, a series of Fe-N-C electrocatalysts are synthesize and the influence of Fe on the ORR activity are speculated both experimentally and theoretically. It is deduced that the active site lies in the structure of Fe-N4, accompanied with the addition of appropriate Fe, and the number of active sites increases without the occurrence of agglomeration particles. Moreover, it is speculated that Fe plays an important role in stabilizing N as well as constituting active sites in the second pyrolyzing process.

Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction reaction

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Papers

Composition-Graded Cu–Pd Nanospheres with Ir-Doped Surfaces on N-Doped Porous Graphene for Highly Efficient Ethanol Electro-Oxidation in Alkaline Media

Comparative Investigation on the Activity Degradation Mechanism of Pt/C and PtCo/C Electrocatalysts in PEMFCs during the Accelerate Degradation Process Characterized by an in Situ X-ray Absorption Fine Structure

Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction reaction