Oxygen reduction and evolution reactions constitute the core process of many vital energy storage or conversion techniques. However, the kinetic sluggishness of the oxygen redox reactions and heavy reliance on noble-metal-based electrocatalysts strongly limit the energy efficiency of the related devices. Developing high-performance noble-metal-free bifunctional ORR and OER electrocatalysts has gained worldwide attention, where much important progress has been made during the last decade. This review systematically addresses the design principles to obtain high-performance noble-metal-free bifunctional oxygen electrocatalysts by emphasizing strategies of both intrinsic activity regulation and active site integration. A statistical analysis of the reported bifunctional electrocatalysts is further carried out to reveal the composition-performance relationship and guide further exploration of emerging candidates. Finally, perspectives for developing advanced bifunctional oxygen electrocatalysts and aqueous rechargeable metal-air batteries are proposed.

Recent advances of noble-metal-free bifunctional oxygen reduction and evolution electrocatalysts

Transition metal sulfides with a multi‐elemental nature represent a class of promising catalysts for oxygen evolution reaction (OER) owing to their good catalytic activity. However, their synthesis remains a challenge due to the thermodynamic immiscibility of the constituent multimetallic elements in a sulfide structure. Herein, for the first time the synthesis of high‐entropy metal sulfide (HEMS, i.e., (CrMnFeCoNi)Sx) solid solution nanoparticles is reported. Computational and X‐ray photoelectron spectroscopy analysis suggest that the (CrMnFeCoNi)Sx exhibits a synergistic effect among metal atoms that leads to desired electronic states to enhance OER activity. The (CrMnFeCoNi)Sx nanoparticles show one of the best activities (low overpotential 295 mV at 100 mA cm−2 in 1 m KOH solution) and good durability (only slight polarization after 10 h by chronopotentiometry) compared with their unary, binary, ternary, and quaternary sulfide counterparts. This work opens up a new synthesis paradigm for high‐entropy compound nanoparticles for highly efficient electrocatalysis applications.

High‐Entropy Metal Sulfide Nanoparticles Promise High‐Performance Oxygen Evolution Reaction

Fuel cells are an incredibly powerful renewable energy technology, but their broad applications remains lagging because of the high cost and poor reliability of cathodic electrocatalysts for the oxygen reduction reaction (ORR). This review focuses on the recent progress of ORR electrocatalysts in fuel cells. More importantly, it highlights the fundamental problems associated with the insufficient activity translation from rotating disk electrode to membrane electrode assembly in the fuel cells. Finally, for the atomic-level in-depth information on ORR catalysts in fuel cells, potential perspectives are suggested, including large-scale preparation, unified assessment criteria, advanced interpretation techniques, advanced simulation and artificial intelligence. This review aims to provide valuable insights into the fundamental science and technical engineering for efficient ORR electrocatalysts in fuel cells.

Oxygen Reduction Electrocatalysts toward Practical Fuel Cells: Progress and Perspectives

Atomically dispersed M-N-C (M refers to transition metals) materials represent the most promising catalyst alternatives to the precious metal Pt for the electrochemical reduction of oxygen (ORR), yet the genuine active sites in M-N-C remain elusive. Here, we develop a two-step approach to fabricate Cu-N-C single-atom catalysts with a uniform and well-defined Cu2+-N4 structure that exhibits comparable activity and superior durability in comparison to Pt/C. By combining operando X-ray absorption spectroscopy with theoretical calculations, we unambiguously identify the dynamic evolution of Cu-N4 to Cu-N3 and further to HO-Cu-N2 under ORR working conditions, which concurrently occurs with reduction of Cu2+ to Cu+ and is driven by the applied potential. The increase in the Cu+/Cu2+ ratio with the reduced potential indicates that the low-coordinated Cu+-N3 is the real active site, which is further supported by DFT calculations showing the lower free energy in each elemental step of the ORR on Cu+-N3 than on Cu2+-N4. These findings provide a new understanding of the dynamic electrochemistry on M-N-C catalysts and may guide the design of more efficient low-cost catalysts.

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N3 as an Active Site for the Oxygen Reduction Reaction.

Lithium-oxygen (Li-O2) batteries have been intensively investigated in recent decades for their utilization in electric vehicles. The intrinsic challenges arising from O2 (electro)chemistry have been mitigated by developing various types of catalysts, porous electrode materials, and stable electrolyte solutions. At the next stage, we face the need to reform batteries by substituting pure O2 gas with air from Earth's atmosphere. Thus, the key emerging challenges of Li-air batteries, which are related to the selective filtration of O2 gas from air and the suppression of undesired reactions with other constituents in air, such as N2, water vapor (H2O), and carbon dioxide (CO2), should be properly addressed. In this review, we discuss all key aspects for developing Li-air batteries that are optimized for operating in ambient air and highlight the crucial considerations and perspectives for future air-breathing batteries.

Lithium–Air Batteries: Air-Breathing Challenges and Perspective

Summary With the ever-increasing demand for higher-performing energy-storage systems, electrocatalysis has become a major topic of interest in an attempt to enhance the electrochemical performance of many electrochemical technologies. Discoveries pertaining to the oxygen reduction reaction catalyst helped enable the commercialization of fuel-cell-based electric vehicles. However, a closely related technology, the metal-air battery, has yet to find commercial application. Much like the Li-ion battery, metal-air batteries can potentially utilize the electrical grid network for charging, bypassing the need for establishing a hydrogen infrastructure. Among the metal-air batteries, Li-air and Zn-air batteries have drawn much interest in the past decade. Unfortunately, state-of-the art metal-air batteries still produce performances that are well below practical levels. In this brief perspective, we hope to bridge some of the ideas from fuel cell to that of metal-air batteries with the aim of inspiring new ideas and directions for future research.

https://www.cell.com/matter/pdf/S2590-2385(19)30277-2.pdf

Relating Catalysis between Fuel Cell and Metal-Air Batteries

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Relating Catalysis between Fuel Cell and Metal-Air Batteries