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

Porous carbon electrodes have emerged as important cathode materials for metal-air battery systems. However, most approaches for fabricating porous carbon electrodes from biomass are highly energy inefficient as they require the breaking down of the biomass and its subsequent reconstitution into powder-like carbon. Here, enzymes are explored to effectively hydrolyze the partial cellulose in bulk raw wood to form a large number of nanopores, which helps to maximally expose the inner parts of the raw wood to sufficiently dope nitrogen onto the carbon skeletons during the subsequent pyrolysis process. The resulting carbons exhibit excellent catalytic activity with respect to the oxygen reduction and oxygen evolution reactions. As-fabricated cellulose-digested, carbonized wood plates are mechanically strong, have high conductivity, and contain a crosslinked network and natural ion-transport channels and can be employed directly as metal-free electrodes without carbon paper, polymer binders, or carbon black. When used as metal-free cathodes in zinc-air batteries, they result in a specific capacity of 801 mA h g-1 and an energy density of 955 W h kg-1 with the long-term stability of the batteries being as high as 110 h. This work paves the way for the ready conversion of abundant biomass into high-value engineering products for energy-related applications.

Hierarchically Porous Carbon Plates Derived from Wood as Bifunctional ORR/OER Electrodes

Sub‐2 nm Thiophosphate Nanosheets with Heteroatom Doping for Enhanced Oxygen Electrocatalysis

Ordered porous carbon materials (PCMs) have potential applications in various fields due to their low mass densities and porous features. However, it yet remains extremely challenging to construct PCMs with multifunctionalization for electromagnetic wave absorption. Herein, the honeycombed-like carbon aerogels with embedded Co@C nanoparticles are fabricated by a directionally freeze-casting and carbonization method. The optimized aerogel possesses low density (0.017 g cm-3 ), fire-retardant, robust mechanical performance (compression moduli reach 1411 and 420 kPa in the longitudinal and transverse directions at 80% strain, respectively), and high thermal management (high thermal insulation capability and high-efficiency electrothermal conversion ability). Notably, the optimized aerogel exhibits the excellent electromagnetic wave absorption properties with broad effective absorption bandwidth (13.12-17.14 GHz) and strong absorption (-45.02 dB) at a thickness of only 1.5 mm. Density functional theory calculations and the experimental results demonstrate that the excellent electromagnetic wave absorption properties stem from the synergetic effects among high electrical conductivity, numerous interfaces and dipoles and unique ordered porous structure. Meanwhile, the computer simulation technology (CST) simulation confirms that the multifunctional aerogel can attenuate more electromagnetic energy in a practical environment. This work paves the way for rational design and fabrication of the next-generation electromagnetic wave absorbing materials.

Lightweight, Fire-Retardant, and Anti-Compressed Honeycombed-Like Carbon Aerogels for Thermal Management and High-Efficiency Electromagnetic Absorbing Properties.

Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are crucial for the large-scale application of rechargeable Zn–air batteries (ZABs). In this work, our density functional theory calculations on the electrocatalyst suggest that the rational construction of interfacial structure can induce local charge redistribution, improve the electronic conductivity and enhance the catalyst stability. In order to realize such a structure, we spatially immobilize heterogeneous CoS/CoO nanocrystals onto N-doped graphene to synthesize a bifunctional electrocatalyst (CoS/CoO@NGNs). The optimization of the composition, interfacial structure and conductivity of the electrocatalyst is conducted to achieve bifunctional catalytic activity and deliver outstanding efficiency and stability for both ORR and OER. The aqueous ZAB with the as-prepared CoS/CoO@NGNs cathode displays a high maximum power density of 137.8 mW cm−2, a specific capacity of 723.9 mAh g−1 and excellent cycling stability (continuous operating for 100 h) with a high round-trip efficiency. In addition, the assembled quasi-solid-state ZAB also exhibits outstanding mechanical flexibility besides high battery performances, showing great potential for applications in flexible and wearable electronic devices.
Highlights:
1 Interface engineering of heterogeneous CoS/CoO nanocrystals and N-doped graphene composite facilitates high-performance oxygen reduction reaction and oxygen evolution reaction.2 Density functional theory calculations and experimental results confirm the enhanced electrocatalytic performances via the proposed interface engineering.3 The bifunctional oxygen electrocatalyst exhibits excellent performances in rechargeable Zn–air batteries.

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Interface Engineering of CoS/CoO@N-Doped Graphene Nanocomposite for High-Performance Rechargeable Zn–Air Batteries

Mechanically stable and foldable air cathodes with exceptional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activities are key components of wearable metal-air batteries Herein, a directional freeze-casting and annealing approach is reported for the construction of a 3D honeycomb nanostructured, N,P-doped carbon aerogel incorporating in situ grown FeP/Fe2 O3 nanoparticles as the cathode in a flexible Zn-air battery (ZAB) The aqueous rechargeable Zn-air batteries assembled with this carbon aerogel exhibit a remarkable specific capacity of 648 mAh g-1 at a current density of 20 mA cm-2 with a good long-term durability, outperforming those assembled with commercial Pt/C+RuO2 catalyst Furthermore, such a foldable carbon aerogel with directional channels can serve as a freestanding air cathode for flexible solid-state Zn-air batteries without the use of carbon paper/cloth and additives, giving a specific capacity of 676 mAh g-1 and an energy density of 517 Wh kg-1 at 5 mA cm-2 together with good cycling stability This work offers a new strategy to design and synthesize highly effective bifunctional air cathodes to be applied in electrochemical energy devices

Chengyu Jiang

Papers

An Iron-Decorated Carbon Aerogel for Rechargeable Flow and Flexible Zn-Air Batteries.

Wood Carbon Based Single-Atom Catalyst for Rechargeable Zn–Air Batteries