Nitrogen-doped graphitic carbon materials hosting single-atom iron (Fe–N–C) are major non-precious metal catalysts for the oxygen reduction reaction (ORR). The nitrogen-coordinated Fe sites are described as the first coordination sphere. As opposed to the good performance in ORR, that in the oxygen evolution reaction (OER) is extremely poor due to the sluggish O–O coupling process, thus hampering the practical applications of rechargeable zinc (Zn)–air batteries. Herein, we succeed in boosting the OER activity of Fe–N–C by additionally incorporating phosphorus atoms into the second coordination sphere, here denoted as P/Fe–N–C. The resulting material exhibits excellent OER activity in 0.1 M KOH with an overpotential as low as 304 mV at a current density of 10 mA cm–2. Even more importantly, they exhibit a remarkably small ORR/OER potential gap of 0.63 V. Theoretical calculations using first-principles density functional theory suggest that the phosphorus enhances the electrocatalytic activity by balancing the *OOH/*O adsorption at the FeN4 sites. When used as an air cathode in a rechargeable Zn–air battery, P/Fe–N–C delivers a charge–discharge performance with a high peak power density of 269 mW cm–2, highlighting its role as the state-of-the-art bifunctional oxygen electrocatalyst.

https://pubs.acs.org/doi/pdf/10.1021/jacs.2c12933

Boosting Oxygen Electrocatalytic Activity of Fe–N–C Catalysts by Phosphorus Incorporation

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric and electronic structure and uncovering the structure-property relationships of single/dual-metal atoms confront with grand challenges. Herein, this review summarizes the latest progress in microenvironment engineering of single/dual-atom active sites via a comprehensive comparison of single-atom catalyst (SACs) and dual-atom catalysts (DACs) in term of design principles, modulation strategy, and theoretical understanding of structure-performance correlations. Subsequently, recent advances in several typical electrocatalysis process are discussed to get general understanding of the reaction mechanisms on finely-tuned SACs and DACs. Finally, full-scaled summaries of the challenges and prospects are given for microenvironment engineering of SACs and DACs. This review will provide new inspiration on the development of atomically dispersed catalysts for electrocatalytic application. This article is protected by copyright. All rights reserved.

Microenvironment Engineering of Single/Dual-atom Catalysts for Electrocatalytic Application.

Acidic water electrolysis enables the production of hydrogen for use as a chemical and as a fuel. The acidic environment hinders water electrolysis on non-noble catalysts, a result of the sluggish kinetics associated with the adsorbate evolution mechanism, reliant as it is on four concerted proton-electron transfer steps. Enabling a faster mechanism with non-noble catalysts will help to further advance acidic water electrolysis. Here, we report evidence that doping Ba cations into a Co3O4 framework to form Co3-xBaxO4 promotes the oxide path mechanism and simultaneously improves activity in acidic electrolytes. Co3-xBaxO4 catalysts reported herein exhibit an overpotential of 278 mV at 10 mA/cm2 in 0.5 M H2SO4 electrolyte and are stable over 110 h of continuous water oxidation operation. We find that the incorporation of Ba cations shortens the Co-Co distance and promotes OH adsorption, findings we link to improved water oxidation in acidic electrolyte.

Doping Shortens the Metal/Metal Distance and Promotes OH Coverage in Non-Noble Acidic Oxygen Evolution Reaction Catalysts.

Multicomponent transition metal oxides and (oxy)hydroxides for oxygen evolution

High‐entropy materials (HEMs) have been in the spotlight as emerging catalysts for electrochemical water splitting. In particular, HEM catalysts feature multi‐element active sites and unsaturated coordination as well as entropy stabilization in comparison with their single‐element counterparts. Herein, a comprehensive overview of HEM catalysts used in electrochemical water splitting is provided, covering both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Particularly, the review begins with discussions of the concept and structure of HEMs. In addition, effective strategies for rationally designing HEMs on the basis of computational techniques and experimental aspects is described. Importantly, the importance of computationally aided methods, that is, density functional theory calculations, high‐throughput screening, and machine learning, to the discovery and design of HEMs, is described. Furthermore, the applications of HEMs in the field of water electrolysis are reviewed. Eventually, an outlook regarding the prospects and future opportunities for HEMs is provided.

High‐Entropy Catalyst—A Novel Platform for Electrochemical Water Splitting

Rationally designed catalysts hold the key to address the sluggish kinetics of oxygen evolution reaction (OER). However, engineering the active sites of such catalysts still faces grand challenges. This study proposes a feasible ligand modulation strategy to boost the OER catalytic activity of cobalt‐iron oxyhydroxide ((Fe,Co)OOH). The 2‐methylimidazole (MI) ligand coordination on (Fe,Co)OOH reduces the orbital overlap between the Fe/Co 3d and O 2p, which weakens the adsorption to oxygen‐containing intermediates and thus facilitates the unfavorable O2 desorption. As a result, the MI ligand modulated (Fe,Co)OOH achieves an excellent OER performance with low overpotentials (230/290 mV at 10/100 mA cm‐2) and excellent durability (>155 h). This study provides a novel ligand modulation strategy for the design of OER catalysts.

Ligand Modulation of Active Sites to Promote Electrocatalytic Oxygen Evolution

Attributing to the high specific capacity and low electrochemical reduction potential, lithium (Li) metal is regarded as the most promising anode for high‐energy Li batteries. However, the growth of lithium dendrites and huge volume change seriously limit the development of lithium metal batteries. To overcome these challenges, an ordered mesoporous N‐doped carbon with lithiophilic single atoms is proposed to induce uniform nucleation and deposition of Li metal. Benefiting from the synergistic effects of interconnected three‐dimensional ordered mesoporous structures and abundant lithiophilic single‐atom sites, regulated local current density and rapid mass transfer can be achieved, leading to the uniform Li deposition with inhibition of dendrites and buffered volume expansion. As a result, the as‐fabricated anode exhibits a high CE of 99.8% for 200 cycles. A stable voltage hysteresis of 14 mV at 5 mA cm−2 could be maintained for more than 1330 h in the symmetric cell. Furthermore, the full cell coupled with commercial LiFePO4 exhibits high reversible capacity of 108 mAh g−1 and average Coulombic efficiency of 99.8% from 5th to 350th cycles at 1 C. The ordered mesoporous carbon host with abundant lithiophilic single‐atom sites delivers new inspirations into rational design of high‐performance Li metal anodes.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/eem2.12466

Single‐Atom Lithiophilic Sites Confined within Ordered Porous Carbon for Ultrastable Lithium Metal Anodes

Amorphous NiMo3S13/nickel foam integrated anode for lithium-ion batteries

The use of electrocatalytic carbon dioxide reduction (ECR) for producing various high-value-added products is critical for achieving carbon neutrality. In the past decades, single-site catalysts (SSCs), such as single-atom catalysts,...

/pdf/single-site-catalysts-for-co2-electroreduction-nhck4s1x.pdf

Single-Site Catalysts for CO2 Electroreduction

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Ligand Modulation of Active Sites to Promote Electrocatalytic Oxygen Evolution

Single‐Atom Lithiophilic Sites Confined within Ordered Porous Carbon for Ultrastable Lithium Metal Anodes

Amorphous NiMo3S13/nickel foam integrated anode for lithium-ion batteries

Single-Site Catalysts for CO2 Electroreduction