Electrochemical Energy Reviews

Electrocatalytic Oxygen Reduction to Produce Hydrogen Peroxide: Rational Design from Single-Atom Catalysts to Devices
Tong Y, Wang L, Hou F, Dou SX and Liang J
Electrocatalytic production of hydrogen peroxide (HO) via the 2e transfer route of the oxygen reduction reaction (ORR) offers a promising alternative to the energy-intensive anthraquinone process, which dominates current industrial-scale production of HO. The availability of cost-effective electrocatalysts exhibiting high activity, selectivity, and stability is imperative for the practical deployment of this process. Single-atom catalysts (SACs) featuring the characteristics of both homogeneous and heterogeneous catalysts are particularly well suited for HO synthesis and thus, have been intensively investigated in the last few years. Herein, we present an in-depth review of the current trends for designing SACs for HO production via the 2e ORR route. We start from the electronic and geometric structures of SACs. Then, strategies for regulating these isolated metal sites and their coordination environments are presented in detail, since these fundamentally determine electrocatalytic performance. Subsequently, correlations between electronic structures and electrocatalytic performance of the materials are discussed. Furthermore, the factors that potentially impact the performance of SACs in HO production are summarized. Finally, the challenges and opportunities for rational design of more targeted HO-producing SACs are highlighted. We hope this review will present the latest developments in this area and shed light on the design of advanced materials for electrochemical energy conversion.
Controlled Synthesis of Carbon-Supported Pt-Based Electrocatalysts for Proton Exchange Membrane Fuel Cells
Liu H, Zhao J and Li X
Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans. However, their performance, cost, and durability are significantly related to Pt-based electrocatalysts, hampering their large-scale commercial application. Hence, considerable efforts have been devoted to improving the activity and durability of Pt-based electrocatalysts by controlled synthesis in recent years as an effective method for decreasing Pt use, and consequently, the cost. Therefore, this review article focuses on the synthesis processes of carbon-supported Pt-based electrocatalysts, which significantly affect the nanoparticle size, shape, and dispersion on supports and thus the activity and durability of the prepared electrocatalysts. The reviewed processes include (i) the functionalization of a commercial carbon support for enhanced catalyst-support interaction and additional catalytic effects, (ii) the methods for loading Pt-based electrocatalysts onto a carbon support that impact the manufacturing costs of electrocatalysts, (iii) the preparation of spherical and nonspherical Pt-based electrocatalysts (polyhedrons, nanocages, nanoframes, one- and two-dimensional nanostructures), and (iv) the postsynthesis treatments of supported electrocatalysts. The influences of the supports, key experimental parameters, and postsynthesis treatments on Pt-based electrocatalysts are scrutinized in detail. Future research directions are outlined, including (i) the full exploitation of the potential functionalization of commercial carbon supports, (ii) scaled-up one-pot synthesis of carbon-supported Pt-based electrocatalysts, and (iii) simplification of postsynthesis treatments. One-pot synthesis in aqueous instead of organic reaction systems and the minimal use of organic ligands are preferred to simplify the synthesis and postsynthesis treatment processes and to promote the mass production of commercial carbon-supported Pt-based electrocatalysts.
Perovskite Oxides Toward Oxygen Evolution Reaction: Intellectual Design Strategies, Properties and Perspectives
Liu LB, Yi C, Mi HC, Zhang SL, Fu XZ, Luo JL and Liu S
Developing electrochemical energy storage and conversion devices (e.g., water splitting, regenerative fuel cells and rechargeable metal-air batteries) driven by intermittent renewable energy sources holds a great potential to facilitate global energy transition and alleviate the associated environmental issues. However, the involved kinetically sluggish oxygen evolution reaction (OER) severely limits the entire reaction efficiency, thus designing high-performance materials toward efficient OER is of prime significance to remove this obstacle. Among various materials, cost-effective perovskite oxides have drawn particular attention due to their desirable catalytic activity, excellent stability and large reserves. To date, substantial efforts have been dedicated with varying degrees of success to promoting OER on perovskite oxides, which have generated multiple reviews from various perspectives, e.g., electronic structure modulation and heteroatom doping and various applications. Nonetheless, the reviews that comprehensively and systematically focus on the latest intellectual design strategies of perovskite oxides toward efficient OER are quite limited. To bridge the gap, this review thus emphatically concentrates on this very topic with broader coverages, more comparative discussions and deeper insights into the synthetic modulation, doping, surface engineering, structure mutation and hybrids. More specifically, this review elucidates, in details, the underlying causality between the being-tuned physiochemical properties [e.g., electronic structure, metal-oxygen (M-O) bonding configuration, adsorption capacity of oxygenated species and electrical conductivity] of the intellectually designed perovskite oxides and the resulting OER performances, coupled with perspectives and potential challenges on future research. It is our sincere hope for this review to provide the scientific community with more insights for developing advanced perovskite oxides with high OER catalytic efficiency and further stimulate more exciting applications.
Structure, Property, and Performance of Catalyst Layers in Proton Exchange Membrane Fuel Cells
Zhao J, Liu H and Li X
Catalyst layer (CL) is the core component of proton exchange membrane (PEM) fuel cells, which determines the performance, durability, and cost. However, difficulties remain for a thorough understanding of the CLs' inhomogeneous structure, and its impact on the physicochemical and electrochemical properties, operating performance, and durability. The inhomogeneous structure of the CLs is formed during the manufacturing process, which is sensitive to the associated materials, composition, fabrication methods, procedures, and conditions. The state-of-the-art visualization and characterization techniques are crucial to examine the CL structure. The structure-dependent physicochemical and electrochemical properties are then thoroughly scrutinized in terms of fundamental concepts, theories, and recent progress in advanced experimental techniques. The relation between the CL structure and the associated effective properties is also examined based on experimental and theoretical findings. Recent studies indicated that the CL inhomogeneous structure also strongly affects the performance and degradation of the whole fuel cell, and thus, the interconnection between the fuel cell performance, failure modes, and CL structure is comprehensively reviewed. An analytical model is established to understand the effect of the CL structure on the effective properties, performance, and durability of the PEM fuel cells. Finally, the challenges and prospects of the CL structure-associated studies are highlighted for the development of high-performing PEM fuel cells.
Stimulating Efficiency for Proton Exchange Membrane Water Splitting Electrolyzers: From Material Design to Electrode Engineering
Zhu Y, Guo F, Zhang S, Wang Z, Chen R, He G, Sun X and Cheng N
Proton exchange membrane water electrolyzers (PEMWEs) are a promising technology for large-scale hydrogen production, yet their industrial deployment is hindered by the harsh acidic conditions and sluggish oxygen evolution reaction (OER) kinetics. This review provides a comprehensive analysis of recent advances in iridium-based electrocatalysts (IBEs), emphasizing novel optimization strategies to enhance both catalytic activity and durability. Specifically, we critically examine the mechanistic insights into OER under acidic conditions, revealing key degradation pathways of Ir species. We further highlight innovative approaches for IBE design, including (i) morphology and support engineering to improve stability, (ii) structure and phase modulation to enhance catalytic efficiency, and (iii) electronic structure tuning for optimizing interactions with reaction intermediates. Additionally, we assess emerging electrode engineering strategies and explore the potential of non-precious metal-based alternatives. Finally, we propose future research directions, focusing on rational catalyst design, mechanistic clarity, and scalable fabrication for industrial applications. By integrating these insights, this review provides a strategic framework for advancing PEMWE technology through highly efficient and durable OER catalysts.