Oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are three key reactions for the development of green and sustainable energy systems. Efficient electrocatalysts for these reactions are highly desired to lower their overpotentials and promote practical applications of related energy devices. Metal–organic frameworks (MOFs) have recently emerged as precursors to fabricate carbon-based electrocatalysts with high electrical conductivity and uniformly distributed active sites. In this review, the current progress of MOF-derived carbon-based materials for ORR/OER/HER electrocatalysis is presented. Materials design strategies of MOF-derived carbon-based materials are firstly summarized to show the rich possibilities of the morphology and composition of MOF-derived carbon-based materials. A wide range of applications based on these materials for ORR, OER, HER and multifunctional electrocatalysis are discussed, with an emphasis on the required features of MOF-derived carbon-based materials for the electrocatalysis of corresponding reactions. Finally, perspectives on the development of MOF-derived carbon-based materials for ORR, OER and HER electrocatalysis are provided.

MOF-derived electrocatalysts for oxygen reduction, oxygen evolution and hydrogen evolution reactions

More than 95% (in volume) of all of today’s chemical products are manufactured through catalytic processes, making research into more efficient catalytic materials a thrilling and very dynamic rese...

Metal–Organic Frameworks in Heterogeneous Catalysis: Recent Progress, New Trends, and Future Perspectives

Water electrolysis represents a promising sustainable hydrogen production technology. However, in practical application which requires extremely large current densities (>500 mA cm−2), the oxygen evolution reaction (OER) becomes unstable and kinetically sluggish, which is a major hurdle to large-scale hydrogen production. Herein, we report an exceptionally active and binder-free NiFe nanowire array based OER electrode that allows durable water splitting at current densities up to 1000 mA cm−2 up to 120 hours. Specifically, NiFe oxyhydroxide (shell)–anchored NiFe alloy nanowire (core) arrays are prepared via a magnetic-field-assisted chemical deposition method. The ultrathin (1–5 nm) and amorphous NiFe oxyhydroxide is in situ formed on the NiFe alloy nanowire surface, which is identified as an intrinsically highly active phase for the OER. Additionally, the fine geometry of the hierarchical electrode can substantially improve charge and mass (reactants and oxygen bubbles) transfer. In an alkaline electrolyte, this OER electrode can yield current densities of 500 and 1000 mA cm−2 stably over 120 hours at overpotentials of only 248 mV and 258 mV respectively, which are dramatically lower than any recently reported overpotentials. Notably, the integrated alkaline electrolyzer (with pure Ni nanowires as HER electrode) is demonstrated to reach the current density of 1000 mA cm−2 with super low voltage of 1.76 V, outperforming the state-of-the-art industrial catalysts. Our result may represent a critical step towards an industrial electrolyzer for large-scale hydrogen production by water splitting.

Exceptional performance of hierarchical Ni–Fe oxyhydroxide@NiFe alloy nanowire array electrocatalysts for large current density water splitting

Lithium-ion batteries (LIBs) with outstanding energy and power density have been extensively investigated in recent years, rendering them the most suitable energy storage technology for application in emerging markets such as electric vehicles and stationary storage. More recently, sodium, one of the most abundant elements on earth, exhibiting similar physicochemical properties as lithium, has been gaining increasing attention for the development of sodium-ion batteries (SIBs) in order to address the concern about Li availability and cost—especially with regard to stationary applications for which size and volume of the battery are of less importance. Compared with traditional intercalation reactions, conversion reaction-based transition metal oxides (TMOs) are prospective anode materials for rechargeable batteries thanks to their low cost and high gravimetric specific capacities. In this review, the recent progress and remaining challenges of conversion reactions for LIBs and SIBs are discussed, covering an overview about the different synthesis methods, morphological characteristics, as well as their electrochemical performance. Potential future research directions and a perspective toward the practical application of TMOs for electrochemical energy storage are also provided.

https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.201902485

Transition Metal Oxide Anodes for Electrochemical Energy Storage in Lithium- and Sodium-Ion Batteries

Recent years have witnessed an upsurge in the development of non-precious catalysts (NPCs) for alkaline water electrolysis (AWE), especially with the strides made in experimental and computational techniques. In this contribution, the most recent advances in NPCs for AWE were systematically reviewed, emphasizing the application of in situ/operando experimental methods and density functional theory (DFT) calculations in their understanding and development. First, we briefly introduced the fundamentals of the anode and cathode reaction for AWE, i.e., the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER), respectively. Next, the most popular in situ/operando approaches for characterizing AWE catalysts, including hard and soft XAS, ambient-pressure XPS, liquid and identical location TEM, electrochemical mass spectrometry, and Raman spectroscopy were thoroughly summarized. Subsequently, we carefully discussed the principles, computational methods, applications, and combinations of DFT with machine learning for modeling NPCs and predicting the alkaline OER and HER. With the improved understanding of the structure-property-performance relationship of NPCs for AWE, we proceeded to overview their current development, summarising state-of-the-art design strategies to boost their activity. In addition, advances in various extensively investigated NPCs for AWE were evaluated. By conveying these methods, progress, insights, and perspectives, this review will contribute to a better understanding and rational development of non-precious AWE electrocatalysts for hydrogen production.

Non-precious-metal catalysts for alkaline water electrolysis: operando characterizations, theoretical calculations, and recent advances

The development of high-performance and cost-effective catalysts for the hydrogen and oxygen evolution reactions is key to efficient electrocatalysis of water, which offers a promising solution to convert and store those green but unsteady energies. Herein, we report a hierarchical nickel–carbon composite, fabricated by directly growing sheet-like Ni–MOFs on commercial nickel foam prior to high-temperature annealing, as a highly efficient bifunctional catalyst. This composite shows remarkable catalytic activities for both the hydrogen and oxygen evolution reactions in an alkaline electrolyte, affording a current density of 10 mA cm−2 at an overpotential of 37 mV for the HER and 265 mV for the OER. Furthermore, an electrolyzer employing the composite as a bifunctional catalyst in both the cathode and the anode delivers a current density of 35.9 mA cm−2 at a cell voltage of 1.60 V with extended stability, which is even superior to the integrated Pt/C and RuO2 counterparts. This excellent performance is believed to be a result of a concerted synergy due to its hierarchical structure, enabling excellent reaction kinetics. Further ex situ XRD and XPS analyses reveal that while metallic nickel is responsible for the HER, Ni nanoparticles with an oxide shell encapsulated in graphitic carbon are the OER catalytically-active sites formed in situ.

A hierarchical nickel–carbon structure templated by metal–organic frameworks for efficient overall water splitting

γ-Fe2O3 nanoparticles embedded in porous carbon fibers as binder-free anodes for high-performance lithium and sodium ion batteries

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A hierarchical nickel–carbon structure templated by metal–organic frameworks for efficient overall water splitting

γ-Fe2O3 nanoparticles embedded in porous carbon fibers as binder-free anodes for high-performance lithium and sodium ion batteries