Single Atoms and Clusters Based Nanomaterials for Hydrogen Evolution, Oxygen Evolution Reactions, and Full Water Splitting

With the increasing demands in energy consumption and increasing environmental concerns, it is of vital significance for developing renewable and clean energy sources to substitute traditional fossil fuels. As an outstanding candidate, hydrogen is recognized as a green energy carrier due to its high gravimetric energy density, zero carbon footprints, and earth-abundance. Currently, water splitting in alkaline electrolytes represents one of the most promising methods for sustainable hydrogen production, and the key challenge lies in the development of high-performance electrocatalysts for the hydrogen evolution reaction (HER). Given the rapid advances in the design and development of efficient catalysts towards the alkaline HER, especially capable transition metal (TM)-based materials, this review aims to summarise recent progress in the theoretical understanding of the alkaline HER and TM-based electrocatalysts. TM-based catalysts classified by their different anionic compositions (metals, alloys, oxides, hydroxides, sulfides, selenides, tellurides, nitrides, phosphides, carbides, and borides) are comprehensively showcased. Special attention is given to mainstream strategies that can improve the catalytic properties of each category, as well as the underlying structure–activity regimes. Additionally, the challenges for the future development of novel catalysts are also analyzed.

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Recent advances in transition metal-based electrocatalysts for alkaline hydrogen evolution

Water splitting is a green strategy for hydrogen generation but greatly hindered by the sluggish anodic oxygen evolution reaction (OER). Herein, ultrathin rhodium-doped nickel iron layered double hydroxide nanosheets are successfully synthesized, which exhibit outstanding hydrogen evolution reaction (HER) and OER performance, and advanced overall water splitting. More impressively, the remarkable mass activity of 960 mA mg1 at 1.55 V (1.7 times larger than NiFe-LDH) for urea electro-oxidation reaction (UOR) shows the great potential to surmount the sluggish OER for overall water splitting. A urine-mediated electrolysis cell is subsequently configured, delivering a current density of 10 mA cm-2 with a potential of 1.35 V, which is 105 mV lower than that of urea-free counterpart. The enhanced catalytic activity and cell performance are attributed to the introduction of Rh into NiFe-LDH matrix by changing the electronic structure, allowing optimization of the adsorbed species, as confirmed by experimental measurements and computational analyses.

Rh-engineered ultrathin NiFe-LDH nanosheets enable highly-efficient overall water splitting and urea electrolysis

Electrochemical water splitting is an appealing and promising approach for energy conversion and storage. As a key half-reaction of electricity-driven water splitting, the oxygen evolution reaction (OER) is a sluggish process due to the transfer of four protons and four electrons. Therefore, development of low-cost and robust OER electrocatalysts is of great importance for improving the efficiency of water splitting. Based on the merits of high surface area, rich pore structure, diverse composition and well-defined metal centers, metal-organic frameworks (MOFs) and their derivatives have been widely exploited as OER electrocatalysts. Herein, the current progress on MOFs and their derivatives for OER electrolysis is summarized, highlighting the design principle, synthetic methods and performance for MOF-based materials. In addition, the structure-performance relationships of MOFs and their derivatives toward the OER are discussed, providing valuable insights into rationally developing OER catalysts with high efficiency. The current scientific and technological challenges and future perspectives towards the purpose of sustainable industrial applications are addressed at the end.

Metal–organic frameworks and their derivatives as electrocatalysts for the oxygen evolution reaction

Hydrogen (H2) production is a latent feasibility of renewable clean energy. The industrial H2 production is obtained from reforming of natural gas, which consumes a large amount of nonrenewable energy and simultaneously produces greenhouse gas carbon dioxide. Electrochemical water splitting is a promising approach for the H2 production, which is sustainable and pollution-free. Therefore, developing efficient and economic technologies for electrochemical water splitting has been an important goal for researchers around the world. The utilization of green energy systems to reduce overall energy consumption is more important for H2 production. Harvesting and converting energy from the environment by different green energy systems for water splitting can efficiently decrease the external power consumption. A variety of green energy systems for efficient producing H2, such as two-electrode electrolysis of water, water splitting driven by photoelectrode devices, solar cells, thermoelectric devices, triboelectric nanogenerator, pyroelectric device or electrochemical water-gas shift device, have been developed recently. In this review, some notable progress made in the different green energy cells for water splitting is discussed in detail. We hoped this review can guide people to pay more attention to the development of green energy system to generate pollution-free H2 energy, which will realize the whole process of H2 production with low cost, pollution-free and energy sustainability conversion.

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Water Splitting: From Electrode to Green Energy System

High-efficient electrocatalysts are crucial for fuel cell applications; however, the whole cell performance is generally restricted by the anodic part because of the sluggish kinetics involved in the oxygen evolution reaction (OER) process. Herein, a hierarchical hollow (Co,Ni)Se2@NiFe layered double hydroxide (LDH) nanocage was synthesized by deriving from the metal–organic framework (MOF) of ZIF-67. Concretely, it involves first fabrication of hollow rhombic (Co,Ni)Se2 nanocages and then deposition of NiFe LDH nanosheets on the surface of nanocages. Notably, the incorporation of Ni into Co-based ZIF-67 (via ion-exchange) could tail the atomic arrangement of the MOF, exposing more additional active sites in the following selenization treatment. The as-synthesized (Co,Ni)Se2@NiFe LDH demonstrates splendid OER performance with a small overpotential of 277 mV (to launch a current density of 10 mA cm–2), a small Tafel slope of 75 mV dec–1, and robust durability (a slight stability decay of 5.1% after 17 h of...

Chenhui Xu

Papers

Metal-Organic Framework-Derived Hierarchical (Co,Ni)Se2@NiFe LDH Hollow Nanocages for Enhanced Oxygen Evolution.

Engineering hierarchical CoSe/NiFe layered-double-hydroxide nanoarrays as high efficient bifunctional electrocatalyst for overall water splitting