Hydrogen fuel is considered as the cleanest renewable resource and the primary alternative to fossil fuels for future energy supply. Sustainable hydrogen generation is the major prerequisite to realize future hydrogen economy. The electrocatalytic hydrogen evolution reaction (HER), as the vital step of water electrolysis to H2 production, has been the subject of extensive study over the past decades. In this comprehensive review, we first summarize the fundamentals of HER and review the recent state-of-the-art advances in the low-cost and high-performance catalysts based on noble and non-noble metals, as well as metal-free HER electrocatalysts. We systemically discuss the insights into the relationship among the catalytic activity, morphology, structure, composition, and synthetic method. Strategies for developing an effective catalyst, including increasing the intrinsic activity of active sites and/or increasing the number of active sites, are summarized and highlighted. Finally, the challenges, perspectives, and research directions of HER electrocatalysis are featured.

Recent Advances in Electrocatalytic Hydrogen Evolution Using Nanoparticles.

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

Even though transition-metal phosphides (TMPs) have been developed as promising alternatives to Pt catalyst for the hydrogen evolution reaction (HER), further improvement of their performance requires fine regulation of the TMP sites related to their specific electronic structure. Herein, for the first time, boron (B)-modulated electrocatalytic characteristics in CoP anchored on the carbon nanotubes (B-CoP/CNT) with impressive HER activities over a wide pH range are reported. The HER performance surpasses commercial Pt/C in both neutral and alkaline media at large current density (>100 mA cm-2 ). A combined experimental and theoretical study identified that the B dopant could reform the local electronic configuration and atomic arrangement of bonded Co and adjacent P atoms, enhance the electrons' delocalization capacity of Co atoms for high electrical conductivity, and optimize the free energy of H adsorption and H2 desorption on the active sites for better HER kinetics.

Boron-Induced Electronic-Structure Reformation of CoP Nanoparticles Drives Enhanced pH-Universal Hydrogen Evolution.

Silver orthophosphate (Ag3PO4) based semiconductor photocatalysis have been widely investigated for environmental purification due to its strong oxidation ability. Yet, its poor photostability and low photoactivity hamper its extensive applications. Here, an inorganic-organic Z-scheme photocatalytic system for antibiotic degradation demonstrated high photoactivity and stability through the use of Ag3PO4/Perylene diimide organic supermolecule (PDIsm). The apparent rate constant of tetracycline hydrochloride (TC-H) degradation with Ag3PO4/PDIsm was 1.5 times that of Ag3PO4 and 8 times that of PDIsm. The photocatalytic activity of Ag3PO4/PDIsm toward TC-H still kept 65 % after four reuses, while pure Ag3PO4 only kept 22 %. We revealed that this high photoactivity and photostability arisen from the efficient carriers separation and the formation of direct Z-scheme junction. Importantly, this Z-scheme electron transfer pathway was confirmed by thorough experimental study and density functional theory (DFT) calculation. This work demonstrated the significant potential of Ag3PO4-based inorganic-organic Z-scheme photocatalyst in environmental remediation.

A promising inorganic-organic Z-scheme photocatalyst Ag3PO4/PDI supermolecule with enhanced photoactivity and photostability for environmental remediation

Promoting Electrocatalytic Hydrogen Evolution Reaction and Oxygen Evolution Reaction by Fields: Effects of Electric Field, Magnetic Field, Strain, and Light

Metallic FePSe3 nanoparticles anchored on N-doped carbon framework for All-pH hydrogen evolution reaction

In-situ growth of CNTs encapsulating P-doped NiSe2 nanoparticles on carbon framework as efficient bifunctional electrocatalyst for overall water splitting

Wei-Jian Li

Papers

Metallic FePSe3 nanoparticles anchored on N-doped carbon framework for All-pH hydrogen evolution reaction

In-situ growth of CNTs encapsulating P-doped NiSe2 nanoparticles on carbon framework as efficient bifunctional electrocatalyst for overall water splitting