Recent Advances in Complex Hollow Electrocatalysts for Water Splitting

Abstract Electrocatalytic water splitting using renewable energy is widely considered as a clean and sustainable way to produce hydrogen as an ideal energy fuel for the future. Electrocatalysts are indispensable elements for large‐scale water electrolysis, which can efficiently accelerate electrochemical reactions occurring at both ends. Benefitting from high specific surface area, well‐defined void space, and tunable chemical compositions, hollow nanostructures can be applied as promising candidates of direct electrocatalysts or supports for loading internal or external electrocatalysts. Herein, some recent progress in the structural design of micro‐/nanostructured hollow materials as advanced electrocatalysts for water splitting is summarized. First, the design principles and corresponding strategies toward highly effective hollow electrocatalysts for oxygen/hydrogen evolution reactions are highlighted. Afterward, an overview of current reports about hollow electrocatalysts with diverse architectural designs and functionalities is given, including direct hollow electrocatalysts with single‐shelled, multi‐shelled, or open features and heterostructured electrocatalysts based on hollow hosts. Finally, some future research directions of hollow electrocatalysts for water splitting are discussed based on personal perspectives.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202105135

Design and Synthesis of Hollow Nanostructures for Electrochemical Water Splitting

Hydrogen is a clean, versatile, and energy-dense fuel that has the potential to play a key role in a low-carbon energy future. However, realizing this potential requires the development of efficient and cost-effective hydrogen generation and storage technologies. Hydrogen can be generated from a variety of sources, including fossil fuels, biomass, and renewable energy sources such as solar and wind. In regard to the renewable energy sources, this paper presents a review of the state-of-the-art in hydrogen generation methods including water electrolysis, gasification, dark fermentation, steam reforming, photocatalytic water splitting and water thermolysis. Further, this paper presents a review of the various hydrogen storage methods, including compression, liquefaction, liquid organic carriers, and solid-state storage. These technologies offer the potential for improved efficiency, safety, and environmental performance, and may play a key role in the transition to a hydrogen-based energy system. Finally, the advantages and challenges of hydrogen energy, and future perspectives on the improvement of hydrogen storage methods are well emphasized. Overall, the development of efficient and cost-effective hydrogen generation and storage technologies is essential for the widespread adoption of hydrogen as a clean energy source. Continued research and development in this field will be critical to advancing the state-of-the-art and realizing the full potential of hydrogen as a key element in a sustainable energy future. 

State-of-the-art hydrogen generation techniques and storage methods: A critical review

Oxygen evolution reaction participated by lattice oxygen oxidation (LOER) on the perovskite catalyst has attracted great interest recently because of its low reaction energy barrier. However, as the surface structure...

Key Roles of Surface Fe Sites and Sr Vacancies in Perovskite for Efficient Oxygen Evolution Reaction Participated by Lattice Oxygen Oxidation

The rational design of efficient electrocatalysts for industrial water splitting is essential to generate sustainable hydrogen fuel. However, a comprehensive understanding of the complex catalytic mechanisms under harsh reaction conditions remains a major challenge. We apply a self-templated strategy to introduce hierarchically nanostructured “all-surface” Fe-doped cobalt phosphide nanoboxes (Co@CoFe–P NBs) as alternative electrocatalysts for industrial-scale applications. Operando Raman spectroscopy and X-ray absorption spectroscopy (XAS) experiments were carried out to track the dynamics of their structural reconstruction and the real catalytically active intermediates during water splitting. Our operando analyses reveal that partial Fe substitution in cobalt phosphides promotes a structural reconstruction into P–Co–O–Fe–P configurations with low-valence metal centers (M0/M+) during the hydrogen evolution reaction (HER). Results from density functional theory (DFT) demonstrate that these in situ reconstructed configurations significantly enhance the HER performance by lowering the energy barrier for water dissociation and by facilitating the adsorption/desorption of HER intermediates (H*). The competitive activity in the oxygen evolution reaction (OER) arises from the transformation of the reconstructed P–Co–O–Fe–P configurations into oxygen-bridged, high-valence CoIV–O–FeIV moieties as true active intermediates. In sharp contrast, the formation of such CoIII/IV–O–FeIII/IV moieties in Co–FeOOH is hindered under the same conditions, which outlines the key advantages of phosphide-based electrocatalysts. Ex situ studies of the as-synthesized reference cobalt sulfides (Co–S), Fe doped cobalt selenides (Co@CoFe–Se), and Fe doped cobalt tellurides (Co@CoFe–Te) further corroborate the observed structural transformations. These insights are vital to systematically exploit the intrinsic catalytic mechanisms of non-oxide, low-cost, and robust overall water splitting electrocatalysts for future energy conversion and storage.

/pdf/dynamics-and-control-of-active-sites-in-hierarchically-3ep60ul2.pdf

Dynamics and control of active sites in hierarchically nanostructured cobalt phosphide/chalcogenide-based electrocatalysts for water splitting

In the study on structure-property relationship for rational material design, hollow multishelled structures (HoMSs) have attracted tremendous attention owing to the optimal balance between mass transfer and surface exposure. Considering the shells structure can significantly affect the properties of HoMSs, in this paper, we provide a novel one-step strategy to continually regulate the shell structures of HoMSs. Through a simple phosphorization process, we can effectively modify the shell from solid to bubble-like and even to duplicate the shells with a narrow spacing. Benefitting from the structure merits, the fabricated CoP HoMSs with close duplicated shells can promote the gas releasing owing to the unbalanced Laplace pressure, while accelerating liquid transfer for the enhanced capillary force. It can provide effectively channels for water and gas and thus exhibit the superior electrocatalytic performance in hydrogen and oxygen evolution reaction.

Delicate Control on the Shell Structure of Hollow Spheres Enables Tunable Mass Transport in Water Splitting

Synthesis of CdSe Nanowires and CuInSe2 Nanosheets for Hydrogen Evolution

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Delicate Control on the Shell Structure of Hollow Spheres Enables Tunable Mass Transport in Water Splitting

Synthesis of CdSe Nanowires and CuInSe2 Nanosheets for Hydrogen Evolution