As a new member of carbon allotropes, graphdiyne (GDY) has the characteristics of being one-atom-thick with two-dimensional layers comprising sp and sp2 hybridized carbon atoms, and represents a trend in the development of carbon materials. Its unique chemical and electronic structures give GDY many unique and fascinating properties such as rich chemical bonds, highly conjugated and super-large π structures, infinitely distributed pores and high inhomogeneity of charge distribution. GDY has entered a period of rapid development, especially with the significant emergence of fundamental research and applied research achievements over the past five years. As one of the frontiers of chemistry and materials science, graphdiyne was listed in the Top 10 research areas in the 2020 Research Frontiers report and was jointly released in the Top 10 in the world by Clarivate and the Chinese Academy of Sciences. The research results have shown the great potential of GDY in the applications of energy, catalysis, environmental science, electronic devices, detectors, biomedicine and therapy, etc. Scientists are eager to explore and fully reveal the new properties, discover new scientific concepts and phenomena, discover the new conversion modes and mechanisms of GDY in photoelectricity, energy, and catalysis, etc., and build the important scientific value of new conversion devices. This review covers research on the foundation and application of GDY, such as the controlled preparation of new methods of GDY and GDY-based materials, studies on new mechanisms and properties in chemistry and physics, and the foundation and applications in energy, catalysis, photoelectric and devices. 

2D graphdiyne: an emerging carbon material

The investigation of highly effective, durable, and cost-effective electrocatalysts for the hydrogen evolution reaction (HER) is a prerequisite for the upcoming hydrogen energy society. To establish a new hydrogen energy system and gradually replace the traditional fossil-based energy, electrochemical water-splitting is considered the most promising, environmentally friendly, and efficient way to produce pure hydrogen. Compared with the commonly used platinum (Pt)-based catalysts, ruthenium (Ru) is expected to be a good alternative because of its similar hydrogen bonding energy, lower water decomposition barrier, and considerably lower price. Analyzing and revealing the HER mechanisms, as well as identifying a rational design of Ru-based HER catalysts with desirable activity and stability is indispensable. In this review, the research progress on HER electrocatalysts and the relevant describing parameters for HER performance are briefly introduced. Moreover, four major strategies to improve the performance of Ru-based electrocatalysts, including electronic effect modulation, support engineering, structure design, and maximum utilization (single atom) are discussed. Finally, the challenges, solutions and prospects are highlighted to prompt the practical applications of Ru-based electrocatalysts for HER.

/pdf/engineering-ruthenium-based-electrocatalysts-for-effective-49238140ub.pdf

Engineering Ruthenium-Based Electrocatalysts for Effective Hydrogen Evolution Reaction

Ru nanoparticles have been demonstrated to be highly active electrocatalysts for the hydrogen evolution reaction (HER). At present, most of Ru nanoparticles-based HER electrocatalysts with high activity are supported by heteroatom-doped carbon substrates. Few metal oxides with large band gap (more than 5 eV) as the substrates of Ru nanoparticles are employed for the HER. By using large band gap metal oxides substrates, we can distinguish the contribution of Ru nanoparticles from the substrates. Here, a highly efficient Ru/HfO2 composite is developed by tuning numbers of Ru-O-Hf bonds and oxygen vacancies, resulting in a 20-fold enhancement in mass activity over commercial Pt/C in an alkaline medium. Density functional theory (DFT) calculations reveal that strong metal-support interaction via Ru-O-Hf bonds and the oxygen vacancies in the supported Ru samples synergistically lower the energy barrier for water dissociation to improve catalytic activities. 

/pdf/the-synergistic-effect-of-hf-o-ru-bonds-and-oxygen-vacancies-1dh563mw.pdf

The synergistic effect of Hf-O-Ru bonds and oxygen vacancies in Ru/HfO2 for enhanced hydrogen evolution

The cost-effective, robust, and efficient electrocatalysts for photoelectrochemical (PEC) water-splitting has been extensively studied over the past decade to address a solution for the energy crisis. The interesting physicochemical properties of CuO have introduced this promising photocathodic material among the few photocatalysts with a narrow bandgap. This photocatalyst has a high activity for the PEC hydrogen evolution reaction (HER) under simulated sunlight irradiation. Here, the recent advancements of CuO-based photoelectrodes, including undoped CuO, doped CuO, and CuO composites, in the PEC water-splitting field, are comprehensively studied. Moreover, the synthesis methods, characterization, and fundamental factors of each classification are discussed in detail. Apart from the exclusive characteristics of CuO-based photoelectrodes, the PEC properties of CuO/2D materials, as groups of the growing nanocomposites in photocurrent-generating devices, are discussed in separate sections. Regarding the particular attention paid to the CuO heterostructure photocathodes, the PEC water splitting application is reviewed and the properties of each group such as electronic structures, defects, bandgap, and hierarchical structures are critically assessed.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/adma.202007285

Photoelectrochemical Water-Splitting Using CuO-Based Electrodes for Hydrogen Production: A Review

Oxygen evolution reaction (OER) in acidic media usually requires a catalyst with high content of noble Ir or Ru, becoming a bottleneck for the electrochemical water splitting. To address this issue, here we report the fabrication of a RuO2/(Co,Mn)3O4 nanocomposite with low Ru loading (2.51 wt%) as a highly efficient OER catalyst in acidic media (0.5 M H2SO4). Spectroscopic and theoretical studies demonstrate that the introduction of Mn in Co3O4 results in redistribution of electrons and the generation of electron-rich Ru species of the RuO2/(Co,Mn)3O4 catalyst. With modulated electronic properties, the adsorption of O on RuO2/(Co,Mn)3O4 is weakened and the rate determining step, formation of OOH*, of the OER process is therefore accelerated. At such a low Ru loading, RuO2/(Co,Mn)3O4 exhibits superior acidic OER activity (η =270 mV at 10 mA/cm2) and long‐term stability to the benchmark RuO2 catalyst. This work provides a new strategy for the design of cost-effective acidic OER electrocatalysts for energy conversion applications.

Low Ru loading RuO2/(Co,Mn)3O4 nanocomposite with modulated electronic structure for efficient oxygen evolution reaction in acid

2D graphdiyne loading ruthenium atoms for high efficiency water splitting

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2D graphdiyne loading ruthenium atoms for high efficiency water splitting