Over the past few decades, the design and development of advanced electrocatalysts for efficient energy conversion technologies have been subjects of extensive study. With the discovery of graphene, two-dimensional (2D) nanomaterials have emerged as some of the most promising candidates for heterogeneous electrocatalysts due to their unique physical, chemical, and electronic properties. Here, we review 2D-nanomaterial-based electrocatalysts for selected electrocatalytic processes. We first discuss the unique advances in 2D electrocatalysts based on different compositions and functions followed by specific design principles. Following this overview, we discuss various 2D electrocatalysts for electrocatalytic processes involved in the water cycle, carbon cycle, and nitrogen cycle from their fundamental conception to their functional application. We place a significant emphasis on different engineering strategies for 2D nanomaterials and the influence these strategies have on intrinsic material performance, such as electronic properties and adsorption energetics. Finally, we feature the opportunities and challenges ahead for 2D nanomaterials as efficient electrocatalysts. By considering theoretical calculations, surface characterization, and electrochemical tests, we describe the fundamental relationships between electronic structure, adsorption energy, and apparent activity for a wide variety of 2D electrocatalysts with the goal of providing a better understanding of these emerging nanomaterials at the atomic level.

Although MnO2 is a promising material for supercapacitors (SCs) due to its excellent electrochemical performance and natural abundance, its wide application is limited by poor electrical conductivity. Inspired by our results that the electrochemical activity and electrical conductivity of ZnO nanowires were greatly improved after hydrogenation, we designed and fabricated hydrogenated single-crystal ZnO@amorphous ZnO-doped MnO2 core-shell nanocables (HZM) on carbon cloth as SC electrodes, showing excellent performance such as areal capacitance of 138.7 mF/cm(2) and specific capacitance of 1260.9 F/g. Highly flexible all-solid-state SCs were subsequently assembled with these novel HZM electrodes using polyvinyl alcohol/LiCl electrolyte. The working devices achieved very high total areal capacitance of 26 mF/cm(2) and retained 87.5% of the original capacitance even after 10 000 charge/discharge cycles. An integrated power pack incorporating series-wound SCs and dye-sensitized solar cells was demonstrated for stand-alone self-powered systems.

All-solid-state flexible supercapacitors based on a carbon/MnO(2) (C/M) core-shell fiber structure were fabricated with high electrochemical performance such as high rate capability with a scan rate up to 20 V s(-1), high volume capacitance of 2.5 F cm(-3), and an energy density of 2.2 × 10(-4) Wh cm(-3). By integrating with a triboelectric generator, supercapacitors could be charged and power commercial electronic devices, such as a liquid crystal display or a light-emitting-diode, demonstrating feasibility as an efficient storage component and self-powered micro/nanosystems.