The advancement of next-generation energy technologies calls for rationally designed and fabricated electrode materials that have desirable structures and satisfactory performance. Three-dimensional (3D) self-supported amorphous nanomaterials have attracted great enthusiasm as the cornerstone for building high-performance nanodevices. In particular, tremendous efforts have been devoted to the design, fabrication, and evaluation of self-supported amorphous nanomaterials as electrodes for energy storage and conversion devices in the past decade. However, the electrochemical performance of devices assembled with 3D self-supported amorphous nanomaterials still remains to be dramatically promoted to satisfy the demands for more practical applications. In this review, we aim to outline the achievements made in recent years in the development of 3D self-supported amorphous nanomaterials for a broad range of energy storage and conversion processes. We firstly summarize different synthetic strategies employed to synthesize 3D nanomaterials and to tailor their composition, morphology, and structure. Then, the performance of these 3D self-supported amorphous nanomaterials in their corresponding energy-related reactions is highlighted. Finally, we draw out our comprehensive understanding towards both challenges and prospects of this promising field, where valuable guidance and inspiration will surely facilitate further development of 3D self-supported amorphous nanomaterials, thus enabling more highly efficient energy storage and conversion devices that play a key role in embracing a sustainable energy future.

The atomic-level interfacial regulation of single metal sites through heteroatom doping can significantly improve the characteristics of the catalyst and obtain surprising activity. Herein, nickel single-site catalysts (SSCs) with dual-coordinated phosphorus and nitrogen atoms were developed and confirmed (denoted as Ni-P_xN_y, x = 1, 2 and y = 3, 2). In CO₂ reduction reaction (CO₂RR), the CO current density on Ni-P_xN_y was significantly higher than that of Ni-N₄ catalyst without phosphorus modification. Besides, Ni-P₁N₃ performed the highest CO Faradaic efficiency (FE_CO) of 85.0%–98.0% over a wide potential range of −0.65 to −0.95 V (vs. the reversible hydrogen electrode (RHE)). Experimental and theoretical results revealed that the asymmetric Ni-P₁N₃ site was beneficial to CO₂ intermediate adsorption/desorption, thereby accelerating the reaction kinetics and boosting CO₂RR activity. This work provides an effective method for preparing well-defined dual-coordinated SSCs to improve catalytic performance, targetting to CO₂RR applications.