• Energy Research

AbstractWith the dramatic developments of renewable and environmental‐friendly electrochemical energy conversion systems, there is an urgent need to fabricate durable and efficient electrocatalysts to address the limitation of high overpotentials exceeding thermodynamic requirements to facilitate practical applications. Recently, tellurium‐based nanomaterials (Te NMs) with unique chemical, electronic, and topological properties, including Te‐derived nanostructures and transition metal tellurides (TMTs), have emerged as one of the most promising electrocatalytic materials. In the absence of comprehensive and guiding reviews, this review comprehensively summarizes the main advances in designing emerging Te NMs for electrocatalysis. First, the engineering strategies and principles of Te NMs to enhance their electrocatalytic activity and stability from the nanostructures to the catalytic atoms are discussed in detail, especially on the chemical/physical/multiplex templating strategies, heteroatom doping, vacancy/defect engineering, phase engineering, and the corresponding mechanisms and structure‐performance correlations. Then, typical applications of Te NMs in electrocatalysis are also discussed in detail. Finally, the existing key issues and main challenges of Te NMs for electrocatalysis are highlighted, and the development trend of Te NMs as electrocatalysts is expounded. This review provides new concepts to guide future directions for developing Te NMs‐based electrocatalysts, thereby promoting their future wide applications in electrochemical energy systems.

AbstractAccelerating insoluble Li2S2−Li2S reduction catalysis to mitigate the shuttle effect has emerged as an innovative paradigm for high‐efficient lithium‐sulfur battery cathodes, such as single‐atom catalysts by offering high‐density active sites to realize in situ reaction with solid Li2S2. However, the profound origin of diverse single‐atom species on solid‐solid sulfur reduction catalysis and modulation principles remains ambiguous. Here we disclose the fundamental origin of Li2S2−Li2S reduction catalysis in ferromagnetic elements‐based single‐atom materials to be from their spin density and magnetic moments. The experimental and theoretical studies disclose that the Fe−N4‐based cathodes exhibit the fastest deposition kinetics of Li2S (226 mAh g−1) and the lowest thermodynamic energy barriers (0.56 eV). We believe that the accelerated Li2S2−Li2S reduction catalysis enabled via spin polarization of ferromagnetic atoms provides practical opportunities towards long‐life batteries.