Abstract

This review systematically examines the structural characteristics, compositional design strategies, and recent research trends of layered double hydroxides (LDHs), which are recognized as promising electrocatalyst materials in electrochemical nitrate-to-ammonia conversion. Despite the rapid growth in related research, achieving simultaneous high selectivity and efficiency remains a significant technical challenge due to the complex mechanisms of the nitrate reduction reaction (NitRR) and its inherent competition with the hydrogen evolution reaction (HER). In this study, we analyzed the structural contributions of LDH catalysts for maximizing nitrate reduction efficiency and systematically established key catalyst design indicators required to ensure optimal performance. Specifically, we provide a detailed investigation of the physicochemical mechanisms for enhancing NH₃ production by precisely regulating the adsorption energies of reaction intermediates and maximizing charge transfer efficiency through compositional control and defect engineering. Furthermore, we discuss advanced structural design strategies, such as core-shell tandem structures, MOF-derived architectures, and interlayer anion control, as effective methods for enhancing catalytic performance and optimizing mass transport processes. These insights offer a strategic roadmap for designing high-performance LDH catalysts and represent a critical step toward the practical implementation of sustainable green ammonia production systems, particularly for integration into high-efficiency membrane electrode assembly (MEA) technologies.

• Keywords: Layered double hydroxide, Electrocatalyst, Electrochemical nitrate reduction, Green ammonia