Surface Geometry‐Electronic Structure Synergy in SbN 4 ‐Rich Multidimensional Nanocarbon Boosts Triiodide Reduction

作者：Yangjun Ma, Xiangtong Meng, Yadong Du, Jun Qi, Hongqi Zou, Xiaoying Wang, Jiachun Li, Jieshan Qiu · 发表于：Small · 年份：2025 · DOI：10.1002/smll.202510239 · 被引用次数：3 · 研究领域：Electrocatalysts for Energy Conversion、Ammonia Synthesis and Nitrogen Reduction、CO2 Reduction Techniques and Catalysts

Abstract The rational design of electrocatalyst surface structures is of great significance for enhancing catalytic activity by increasing the number of active sites, improving charge‐transfer dynamics, and tuning the adsorption behavior of intermediates. Herein, a multidimensional carbon catalyst enriched with atomic antimony coordinated with four nitrogen atoms (i.e., SbN 4 ) is fabricated for triiodide reduction via controlled chemical unzipping of carbon nanotubes (CNTs) followed by Sb incorporation. This catalyst features a carbon heterostructure comprising CNTs covalently bonded to graphene nanoribbons, along with a tunable surface geometry. Thanks to the unique attributes of the Sb‐NDHC‐800, it exhibits more than twice the electrochemically active surface area of pristine CNTs (0.98 cm 2 ) and suppresses the inter‐component interface. When functioning as an electrocatalyst for triiodide reduction, the Sb‐NDHC‐800 showcases an ultralow charge‐transfer resistance (0.14 Ω cm 2 ) coupled with a short electron lifetime (159.15 µs) on the catalyst‐electrolyte interface, exceeding those of the CNTs and DHC‐800 counterparts. Theoretical investigations unveil that the tuned electronic structure of the catalyst and SbN 4 geometries synergistically optimize the adsorption process of intermediates, thereby modulating the rate‐determining step. This work provides insights for manipulating the surface structure of carbon‐based electrocatalysts and elucidating the structure‐performan...