Biomimetic Design of “Trunk‐Branch‐Leaf” Metallene Electrode for Efficient CO 2 Electroreduction

作者：Min Zhang, Ronghao Bai, Liang Yuan, Xun Zhu, Qian Fu, Qiang Liao · 发表于：Carbon Energy · 年份：2025 · DOI：10.1002/cey2.70122 · 被引用次数：3 · 研究领域：CO2 Reduction Techniques and Catalysts、Ammonia Synthesis and Nitrogen Reduction、Electrocatalysts for Energy Conversion

ABSTRACT Controllable synthesis of ultrathin metallene nanosheets and rational design of their spatial arrangement in favor of electrochemical catalysis are critical for their renewable energy applications. Here, a biomimetic design of “Trunk‐Branch‐Leaf” strategy is proposed to prepare the ultrathin edge‐riched Zn‐ene “leaves” with a thickness of ~2.5 nm, adjacent Zn‐ene cross‐linked with each other, which are supported by copper nanoneedle “branches” on copper mesh “trunks,” named as Zn‐ene/Cu‐CM. The resulting superstructure enables the formation of an interconnected network and multiple channels, which can be used as an electrocatalytic CO 2 reduction reaction (CO 2 RR) electrode to allow a fast charge and mass transfer as well as a large electrolyte reservoir. By virtue of the distinctive structure, the obtained Zn‐ene/Cu‐CM electrode exhibits excellent selectivity and activity toward CO production with a maximum Faradaic efficiency of 91.3% and incredible partial current density up to 40 mA cm −2 , outperforming most of the state‐of‐the‐art Zn‐based electrodes for CO 2 reduction. The phenolphthalein color probe combined with in situ attenuated total reflection‐infrared spectroscopy uncovered the formation of the localized pseudo‐alkaline microenvironment at the interface of the Zn‐ene/Cu‐CM electrode. Theoretical calculations confirmed that the localized pH as the origin is responsible for the adsorption of CO 2 at the interface and the generation of *COOH and *CO inter...