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Preferentially Stabilizing the Watershed Intermediates by Adsorbate‐adsorbate Interaction to Accelerate CO2 Electroreduction to Ethanol
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2024-12-26 , DOI: 10.1002/adfm.202424583
Pu Huang, Bingling He, Yuming Dong, Jing Zhou, Jing Xu, Chengsi Pan, Yang Lou, Yao Wang, Ying Zhang, Hongwen Huang, Jiawei Zhang

Returning CO2 to liquid ethanol powered by clean energy offers considerable economic benefits and contributes to reaching the goal of carbon neutrality, but it remains a formidable challenge to achieve high ethanol selectivity due to the inevitable strong competition among various pathways. Herein, an investigation is presented to accelerate CO2 electroreduction to ethanol via preferentially stabilizing the precarious watershed intermediates (*CHCOH) by creating strong adsorbate‐adsorbate interaction. The highly ordered CuOx nanoplates (HO‐CuOx NPLs) featuring abundant amorphous‐crystalline interface exhibit an exceptional ethanol Faradaic efficiency (FEEtOH) of 63.8% and an ethanol‐to‐ethylene ratio of 6.1 at a large ethanol partial current density (jethanol) of 232.8 mA cm−2. The findings decipher that abundant in‐between nanogaps in the amorphous‐crystalline interface enhance the adsorption of *OH, which can preferentially strengthen C─O bonds while weakening the Cu─C interaction of *CHCOH through adsorbate‐adsorbate interaction, thereby enabling a predilection for CO2 to ethanol conversion. Beyond an efficient ethanol‐oriented CO2RR electrocatalyst, the investigations provide an in‐depth understanding of adsorbate‐adsorbate interaction on key CO2RR steps and precise intermediates regulation, which can be extended to a range of energy conversion technologies.

中文翻译:


通过吸附物-吸附物相互作用优先稳定流域中间体,以加速 CO2 电还原为乙醇



将 CO2 回归为由清洁能源驱动的液态乙醇可提供可观的经济效益,并有助于实现碳中和的目标,但由于各种途径之间不可避免的激烈竞争,实现高乙醇选择性仍然是一项艰巨的挑战。在此,提出了一项研究,通过产生强吸附物-吸附物相互作用优先稳定不稳定的流域中间体 (*CHCOH) 来加速 CO2 电还原为乙醇。高度有序的 CuOx 纳米板 (HO-CuOx NPLs) 具有丰富的非晶-结晶界面,在 232.8 mA cm-2 的大乙醇部分电流密度 (jethanol) 下表现出 63.8% 的出色乙醇法拉第效率 (FEEtOH) 和 6.1 的乙醇与乙烯比率。研究结果破译了非晶-结晶界面中丰富的纳米间隙增强了 *OH 的吸附,这可以优先加强 C─O 键,同时通过吸附物-吸附物相互作用削弱 *CHCOH 的 Cu─C 相互作用,从而有利于 CO2 转化为乙醇。除了高效的乙醇导向型 CO2RR 电催化剂外,这些研究还提供了对 CO2RR 关键步骤中吸附物-吸附物相互作用和精确中间体调节的深入了解,这可以扩展到一系列能量转换技术。
更新日期:2024-12-26
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