Wu Tong, Wu Zihao, Shi Ziqian, Zhang Lihua, Zhan Yinbo, Dong Yilin, Zhou Bowei, Wei Fei, Zhang Dongliang, Gao Yukun, Yin Penggang, Zhao Yixin, Qi Limin, Long Xia
China-UK Low Carbon College, Shanghai Jiao Tong University, Shanghai, 201306, P. R. China.
College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
Small. 2025 Jan;21(1):e2406906. doi: 10.1002/smll.202406906. Epub 2024 Oct 23.
Both the physicochemical properties of catalytic material and the structure of loaded catalyst layer (CL) on gas diffusion electrode (GDE) are of crucial importance in determining the conversion efficiency and product selectivity of carbon dioxide reduction reaction (CORR). However, the highly reducing reaction condition of CORR will lead to the uncontrollable structural and compositional changes of catalysts, making it difficult to tailor surface properties and microstructure of the real active species for favored products. Herein, the interlayer microenvironment of copper-based layered double hydroxides (LDHs) is rationally tuned by a facile ink solvent engineering, which affects both the surface characters and microstructure of CL on GDE, leading to distinct catalytic activity and product selectivity. According to series of in situ and ex situ techniques, the appropriate surface wettability and thickness of porous CL are found to play critical roles in controlling the local CO concentration and water dissociation steps that are key for hydrogenation during CORR, leading to a high Faradaic efficiency of 75.3% for C products and a partial current density of 275 mA cm at -0.8 V versus RHE. This work provides insights into rational design of efficient electrocatalysts toward CORR for multi-carbon generation.
催化材料的物理化学性质和气态扩散电极（GDE）上负载催化剂层（CL）的结构对于确定二氧化碳还原反应（CORR）的转化效率和产物选择性都至关重要。然而，CORR的高还原反应条件会导致催化剂的结构和组成发生不可控变化，使得难以针对所需产物定制实际活性物种的表面性质和微观结构。在此，通过简便的油墨溶剂工程合理调节了铜基层状双氢氧化物（LDHs）的层间微环境，这影响了GDE上CL的表面特征和微观结构，从而导致不同的催化活性和产物选择性。根据一系列原位和非原位技术，发现多孔CL合适的表面润湿性和厚度在控制局部CO浓度和水离解步骤中起着关键作用，而这些步骤是CORR氢化过程的关键，从而在相对于可逆氢电极（RHE）为-0.8 V时实现了75.3%的C产物法拉第效率和275 mA cm⁻²的分电流密度。这项工作为合理设计用于多碳生成的CORR高效电催化剂提供了见解。
