Guo Zhongyuan, Yu Yihong, Li Congcong, Campos Dos Santos Egon, Wang Tianyi, Li Huihui, Xu Jiang, Liu Chuangwei, Li Hao
College of Environmental and Resource Sciences, Zhejiang University, Hangzhou, 310058, China.
Advanced Institute for Materials Research (WPI-AIMR), Tohoku University, Sendai, 980-8577, Japan.
Angew Chem Int Ed Engl. 2024 Mar 18;63(12):e202319913. doi: 10.1002/anie.202319913. Epub 2024 Feb 13.
Authentic surface structures under reaction conditions determine the activity and selectivity of electrocatalysts, therefore, the knowledge of the structure-activity relationship can facilitate the design of efficient catalyst structures for specific reactivity requirements. However, understanding the relationship between a more realistic active surface and its performance is challenging due to the complicated interface microenvironment in electrocatalysis. Herein, we proposed a standard research paradigm to effectively decipher the structure-activity relationship in electrocatalysis, which is exemplified in the CO electroreduction over SnO . The proposed practice has aided in discovering authentic/resting surface states (Sn layer) of SnO accountable for the electrochemical CO reduction reaction (CO RR) performance under electrocatalytic conditions, which then is corroborated in the subsequent CO RR experiments over SnO with different morphologies (nanorods, nanoparticles, and nanosheets) in combination with in situ characterizations. This proposed methodology is further extended to the SnO electrocatalysts, providing helpful insights into catalytic structures. It is believed that our proposed standard research paradigm is also applicable to other electrocatalytic systems, in the meantime, decreases the discrepancy between theory and experiments, and accelerates the design of catalyst structures that achieve sustainable performance for energy conversion.
反应条件下的真实表面结构决定了电催化剂的活性和选择性，因此，了解结构-活性关系有助于设计出满足特定反应活性要求的高效催化剂结构。然而，由于电催化中复杂的界面微环境，理解更真实的活性表面与其性能之间的关系具有挑战性。在此，我们提出了一种标准研究范式，以有效解读电催化中的结构-活性关系，这在SnO上的CO电还原中得到了例证。所提出的方法有助于发现SnO在电催化条件下负责电化学CO还原反应（CO RR）性能的真实/静止表面状态（Sn层），随后通过对不同形貌（纳米棒、纳米颗粒和纳米片）的SnO进行CO RR实验，并结合原位表征对其进行了证实。所提出的方法进一步扩展到SnO电催化剂，为催化结构提供了有益的见解。相信我们提出的标准研究范式也适用于其他电催化系统，同时减少理论与实验之间的差异，并加速设计出实现可持续能量转换性能的催化剂结构。
