Yang Ming, Li Yingying, Dong Chung-Li, Li Shengkai, Xu Leitao, Chen Wei, Wu Jingcheng, Lu Yuxuan, Pan Yuping, Wu Yandong, Luo Yongxiang, Huang Yu-Cheng, Wang Shuangyin, Zou Yuqin
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, Hunan, 410082, P. R. China.
Research Center for X-ray Science & Department of Physics, Tamkang University, New Taipei City, 25137, Taiwan.
Adv Mater. 2023 Sep;35(39):e2304203. doi: 10.1002/adma.202304203. Epub 2023 Aug 7.
The low-potential furfural oxidation reaction (FFOR) on a Cu-based electrocatalyst can produce H at the anode, thereby providing a bipolar H production system with an ultralow cell voltage. However, the intrinsic activity and stability of the Cu-based electrocatalyst for the FFOR remain unsatisfactory for practical applications. This study investigates the correlation between the valence state and the adsorption behavior of the Cu-based electrocatalyst in furfural oxidation. Cu is the adsorption site with low intrinsic activity. Cu , which exists in the form of Cu(OH) in alkaline electrolytes, has no adsorption ability but can improve the performance of Cu by promoting the adsorption of FF. Moreover, a mixed-valence Cu-based electrocatalyst (MV Cu) with high intrinsic activity and stability is prepared electrochemically. With the MV Cu catalyst, the assembled dual-side H production electrolyzer has a low electricity requirement of only 0.24 kWh m at an ultralow cell voltage of 0.3 V, and it exhibits sufficient stability. This study not only correlates the valence state with the adsorption behavior of the Cu-based electrocatalyst for the low-potential FFOR with anodic H production but also reveals the mechanism of deactivation to provide design principles for Cu-based electrocatalysts with satisfactory stability.
铜基电催化剂上的低电位糠醛氧化反应（FFOR）可在阳极产生氢气，从而为双极制氢系统提供超低的电池电压。然而，用于FFOR的铜基电催化剂的本征活性和稳定性在实际应用中仍不尽人意。本研究探讨了铜基电催化剂在糠醛氧化中的价态与吸附行为之间的相关性。铜是本征活性较低的吸附位点。在碱性电解质中以Cu(OH)形式存在的Cu没有吸附能力，但可以通过促进FF的吸附来提高Cu的性能。此外，通过电化学方法制备了具有高本征活性和稳定性的混合价铜基电催化剂（MV Cu）。使用MV Cu催化剂，组装的双侧制氢电解槽在0.3 V的超低电池电压下仅需0.24 kWh m的低电耗，并且具有足够的稳定性。本研究不仅将价态与用于阳极制氢的低电位FFOR的铜基电催化剂的吸附行为相关联，还揭示了失活机理，为具有令人满意稳定性的铜基电催化剂提供了设计原则。
