Zhou Peng, Lv Xingshuai, Tao Shasha, Wu Jingcheng, Wang Hongfang, Wei Xiaoxiao, Wang Tehua, Zhou Bo, Lu Yuxuan, Frauenheim Thomas, Fu Xianzhu, Wang Shuangyin, Zou Yuqin
State Key Laboratory of Chemo/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Advanced Catalytic Engineering Research Center of the Ministry of Education, Hunan University, Changsha, 410082, China.
College of Materials Science and Engineering, College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen, 518060, China.
Adv Mater. 2022 Oct;34(42):e2204089. doi: 10.1002/adma.202204089. Epub 2022 Sep 18.
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) provides an efficient way to obtain high-value-added biomass-derived chemicals. Compared with other transition metal oxides, CuO exhibits poor oxygen evolution reaction performance, leading to high Faraday efficiency for HMF oxidation. However, the weak adsorption and activation ability of CuO to OH species restricts its further development. Herein, the CuO-PdO heterogeneous interface is successfully constructed, resulting in an advanced onset-potential of the HMF oxidation reaction (HMFOR), a higher current density than CuO. The results of open-circuit potential, in situ infrared spectroscopy, and theoretical calculations indicate that the introduction of PdO enhances the adsorption capacity of the organic molecule. Meanwhile, the CuO-PdO heterogeneous interface promotes the adsorption and activation of OH species, as demonstrated by zeta potential and electrochemical measurements. This work elucidates the adsorption enhancement mechanism of heterogeneous interfaces and provides constructive guidance for designing efficient multicomponent electrocatalysts in organic electrocatalytic reactions.
5-羟甲基糠醛（HMF）的电催化氧化为获得高附加值的生物质衍生化学品提供了一种有效途径。与其他过渡金属氧化物相比，CuO的析氧反应性能较差，导致HMF氧化具有较高的法拉第效率。然而，CuO对OH物种的弱吸附和活化能力限制了其进一步发展。在此，成功构建了CuO-PdO异质界面，使得HMF氧化反应（HMFOR）具有提前的起始电位，电流密度高于CuO。开路电位、原位红外光谱和理论计算结果表明，PdO的引入增强了有机分子的吸附能力。同时，zeta电位和电化学测量表明，CuO-PdO异质界面促进了OH物种的吸附和活化。这项工作阐明了异质界面的吸附增强机制，并为有机电催化反应中高效多组分电催化剂的设计提供了建设性指导。
