Wu Jia, Wang Ke, Yu Tianqi, Huang Shuaiqin, Zhai Zhixiang, Wen Huan, Yin Shibin
Guangxi Key Laboratory of Electrochemical Energy Materials, Guangxi Colleges and Universities Key Laboratory of Applied Chemistry Technology and Resource Development, School of Chemistry and Chemical Engineering, Guangxi University, 100 Daxue Road, Nanning 530004, China.
Guangxi Key Laboratory of Electrochemical Energy Materials, Guangxi Colleges and Universities Key Laboratory of Applied Chemistry Technology and Resource Development, School of Chemistry and Chemical Engineering, Guangxi University, 100 Daxue Road, Nanning 530004, China.
J Colloid Interface Sci. 2024 Feb;655:676-684. doi: 10.1016/j.jcis.2023.11.061. Epub 2023 Nov 10.
The development of catalysts with high activity, selectivity, and stability is critical for biomass upgrading coupled with hydrogen evolution. In this study, we present a simple method for fabricating crystalline-amorphous phase heterostructures using the etching effect of the acidic medium generated during cobalt salt hydrolysis, resulting in the formation of NiCo(OH)-modified Ni/NiMoO nanosheets electrode (NiCo(OH)/Ni/NiMoO/NF). The nanosheets array formed during the synthesis process enlarges the surface area of the prepared catalyst, which facilitates the exposure of electrochemically active sites and improves mass transfer. Unexpectedly, the strong coupling interactions between the amorphous-crystalline heterointerface optimize the adsorption of reaction molecules and the corresponding charge transfer process, consequently boosting the catalytic activity for the 5-hydroxymethylfurfural oxidation reaction (HMFOR) and hydrogen evolution reaction (HER). Specifically, NiCo(OH)/Ni/NiMoO/NF catalyst requires only 1.34 V to obtain a current density of 10 mA cm for HMFOR-coupled H evolution, and operates stably for 13 consecutive cycles with good product selectivity. This work thus provides insights into the design of efficient and robust catalysts for HMFOR-assisted H evolution.
开发具有高活性、选择性和稳定性的催化剂对于生物质升级与析氢耦合至关重要。在本研究中，我们提出了一种利用钴盐水解过程中产生的酸性介质的蚀刻效应制备晶态-非晶态相异质结构的简单方法，从而形成了NiCo(OH)修饰的Ni/NiMoO纳米片电极（NiCo(OH)/Ni/NiMoO/NF）。合成过程中形成的纳米片阵列扩大了制备的催化剂的表面积，这有利于电化学活性位点的暴露并改善传质。出乎意料的是，非晶-晶态异质界面之间的强耦合相互作用优化了反应分子的吸附和相应的电荷转移过程，从而提高了对5-羟甲基糠醛氧化反应（HMFOR）和析氢反应（HER）的催化活性。具体而言，NiCo(OH)/Ni/NiMoO/NF催化剂在HMFOR耦合析氢反应中仅需1.34 V即可获得10 mA cm的电流密度，并能连续稳定运行13个循环，且具有良好的产物选择性。因此，这项工作为设计用于HMFOR辅助析氢的高效且稳健的催化剂提供了见解。
