Liu Junbo, Tao Shengyang
School of Chemistry, Dalian University of Technology, Dalian, 116024, China.
State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian, 116024, China.
Adv Sci (Weinh). 2023 Sep;10(27):e2302641. doi: 10.1002/advs.202302641. Epub 2023 Jul 23.
It is well known that nickel-based catalysts have high electrocatalytic activity for the 5-hydroxymethylfurfural oxidation reaction (HMFOR), and NiOOH is the main active component. However, the price of nickel and the catalyst's lifetime still need to be solved. In this work, NiOOH containing oxygen vacancies is formed on the surface of Ni alloy by UV laser (1J85-laser). X-ray absorption fine structure (XAFS) analyses indicate an interaction between Mo and Ni, which affects the coordination environment of Ni with oxygen. The chemical valence of Ni is between 0 and 2, indicating the generation of oxygen vacancies. Density functional theory (DFT) suggests that Mo can increase the defect energy and form more oxygen vacancies. In situ Raman electrochemical spectroscopy shows that Mo can promote the formation of NiOOH, thus enhancing the HMFOR activity. The 1J85-laser electrode shows a longer electrocatalytic lifetime than Ni-laser. After 15 cycles, the conversion of HMF is 95.92%.
众所周知,镍基催化剂对5-羟甲基糠醛氧化反应(HMFOR)具有较高的电催化活性,且NiOOH是主要活性成分。然而,镍的价格以及催化剂的寿命仍有待解决。在这项工作中,通过紫外激光(1J85-激光)在镍合金表面形成了含有氧空位的NiOOH。X射线吸收精细结构(XAFS)分析表明Mo与Ni之间存在相互作用,这影响了Ni与氧的配位环境。Ni的化学价在0到2之间,表明产生了氧空位。密度泛函理论(DFT)表明Mo可以增加缺陷能量并形成更多的氧空位。原位拉曼电化学光谱表明Mo可以促进NiOOH的形成,从而增强HMFOR活性。1J85-激光电极显示出比镍激光更长的电催化寿命。经过15个循环后,HMF的转化率为95.92%。