Ma Shasha, Chen Di, Ye Zhaobin, Wang Yuanlong, Xu Jie, Zhang Jianyong
Sun Yat-Sen University, MOE Laboratory of Polymeric Composite and Functional Materials, School of Materials Science and Engineering, Guangzhou 510275, China.
Dalton Trans. 2025 Sep 30;54(38):14349-14358. doi: 10.1039/d5dt01777g.
The main bottleneck faced by traditional hydrogen production technology through water electrolysis lies in the high energy consumption of the anodic oxygen evolution reaction (OER). Combining the thermodynamically favorable ethanol oxidation reaction (EOR) with the hydrogen evolution reaction provides a promising route to reduce the energy consumption of hydrogen production and generate high value-added products. In this study, a facile method was developed for nickel oxyhydroxide (NiOOH) fabrication. Diverse carboxylic acids were utilized to adjust the surface structure of nickel foam. A self-supporting nickel foam electrode with Ni(OH) nanosheets (FU-NF) was obtained by reacting fumaric acid and nickel foam in DMF through solvothermal treatment. The interconnected Ni(OH) nanosheets form a uniform 3D skeleton network architecture that exposes abundant active sites toward the EOR. Electrochemical studies in the EOR showed that the Ni(OH) nanosheets were oxidized into a higher valence state to form NiOOH species, which is evidenced by Raman spectroscopy. The reconstructed NiOOH served as an active species, thereby enhancing the EOR electrocatalytic activity of FU-NF. The FU-NF electrode exhibited remarkable EOR catalytic activity with current densities of 10 and 100 mA cm at 1.314 and 1.353 V, respectively, and achieved a high faradaic efficiency of 99.84% and maintained outstanding stability for over 100 h. This work provides a new strategy to prepare Ni-based catalysts to convert ethanol into high value-added products.
传统水电解制氢技术面临的主要瓶颈在于阳极析氧反应（OER）的高能耗。将热力学上有利的乙醇氧化反应（EOR）与析氢反应相结合，为降低制氢能耗和生产高附加值产品提供了一条有前景的途径。在本研究中，开发了一种简便的方法来制备氢氧化镍（NiOOH）。使用多种羧酸来调节泡沫镍的表面结构。通过在DMF中使富马酸与泡沫镍进行溶剂热处理，获得了具有Ni(OH)纳米片的自支撑泡沫镍电极（FU-NF）。相互连接的Ni(OH)纳米片形成了一个均匀的三维骨架网络结构，向EOR暴露了丰富的活性位点。EOR的电化学研究表明，Ni(OH)纳米片被氧化成更高价态，形成NiOOH物种，拉曼光谱证实了这一点。重构的NiOOH作为活性物种，从而增强了FU-NF的EOR电催化活性。FU-NF电极在1.314和1.353 V时分别表现出显著的EOR催化活性，电流密度分别为10和100 mA cm，实现了99.84%的高法拉第效率，并在超过100小时内保持了出色的稳定性。这项工作为制备将乙醇转化为高附加值产品的镍基催化剂提供了一种新策略。
