Zhang Geng, Yu Rui, Zhou Yu-Qi, Lu Wang-Ting, Cao Fei-Fei
College of Chemistry, Huazhong Agricultural University, 430070, Wuhan, P. R. China.
Key Laboratory of Optoelectronic Chemical Materials and Devices, Ministry of Education, Jianghan University, 430056, Wuhan, P. R. China.
Nanoscale. 2023 Aug 25;15(33):13750-13759. doi: 10.1039/d3nr02896h.
The construction of heterostructures is an effective strategy to enhance electrocatalysis for hydrogen evolution reactions (HERs) and biomass oxidative upgrading. In this work, a Ni/TiO heterostructure prepared by a phase-separation strategy was adopted as a bifunctional electrocatalyst for HERs and biomass oxidation in alkaline media. Due to the optimized hydrogen adsorption energetics as well as the interfacial water structure and hydrogen bond connectivity in the electrical double layer, Ni/TiO exhibited high activity for HERs with an overpotential of 28 mV at 10 mA cm and good durability at 1000 mA cm for over 100 h in an anion exchange membrane (AEM) electrolyzer. In addition, Ni/TiO showed high catalytic performance for the oxidation of biomass-based platform compound 5-hydroxymethylfurfural (HMF) to high-value added compound 2,5-furandicarboxylic acid (FDCA). Continuous production of FDCA with a yield >95% was achieved in the AEM electrolyzer for over 50 h. The superior HMF oxidation performance on the Ni/TiO heterostructure compared to Ni resulted from stronger HMF adsorption, lower Ni-O formation potential, longer Ni-O bond and smaller Ni crystal size.
构建异质结构是增强析氢反应（HERs）电催化和生物质氧化升级的有效策略。在这项工作中，采用相分离策略制备的Ni/TiO异质结构作为碱性介质中HERs和生物质氧化的双功能电催化剂。由于优化了氢吸附能以及双电层中的界面水结构和氢键连接性，Ni/TiO在10 mA cm时具有28 mV的过电位，对HERs表现出高活性，并且在阴离子交换膜（AEM）电解槽中在1000 mA cm下具有超过100小时的良好耐久性。此外，Ni/TiO对生物质基平台化合物5-羟甲基糠醛（HMF）氧化为高附加值化合物2,5-呋喃二甲酸（FDCA）表现出高催化性能。在AEM电解槽中超过50小时实现了FDCA的连续生产，产率>95%。与Ni相比，Ni/TiO异质结构上优异的HMF氧化性能源于更强的HMF吸附、更低的Ni-O形成电位、更长的Ni-O键和更小的Ni晶体尺寸。
