自模板法合成等级结构Co3O4@NiO双功能电极用于选择性硝酸根还原和四氢异喹啉类半脱氢

Self-template synthesis of hierarchically structured Co3O4@NiO bifunctional electrodes for selective nitrate reduction and tetrahydroisoquinolines semidehydrogenation

等级中空结构的纳米材料具有丰富的活性位点和畅通的电子/物质传递通道,因此在电催化领域具有广阔的应用前景.从环保和节能的角度考虑,电催化硝酸根还原合成铵具有重要意义.高效电催化剂短缺,以及动力学缓慢的阳极析氧反应,严重限制了该技术的发展.本论文发展了一种新颖的自模板转化法,将无机有机杂化的钴基纳米棒成功转化为Co3O4纳米管@NiO多孔纳米片等级材料.该材料在阴极硝酸根电还原为铵和阳极四氢异喹啉类半脱氢为二氢异喹啉类物质的反应中均表现出了优异的性能.更重要的是,合成的Co3O4@NiO等级纳米管还可作为双功能电极,同时合成铵和二氢异喹啉化合物,并具有良好的的选择性和稳定性.

The rational design and synthesis of hierarchically hollow nanostructures with controlled spatial architecture and composition are significant in electrocatalysis owing to their abundant active sites and the expedited electron/mass transfer.Electrocatalytic nitrate reduction to ammonia is of great interest from the points of environmental protection and energy saving.However,the development of this technology is hindered by the lack of efficient nitrate-toammonia electrocatalysts and the kinetically sluggish oxygen evolution reaction at the anode.Herein,a novel self-template conversion method was developed for the synthesis of Co3O4@Ni O hierarchical nanotubes(Co3O4@Ni O HNTs)with Ni O porous nanosheets assembled on Co3O4nanotubes.The as-obtained Co3O4@Ni O HNTs exhibited an outstanding performance for both the cathodic nitrate electroreduction to ammonia reaction and the anodic tetrahydroisoquinolines(THIQs)semi-dehydrogenation to dihydroisoquinolines(DHIQs).Importantly,a two-electrode system of Co3O4@Ni O HNTs||Co3O4@Ni O HNTs was constructed for the simultaneous synthesis of ammonia and DHIQs with high selectivity and robust stability.