【作者】 宋涛；

【导师】 张培立；

【作者基本信息】 大连理工大学 ， 化学工程（应用化学方向）（专业学位）， 2021， 硕士

【摘要】 产氧反应是一个关键的半反应,可生成质子,用于电化学和光电化学水分解、CO₂还原和N₂还原。该反应是四质子、四电子转移过程,在动力学上反应迟缓。开发高效、耐用且具有成本效益的水氧化催化剂仍然是该领域面临的最大挑战之一。（1）电催化水氧化需要高效的催化剂来减少过电位并加速缓慢的析氧动力学过程。通过Ba²⁺,Ni²⁺和Fe³⁺的共电沉积法制备了NiFeBa三金属材料,作为高效的电催化水氧化催化剂。与Ni Fe层状双氢氧化物和Ni Fe氧化物相比,NiFeBa表现出优异的水氧化性能,可以在180 m V的过电势下提供10 m A cm^-2的电流密度。掺杂的Ba²⁺用于稳定电生成的Ni³⁺中间体,产生更多的八面体Ni-O用于水氧化,并最终调节催化机理,提高催化效率。（2）镍基材料在电催化水氧化过程中会产生Ni³⁺活性中间体,基于此现象的启发,本文制备了规整的Ni（OH）₂纳米片作为催化剂,用于以水为氧源的电驱动有机物氧化。结果表明,在水溶液中,电驱动Ni（OH）₂成功实现了多种芳基伯胺在阳极处被选择性地电氧化为相应的腈,转化率和选择性均达到98%以上。Ni²⁺/Ni³⁺可以作为芳基伯胺转化的氧化还原活性物质。更多还原

【Abstract】 The oxygen evolution reaction（OER）is a crucial half-reaction that produces protons for electrochemical and photoelectrochemical water splitting,CO₂ reduction,and N₂ reduction.Unfortunately,the OER is a kinetically sluggish half-reaction owing to its four-proton and four-electron process.The development of highly efficient,robust,and cost-effective OER catalysts is one of the biggest challenges in this field.（1）Electrocatalytic water oxidation requires efficient catalysts to reduce the overpotential and accelerate the sluggish kinetics of oxygen formation.Here,NiFeBa trimetal material was prepared by the co-electrodeposition of Ba²⁺,Ni²⁺,and Fe³⁺as an efficient catalyst for electrocatalytic water oxidation.NiFeBa showed enhanced water oxidation performance compared with NiFelayered double hydroxide and NiFeoxide,delivering a current density of 10 m A cm^-2 at an overpotential of 180 m V.Doped Ba ions played a key role in stabilizing the electro-generated Ni³⁺species,producing more octahedral Ni-O structures for water oxidation,adjusting the catalytic mechanism,and finally leading to an enhancement of catalytic efficiency.（2）Inspired by the active Ni³⁺intermediates involved in electrocatalytic water oxidation by Ni-based materials,we prepared Ni（OH）₂ nanosheets as a catalyst and used water as the oxygen source for the oxygenations of various organics.The electrically driven Ni（OH）₂successfully realized the selective electrooxidation of aryl primary amines to the corresponding nitriles at the anode in an aqueous solution,with the conversions efficiencies and selectivity reached more than 98%.Ni²⁺/Ni³⁺can be used as the redox active substance for the conversion of aryl primary amines.更多还原