南方科技大学知识苑(SUSTech KC): 非贵金属羟基氧化物的制备及其在析氧反应中的应用

题名	非贵金属羟基氧化物的制备及其在析氧反应中的应用
其他题名	Preparation of non-noble metal oxyhydroxides and their application in oxygen evolution reaction
姓名	陈宇萍
姓名拼音	CHEN Yuping
学号	12232070
学位类型	硕士
学位专业	0856 材料与化工
学科门类/专业学位类别	08 工学
导师	JOKYO（徐强）
导师单位	化学系
论文答辩日期	2024-04-24
论文提交日期	2024-06-24
学位授予单位	南方科技大学
学位授予地点	深圳
摘要	析氧反应（Oxygen Evolution Reaction, OER）在电解水产氢中占据主导地位，但因其涉及四电子转移而具有缓慢的动力学，严重影响了产氢的效率，因此，亟需开发高效的催化剂以降低反应能垒，从而加速OER的进行。过渡金属羟基氧化物（MOOH）因其对催化OER具有较高的本征活性而备受关注，但目前大多数MOOH的催化性能受限于导电性较差、比表面积小、结构单一等。本论文通过元素掺杂调控MOOH的微观形貌和电子结构，以此实现高活性和强稳定性OER催化剂的可控制备。具体研究内容如下：通过将W和Fe原子锚定在含有缺陷的CoOOH纳米片的不同位点，成功制备了 W,Fe-CoOOH 催化剂。W 和 Fe 以单原子的形式被锚定在了CoOOH表面，其中，观察到的锚定位置有两种，一种为表面的氧空位位点，另一种为密排六方堆积（HCP）位点。得益于其表面三种原子的特殊排列对CoOOH晶面间距和微观电子结构的影响，W,Fe-CoOOH对OER具有优异的催化性能，在10 mA cm^-2的电流密度下的过电位仅为269 mV并可稳定运行超过700 h。通过采用室温浸渍法在泡沫铁上成功制备了自支撑结构的Ni掺杂的FeOOH催化剂（Ni-FeOOH/IF）。由于三维垂直结构的构筑以及Ni离子对FeOOH电子结构的调控作用，Ni-FeOOH/IF催化剂具有充分暴露的活性位点以及快速的电子传输能力。其在碱性纯水和海水中对 OER 均表现出突出的催化活性，分别仅需183和234 mV的过电位即可达到10 mA cm^-2的电流密度。
其他摘要	Oxygen evolution reaction (OER) plays a dominant role in water electrolysis for hydrogen production, but its slow kinetics caused by the four-electron transfer seriously affect the efficiency of hydrogen production. Therefore, it is urgent to develop efficient catalysts to reduce the reaction energy barrier to accelerate OER process. Transition metal oxyhydroxides (MOOHs) have attracted much attention due to their high intrinsic activity for OER, but the catalytic performance of most MOOHs is currently limited by the poor electrical conductivity, small specific surface area, and single structure. In this thesis, the micromorphology and electronic structures of MOOHs are modulated by element doping, thus achieving the controllable preparation of highly active and strongly stable OER catalysts. The details are as follows: A W,Fe-CoOOH catalyst is successfully prepared by anchoring W and Fe atoms at different sites of defective CoOOH nanosheets. W and Fe were anchored to the CoOOH surface as single atoms. Two types of anchoring positions were observed, one for the oxygen vacancy sites on the surface and the other for Hexagonal Close Packed (HCP) sites. Due to the special arrangement of three kinds of atoms on the surface of CoOOH, the interplanar distance and the microscopic electronic structure are affected, and thus the resultant W,Fe-CoOOH exhibits excellent catalytic performance for OER with an overpotential of only 269 mV at a current density of 10 mA cm^-2 and stable operation for more than 700 h. A self-supported Ni-doped FeOOH catalyst is successfully prepared on iron foam by an impregnation method at room temperature (Ni-FeOOH/IF). Due to the construction of three-dimensional vertical structure and the modulation of the electronic structure of FeOOH by Ni ions, the Ni-FeOOH/IF catalyst has fully exposed active sites and fast electron transfer ability. It exhibits outstanding catalytic activity for OER in both alkaline pure water and seawater, reaching a current density of 10 mA cm^-2 with only 183 and 234 mV, respectively.
关键词	羟基氧化物析氧反应掺杂电子结构微观形貌
其他关键词	Metal Oxyhydroxides Oxygen Evolution Reaction Doping Electronic Structure Micromorphology
语种	中文
培养类别	独立培养
入学年份	2022
学位授予年份	2024-06
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所在学位评定分委会	材料与化工
国内图书分类号	TQ151.1
来源库	人工提交
成果类型	学位论文
条目标识符	http://sustech.caswiz.com/handle/2SGJ60CL/765901
专题	南方科技大学工学院_材料科学与工程系
推荐引用方式 GB/T 7714	陈宇萍. 非贵金属羟基氧化物的制备及其在析氧反应中的应用[D]. 深圳. 南方科技大学,2024.

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