硫掺杂镍铁层状双氢氧化物的氧析出电催化性能

引用本文: 李申宙, 刘健云, 段烁, 王谭源, 李箐. 硫掺杂镍铁层状双氢氧化物的氧析出电催化性能[J]. 催化学报, 2020, 41(5): 847-852. doi: S1872-2067(19)63356-5 shu

Citation: Shenzhou Li, Jianyun Liu, Shuo Duan, Tanyuan Wang, Qing Li. Tuning the oxygen evolution electrocatalysis on NiFe-layered double hydroxides via sulfur doping[J]. Chinese Journal of Catalysis, 2020, 41(5): 847-852. doi: S1872-2067(19)63356-5 shu

硫掺杂镍铁层状双氢氧化物的氧析出电催化性能

华中科技大学材料科学与工程学院, 湖北武汉 430074
基金项目:
国家自然科学基金（21603078，21705052，51602223）.

摘要: 氧析出反应（OER）是裂解水、二氧化碳还原、以及可充电的锌空电池等许多技术中重要的半反应，但受限于其迟缓的反应动力学，开发高效的氧析出催化剂迫在眉睫.在OER出反应中，性能较好的非贵金属催化剂主要是第四周期过渡金属的一些化合物，如氧化物、氢氧化物、硫化物、硒化物、磷化物等等.在这些材料中，镍铁双金属化合物被认为是最优的氧析出材料，尤其是镍铁层状双氢氧化物（NiFe-LDHs）它拥有较大的电化学活性面积以暴露较多活性位点，同时镍铁两种过渡金属元素存在协同效应，使得其具有良好的催化性能.然而，这一类材料的OER性能仍然有优化的空间.研究表明，将硫化物氧化得到的氢氧化物会有少量的硫元素残留，这种硫残留的氢氧化物拥有十分优异的OER性能.为了进一步认识硫的引入对NiFe-LDHs的OER行为的影响，本文通过水热法合成了硫掺杂的NiFe-LDHs，考察了硫的掺杂量对催化剂性能的影响，验证了微量硫的存在对NiFe-LDHs的OER性能的贡献.
扫描电镜图片显示，水热合成的催化剂是厚度为几十纳米的薄片，拥有较高的比表面积，X射线荧光光谱分析证明合成的硫掺杂NiFe-LDHs中镍铁的元素比例为4：1，而且硫的掺杂量并不影响催化剂的形貌和其中镍铁元素比.X射线光电子能谱分析表明，硫原子的引入使得铁原子结合能降低，即硫与铁的相互作用部分降低了铁的价态，这种硫和铁的相互作用能够优化OER反应中间体OH^*与O^*在铁活性位点上的吸附自由能，降低氧析出反应的过电势.电化学测试表明，拥有0.43%的硫掺杂NiFe-LDHs拥有最好的氧析出性能，10mA cm^-1下超电势仅有257mV，Tafel斜率61.5mV dec^-1.此后，随着硫掺杂量的提升，其性能先保持稳定，随后有所下降.在稳定测试中，硫掺杂的镍铁层状双氢氧化物在10mA cm^-1电流密度下循环30h后过电位仅衰减14mV.在对稳定性测试后的催化剂进行表征表明，催化剂发生了轻微了变形，但这对性能的影响不大.综上，本文提供了一种简便的通过非金属元素掺杂调控过渡金属氧化物的结构和电子态的方法，有望为设计高活性OER电催化剂提供新思路.

关键词:

English

Tuning the oxygen evolution electrocatalysis on NiFe-layered double hydroxides via sulfur doping

State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China
Received Date: 14 October 2019
Revised Date: 18 November 2019
Fund Project:
This work was supported by the National Natural Science Foundation of China (21603078, 21705052, 51602223).

Abstract: We report a facile way to prepare sulfur (S) doped Ni_4/5Fe_1/5-layered double hydroxide (LDH) electrocatalysts for oxygen evolution reaction (OER). The influence of S doping amount on the OER activity of the resulted NiFe-LDHs was studied and the optimal surface S content was ca. 0.43 at%. The developed S-doped NiFe-LDH exhibits excellent OER catalyst activity in 1.0 M KOH with overpotential of only 257 mV at the current density of 10 mA cm^-2. Moreover, the catalyst could maintain high activity after 30 h stability test. The high activity of the S-doped NiFe-LDH catalysts may originate from the synergistic effect between S and the Fe sites. This work provides a simple but efficient way to improve the OER performance of transition metal oxides/(oxy)hydroxides.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

硫掺杂镍铁层状双氢氧化物的氧析出电催化性能

English

Tuning the oxygen evolution electrocatalysis on NiFe-layered double hydroxides via sulfur doping

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

硫掺杂镍铁层状双氢氧化物的氧析出电催化性能

English

Tuning the oxygen evolution electrocatalysis on NiFe-layered double hydroxides via sulfur doping

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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