选择性硒掺杂提高NiFe2O4/NiOOH异质结电催化析氧性能

doi:10.1016/S1872-2067(20)63739-1

催化学报 ›› 2021, Vol. 42 ›› Issue (8): 1395-1403.DOI: 10.1016/S1872-2067(20)63739-1

选择性硒掺杂提高NiFe₂O₄/NiOOH异质结电催化析氧性能

黄远^a^,^b, 王建军^a^,^b^,^$(), 邹杨^a, 蒋立文^a, 刘晓龙^d, 江文杰^d, 刘宏^a^,^c^,^#(), 胡劲松^d^,^*()

^a山东大学晶体材料国家重点实验室, 山东济南 250100
^b山东大学深圳研究院, 广东深圳 518057
^c济南大学前沿交叉科学研究院, 山东济南 250022
^d中国科学院化学研究所, 分子纳米结构与纳米技术重点实验室, 北京分子科学国家研究中心, 北京 100190

收稿日期:2020-09-24 接受日期:2020-11-18 出版日期:2021-08-18 发布日期:2020-12-10
通讯作者: 王建军,刘宏,胡劲松
作者简介:^$wangjianjun@sdu.edu.cn
^#hongliu@sdu.edu.cn,
^*. 电子信箱: hujs@iccas.ac.cn,
基金资助:
国家自然科学基金(21802086);国家自然科学基金(51732007);国家自然科学基金(21902162);山东省自然科学基金(ZR2019MB048);山东大学齐鲁青年学者项目; 北京分子科学国家研究中心课题(BNLMS201802);深圳市科技创新委员会基础研究计划(JCYJ20190807093411445);山东省高校生物诊断与治疗技术与设备协同创新中心.

Selective Se doping of NiFe₂O₄ on an active NiOOH scaffold for efficient and robust water oxidation

Yuan Huang^a^,^b, Jian-Jun Wang^a^,^b^,^$(), Yang Zou^a, Li-Wen Jiang^a, Xiao-Long Liu^d, Wen-Jie Jiang^d, Hong Liu^a^,^c^,^#(), Jin-Song Hu^d^,^*()

^aState Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, Shandong, China
^bShenzhen Research Institute of Shandong University, Shenzhen 518057, Guangdong, China
^cInstitute for Advanced Interdisciplinary Research (IAIR), University of Jinan, Jinan 250022, Shandong, China
^dBeijing National Laboratory for Molecular Sciences (BNLMS), CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Science, Beijing 100190, China

Received:2020-09-24 Accepted:2020-11-18 Online:2021-08-18 Published:2020-12-10
Contact: Jian-Jun Wang,Hong Liu,Jin-Song Hu
About author:^$. E-mail: wangjianjun@sdu.edu.cn
^#. E-mail: hongliu@sdu.edu.cn,
^*. E-mail: hujs@iccas.ac.cn,
Supported by:
This work was supported by the National Natural Science Foundation of China(21802086);This work was supported by the National Natural Science Foundation of China(51732007);This work was supported by the National Natural Science Foundation of China(21902162);Shandong Provincial Natural Science Foundation(ZR2019MB048);QiLu Young Scientist Program of Shandong University, Beijing National Laboratory for Molecular Sciences Program(BNLMS201802);Shenzhen Fundamental Research Program(JCYJ20190807093411445);the Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong.

摘要/Abstract

摘要：

氢能具有能量密度高、清洁无污染等优势, 被认为是理想的能源, 受到越来越多的关注. 利用太阳能和风能等可再生能源电解水制氢是一种极具发展前景的可以规模化获取清洁氢气的能源技术, 其挑战在于如何降低电能消耗并实现稳定地高速电解制氢. 由于电解水阳极析氧反应(OER)涉及四电子转移, 动力学过程缓慢, 是电解水过程的决速步骤. 因此, 开发高效、廉价、稳定的OER电催化剂对于推动电解水制氢的应用至关重要. 硫族化合物具有良好的导电性, 对OER中间体表现出适宜的吸附/脱附能力, 是一类高活性的析氧电催化剂. 但在析氧反应中硫族化合物会不可避免地发生氧化, 导致其结构坍塌, 使其性能发生大幅衰减. NiOOH被认为是Ni(OH)₂、NiSe和NiS等镍基电催化剂析氧过程中的真实催化活性位点, 在析氧反应过程中表现出优异的稳定性. 因此, 结合硫族化合物的高催化活性和羟基氧化物的高稳定性, 将有望获得高效稳定的析氧电催化剂.
本文提出了一种选择性硒掺杂的策略, 实现了不锈钢基底上NiFe₂O₄/NiOOH异质结的选择性硒掺杂, 获得了硒掺杂浓度可调的NiFe₂O_4-_xSe_x/NiOOH异质结电催化剂, 大幅提升了其电催化析氧性能. 采用X射线衍射技术、拉曼光谱、扫描电镜和透射电镜技术等对NiFe₂O₄/NiOOH异质结的结构、形貌和组分进行了表征. 利用X射线光电子能谱和透射电镜的能量色散光谱仪对硒掺杂产物的元素组成和分布进行了分析. 结果表明, 硒元素仅掺杂到NiFe₂O₄纳米颗粒中, 而NiOOH纳米片骨架保持不变, 保证了催化剂在析氧过程的稳定性. NiFe₂O_4-_xSe_x/NiOOH异质结电极在1 M KOH溶液中表现出较好的析氧性能, 达到10和500 mA cm ^-2电流密度所需要的过电位分别仅为153和259 mV, 塔菲尔斜率为22.2 mV dec ^-1. 更重要的是, NiFe₂O_4-_xSe_x/NiOOH电催化剂的电化学性能稳定性, 计时电流测试表明, 在10~400 mA cm ^-2电流密度下可稳定工作. 稳定性测试表明, 催化剂在100 mA cm ^-2的电流密度下可稳定工作至少300 h. 电催化过程研究表明, 选择性硒掺杂提高了界面间电荷输运能力, 改善了电极表面的浸润性, 优化了活性位点的电子结构, 从而大幅提高催化剂的电催化性能. 密度泛函理论计算结果表明, 硒掺杂会导致NiFe₂O₄表面晶格发生畸变, 显著改善了反应中间体的吸附过程, 因此明显降低了析氧反应决速步骤的能垒. 本研究结果将为未来探索高效和稳定的电催化剂提供新的研究思路.

关键词: 水氧化反应, 选择性硒化, 镍铁尖晶石, 羟基氧化镍, 异质结

Abstract:

There remains a challenge in designing electrocatalysts for water oxidation to create highly efficient catalytic sites for the oxygen evolution reaction (OER) while maintaining their robustness at large outputs. Herein, an etching-assisted synthesis approach was developed to integrate highly active NiFe₂O₄ nanoparticles with a robust and active NiOOH scaffold directly on commercial stainless steel. A precise selenization strategy was then introduced to achieve selective Se doping of NiFe₂O₄ to further enhance its intrinsic OER activity while maintaining a three-dimensional NiOOH nanosheet array as a robust scaffold for prompt mass transfer and gas evolution. The resulting NiFe₂O_4‒_xSe_x/NiOOH electrode exhibited superior electrocatalytic activity with low overpotentials of 153 and 259 mV to deliver benchmark current densities of 10 and 500 mA cm ^-2, respectively. More importantly, the catalyst exhibited remarkable durability at a stable current output of 100 mA cm ^-2 for hundreds of hours. These findings may open up opportunities for exploring efficient and robust electrocatalysts for scalable hydrogen production with practical materials.

Key words: Water oxidation, Selective selenization, NiFe2O4, NiOOH, Heterostructure

黄远, 王建军, 邹杨, 蒋立文, 刘晓龙, 江文杰, 刘宏, 胡劲松. 选择性硒掺杂提高NiFe₂O₄/NiOOH异质结电催化析氧性能[J]. 催化学报, 2021, 42(8): 1395-1403.

Yuan Huang, Jian-Jun Wang, Yang Zou, Li-Wen Jiang, Xiao-Long Liu, Wen-Jie Jiang, Hong Liu, Jin-Song Hu. Selective Se doping of NiFe₂O₄ on an active NiOOH scaffold for efficient and robust water oxidation[J]. Chinese Journal of Catalysis, 2021, 42(8): 1395-1403.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(20)63739-1

https://www.cjcatal.com/CN/Y2021/V42/I8/1395

图/表 5

Fig. 1. (a) Scheme for the preparation of NiFe2O4-xSex/NiOOH. XRD patterns (b) and Raman spectra (c). (I) NiFe2O4-xSex/NiOOH; (II) NiFe2O4/NiOOH; (III) stainless steel. High-resolution XPS spectra of NiFe2O4-xSex/NiOOH and NiFe2O4/NiOOH. (d) Fe 2p; (e) Ni 2p; (f) O 1s; (g) Se 3d.

Fig. 2. Typical SEM images of stainless steel (a), NiFe2O4/NiOOH (b), and NiFe2O4-xSex/NiOOH (c); (d) TEM image of NiFe2O4-xSex/NiOOH; (e) HRTEM image of the nanoparticle in (d); HRTEM image (f) and SAED pattern (g) of the nanosheet in (d); (h) STEM image and corresponding elemental mapping images of NiFe2O4-xSex/NiOOH.

Fig. 3. (a) LSV polarization curves of various catalysts for OER without iR-correction. The orange dashed line and the inset are LSV curves of NiFe2O4-xSex/NiOOH with iR-correction. (b) Corresponding Tafel plots. (c) Comparison of overpotentials and Tafel slopes of NiFe2O4-xSex/NiOOH with state-of-the-art analogs. (d) OER Faradaic efficiency of NiFe2O4-xSex/NiOOH. (e) Stability test of NiFe2O4-xSex/NiOOH for OER at different potentials. (f) Multi-chronoamperometric curves for NiFe2O4-xSex/NiOOH recorded at various overpotentials.

Fig. 4. Nyquist plots (the inset is the model of equivalent circuit) (a) and ECSA-normalized LSV curves (b) of NiFe2O4/NiOOH, NiFe2O4-xSex/ NiOOH, and RuO2/SS. Contact angle images of NiFe2O4/NiOOH (c) and NiFe2O4-xSex/NiOOH (d) at different contact times.

Fig. 5. (a) Structures of NiFe2O4 and Se-doped NiFe2O4. Fe atom (golden), Ni atom (gray), O atom (red), Se atom (green). (b) The free-energy landscape of NiFe2O4 and Se-doped NiFe2O4 for OER.

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选择性硒掺杂提高NiFe₂O₄/NiOOH异质结电催化析氧性能

Selective Se doping of NiFe₂O₄ on an active NiOOH scaffold for efficient and robust water oxidation

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