Wang Zekun, Niu Xueqing, Ye Lin, Wang Xiaoyu, Wang Chao, Wen Yonghong, Zong Lingbo, Wang Lei, Gao Hongtao, Li Xingwei, Zhan Tianrong
Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science (Ministry of Education), College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science (Ministry of Education), College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
J Colloid Interface Sci. 2024 Aug 15;668:607-617. doi: 10.1016/j.jcis.2024.04.198. Epub 2024 Apr 29.
Transition metal-based electrocatalysts generally take place surface reconstruction in alkaline conditions, but little is known about how to improve the reconstruction to a highly active oxyhydroxide surface for an efficient and stable oxygen evolution reaction (OER). Herein, we develop a strategy to accelerate surface reconstruction by combining boron modification and cyclic voltammetry (CV) activation. Density functional theory calculations and in-situ/ex-situ characterizations indicate that both B-doping and electrochemical activation can reduce the energy barrier and contribute to the surface evolution into highly active oxyhydroxides. The formed oxyhydroxide active phase can tune the electronic configuration and boost the OER process. The reconstructed catalyst of CV-B-NiFe-LDH displays excellent alkaline OER performance in freshwater, simulated seawater, and natural seawater with low overpotentials at 100 mA cm (η: 219, 236, and 255 mV, respectively) and good durability. This catalyst also presents outstanding Cl corrosion resistance in alkalized seawater electrolytes. The CV-B-NiFe-LDH||Pt/C electrolyzer reveals prominent performance for alkalized freshwater/seawater splitting. This study provides a guideline for developing advanced OER electrocatalysts by promoting surface reconstruction.
基于过渡金属的电催化剂在碱性条件下通常会发生表面重构，但对于如何将重构提升至高效稳定析氧反应（OER）所需的高活性羟基氧化物表面却知之甚少。在此，我们开发了一种通过硼修饰与循环伏安法（CV）活化相结合来加速表面重构的策略。密度泛函理论计算以及原位/非原位表征表明，硼掺杂和电化学活化均可降低能垒，并促使表面演变为高活性羟基氧化物。形成的羟基氧化物活性相可调节电子构型并促进OER过程。CV-B-NiFe-LDH重构催化剂在淡水、模拟海水和天然海水中均表现出优异的碱性OER性能，在100 mA cm⁻²时过电位较低（η分别为219、236和255 mV）且耐久性良好。该催化剂在碱化海水电解质中还表现出出色的抗Cl⁻腐蚀性。CV-B-NiFe-LDH||Pt/C电解槽在碱化淡水/海水分解方面展现出卓越性能。本研究为通过促进表面重构来开发先进的OER电催化剂提供了指导。
