Activating lattice oxygen in NiFe-based (oxy)hydroxide for water electrolysis

• Published in: Nature communications Vol. 13; no. 1; pp. 2191 - 12
• Main Authors: He, Zuyun, Zhang, Jun, Gong, Zhiheng, Lei, Hang, Zhou, Deng, Zhang, Nian, Mai, Wenjie, Zhao, Shijun, Chen, Yan
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 21.04.2022; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/133; 140/146; 140/58; 147/135; 147/143; 147/3; 639/301/299/886; 639/638/77/885; 639/925/357; Carbon fibers; Catalysts; Density functional theory; Dopants; Electrocatalysts; Electrolysis; Energy; Evolution; Humanities and Social Sciences; Hydroxides; Intermetallic compounds; Investigations; Iron compounds; Laboratories; Lattice vacancies; Metal oxides; Microscopy; multidisciplinary; Nickel compounds; Oxidation; Oxygen; Oxygen evolution reactions; Science; Science (multidisciplinary); Spectroscopy; Surface reactions; Transition metal oxides
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-022-29875-4

Transition metal oxides or (oxy)hydroxides have been intensively investigated as promising electrocatalysts for energy and environmental applications. Oxygen in the lattice was reported recently to actively participate in surface reactions. Herein, we report a sacrificial template-directed approach to synthesize Mo-doped NiFe (oxy)hydroxide with modulated oxygen activity as an enhanced electrocatalyst towards oxygen evolution reaction (OER). The obtained MoNiFe (oxy)hydroxide displays a high mass activity of 1910 A/g metal at the overpotential of 300 mV. The combination of density functional theory calculations and advanced spectroscopy techniques suggests that the Mo dopant upshifts the O 2 p band and weakens the metal-oxygen bond of NiFe (oxy)hydroxide, facilitating oxygen vacancy formation and shifting the reaction pathway for OER. Our results provide critical insights into the role of lattice oxygen in determining the activity of (oxy)hydroxides and demonstrate tuning oxygen activity as a promising approach for constructing highly active electrocatalysts. While (oxy)hydroxides are effective oxygen evolution electrocatalysts, the impacts of pre-catalyst properties on catalyst activities are challenging to assess. Here, authors find Mo dopants in Ni-Fe (oxyhydroxides) to promote lattice oxygen participation and to boost oxygen evolution activities.