Ligand-regulated Ni-based coordination compounds to promote self-reconstruction for improved oxygen evolution reaction

Ni-based coordination compounds, during the oxygen evolution reaction (OER), self-reconstruct to produce NiOOH, which are the real active sites. Thus, encouraging the self-reconstruction of pre-catalysts to generate more NiOOH species has emerged as an effective strategy for enhancing the activity. In this research, we utilized three coordination compounds, Ni(N(CN) 2 ) 2 , Ni(NCN), and Ni(HNCN) 2 , to examine the effect of three distinct ligands (–N(CN) 2 –, –HNCN–, and –NCN–) on the local electronic structure of coordinated Ni, aiming to promote the degree of self-reconstruction during the OER. XPS studies and in situ Raman spectroscopy revealed a significant relationship between the electron-donating properties of coordinated Ni and the self-reconstruction abilities of the pre-catalysts. Notably, Ni coordinated with –N(CN) 2 – exhibits a high tendency to donate electrons, leading to facile reconstruction of Ni(N(CN) 2 ) 2 into Ni(OOH)–(N(CN) 2 ). As a result, Ni(OOH)–(N(CN) 2 ) displays high OER activity (264 mV @ 10 mA cm −2 and Tafel slope of 40.80 mV dec −1 ) in comparison to Ni(OOH)–(NCN) (290 mV @ 10 mA cm −2 and Tafel slope of 55.63 mV dec −1 ) and Ni(OOH)–(HNCN) (307 mV @ 10 mA cm −2 and Tafel slope of 77.70 mV dec −1 ). These findings offer new perspectives on designing and developing innovative catalysts to enhance OER efficiency.