3 years ago

Dual-Ligand Synergistic Modulation: A Satisfactory Strategy for Simultaneously Improving the Activity and Stability of Oxygen Evolution Electrocatalysts

Dual-Ligand Synergistic Modulation: A Satisfactory Strategy for Simultaneously Improving the Activity and Stability of Oxygen Evolution Electrocatalysts
Kun Xiong, Lishan Peng, Ling Zhang, Yao Wang, Jun Wang, Yao Nie, Li Li, Zidong Wei, Wei Ding, Ke Chen
The sluggish kinetics of the oxygen evolution reaction (OER) is the bottleneck of water electrolysis for hydrogen generation. Developing cost-effective OER materials with a high value of practical application is a prerequisite to achieve extreme performance in both activity and stability. Herein, we report a “dual ligand synergistic modulation” strategy to accurately tune the structure of transition-metal materials at atomic level, which finally achieves satisfactory results for the unity between robust stability and high activity. Remarkably, the elaborately designed S and OH dual-ligand NiCo2(SOH)x catalyst exhibits an excellent OER activity with a very small overpotential of 0.29 V at a current density of 10 mA cm–2 and a strong durability even after 30 h accelerated aging at a large current density of 100 mA cm–2, both of which are superior to most of the state-of-the-art OER catalysts so far. The density functional theory (DFT) calculations disclose that the synergy of OH and S ligands on the surface of NiCo2(SOH)x can delicately tune the electronic structure of metal active centers and their chemical environment, which results in optimal binding energies of the OER intermediates (*OH, *O, and *OOH) and a strengthened binding energy between metal and anion ligands, thus leading to an excellent intrinsically enhanced OER activity and stability, respectively. Meanwhile, the special nonmagnetism of NiCo2(SOH)x can significantly weaken the resistance of O2 desorption on the catalyst surface, thus facilitating the O2 evolution proceedings.

Publisher URL: http://dx.doi.org/10.1021/acscatal.7b01971

DOI: 10.1021/acscatal.7b01971

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