Construction of Polarized Carbon-Nickel Catalytic Surfaces for Potent, Durable, and Economic Hydrogen Evolution Reactions

Authors

Min Zhou, Yangzhou University, National Institute for Materials Science
Qunhong Weng, National Institute for Materials Science
Zakhar Popov, National University of Science and Technology
Yijun Yang, Beijing Jiaotong University
Liubov Antipina, National University of Science and Technology, Technological Institute for Superhard and Novel Carbon Materials
Pavel Sorokin, National University of Science and Technology, Technological Institute for Superhard and Novel Carbon Materials
Xi Wang, Beijing Jiaotong University, Tianjin University and Collaborative Innovation Center of Chemical Science and Engineering
Yoshio Bando, National Institute for Materials Science, University of Wollongong,Follow
Dmitri Golberg, National Institute for Materials Science, Queensland University of Technology

RIS ID

127817

Publication Details

Zhou, M., Weng, Q., Popov, Z., Yang, Y., Antipina, L., Sorokin, P., Wang, X., Bando, Y. & Golberg, D. (2018). Construction of Polarized Carbon-Nickel Catalytic Surfaces for Potent, Durable, and Economic Hydrogen Evolution Reactions. ACS Nano, 12 (5), 4148-4155.

Abstract

Electrocatalytic hydrogen evolution reaction (HER) in alkaline solution is hindered by its sluggish kinetics toward water dissociation. Nickel-based catalysts, as low-cost and effective candidates, show great potentials to replace platinum (Pt)-based materials in the alkaline media. The main challenge regarding this type of catalysts is their relatively poor durability. In this work, we conceive and construct a charge-polarized carbon layer derived from carbon quantum dots (CQDs) on Ni 3 N nanostructure (Ni 3 N@CQDs) surfaces, which simultaneously exhibit durable and enhanced catalytic activity. The Ni 3 N@CQDs shows an overpotential of 69 mV at a current density of 10 mA cm -2 in a 1 M KOH aqueous solution, lower than that of Pt electrode (116 mV) at the same conditions. Density functional theory (DFT) simulations reveal that Ni 3 N and interfacial oxygen polarize charge distributions between originally equal C-C bonds in CQDs. The partially negatively charged C sites become effective catalytic centers for the key water dissociation step via the formation of new C-H bond (Volmer step) and thus boost the HER activity. Furthermore, the coated carbon is also found to protect interior Ni 3 N from oxidization/hydroxylation and therefore guarantees its durability. This work provides a practical design of robust and durable HER electrocatalysts based on nonprecious metals.