Modulating the synergy of Pt single atoms and quantum dots on NiFe LDH for efficient and robust hydrogen evolution

doi:10.1016/j.jmst.2024.07.025

Abstract

Abstract: Hydrogen evolution reaction (HER) from water electrolysis is an ideal alternative solution to address the energy crisis and develop clean energy. However, the construction of an efficient electrocatalyst with multiple active sites that can ensure high metal utilization and promote reaction kinetics simultaneously still leaves a major challenge. Herein, we present a facile strategy to synthesize a HER catalyst comprising Pt single atoms (Pt_SA) anchored in Fe vacancies and Pt quantum dots (Pt_QD) on the surface of NiFe LDH. Benefitting from the hierarchical and ultrathin nanosheet arrays and strong electronic interaction between Pt_SA/Pt_QD and NiFe LDH matrix, the optimized sample (Pt_SA/QD-NiFe_V9 LDH) exhibits outstanding HER performance in 1 M KOH with ultra-low overpotentials of 20 and 67 mV at 10 and 100 mA cm^-2, respectively, outperforming the benchmark Pt/C electrocatalyst. In addition, the electrolyzer using Pt_SA/QD-NiFe_V9 LDH as a cathode requires voltages of only 1.48 and 1.73 V to yield current densities of 10 and 1000 mA cm^-2, respectively. The combination of in situ tests and density functional theory (DFT) calculations reveal that the synergy of Pt_SA and Pt_QD can optimize the kinetics of water dissociation and hydrogen desorption, thus the Volmer-Tafel pathway prevailing the HER process. This work provides a promising surface engineering strategy to develop catalysts for efficient and robust hydrogen evolution.

Key words: Hydrogen evolution reaction, Pt_SA/QD-NiFe_V9 LDH nanostructure, Alkaline water electrolysis, Metal-support interaction, Synergistic effect

Yuewen Wu, Mingpeng Chen, Di Liu, Huachuan Sun, Tong Zhou, Guohao Na, Guoyang Qiu, Dequan Li, Yun Chen, Jianhong Zhao, Yumin Zhang, Jin Zhang, Hui Pan, Feng Liu, Hao Cui, Qingju Liu. Modulating the synergy of Pt single atoms and quantum dots on NiFe LDH for efficient and robust hydrogen evolution[J]. J. Mater. Sci. Technol., 2025, 215: 111-120.

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