Details

Autor(en) / Beteiligte

• Liu, Yingjie
• Wu, Zhaohui
• Bai, Sha
• Shen, Tianyang
• Li, Qian
• Liu, Guihao
• Sun, Xiaoliang
• Hu, Yihang
• Song, Ziheng
• Chu, Jinfeng
• Song, Yu-Fei

Titel

Revealing the synergistic effect of Ni single atoms and adjacent 3d metal doped Ni nanoparticles in electrocatalytic CO2 reduction

Ist Teil von

• Nanoscale advances, 2024-04, Vol.6 (9), p.2363-2370

Ort / Verlag

RSC

Erscheinungsjahr

2024

Link zum Volltext

Quelle

EZB Electronic Journals Library

Beschreibungen/Notizen

• Herein, we report the successful fabrication of a series of transition metal doped Ni nanoparticles (NPs) coordinated with Ni single atoms in nitrogen-doped carbon nanotubes (denoted as Ni1+NPsM-NCNTs, M = Mn, Fe, Co, Cu and Zn; Ni1 = Ni single atom). X-ray absorption fine structure reveals the coexistence of Ni single atoms with Ni-N4 coordination and NiM NPs. When applied for electrocatalytic CO2RR, the Ni1+NPsM-NCNT compounds show the Faradaic efficiency of CO (FECO) with a volcano-like tendency of Mn < Fe ≈ Co < Zn < Cu, in which the Ni1+NPsCu-NCNT exhibits the highest FECO of 96.92%, a current density of 171.25 mA cm-2 and a sustainable stability over 24 hours at a current density of 100 mA cm-2, outperforming most reported examples in the literature. Detailed experiments and theoretical calculations reveal that for Ni1+NPsCu-NCNTs, the electron transfer from NiCu NPs to Ni single atoms strengthens the adsorption of *COOH intermediates. Moreover, the d-band center of Ni-N in Ni1+NPsCu-NCNT is upshifted, providing stronger binding with the reaction intermediates of *COOH, whereas the NiCu NPs increase the Gibbs free energy change of the Volmer step, suppressing the competitive HER.