Self-supported film catalyst integrated with multifunctional carbon nanotubes and Ni-Ni(OH)2 heterostructure for promoted hydrogen evolution

doi:10.1016/S1872-2067(24)60057-4

Abstract

Abstract:

In order to reduce energy consumption in water electrolysis, it is of great importance to design active and stable electrocatalysts for hydrogen evolution reaction (HER) in alkaline solution, especially based on earth-abundant metal. Here we integrate carbon nanotubes (CNTs) and Ni-Ni(OH)₂ heterostructure multifunctional components to design a self-supported 3D CNTs-Ni-Ni(OH)₂ catalyst for HER by composite deposition and subsequent in-situ oxidation. In alkaline solution, this designed CNTs-Ni-Ni(OH)₂ catalyst exhibits 0 mV onset overpotential, and overpotentials of 65 mV and 109 mV at 10 and 50 mA/cm² respectively. Electrochemical measurements, characterizations, and simulation results attribute the outstanding performance to the incorporation of CNTs and heterostructure. CNTs induce the formation 3D catalytic surface, enhance electrochemical active surface area, and more importantly weaken the adsorption of H. Moreover, the formation of heterostructure, especially reversible Ni(OH)₂, supplies active sites and adjusts the adsorption strength of H atom to an optimal value. CNTs and heterostructure synergistically facilitate water adsorption, promote water dissociation, and accelerate H₂ desorption. Significantly, integration of multifunctional components supplies a distinct strategy for development of cost-effective electrocatalyst with outstanding performance.

Key words: Ni-Ni(OH)₂ heterostructure, Electrocatalyst, Hydrogen evolution reaction, Carbon nanotubes, Adsorption free energy

Wancheng Zhao, Jiapeng Ma, Dong Tian, Baotao Kang, Fangquan Xia, Jing Cheng, Yajun Wu, Mengyao Wang, Gang Wu. Self-supported film catalyst integrated with multifunctional carbon nanotubes and Ni-Ni(OH)₂ heterostructure for promoted hydrogen evolution[J]. Chinese Journal of Catalysis, 2024, 62: 287-295.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60057-4

https://www.cjcatal.com/EN/Y2024/V62/I7/287

Figures/Tables 7

Fig. 1. Schematic representation of synthesis process of the designed 3D CNTs-Ni-Ni(OH)2 film as well as the corresponding characterizations of solution and films in each step. (a) Illustration of the synthesis process. (b) Image of the electrodeposition solution. (c) SEM images of prepared films corresponding to different stages.

Fig. 2. Elements mappings (a), XPS analysis (b), and XRD pattern (c) of the designed 3D CNTs-Ni-Ni(OH)2 film.

Fig. 3. Performance comparison of the synthesized 3D CNTs-Ni-Ni(OH)2 catalyst with commercial Pt/C in 1.0 mol/L NaOH. (a) Linear sweep voltammograms. (b) Chronopotentiometric curves.

Fig. 4. Influence of CNTs on catalytic activity and morphology of synthesized CNTs-Ni. (a) Linear sweep voltammograms in 1.0 mol/L NaOH for CNTs-Ni films with different deposition time. (b?g) Influence of deposition time on morphology of 3D CNTs-Ni films. (b,c) 15 min; (d,e) 30 min; (f,g) 60 min. Scale bars in (b), (d) and (f), 1 μm. Scale bars in (c), (e) and (g), 200 nm.

Fig. 5. Linear sweep voltammograms (a) and ECSA-normalized linear sweep voltammograms (b) in 1.0 mol/L NaOH for CNTs-Ni films before and after oxidation treatment.

Fig. 6. Theoretical calculations. (a) Crystal structures of CNT-Ni and CNT-Ni(OH)2-Ni. (b) The calculated adsorption free energies of H on pure Ni, CNT-Ni, and CNT-Ni(OH)2-Ni. (c) Calculated d band center of Ni by the partial DOS of pure Ni, CNT-Ni and CNT-Ni(OH)2-Ni.

Fig. 7. Schematic illustration of synergistic effect between CNTs and heterostructure on HER in alkaline solution.

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Self-supported film catalyst integrated with multifunctional carbon nanotubes and Ni-Ni(OH)₂ heterostructure for promoted hydrogen evolution

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