Breaking the Ni loading-reducibility-dispersion dependence achieved by solid-state co-grinding

Abstract

The loading-dispersion-reducibility dependence has always been one of the most critical issues in the development of high-performance supported metal catalysts. Herein, up to 40 wt % NiO over ordered mesoporous alumina (OMA) was prepared by co-grinding the hybrid of template-containing OMA and Ni(NO₃)₂·6H₂O. Characterization results confirmed that the OMA mesostructure was still preserved even after loading NiO at a content as high as 40 wt %. More importantly, the reduction extent, dispersion, and average particle size of the Ni/OMA catalysts were maintained at ≥ 91.0%, ~13.5%, and ~4.0–5.0 nm, respectively, when the NiO loading was increased from 20 to 40 wt %. The catalysts were evaluated for the CO methanation as a model reaction, and the similarly high turnover frequency of 24.0 h^–1 was achieved at 300 °C for all of the Ni/OMA catalysts. For the catalyst with the highest NiO loading of 40 wt % (40Ni/OMA), the low-temperature activity at 300 °C indexed by the space-time yield of methane (over 325.8 {\mathrm{m}\mathrm{o}\mathrm{l}}_{{\mathrm{C}\mathrm{H}}_4}\cdot {{\mathrm{k}\mathrm{g}}_{\mathrm{c}\mathrm{a}\mathrm{t}}}^{-1}\cdot {\mathrm{h}}^{-1}) was achieved, while the catalyst was operated without an observable deactivation for a time on stream of 120 h under severe reaction conditions of 600 °C and a very high gas hourly space velocity of 240000 mL·g^–1·h^–1. With these significant results, this work paves the way for a rational and controllable design of supported Ni catalysts by breaking the loading-dispersion-reducibility dependence and stabilizing Ni nanoparticles under harsh reaction conditions.

Graphical abstract

Keywords

Ni-supported catalyst / solid-state grinding / metal-support interactions / high Ni loading / high dispersion / CO methanation

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Competing interests

The authors declare that they have no competing interests.

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant No. 22208205), the Fundamental Research Funds for the Central Universities (Grant No. GK202304042), and the Key Research and Development Program of Shaanxi Province (Grant No. 2024SF-YBXM-613).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-024-2499-9 and is accessible for authorized users.

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