Yang Bo, Deng Jiang, Li Hongrui, Yan Tingting, Zhang Jianping, Zhang Dengsong
International Joint Laboratory of Catalytic Chemistry, Department of Chemistry, Research Center of Nano Science and Technology, College of Sciences, Shanghai University, 200444 Shanghai, China.
iScience. 2021 Jun 17;24(7):102747. doi: 10.1016/j.isci.2021.102747. eCollection 2021 Jul 23.
The coking issue is the main challenge for dry reforming of methane (DRM) over Ni-based catalysts. Herein, we excavate the reasons for the enhanced coking resistance of the bounded Ni over the free state Ni in Ni/γ-AlO catalysts for DRM. Rational metal-support interaction of the bounded Ni would facilitate desorption of CO, thus suppressing CO disproportionation and decreasing carbon deposition. The higher activity of the bounded Ni is ascribed to better methane cracking ability, stronger adsorption, and activation of CO by forming polydentate carbonate. The better activation of CO over the bounded Ni would also contribute to the gasification of formed coke. We gain an insight into the anti-coking mechanism of DRM determined by metal-support interaction in Ni/γ-AlO catalysts through mechanistic studies. It is believed that our findings would enlighten the design of more efficient catalysts for DRM.
积碳问题是镍基催化剂上甲烷干重整(DRM)的主要挑战。在此,我们探究了在用于DRM的Ni/γ -AlO催化剂中,键合态镍比自由态镍具有更高抗积碳性能的原因。键合态镍合理的金属 - 载体相互作用会促进CO的脱附,从而抑制CO歧化反应并减少碳沉积。键合态镍较高的活性归因于更好的甲烷裂解能力、更强的吸附以及通过形成多齿碳酸盐对CO的活化。键合态镍对CO更好的活化作用也有助于所形成焦炭的气化。通过机理研究,我们深入了解了由Ni/γ -AlO催化剂中金属 - 载体相互作用决定的DRM抗积碳机理。相信我们的研究结果将为设计更高效的DRM催化剂提供启示。