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铁促进的氧化锆-氧化铝负载镍催化剂用于通过甲烷干重整高效且经济地生产氢气。

Iron-promoted zirconia-alumina supported Ni catalyst for highly efficient and cost-effective hydrogen production via dry reforming of methane.

机构信息

Chemical Engineering Department, College of Engineering, King Saud University, P.O. Box 800, Riyadh 11421, Saudi Arabia.

Department of Chemistry, Indus University, Ahmedabad, Gujarat 382115, India.

出版信息

J Environ Sci (China). 2025 Feb;148:274-282. doi: 10.1016/j.jes.2023.06.024. Epub 2023 Jun 27.

Abstract

Developing cost-effective and high-performance catalyst systems for dry reforming of methane (DRM) is crucial for producing hydrogen (H) sustainably. Herein, we investigate using iron (Fe) as a promoter and major alumina support in Ni-based catalysts to improve their DRM performance. The addition of iron as a promotor was found to add reducible iron species along with reducible NiO species, enhance the basicity and induce the deposition of oxidizable carbon. By incorporating 1 wt.% Fe into a 5Ni/10ZrAl catalyst, a higher CO interaction and formation of reducible "NiO-species having strong interaction with support" was observed, which led to an ∼80% H yield in 420 min of Time on Stream (TOS). Further increasing the Fe content to 2wt% led to the formation of additional reducible iron oxide species and a noticeable rise in H yield up to 84%. Despite the severe weight loss on Fe-promoted catalysts, high H yield was maintained due to the proper balance between the rate of CH decomposition and the rate of carbon deposit diffusion. Finally, incorporating 3 wt.% Fe into the 5Ni/10ZrAl catalyst resulted in the highest CO interaction, wide presence of reducible NiO-species, minimum graphitic deposit and an 87% H yield. Our findings suggest that iron-promoted zirconia-alumina-supported Ni catalysts can be a cheap and excellent catalytic system for H production via DRM.

摘要

开发具有成本效益和高性能的甲烷干重整(DRM)催化剂体系对于可持续生产氢气(H)至关重要。在此,我们研究了在镍基催化剂中使用铁(Fe)作为促进剂和主要氧化铝载体来提高其 DRM 性能。研究发现,添加铁作为促进剂可以增加可还原铁物种和可还原 NiO 物种,增强碱性并诱导可氧化碳的沉积。通过将 1wt.%的铁掺入 5Ni/10ZrAl 催化剂中,可以观察到更高的 CO 相互作用和可还原“与载体具有强相互作用的 NiO 物种”的形成,这导致在 420 分钟的时间内 H 的产率约为 80%。进一步将铁含量增加到 2wt%,导致形成了额外的可还原氧化铁物种,H 的产率显著提高,达到 84%。尽管在铁促进的催化剂上存在严重的重量损失,但由于 CH 分解的速率和碳沉积物扩散的速率之间的适当平衡,高 H 产率得以维持。最后,将 3wt.%的铁掺入 5Ni/10ZrAl 催化剂中,导致 CO 的相互作用最强,可还原 NiO 物种广泛存在,石墨沉积物最少,H 的产率达到 87%。我们的研究结果表明,铁促进的氧化锆-氧化铝负载镍催化剂可以作为一种廉价且优异的 DRM 制氢催化体系。

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