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