Combined Steam and CO2 Reforming of Methane over the Hierarchical Ni-ZrO2 Nanosheets/Al2O3 Catalysts at Ultralow Temperature and under Low Steam,ACS Omega

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Combined Steam and CO2 Reforming of Methane over the Hierarchical Ni-ZrO2 Nanosheets/Al2O3 Catalysts at Ultralow Temperature and under Low Steam
ACS Omega ( IF 3.7 ) Pub Date : 2023-12-03 , DOI: 10.1021/acsomega.3c03676
Wassachol Sumarasingha ₁ , Sabaithip Tungkamani _{1,

2} , Tanakorn Ratana _{1,

2} , Somsak Supasitmongkol ₃ , Monrudee Phongaksorn _{1,

2}

Affiliation

This research developed hierarchical 10 wt % Ni-1 wt % ZrO₂/Al₂O₃ catalysts for combined steam and CO₂ reforming of methane (CSCRM) reaction to produce syngas for gas-to-liquid (GTL) application under the ultralow temperature and low steam condition. The hierarchical nanosheet catalysts were prepared via a novel impregnation technique assisted by ammonia vapor diffusion with various times (1, 6, and 12 h) to develop the different magnitude of hierarchical nanosheets on the surface. Then, CSCRM at 600 °C was performed on the catalysts for 6 h. The results evidenced the improvement of H₂ selectivity, reaching an appropriate H₂/CO ratio (1.9–2.0) in FT subunits in the GTL process when nanosheets existed on the surface due to the increase in H₂O adsorption-dissociation sites. The good dispersion of hierarchical nanosheets accompanied by the ZrO₂ promoter successfully enhanced the CH₄ conversion and the coke prevention through the spread nanosheets because of the increase in the number of active sites and the surface interaction. The interaction of hierarchical nanosheets created the H₂O activation-dissociation sites that allowed CO₂ to be selective on the oxygen vacancy sites, producing more OH* and OH* on the catalyst surface to resist the carbon deposition during CSCRM operation.

中文翻译：

多级 Ni-ZrO2 纳米片/Al2O3 催化剂在超低温低蒸汽下联合蒸汽和 CO2 重整甲烷

本研究开发了多级10 wt % Ni-1 wt % ZrO ₂ /Al ₂ O ₃催化剂，用于甲烷蒸汽和CO ₂组合重整（CSCRM）反应，在超低温下生产用于气制油（GTL）应用的合成气和低蒸汽条件。分级纳米片催化剂是通过一种新颖的浸渍技术制备的，辅以不同时间（1、6和12小时）的氨蒸气扩散，以在表面上形成不同大小的分级纳米片。然后，在600℃下对催化剂进行CSCRM 6小时。结果证明，当表面存在纳米片时，由于H ₂ O吸附解离位点的增加，H ₂选择性得到改善，在GTL过程中FT亚基达到适当的H ₂ /CO比（1.9-2.0）。由于活性位点数量和表面相互作用的增加，分层纳米片与ZrO ₂促进剂相伴的良好分散性通过铺展的纳米片成功地增强了CH ₄转化率和防焦炭。分层纳米片的相互作用产生了H ₂ O活化解离位点，使CO ₂能够选择性地选择性地选择氧空位位点，在催化剂表面产生更多的OH*和OH*，以抵抗CSCRM操作期间的碳沉积。

更新日期：2023-12-03

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