Impact of trace noble metals on the catalytic performance of LaNiMgO towards methane dry reforming

CO 2 reforming of methane was investigated using trace noble metal anchored MgO-promoted Ni/La 2 O 3 catalyst (LaNiMgO-X), where X = Ir, Pt, Ru, Pd, and Rh. The incorporation of noble metals enhanced Ni dispersion on the support and facilitated the Ni reducibility due to the H 2 spillover effect. At 650 °C and in the early stages of the reaction, all catalysts exhibited enhancement in the catalytic activity. However, at longer times, the control and Pd-embedded catalysts revealed sharp decay in the catalytic activity compared to counterparts, which was assigned to the extensive coke deposition originated by methane cracking methane and Boudouard reactions. Whereas, other noble metals embedded catalysts, in particular, Rh- and Ir-anchored catalysts exhibited high chemical durability with minor decay in the catalytic activity. For instance, after 25h, LaNiMgO-Pd exhibited 22.7 % and 33.2 % decay of its maximum CO 2 and CH 4 conversion, respectively, while LaNiMgO lost 19.7 % and 27.2 % of its maximum CO 2 and CH 4 conversion, respectively. On the other hand, at the same time-on-stream LaNiMgO-Rh lost 0.3 and 0.7 % of its maximum CO 2 and CH 4 conversions, respectively. In durability measurements, and after 140h LaNiMgO-Rh exhibited slight decay in the CO 2 conversion from 77.6 % to 70.5%, the CH 4 conversion decreased from 72.3% to 64.2%. On the other hand, LaNiMgO-Pd depicted rapid decay in the CO 2 conversion from 68.3 % to 49.3 % and the CH 4 conversion felled from 66.5 % to 41.5 % after 50h. In addition, the reactor was blocked in case of LaNiMgO-Pd after about 54h. Excluding Pd, the enhancement of noble metals was assigned to the formation of noble metal-rich Ni surfaces, which suppressed the oxidation of nickel and enhanced the gasification of deposited coke. In addition, the presence of noble metals at the Ni surface afforded a high density of adsorbed oxygen species, which enhanced coke gasification and consequently decreased the extent of deactivation of the catalysts by coke formation. While Pd-anchored sample showed extensive carbon deposition, in particular, recalcitrant γ-carbon, which is hardly gasified, encapsulating the active Ni catalyst, which causes catalyst deactivation. • The DRM performance of noble metals-anchored LaNiMgO was studied. • Noble metals enhanced the Ni dispersion, reducibility, the moderate basic sites and adsorbed oxygenated species. • Rh-anchored catalyst exhibited the highest CO 2 and CH 4 conversions, i.e., 75.7% and 70.0%, respectively. • LaNiMgO-Pd showed the highest decay in CO 2 and CH 4 conversions over 25h, i.e., 22.7% and 33.2%, respectively. • Spent Pd-catalyst showed the highest Cγ content, while spent Rh-catalyst depicted the absence of Cγ.

Authors

Institutions

Publication Details

Journal
Gas Science and Engineering
Published
2024-12-28
DOI
https://doi.org/10.1016/j.jgsce.2024.205533
Citations
8
Primary Topic
Catalytic Processes in Materials Science
Type
article
Field-Weighted Citation Impact
0.94

Funders

Controls
|||
ALL TIME
JAN
FEB
MAR
APR
MAY
JUN
JUL
AUG
SEP
OCT
article

Impact of trace noble metals on the catalytic performance of LaNiMgO towards methane dry reforming

Ahmed Abotaleb, Yahia H. Ahmad, Anand Kumar, Siham Y. Al-Qaradawi et al.
8 citations
Gas Science and Engineering
Catalytic Processes in Materials Science
0.94
article

Impact of trace noble metals on the catalytic performance of LaNiMgO towards methane dry reforming

Ahmed Abotaleb, Yahia H. Ahmad, Anand Kumar, Siham Y. Al-Qaradawi, Assem T. Mohamed, Alessandro Sinopoli, Atef Zekri
article en
8 citations

Abstract

CO 2 reforming of methane was investigated using trace noble metal anchored MgO-promoted Ni/La 2 O 3 catalyst (LaNiMgO-X), where X = Ir, Pt, Ru, Pd, and Rh. The incorporation of noble metals enhanced Ni dispersion on the support and facilitated the Ni reducibility due to the H 2 spillover effect. At 650 °C and in the early stages of the reaction, all catalysts exhibited enhancement in the catalytic activity. However, at longer times, the control and Pd-embedded catalysts revealed sharp decay in the catalytic activity compared to counterparts, which was assigned to the extensive coke deposition originated by methane cracking methane and Boudouard reactions. Whereas, other noble metals embedded catalysts, in particular, Rh- and Ir-anchored catalysts exhibited high chemical durability with minor decay in the catalytic activity. For instance, after 25h, LaNiMgO-Pd exhibited 22.7 % and 33.2 % decay of its maximum CO 2 and CH 4 conversion, respectively, while LaNiMgO lost 19.7 % and 27.2 % of its maximum CO 2 and CH 4 conversion, respectively. On the other hand, at the same time-on-stream LaNiMgO-Rh lost 0.3 and 0.7 % of its maximum CO 2 and CH 4 conversions, respectively. In durability measurements, and after 140h LaNiMgO-Rh exhibited slight decay in the CO 2 conversion from 77.6 % to 70.5%, the CH 4 conversion decreased from 72.3% to 64.2%. On the other hand, LaNiMgO-Pd depicted rapid decay in the CO 2 conversion from 68.3 % to 49.3 % and the CH 4 conversion felled from 66.5 % to 41.5 % after 50h. In addition, the reactor was blocked in case of LaNiMgO-Pd after about 54h. Excluding Pd, the enhancement of noble metals was assigned to the formation of noble metal-rich Ni surfaces, which suppressed the oxidation of nickel and enhanced the gasification of deposited coke. In addition, the presence of noble metals at the Ni surface afforded a high density of adsorbed oxygen species, which enhanced coke gasification and consequently decreased the extent of deactivation of the catalysts by coke formation. While Pd-anchored sample showed extensive carbon deposition, in particular, recalcitrant γ-carbon, which is hardly gasified, encapsulating the active Ni catalyst, which causes catalyst deactivation. • The DRM performance of noble metals-anchored LaNiMgO was studied. • Noble metals enhanced the Ni dispersion, reducibility, the moderate basic sites and adsorbed oxygenated species. • Rh-anchored catalyst exhibited the highest CO 2 and CH 4 conversions, i.e., 75.7% and 70.0%, respectively. • LaNiMgO-Pd showed the highest decay in CO 2 and CH 4 conversions over 25h, i.e., 22.7% and 33.2%, respectively. • Spent Pd-catalyst showed the highest Cγ content, while spent Rh-catalyst depicted the absence of Cγ.

Gas Science and EngineeringVol. 134
Hamad bin Khalifa University (QA), Qatar University (QA)
Qatar University
Openalex Percentile: Top 22%
Catalytic Processes in Materials Science
0.94
AI Navigator

Ask Laika to Summarize, Analyze, and Connect papers live on the map.

Summarize Papers & Methodologies

Extract key findings, datasets, and comparative methods across publications.

Benchmark Rankings & Visual Analytics

Rank top research institutions, authors, funders, topics, and journals by Field-Weighted Citation Impact (FWCI) and paper volume with instant charts.

Connect Distant Disciplines

Bridge topological clusters on the map to find hidden collaborative intersections.