Grafted nickel-promoter catalysts for dry reforming of methane identified through high-throughput experimentation
Abstract
High-throughput synthesis of a series of monometallic and bimetallic catalysts (45 bimetallic and 50 monometallic samples) consisting of nickel and one of nine different metal promoters (B, Co, Cu, Fe, Mg, Mn, Sn, V and Zn) supported on one of six different metal oxides alumina, ceria, magnesia, silica and titania) is carried out via organometallic grafting using a robotic platform. The catalysts are evaluated for their activity and selectivity for the dry reforming of methane at a feed ratio of CH4:CO2 of 1 at 650–800 °C in a parallel flow reactor system. The type of oxide support prevails over the type of additive for both catalyst activity and stability. On Al2O3 and MgO, Fe was found to be the best promoter; on SiO2, Cu is the best promoter at 700 °C and higher, while on TiO2, Mn is found to enhance the conversion at 800 °C. On CeO2, all additives except Fe have beneficial effects. Twenty-five catalysts show > 90% methane conversion with ten catalysts showing > 95% conversion at 800 °C with the H2:CO ratios ranging from 0.8 to 1.2. Amongst the ten highest performers, NiFe/Al2O3 and NiFe/MgO are more active than Ni/Al2O3 and Ni/MgO, respectively and were stablemore »
- Authors:
-
[2];
[3];
[2];
[1]
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Univ. of Delaware, Newark, DE (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); Middle East Technical Univ., Ankara (Turkey)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1837073
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Catalysis. A, General
- Additional Journal Information:
- Journal Volume: 629; Journal ID: ISSN 0926-860X
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2; dry reforming; high throughput; methane; nickel; promoter; deactivitation; coke; Raman; XPS; XRD; SEM; TEM; TPR
Citation Formats
Ferrandon, Magali S., Byron, Carly, Celik, Gokhan, Zhang, Yuying, Ni, Chaoying, Sloppy, Jennifer, McCormick, Rachel A., Booksh, Karl, Teplyakov, Andrew V., and Delferro, Massimiliano. Grafted nickel-promoter catalysts for dry reforming of methane identified through high-throughput experimentation. United States: N. p., 2021.
Web. doi:10.1016/j.apcata.2021.118379.
Ferrandon, Magali S., Byron, Carly, Celik, Gokhan, Zhang, Yuying, Ni, Chaoying, Sloppy, Jennifer, McCormick, Rachel A., Booksh, Karl, Teplyakov, Andrew V., & Delferro, Massimiliano. Grafted nickel-promoter catalysts for dry reforming of methane identified through high-throughput experimentation. United States. https://doi.org/10.1016/j.apcata.2021.118379
Ferrandon, Magali S., Byron, Carly, Celik, Gokhan, Zhang, Yuying, Ni, Chaoying, Sloppy, Jennifer, McCormick, Rachel A., Booksh, Karl, Teplyakov, Andrew V., and Delferro, Massimiliano. Wed .
"Grafted nickel-promoter catalysts for dry reforming of methane identified through high-throughput experimentation". United States. https://doi.org/10.1016/j.apcata.2021.118379. https://www.osti.gov/servlets/purl/1837073.
@article{osti_1837073,
title = {Grafted nickel-promoter catalysts for dry reforming of methane identified through high-throughput experimentation},
author = {Ferrandon, Magali S. and Byron, Carly and Celik, Gokhan and Zhang, Yuying and Ni, Chaoying and Sloppy, Jennifer and McCormick, Rachel A. and Booksh, Karl and Teplyakov, Andrew V. and Delferro, Massimiliano},
abstractNote = {High-throughput synthesis of a series of monometallic and bimetallic catalysts (45 bimetallic and 50 monometallic samples) consisting of nickel and one of nine different metal promoters (B, Co, Cu, Fe, Mg, Mn, Sn, V and Zn) supported on one of six different metal oxides alumina, ceria, magnesia, silica and titania) is carried out via organometallic grafting using a robotic platform. The catalysts are evaluated for their activity and selectivity for the dry reforming of methane at a feed ratio of CH4:CO2 of 1 at 650–800 °C in a parallel flow reactor system. The type of oxide support prevails over the type of additive for both catalyst activity and stability. On Al2O3 and MgO, Fe was found to be the best promoter; on SiO2, Cu is the best promoter at 700 °C and higher, while on TiO2, Mn is found to enhance the conversion at 800 °C. On CeO2, all additives except Fe have beneficial effects. Twenty-five catalysts show > 90% methane conversion with ten catalysts showing > 95% conversion at 800 °C with the H2:CO ratios ranging from 0.8 to 1.2. Amongst the ten highest performers, NiFe/Al2O3 and NiFe/MgO are more active than Ni/Al2O3 and Ni/MgO, respectively and were stable over a period of 25 h at 800 °C. Characterization on the as-prepared samples reveals highly dispersed phase, while after reduction in H2, highly dispersed and reduced nickel particles up to 10 nm are formed. The particles do not increase in size under dry reforming reaction conditions at 800 °C. An increased hydrogen consumption observed during H2-TPR of the nickel particles is positively correlated with methane conversion for Al2O3-based catalysts. The resistance to deactivation by coking and variation in coke structure are investigated by spectroscopic and microscopic methods to identify the relationship between metal promoters, alloy formation, and type of surface carbon deposits. Carbon whiskers were observed on the ten selected spent samples and are preferentially deposited on Ni rather than on the promoters. Carbon nanotube formation and metal particle removal from support were not observed to cause deactivation while amorphous carbon formation was clearly linked to catalyst deactivation, as amorphous carbon could encapsulate nickel, either on the support or at the end of the carbon nanotube. Furthermore, the organometallic grafting technique is an efficient and suitable technique for synthesizing highly dispersed and homogeneous phases which lead to high conversion and high durability for dry reforming of methane.},
doi = {10.1016/j.apcata.2021.118379},
journal = {Applied Catalysis. A, General},
number = ,
volume = 629,
place = {United States},
year = {Wed Sep 29 00:00:00 EDT 2021},
month = {Wed Sep 29 00:00:00 EDT 2021}
}
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