Promoted cobalt metal catalysts suitable for the production of lower olefins from natural gas

Xie, Jingxiu; Paalanen, Pasi P.; Deelen, Tom W. van; Weckhuysen, Bert M.; Louwerse, Manuel J.; Jong, Krijn P. de

doi:10.1038/s41467-018-08019-7

Cited by 96 publications

(60 citation statements)

References 52 publications

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“…[51][52] According to our kinetic analysis, addition of Ba alleviates to a certain degree this limitation, most likely by decreasing H 2 affinity of cobalt. [53][54][55] As well as by the increase in the basic properties of the catalyst surface, weakening the H 2 adsorption, and limiting the H 2 poisoning. 46,[56][57] The XPS measurements confirmed that no electronic effect induced by the addition of Ba is expected, since there was no change in the Co binding energy in the sample with Ba.…”

Section: Co-redmentioning

confidence: 99%

Development of a Ba–CoCe catalyst for the efficient and stable decomposition of ammonia

Morlanés

Sayas

Shterk

et al. 2021

Catal. Sci. Technol.

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Section: Co-redmentioning

confidence: 99%

Development of a Ba–CoCe catalyst for the efficient and stable decomposition of ammonia

Morlanés

Sayas

Shterk

et al. 2021

Catal. Sci. Technol.

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“…S11). To obtain satisfying Rietveld refinement results, it was necessary to allow preferred orientations of hcp Co crystallites, similar to what has been reported before [55]. We ascribe this to polymorphism of Co in the Co-NC/SiO 2 samples, since XRD analysis of metallic cobalt is complicated by the propensity of cobalt to include stacking faults [22,59].…”

Section: Resultsmentioning

confidence: 70%

“…The setup was equipped with an energy dispersive LynxEye XE Position Sensitive Detector (PSD). Details on the complete setup can be found in recent publications [54,55]. The patterns were measured between 5 and 39° 2θ with an increment of 0.07° and time per step of 20.5 s. Multiple scans were accumulated to improve the signal-to-noise ratio only if the patterns were identical.…”

Section: Characterizationmentioning

confidence: 99%

Disk-Shaped Cobalt Nanocrystals as Fischer–Tropsch Synthesis Catalysts Under Industrially Relevant Conditions

et al. 2020

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Colloidal synthesis of metal nanocrystals (NC) offers control over size, crystal structure and shape of nanoparticles, making it a promising method to synthesize model catalysts to investigate structure-performance relationships. Here, we investigated the synthesis of disk-shaped Co-NC, their deposition on a support and performance in the Fischer–Tropsch (FT) synthesis under industrially relevant conditions. From the NC synthesis, either spheres only or a mixture of disk-shaped and spherical Co-NC was obtained. The disks had an average diameter of 15 nm, a thickness of 4 nm and consisted of hcp Co exposing (0001) on the base planes. The spheres were 11 nm on average and consisted of ε-Co. After mild oxidation, the CoO-NC were deposited on SiO2 with numerically 66% of the NC being disk-shaped. After reduction, the catalyst with spherical plus disk-shaped Co-NC had 50% lower intrinsic activity for FT synthesis (20 bar, 220 °C, H2/CO = 2 v/v) than the catalyst with spherical NC only, while C5+-selectivity was similar. Surprisingly, the Co-NC morphology was unchanged after catalysis. Using XPS it was established that nitrogen-containing ligands were largely removed and in situ XRD revealed that both catalysts consisted of 65% hcp Co and 21 or 32% fcc Co during FT. Furthermore, 3–5 nm polycrystalline domains were observed. Through exclusion of several phenomena, we tentatively conclude that the high fraction of (0001) facets in disk-shaped Co-NC decrease FT activity and, although very challenging to pursue, that metal nanoparticle shape effects can be studied at industrially relevant conditions.

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“…Recently, Zhong et al and our group demonstrated that the CO hydrogenation selectivity of cobalt catalysts can be modified to produce light olefins, though the selectivity to CO 2 also remained high in each of these works indicating that the water gas shift (WGS) reaction (CO + H 2 O → CO 2 + H 2 ) remained the dominant overall reaction. A recent work identified the synergetic effects of Na and S in promoting CO hydrogenation to olefins over Co/MnO catalysts, resulting in a low CO 2 selectivity . Ruthenium catalysts have very strong hydrogenation ability, thus are generally unsuitable for producing olefins.…”

Section: Performance Comparison Of Various Ni‐based Catalysts For Ftsmentioning

confidence: 99%

Manganese Oxide Modified Nickel Catalysts for Photothermal CO Hydrogenation to Light Olefins

Wang

Zhao

Liu

et al. 2019

Advanced Energy Materials

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from FTS reactions include light olefins, [2] higher hydrocarbons, methanol, [3] ethylene glycol, [4] dimethyl ether, [5] and aromatics. [6] Among all the products of FTS, light olefins (ethene, propene, and butene) are perhaps the most valuable and widely used in the production of fine chemicals, plastics, coatings, and cosmetics. [7] In FTS, the most commonly used catalysts are group VIIIB transition metals, especially iron, cobalt, nickel, and ruthenium. These catalysts differ in their CO hydrogenation activity and product selectivity, with several of these metals often being used together (in alloy form) to achieve a high CO conversion or to enhance the selectivity toward a specific product or group of products. Iron-based catalysts show good initial selectivity toward light olefins during FTS. [8] During FTS, metallic iron is gradually transformed to iron carbide during reaction (which is considered the true active phase of iron-based FTS catalysts). Iron carbide has a relatively mild hydrogenation ability and the ability to promote CC coupling reactions. However, FTS over iron-based catalysts typically requires temperatures above 300 °C, which can lead to coke formation and sintering of active sites, leading to catalyst deactivation. Co-based catalysts are suitable for CO hydrogenation to Ni-based catalysts are traditionally considered unsuitable for the Fischer-Tropsch syntheses of olefins, due to the very strong hydrogenation ability of metallic Ni. Herein, this paradigm is challenged. A series of MnO supports nickel catalysts (denoted herein as Ni-x) are fabricated by H 2 reduction of a nickel-manganese mixed metal oxide at temperatures (x) ranging from 250 to 600 °C. The Ni-500 catalyst displays unprecedented performance for photothermal CO hydrogenation to olefins, with an olefin selectivity of 33.0% under ultraviolet-visible irradiation. High-resolution transmission electron microscopy, X-ray absorption spectroscopy (XAS), and X-ray diffraction analyses reveal that the Ni-x catalysts contain metallic Ni nanoparticles supported by MnO. X-ray photoelectron spectroscopy and XAS establish that electron transfer from MnO to the Ni 0 nanoparticles is responsible for modifying the electronic structure of nickel (creating Ni δ− states), thereby shifting the CO hydrogenation selectivity toward light olefins. Further, density functional theory calculations show that this electron transfer lowers the adsorption energies of olefins on Ni surfaces, thus minimizing the undesirable deep hydrogenation reactions to higher alkanes. This study conclusively demonstrates that MnO-modified Ni-based catalyst systems can be highly selective for CO hydrogenation to light olefins.

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Promoted cobalt metal catalysts suitable for the production of lower olefins from natural gas

Cited by 96 publications

References 52 publications

Development of a Ba–CoCe catalyst for the efficient and stable decomposition of ammonia

Development of a Ba–CoCe catalyst for the efficient and stable decomposition of ammonia

Disk-Shaped Cobalt Nanocrystals as Fischer–Tropsch Synthesis Catalysts Under Industrially Relevant Conditions

Manganese Oxide Modified Nickel Catalysts for Photothermal CO Hydrogenation to Light Olefins

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