Selective conversion of syngas to light olefins

Jiao, Feng; Li, Jinjing; Pan, Xiulian; Xiao, Jianping; Li, Haobo; Ma, Heng; Wei, Mingming; Pan, Yang; Zhou, Zhongyue; Li, Mingrun; Miao, Shu; Li, Jian; Zhu, Yulong; Xiao, Dong; He, Ting; Yang, Jun; Qi, Fei; Fu, Qiang; Bao, Xinhe

doi:10.1126/science.aaf1835

Cited by 1,191 publications

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“…We then repeated this hydrogenation test with the reactor heated to a temperature of 150 °C, and were still unable to detect any carbonaceous species. The TGA experiments were performed on Pd@Nb 2 O 5 catalysts that had been used under high light intensity testing conditions reported in the paper for over 40 h 32. The results from the TGA analysis, plotted in Figure S10 (Supporting Information), showed no weight loss in the temperature range of 400–700 °C for two tests, one performed under flowing CO 2 and the other flowing air.…”

Section: Resultsmentioning

confidence: 99%

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Visible and Near‐Infrared Photothermal Catalyzed Hydrogenation of Gaseous CO₂ over Nanostructured Pd@Nb₂O₅

et al. 2016

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The reverse water gas shift (RWGS) reaction driven by Nb2O5 nanorod‐supported Pd nanocrystals without external heating using visible and near infrared (NIR) light is demonstrated. By measuring the dependence of the RWGS reaction rates on the intensity and spectral power distribution of filtered light incident onto the nanostructured Pd@Nb2O5 catalyst, it is determined that the RWGS reaction is activated photothermally. That is the RWGS reaction is initiated by heat generated from thermalization of charge carriers in the Pd nanocrystals that are excited by interband and intraband absorption of visible and NIR light. Taking advantage of this photothermal effect, a visible and NIR responsive Pd@Nb2O5 hybrid catalyst that efficiently hydrogenates CO2 to CO at an impressive rate as high as 1.8 mmol gcat−1 h−1 is developed. The mechanism of this photothermal reaction involves H2 dissociation on Pd nanocrystals and subsequent spillover of H to the Nb2O5 nanorods whereupon adsorbed CO2 is hydrogenated to CO. This work represents a significant enhancement in our understanding of the underlying mechanism of photothermally driven CO2 reduction and will help guide the way toward the development of highly efficient catalysts that exploit the full solar spectrum to convert gas‐phase CO2 to valuable chemicals and fuels.

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Section: Resultsmentioning

confidence: 99%

“…TGA was performed to determine whether or not carbon deposits reside on the used catalyst 32. These experiments were carried out using a Discovery TGA (TA Instruments).…”

Section: Methodsmentioning

confidence: 99%

Visible and Near‐Infrared Photothermal Catalyzed Hydrogenation of Gaseous CO₂ over Nanostructured Pd@Nb₂O₅

et al. 2016

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“…The FT process can be potentially used in synthesis of chemicals with high commercial value, such as light olefins [1,2], alcohols [3,4] and other oxygenates [5]. The yield of products with secondary functional group (i.e., OH or unsaturated bond) is usually low.…”

Section: Introductionmentioning

confidence: 99%

Investigating the Plasma-Assisted and Thermal Catalytic Dry Methane Reforming for Syngas Production: Process Design, Simulation and Evaluation

2017

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Abstract:The growing surplus of green electricity generated by renewable energy technologies has fueled research towards chemical industry electrification. By adapting power-to-chemical concepts, such as plasma-assisted processes, cheap resources could be converted into fuels and base chemicals. However, the feasibility of those electrified processes at large scale has not been investigated yet. Thus, the current work strives to compare, for first time in the literature, plasma-assisted production of syngas, from CH 4 and CO 2 (dry methane reforming), with thermal catalytic dry methane reforming. Specifically, both processes are conceptually designed to deliver syngas suitable for methanol synthesis (H 2 /CO ≥ 2 in mole). The processes are simulated in the Aspen Plus process simulator where different process steps are investigated. Heat integration and equipment cost estimation are performed for the most promising process flow diagrams. Collectively, plasma-assisted dry methane reforming integrated with combined steam/CO 2 methane reforming is an effective way to deliver syngas for methanol production. It is more sustainable than combined thermal catalytic dry methane reforming with steam methane reforming, which has also been proposed for syngas production of H 2 /CO ≥ 2; in the former process, 40% more CO 2 is captured, while 38% less H 2 O is consumed per mol of syngas. Furthermore, the plasma-assisted process is less complex than the thermal catalytic one; it requires higher amount of utilities, but comparable capital investment.

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“…[3,4] Beide Methoden unterscheiden sich mechanistisch stark voneinander.S on utzt der FT-Prozess trägerfixierte Eisenoder Cobaltkatalysatoren. Die Bildung der Produkte erfolgt über einen Oberflächencarbid-Mechanismus,b ei dem hauptsächlich lineare Olefine und Paraffine entstehen.…”

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Katalytische Umwandlung von Synthesegas in Olefine über Methanol in einem Arbeitsgang

Olsbye

2016

Angewandte Chemie

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[1] Jüngst wurde ein Mischoxidkatalysator in Kombination mit einem MTO-Katalysator für die Umwandlung von Synthesegas mithilfe einer Oxygenat-Zwischenstufe in einem einzigen Reaktor entwickelt (Abbildung 1). [3,4] Beide Methoden unterscheiden sich mechanistisch stark voneinander.S on utzt der FT-Prozess trägerfixierte Eisenoder Cobaltkatalysatoren. Die Bildung der Produkte erfolgt über einen Oberflächencarbid-Mechanismus,b ei dem hauptsächlich lineare Olefine und Paraffine entstehen. Die Kettenlängenverteilung ist abhängig von der relativen Geschwindigkeit der Insertion von CH 2 -Gruppen und von derjenigen der Kettenabbruchreaktion (Schulz-Anderson-FloryVerteilung). Der Katalysator sowie die Reaktionsbedingungen kçnnen so variiert werden, dass einerseits Produkte im Bereich zwischen Methan und leichten Olefinen und andererseits Produkte wie schwere Wachse bevorzugt gebildet werden. Es konnte gezeigt werden, dass eine Zugabe von Natrium und Schwefel zum Eisenkatalysator die Bildung von C 2 -C 4 -Olefinen fçrdert, während die Methanbildung unterdrückt wird, was zu einer stabilen Leistung mit einer Selektivität von 50 %für C 2 -C 4 -Olefine bei einem CO-Umsatz von > 70 %führt. [5] Beim industriellen MTO-Prozess wird der kristalline mikroporçse Silicoaluminiumphosphat-Katalysator H-SAPO-34 eingesetzt. Hierbei wird eine hohe Ausbeute von 91 %C 2 -C 4 -Olefin bei vollständiger Umwandlung des Methanols erhalten.[6] Die hohe Selektivität für die C 2 -C 4 -Olefine ist auf die Struktur von H-SAPO-34 (Abbildung 2) in Verbindung mit einer moderaten Säurestärke zurückführbar. Die Porenstruktur dieses Katalysators besteht aus großen Hohlräumen mit einem Durchmesser von 7.3 12 ; diese Hohlräume sind über kleine Fenster mit einem Durchmesser von 3.8 Abbildung 1. Allgemeines Schema für den FTO-Prozess (oben) und MTO-Prozess (unten).

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Selective conversion of syngas to light olefins

Cited by 1,191 publications

References 28 publications

Visible and Near‐Infrared Photothermal Catalyzed Hydrogenation of Gaseous CO₂ over Nanostructured Pd@Nb₂O₅

Visible and Near‐Infrared Photothermal Catalyzed Hydrogenation of Gaseous CO₂ over Nanostructured Pd@Nb₂O₅

Investigating the Plasma-Assisted and Thermal Catalytic Dry Methane Reforming for Syngas Production: Process Design, Simulation and Evaluation

Katalytische Umwandlung von Synthesegas in Olefine über Methanol in einem Arbeitsgang

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Selective conversion of syngas to light olefins

Cited by 1,191 publications

References 28 publications

Visible and Near‐Infrared Photothermal Catalyzed Hydrogenation of Gaseous CO2 over Nanostructured Pd@Nb2O5

Visible and Near‐Infrared Photothermal Catalyzed Hydrogenation of Gaseous CO2 over Nanostructured Pd@Nb2O5

Investigating the Plasma-Assisted and Thermal Catalytic Dry Methane Reforming for Syngas Production: Process Design, Simulation and Evaluation

Katalytische Umwandlung von Synthesegas in Olefine über Methanol in einem Arbeitsgang

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Product

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Visible and Near‐Infrared Photothermal Catalyzed Hydrogenation of Gaseous CO₂ over Nanostructured Pd@Nb₂O₅

Visible and Near‐Infrared Photothermal Catalyzed Hydrogenation of Gaseous CO₂ over Nanostructured Pd@Nb₂O₅