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Syngas

About: Syngas is a research topic. Over the lifetime, 25825 publications have been published within this topic receiving 508328 citations. The topic is also known as: Syngas, or synthesis gas & Syngas/synthesis gas.


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Journal ArticleDOI
07 Mar 2013-Nature
TL;DR: A crystal engineering or reticular chemistry strategy that controls pore functionality and size in a series of MOMs with coordinately saturated metal centres and periodically arrayed hexafluorosilicate anions enables a ‘sweet spot’ of kinetics and thermodynamics that offers high volumetric uptake at low CO2 partial pressure (less than 0.15 bar).
Abstract: A series of porous crystalline materials known as metal–organic materials are prepared, and a full sorption study shows that controlled pore size (rather than large surface area) coupled with appropriate chemistry lead to materials exhibiting fast and highly selective CO2 sorption. Metal organic frameworks are porous crystalline materials widely studied as potential gas separation and storage materials for clean energy applications. A general trend in this field has been the development of materials with the largest possible surface area with the aim of maximizing uptake of gases. In this paper the authors generate a series of metal organic frameworks and carry out sorption experiments that suggest that surface area may not be as important as was thought. Rather, pore size, coupled with appropriate chemistry, are the keys to fast CO2 uptake and strong CO2 sorption. Materials designed on these principles attain high selectivity for CO2 over nitrogen, oxygen, methane and hydrogen even in the presence of moisture. The energy costs associated with the separation and purification of industrial commodities, such as gases, fine chemicals and fresh water, currently represent around 15 per cent of global energy production, and the demand for such commodities is projected to triple by 2050 (ref. 1). The challenge of developing effective separation and purification technologies that have much smaller energy footprints is greater for carbon dioxide (CO2) than for other gases; in addition to its involvement in climate change, CO2 is an impurity in natural gas, biogas (natural gas produced from biomass), syngas (CO/H2, the main source of hydrogen in refineries) and many other gas streams. In the context of porous crystalline materials that can exploit both equilibrium and kinetic selectivity, size selectivity and targeted molecular recognition are attractive characteristics for CO2 separation and capture, as exemplified by zeolites 5A and 13X (ref. 2), as well as metal–organic materials (MOMs)3,4,5,6,7,8,9. Here we report that a crystal engineering7 or reticular chemistry5,9 strategy that controls pore functionality and size in a series of MOMs with coordinately saturated metal centres and periodically arrayed hexafluorosilicate (SiF62−) anions enables a ‘sweet spot’ of kinetics and thermodynamics that offers high volumetric uptake at low CO2 partial pressure (less than 0.15 bar). Most importantly, such MOMs offer an unprecedented CO2 sorption selectivity over N2, H2 and CH4, even in the presence of moisture. These MOMs are therefore relevant to CO2 separation in the context of post-combustion (flue gas, CO2/N2), pre-combustion (shifted synthesis gas stream, CO2/H2) and natural gas upgrading (natural gas clean-up, CO2/CH4).

1,877 citations

Journal ArticleDOI
TL;DR: In this paper, the authors proposed to use CO2 for environmentally-benign physical and chemical processing that adds value to the process, using CO2 as an alternate medium or solvent or co-reactant or a combination of them.

1,541 citations

Journal ArticleDOI
TL;DR: Dry (CO2) reforming of methane literature for catalysts based on Rh, Ru, Pt, and Pd metals is reviewed, including the effect of these noble metals on the kinetics, mechanism and deactivation of these catalysts.
Abstract: Dry (CO2) reforming of methane (DRM) is a well-studied reaction that is of both scientific and industrial importance. This reaction produces syngas that can be used to produce a wide range of products, such as higher alkanes and oxygenates by means of Fischer–Tropsch synthesis. DRM is inevitably accompanied by deactivation due to carbon deposition. DRM is also a highly endothermic reaction and requires operating temperatures of 800–1000 °C to attain high equilibrium conversion of CH4 and CO2 to H2 and CO and to minimize the thermodynamic driving force for carbon deposition. The most widely used catalysts for DRM are based on Ni. However, many of these catalysts undergo severe deactivation due to carbon deposition. Noble metals have also been studied and are typically found to be much more resistant to carbon deposition than Ni catalysts, but are generally uneconomical. Noble metals can also be used to promote the Ni catalysts in order to increase their resistance to deactivation. In order to design catalysts that minimize deactivation, it is necessary to understand the elementary steps involved in the activation and conversion of CH4 and CO2. This review will cover DRM literature for catalysts based on Rh, Ru, Pt, and Pd metals. This includes the effect of these noble metals on the kinetics, mechanism and deactivation of these catalysts.

1,472 citations

Journal ArticleDOI
29 Jan 2004-Nature
TL;DR: Time-resolved, high-resolution in situ transmission electron microscope observations of the formation of carbon nanofibres from methane decomposition over supported nickel nanocrystals show that metallic step edges act as spatiotemporal dynamic growth sites and may be important for understanding other types of catalytic reactions and nanomaterial syntheses.
Abstract: The synthesis of carbon nanotubes with predefined structure and functionality plays a central role in the field of nanotechnology1,2, whereas the inhibition of carbon growth is needed to prevent a breakdown of industrial catalysts for hydrogen and synthesis gas production3. The growth of carbon nanotubes and nanofibres has therefore been widely studied4,5,6,7,8,9,10. Recent advances in in situ techniques now open up the possibility of studying gas–solid interactions at the atomic level11,12. Here we present time-resolved, high-resolution in situ transmission electron microscope observations of the formation of carbon nanofibres from methane decomposition over supported nickel nanocrystals. Carbon nanofibres are observed to develop through a reaction-induced reshaping of the nickel nanocrystals. Specifically, the nucleation and growth of graphene layers are found to be assisted by a dynamic formation and restructuring of mono-atomic step edges at the nickel surface. Density-functional theory calculations indicate that the observations are consistent with a growth mechanism involving surface diffusion of carbon and nickel atoms. The finding that metallic step edges act as spatiotemporal dynamic growth sites may be important for understanding other types of catalytic reactions and nanomaterial syntheses.

1,357 citations

Journal ArticleDOI
TL;DR: Improved new methods for the efficient reductive conversion of CO(2) to methanol and/or DME that the authors have developed include bireforming with methane and ways of catalytic or electrochemical conversions.
Abstract: Nature’s photosynthesis uses the sun’s energy with chlorophyll in plants as a catalyst to recycle carbon dioxide and water into new plant life. Only given sufficient geological time can new fossil fuels be formed naturally. In contrast, chemical recycling of carbon dioxide from natural and industrial sources as well as varied human activities or even from the air itself to methanol or dimethyl ether (DME) and their varied products can be achieved via its capture and subsequent reductive hydrogenative conversion. The present Perspective reviews this new approach and our research in the field over the last 15 years. Carbon recycling represents a significant aspect of our proposed Methanol Economy. Any available energy source (alternative energies such as solar, wind, geothermal, and atomic energy) can be used for the production of needed hydrogen and chemical conversion of CO2. Improved new methods for the efficient reductive conversion of CO2 to methanol and/or DME that we have developed include bireformin...

1,236 citations


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Performance
Metrics
No. of papers in the topic in previous years
YearPapers
20241
2023942
20221,711
20211,195
20201,473
20191,426