Microwave-initiated catalytic dehydrogenation of fossil fuels for the facile production and safe storage of hydrogen

Jie, X

Abstract:: Hydrogen offers the prospect of a highly effective fuel for future sustainable energy, not only because of its intensive energy density per unit-mass but also because its combustion produces no environmentally damaging CO₂ at its point-of-use. Hydrogen is presently manufactured on an industrial scale by steam reforming or partial oxidation of methane and to a lesser degree by gasification of coal. However, these processes also generate significant quantities of CO₂, w...
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APA Style

Jie, X. (2019). Microwave-initiated catalytic dehydrogenation of fossil fuels for the facile production and safe storage of hydrogen [PhD thesis]. University of Oxford.

MLA Style

Jie, X. Microwave-Initiated Catalytic Dehydrogenation of Fossil Fuels for the Facile Production and Safe Storage of Hydrogen. 2019. University of Oxford, PhD thesis.

Chicago Style

Jie, X. 2019. “Microwave-Initiated Catalytic Dehydrogenation of Fossil Fuels for the Facile Production and Safe Storage of Hydrogen.” PhD thesis, University of Oxford.
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+ Jie, X More by this author

Division:: MPLS
Department:: Chemistry
Sub department:: Inorganic Chemistry
Department:: Inorganic Chemistry
Role:: Author

Contributors

+ Edwards, PP

Department:: Inorganic Chemistry
Role:: Supervisor

+ Compton, RG

Department:: Chemistry
Role:: Supervisor

DOI:: 10.5287/ora-ga8n7py8y
Type of award:: DPhil
Level of award:: Doctoral
Awarding institution:: University of Oxford

UUID:: uuid:66f1fb37-472d-4f6d-b456-f5adca703c58
Deposit date:: 2020-05-27
ARK identifier:: ark:/29072/ora_66f1fb37472d4f6db456f5adca703c58

Related item:: The decarbonisation of petroleum and other fossil hydrocarbon fuels for the facile production and safe storage of hydrogen
Description:: The importance of extracted and refined fossil carbonaceous fuels (petroleum, diesel etc.) to the development of human society cannot be overestimated. These natural resources have improved billions of lives, worldwide, in providing accessible, relatively inexpensive energy at nearly every scale. Notwithstanding the credible advances in renewable energy production over the past decade or so, the aerial combustion of coal, natural gas and liquid fossil fuels, given humankinds insatiable demand for power, will continue to be the ready source of more than 85% of the world's energy in the foreseeable and possibly the distant future. Human activities based on the combustion of fossil fuels, however, has led to significant anthropogenic emissions of carbon dioxide (CO2) to the atmosphere – and that fact is now seen as the major contributor to global warming and climate change. To stabilise global mean temperatures will depend on the ultimate transformation of humankind's energy system to one that does not introduce CO2 into the atmosphere. The hydrogen economy has long been mooted as a route to achieving the required net-zero emissions energy future. Paradoxically, fossil fuel sources such as petroleum, crude and extra-heavy crude oil, petrol, diesel and methane are reported here to produce high volumes of high-purity hydrogen through their microwave-initiated catalytic dehydrogenation using fine iron particles. The co-product of this dehydrogenation process, solid carbon, can be safely stored underground in perpetuity or converted in future to valuable hydrocarbons and other materials. Through their catalytic dehydrogenation to yield carbon-free hydrogen – rather than through their aerial combustion to produce carbon dioxide – petroleum and other fossil fuels can now serve as an energy pathway to stabilising global mean temperatures.
Related item:: Rapid Production of High‐Purity Hydrogen Fuel through Microwave‐Promoted Deep Catalytic Dehydrogenation of Liquid Alkanes with Abundant Metals
Description:: Hydrogen as an energy carrier promises a sustainable energy revolution. However, one of the greatest challenges for any future hydrogen economy is the necessity for large scale hydrogen production not involving concurrent CO2 production. The high intrinsic hydrogen content of liquid‐range alkane hydrocarbons (including diesel) offers a potential route to CO2‐free hydrogen production through their catalytic deep dehydrogenation. We report here a means of rapidly liberating high‐purity hydrogen by microwave‐promoted catalytic dehydrogenation of liquid alkanes using Fe and Ni particles supported on silicon carbide. A H2 production selectivity from all evolved gases of some 98 %, is achieved with less than a fraction of a percent of adventitious CO and CO2. The major co‐product is solid, elemental carbon.
Related item:: On the performance optimisation of Fe catalysts in the microwave - assisted H2 production by the dehydrogenation of hexadecane
Description:: Microwave - assisted catalysis has previously been shown to offer unique advantages in the rapid production of hydrogen from hydrocarbons fuels. In this work, we have prepared a series of supported catalysts with varying iron content and support materials, and evaluated the resulting H2 production from hexadecane, a key representative component of diesel fuel. These catalysts, under microwave activation, exhibit high selectivity for H2 over hydrocarbons in the effluent gas. Microwave-assisted Fe catalysts supported on SiC at low Fe loading levels (<10 wt.%) are found to be the most effective catalytic system for rapid and high-purity H2 production from hexadecane.

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Licence:: Terms and Conditions of Use for Oxford University Research Archive

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Thesis

Microwave-initiated catalytic dehydrogenation of fossil fuels for the facile production and safe storage of hydrogen

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Microwave-initiated catalytic dehydrogenation of fossil fuels for the facile production and safe storage of hydrogen

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