In-situ conversion of subsurface hydrocarbons via electromagnetic(EM)heating has emerged as a promising technology for producing carbon-zero and affordable hydrogen(H_(2))directly from natural gas reservoirs.However,t...In-situ conversion of subsurface hydrocarbons via electromagnetic(EM)heating has emerged as a promising technology for producing carbon-zero and affordable hydrogen(H_(2))directly from natural gas reservoirs.However,the reaction pathways and role of water as an additional hydrogen donor in EM-assisted methane-to-hydrogen(CH_(4)-to-H_(2))conversion are poorly understood.Herein,we employ a combination of lab-scale EM-heating experiments and reaction modeling analyses to unravel reaction pathways and elucidate water's role in enhancing hydrogen production.The labelled hydrogen isotope of deuterium oxide(D_(2)O)is used to trace the sources of hydrogen.The results show that water significantly boosts hydrogen yield via coke gasification at around 400℃and steam methane reforming(SMR)reaction at over 600℃in the presence of sandstone.Water-gas shift reaction exhibits a minor impact on this enhancement.Reaction mechanism analyses reveal that the involvement of water can initiate auto-catalytic loop reactions with methane,which not only generates extra hydrogen but also produces OH radicals that enhance the reactants'reactivity.This work provides crucial insights into the reaction mechanisms involved in water-carbon-methane interactions and underscores water's potential as a hydrogen donor for in-situ hydrogen production from natural gas reservoirs.It also addresses the challenges related to carbon deposition and in-situ catalyst regeneration during EM heating,thus derisking this technology and laying a foundation for future pilots.展开更多
基金supported by a generous gift from The CH Foundationthe support from the Distinguished Graduate Student Assistantship and the Graduate Research Support Award at Texas Tech University+1 种基金the Aid fund from AAPGthe Matejek Family Faculty Fellowship。
文摘In-situ conversion of subsurface hydrocarbons via electromagnetic(EM)heating has emerged as a promising technology for producing carbon-zero and affordable hydrogen(H_(2))directly from natural gas reservoirs.However,the reaction pathways and role of water as an additional hydrogen donor in EM-assisted methane-to-hydrogen(CH_(4)-to-H_(2))conversion are poorly understood.Herein,we employ a combination of lab-scale EM-heating experiments and reaction modeling analyses to unravel reaction pathways and elucidate water's role in enhancing hydrogen production.The labelled hydrogen isotope of deuterium oxide(D_(2)O)is used to trace the sources of hydrogen.The results show that water significantly boosts hydrogen yield via coke gasification at around 400℃and steam methane reforming(SMR)reaction at over 600℃in the presence of sandstone.Water-gas shift reaction exhibits a minor impact on this enhancement.Reaction mechanism analyses reveal that the involvement of water can initiate auto-catalytic loop reactions with methane,which not only generates extra hydrogen but also produces OH radicals that enhance the reactants'reactivity.This work provides crucial insights into the reaction mechanisms involved in water-carbon-methane interactions and underscores water's potential as a hydrogen donor for in-situ hydrogen production from natural gas reservoirs.It also addresses the challenges related to carbon deposition and in-situ catalyst regeneration during EM heating,thus derisking this technology and laying a foundation for future pilots.
