Hydrogen　is　a　clean　secondary　energy　as　well　as　an　efficient　energy　carrier,　but　the　low　density　and　small　molecular　hydrogen　result　in　high　economic　and　energetic　efforts　to　store　and　transport　hydrogen.　In　addition,　the　hydrogen　produced　by　the　current　industry　is　usually　impure　and　requires　gas　separation,　which　consequently　increases　the　cost　of　hydrogen.　A　promising　hydrogen　storage　technology　using　liquid　organic　hydrogen　carrier　(LOHC)　can　permit　the　safe　storage　of　hydrogen　for　long　time　through　the　reversible　chemical　reaction　in　the　presence　of　catalyst.　The　selective　hydrogenation　reaction　of　N-ethylcarbazole　(NEC),　an　attractive　LOHC　compound　due　to　the　low　dehydrogenation　temperature　of　perhydro-N-ethylcarbazole　(12H-NEC),　with　hydrogen　was　conducted　in　this　study　to　achieve　both　separation　and　hydrogen　storage　for　hydrogen-rich　raw　gas　from　natural　gas　steam　reforming.　First,　hydrogenation　experiments　of　molten　NEC　under　a　pure　hydrogen　atmosphere　were　carried　out　to　determine　the　suitable　hydrogenation　conditions　and　reaction　pathways.　Then,　the　effect　of　methane　addition　on　NEC　hydrogenation　was　analyzed.　Results　indicate　that　there　are　multiple　parallel　pathways　in　the　hydrogenation　of　NEC.　The　reaction　rate　from　8H-NEC　to　12H-NEC　step　is　extremely　slow　and　this　step　is　unstable　at　453　K.　The　optimal　hydrogenation　temperature　of　NEC　is　443　K　and　the　apparent　activation　energy　is　67.6　kJ·mol−1.　The　addition　of　methane　reduces　the　initial　reaction　rate　from　0.877　gH2·(gRu·min)−1　to　0.640　gH2·(gRu·min)−1　but　increases　the　maximum　degree　of　hydrogenation　(DoH)　from　0.870　to　0.909.　©　2022