S1 Supporting Information Efficient Reversible Hydrogen Carrier System Based on Amine Reforming of Methanol Jotheeswari Kothandaraman, Sayan Kar, Raktim Sen, Alain Goeppert, George A. Olah* and G. K. Surya Prakash* Loker Hydrocarbon Research Institute and Department of Chemistry, University of Southern California, University Park, Los Angeles, California 90089-1661, United States. 1. Materials and methods All experiments were carried out under inert atmosphere using standard schlenk techniques with the exclusion of moisture. Complexes Ru-Macho ® -BH (C-1) (Strem Chemicals, 98%), Ru- Macho ® (C-2) (Strem Chemicals, 98%), Carbonylhydrido[6-(di-t-butylphosphinomethylene)-2- (N,N-diethylaminomethyl)-1,6-dihydropyridine]ruthenium(II) (C-4) (Strem Chemicals, 98%), (R,R)-Ts-DENEB ® (C-7) (Strem Chemicals, 16% Ru), (R)-RUCY ® -xylBINAP (C-8) (Strem Chemicals, 8% Ru), and anhydrous K 3 PO 4 (Aldrich, 97%) were weighed inside an argon filled glove box without any further purification (Figure S1). Complexes RuHClPN Me P Ph (CO) (C-3) 1 , RuHClPNP iPr (CO) (C-5) 2 , FeHBrPNP iPr (CO) (C-6) 3 were prepared by previously reported methods. N,N’-Dimethylethylenediamine (7) (Combi-Blocks, 98%) was sparged with N 2 for 2 hours and stored in a schlenk flask. Amines 1 (Aldrich, 99%), 2 (Aldrich, 99%), 3 (Aldrich, 99%), 4 (Aldrich, 99%), 6 (Aldrich, 99%) were purified through distillation and amine 5 (Aldrich, 99%) through sublimation prior to use. Methanol (DriSolv) and toluene (DriSolv) were sparged with N 2 for 2 hours and stored over 3 Å molecular sieves. Freshly distilled 1,4-dioxane