Hydrogen (H 2 ) was produced via sorption-enhanced steam reforming of ethanol (SESRE) over multifunctional hybrid materials made of cobalt (10 wt %) and a Ca-based sorbent modified by CeO 2 , ZrO 2 , and MgO. SESRE provides an excellent opportunity for producing pure H 2 from renewable ethanol by merging catalytic steam reforming and removal of the co-product carbon dioxide (CO 2 ) in a single process. The chosen hybrid materials were synthesized using the coprecipitation method and denoted as Co−CaO/CeO 2 (or HM1), Co−CaO/ZrO 2 (or HM2), and Co−CaO/MgO (or HM3). Their features were investigated using electron microscopy, X-ray diffraction, and CO 2 -temperature-programmed desorption. Their sorption capacity and adsorption breakthrough time were determined. All of the chosen materials performed remarkably well and improved H 2 production. Especially, hybrid materials containing cerium (HM1) and zirconium (HM2) displayed better adsorption capacity and extended breakthrough time than those bearing magnesium (HM3). At T = 773 K, HM1 showed the longest breakthrough time (45 min) and adsorption capacity (5.61 mol CO 2 /kg sorbent). Material HM2 demonstrated its highest breakthrough time (30 min) and adsorption capacity (3.78 mol CO 2 /kg sorbent) at T = 723 K and produced >85 mol % H 2 . HM3 displayed the highest breakthrough time (15 min) and adsorption capacity (1.51 mol CO 2 /kg sorbent) at T = 773 K, producing >75 mol % H 2 . The effects of reaction temperature, steam-tocarbon ratio in the feed, and gas hourly space velocity on the SESRE process were investigated. The performance of HM1, HM2, and HM3 was assessed over 20 cycles, and it was found that they were stable for up to 13, 10, and 5 cycles. Finally, probable reaction pathways for SESRE were discussed.

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