Calcium-looping reforming of methane realizes in situ CO ₂ utilization with improved energy efficiency

Abstract

Closing the anthropogenic carbon cycle is one important strategy to combat climate change, and requires the chemistry to effectively combine CO2 capture with its conversion. Here, we propose a novel in situ CO2 utilization concept, calcium-looping reforming of methane, to realize the capture and conversion of CO2 in one integrated chemical process. This process couples the calcium-looping CO2 capture and the CH4 dry reforming reactions in the CaO-Ni bifunctional sorbent-catalyst, where the CO2 captured by CaO is reduced in situ by CH4 to CO, a reaction catalyzed by catalyzed by the adjacent metallic Ni. The process coupling scheme exhibits excellent decarbonation kinetics by exploiting Le Chatelier’s principle to shift reaction equilibrium through continuous conversion of CO2, and results in an energy consumption 22% lower than that of conventional CH4 dry reforming for CO2 utilization. The proposed CO2 utilization concept offers a promising option to recycle carbon directly at large CO2 stationary sources in an energy-efficient manner.

CO2 capture using solid sorbents: Fundamental aspects, mechanistic insights and recent advances

“…a higher binding energy) with increased CO2 absorption. Further studies of CaO/NiO particles for methane reforming also used XPS to identify two distinct Ni sites, one corresponding to NiO interacting with CaO, and one without interaction [521]. These two phases aligned well with the observed temperature-programmed reduction curves, which all showed the presence of two separate reduction peaks.…”

Enhancing Thermocatalytic Activities by Upshifting the d‐Band Center of Exsolved Co‐Ni‐Fe Ternary Alloy Nanoparticles for the Dry Reforming of Methane

“…[1,2] Carbon dioxide (CO 2 )a nd methane (CH 4 )a re the most contributing gases to the greenhouse effect, [3,4] and the recent discovery of abundant shale gas reserves and methane hydrate has further highlighted the need for their utilization. [1] Thedry reforming of methane (DRM) has been studied as apromising way to utilize CH 4 and CO 2 at the same time by converting these to syngas (a mixture of H 2 and CO) which can be used as fuel or feedstock in the chemical industry. [5][6][7] Despite the economic and environmental advantages of DRM, it has not fully matured for industrial applications because of the deactivation of the conventional Ni-based catalysts from carbon coking and sintering during the reaction.…”

Electrochemical Fixation of Carbon Dioxide in Molten Salts on Liquid Zinc Cathode to Zinc@Graphitic Carbon Spheres for Enhanced Energy Storage

“…[6][7][8][9][10][11][12] Fixation of CO 2 into valuable chemicals could simultaneously realize carbon reduction and reutilization of CO 2. [6,13] For example, high-efficiency fixation of CO 2 enabling a high capacity of ≈123 mAh g −1 at 5 A g −1 , a high Coulombic efficiency of more than 98%, and a long-term stability up to 10 000 cycles as well as a high rate performance. [28] Also, Gao and co-workers designed a special "trihigh tricontinuous" graphene film cathode, presenting a high capacity of ≈120 mAh g −1 at an ultrahigh current density of 400 A g −1 .…”