Research Article

Self-assembled iron-containing mordenite monolith for carbon dioxide sieving

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Science  16 Jul 2021:
Vol. 373, Issue 6552, pp. 315-320
DOI: 10.1126/science.aax5776

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Channeling carbon dioxide

The separation of gas molecules with physisorbents can be challenging because there is often a tradeoff between capacity and selectivity. Zhou et al. report a template-free hydrothermal synthesis of the one-dimensional channel zeolite mordenite, in which some silicon was replaced by iron. Rather than forming a powder that requires further shaping, this mechanically stable material self-assembled into monoliths. Iron atoms bound in tetrahedral zeolite sites narrowed the channels and enabled the size-exclusion separation of carbon dioxide (CO2) over nitrogen (N2) and methane. High CO2 uptake and highly efficient CO2–N2 separation was demonstrated for both dry and humid conditions.

Science, aax5776, this issue p. 315

Abstract

The development of low-cost, efficient physisorbents is essential for gas adsorption and separation; however, the intrinsic tradeoff between capacity and selectivity, as well as the unavoidable shaping procedures of conventional powder sorbents, greatly limits their practical separation efficiency. Herein, an exceedingly stable iron-containing mordenite zeolite monolith with a pore system of precisely narrowed microchannels was self-assembled using a one-pot template- and binder-free process. Iron-containing mordenite monoliths that could be used directly for industrial application afforded record-high volumetric carbon dioxide uptakes (293 and 219 cubic centimeters of carbon dioxide per cubic centimeter of material at 273 and 298 K, respectively, at 1 bar pressure); excellent size-exclusive molecular sieving of carbon dioxide over argon, nitrogen, and methane; stable recyclability; and good moisture resistance capability. Column breakthrough experiments and process simulation further visualized the high separation efficiency.

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