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.

Single-atom catalysts (SACs) are promising in some reactions typically promoted by homogeneous catalysts.However, the leaching of active species from the support in liquid-phase reactions hinders their potential applications. Herein, taking hydroformylation reaction as an example, we report ionic liquid-induced stabilization of single Rh atoms against leaching. Among the ionic liquids examined, [OHEmim][Tf 2 N] stabilized single-atom Rh 1 /TiO 2 showed a turnover frequency (TOF) of around 800 h -1 in styrene hydroformylation and was able to be recycled for 5 runs without significant deactivation, while the activity for unprotected Rh 1 /TiO 2 decreased over two orders of magnitude under similar conditions. DFT simulations reveal that the IL acts as a linker to connect both Rh and TiO 2 , thereby enhancing the binding energy of Rh species on TiO 2 from 0.69 to

Heterogeneous thermocatalytic hydrogenation is widely believed to occur via co-adsorption of H 2 and other reactants, but in aqueous phase an ionic or electrochemical mechanism was also proposed. Herein, we conduct 4-nitrophenol hydrogenation in an unbiased H-cell, where the H 2 and substrate are separately supplied into two chambers connected by a proton exchange membrane, in comparison with the same reaction in a single cell in which H 2 and 4-nitrophenol are co-fed. Based on the observation of the almost identical hydrogenation performance between the H-cell and the single cell, we conclude that coadsorption of H 2 and 4-nitrophenol is not a prerequisite for hydrogenation in aqueous phase in the tested pH range. Isotope experiments, scavenger test, DFT calculations, and reaction kinetics suggest that a coupled electrochemical half-reaction mechanism for 4-nitrophenol hydrogenation in acidic aqueous phase is predominant. Importantly, while H 2 oxidation primarily occurs on metal sites, 4-nitrophenol reduction occurs on both metal sites and conductive support, highlighting the non-innocent role of the support if the hydrogenation reaction follows the electron− proton-transfer pathway.