Although numerous porous adsorbents have been investigated for NH3 capture applications, these materials often exhibit insufficient NH3 uptake, low NH3 affinity at the ppm level, and poor chemical stability against wet NH3 conditions. The NH3 capture properties of M2(dobpdc) complexes (M=Mg2+, Mn2+, Co2+, Ni2+, and Zn2+; dobpdc4−=4,4‐dioxidobiphenyl‐3,3‐dicarboxylate) that contain open metal sites is presented. The NH3 uptake of Mg2(dobpdc) at 298 K was 23.9 mmol g−1 at 1 bar and 8.25 mmol g−1 at 570 ppm, which are record high capacities at both pressures among existing porous adsorbents. The structural stability of Mg2(dobpdc) upon exposure to wet NH3 was superior to that of the other M2(dobpdc) and the frameworks tested. Overall, these results demonstrate that Mg2(dobpdc) is a recyclable compound that exhibits significant NH3 affinity and capacity, making it a promising candidate for real‐world NH3‐capture applications.
Diamine-functionalized metal−organic frameworks (MOFs) are known as desirable adsorbents that can capture CO 2 even at low pressures, but the humidity instability of bare MOF powders as well as their shaping have not yet adequately addressed for practical applications. Herein, we report an effective synthetic strategy for fabricating millimeter-sized MOF/poly(vinylidene fluoride) (PVDF) composite beads with different amounts of PVDF binders (30, 40, and 50 wt %) via a phase inversion method, followed by the postfunctionalization of 1-ethylpropane-1,3-diamine (epn). Compared with the pristine MOF powder, the diamine-grafted bead, epn-MOF/PVDF40, upon mixing with 40% binder polymers, exhibited a superior long-term performance without structural collapse for up to 1 month. The existence of the hydrophobic PVDF polymer in the composite material is responsible for such durability. This work provides a promising preparative route toward developing stable and shaped MOFs for the removal of indoor CO 2 .
Although metal-organic framework (MOF) powders can be successfully shaped by conventional methods, postsynthetic functionalization of the shaped MOFs remains almost unexplored, yet is required to overcome intrinsic limitations, such as CO2 adsorption capacity and stability. Here, we present a scalable synthesis method for Mg2(dobpdc) MOF and its shaped beads, which are obtained by using a spray dry method after mixing Mg2(dobpdc) powders with alumina sol. The synthesized MOF/Al beads have micron-sized diameters with a moderate particle size distribution of 30–70 μm. They also maintain a high mechanical strength. N-ethylethylenediamine (een) functionalization and coating with long alkyl chain silanes results in een-MOF/Al-Si, which exhibits a significant working capacity of >11 wt% CO2 capture and high hydrophobicity. The een-MOF/Al-Si microbeads retain their crystallinity and improved CO2 uptake upon exposure to humid conditions for three days at a desorption temperature of 140 °C.
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