As CO2 emissions increase and the global climate deteriorates, converting CO2 into valuable chemicals has become a topic of wide concern. The development of multifunctional catalysts for efficient CO2 conversion remains a major challenge. Herein, two porous organic polymers (NPOPs) functionalized with covalent triazine and triazole N-heterocycles are synthesized through the copper(I)-catalyzed azide–alkyne cycloaddition (CuAAC) reaction. The NPOPs have an abundant microporous content and high specific surface area, which confer them excellent CO2 affinities with a CO2 adsorption capacity of 84.0 mg g−1 and 63.7 mg g−1, respectively, at 273 K and 0.1 MPa. After wet impregnation and in situ reductions, Ag nanoparticles were supported in the NPOPs to obtain Ag@NPOPs with high dispersion and small particle size. The Ag@NPOPs were applied to high-value conversion reactions of CO2 with propargylic amines and terminal alkynes under mild reaction conditions. The carboxylative cyclization transformation of propargylic amine into 2-oxazolidinone and the carboxylation transformation of terminal alkynes into phenylpropiolic acid had the highest TOF values of 1125.1 and 90.9 h−1, respectively. The Ag@NPOP-1 was recycled and used five times without any significant decrease in catalytic activity, showing excellent catalytic stability and durability.
Aqueous zinc metal batteries (ZMBs) are a promising sustainable technology for large‐scale energy storage applications. However, the water is often associated with problematic parasitic reactions on both anode and cathode, leading to the low durability and reliability of ZMBs. Here, a multifunctional separator for the Zn‐V2O5 batteries by growing the coordination supramolecular network (CSN:Zn‐MBA, MBA = 2‐mercaptobenzoic acid) on the conventional non‐woven fabrics (NWF) is developed. CSN tends to form a stronger coordination bond as a softer cation, enabling a thermodynamically preferred Zn2+ to VO2+ substitution in the network, leading to the formation of VO2‐MBA interface, that strongly obstructs the VO2(OH)2− penetration but simultaneously allows Zn2+ transfer. Moreover, Zn‐MBA molecules can adsorb the OTF− and distribute the interfacial Zn2+ homogeneous, which facilitate a dendrite‐free Zn deposition. The Zn‐V2O5 cells with Zn‐MBA@NWF separator realize high capacity of 567 mAh g−1 at 0.2 A g−1, and excellent cyclability over 2000 cycles with capacity retention of 82.2% at 5 A g−1. This work combines the original advantages of the template and new function of metals via cation metathesis within a CSN, provides a new strategy for inhibiting vanadium oxide dissolution.
Metal nanoparticles immobilized in the confined space are a catalogue of efficient and widely used catalysts. Herein we develop a gel‐based bimetallic nanoparticle catalytic system with different ratios of Pd/Cu NPs by wet impregnation and reduction using a stable covalent gel (triazole‐A1B1) as a porous support. Triazole‐A1B1 gel is synthesized from 1,4‐diazidobenzene (A1) and tetrakis(4‐ethynylphenyl)methane (B1) via Cu(I)‐catalyzed azide‐alkyne clcloaddition. The bimetallic Pd/Cu metal nanoparticles are highly dispersed and uniformly distributed with an average particle size distribution of 2.06–3.29 nm. Cu/Pd@A1B1 shows high catalytic efficiency in catalyzing Sonogashira‐Hagihara and Mizoroki‐Heck coupling reactions. The introduction of oxygenophilic Cu effectively improves the catalytic activity of the system. In addition, Cu1Pd2@A1B1 shows good reusability. Especially, it can be reused five times and maintains high catalytic activity without significant deactivation in Mizoroki‐Heck coupling reaction.
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