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This review focuses on the mechanism and driving force in the intractable gas separation using porous adsorbents. A variety of intractable mixtures have been discussed, including air separation, carbon capture, and hydrocarbon purification. Moreover, the separation systems are categorized according to distinctly biased modes depending on the minor differences in the kinetic diameter, dipole/quadruple moment, and polarizability of the adsorbates, or sorted by the varied separation occasions (e.g., CO2 capture from flue gas or air) and driving forces (thermodynamic and kinetic separation, molecular sieving). Each section highlights the functionalization strategies for porous materials, like synthesis condition optimization and organic group modifications for porous carbon materials, cation exchange and heteroatom doping for zeolites, and metal node‐organic ligand adjustments for MOFs. These functionalization strategies are subsequently associated with enhanced adsorption performances (capacity, selectivity, structural/thermal stability, moisture resistance, etc.) toward the analog gas mixtures. Finally, this review also discusses future challenges and prospects for using porous materials in intractable gas separation. Therein, the combination of theoretical calculation with the synthesis condition and adsorption parameters optimization of porous adsorbents may have great potential, given its fast targeting of candidate adsorbents and deeper insights into the adsorption forces in the confined pores and cages.
This review focuses on the mechanism and driving force in the intractable gas separation using porous adsorbents. A variety of intractable mixtures have been discussed, including air separation, carbon capture, and hydrocarbon purification. Moreover, the separation systems are categorized according to distinctly biased modes depending on the minor differences in the kinetic diameter, dipole/quadruple moment, and polarizability of the adsorbates, or sorted by the varied separation occasions (e.g., CO2 capture from flue gas or air) and driving forces (thermodynamic and kinetic separation, molecular sieving). Each section highlights the functionalization strategies for porous materials, like synthesis condition optimization and organic group modifications for porous carbon materials, cation exchange and heteroatom doping for zeolites, and metal node‐organic ligand adjustments for MOFs. These functionalization strategies are subsequently associated with enhanced adsorption performances (capacity, selectivity, structural/thermal stability, moisture resistance, etc.) toward the analog gas mixtures. Finally, this review also discusses future challenges and prospects for using porous materials in intractable gas separation. Therein, the combination of theoretical calculation with the synthesis condition and adsorption parameters optimization of porous adsorbents may have great potential, given its fast targeting of candidate adsorbents and deeper insights into the adsorption forces in the confined pores and cages.
The rational design of metal‐nitrogen‐doped carbons (M‐N‐C) from available and cost‐effective sources featuring high electrocatalytic performance and stability is attractive for the development of viable low‐temperature fuel cells. Herein, mimosa tannin, an abundant polyphenol easily extracted from the Mimosa plant, is used as a natural carbon source to produce a tannin‐Fe(III) coordination complex. This process is assisted by Pluronic F127, which acts as both a surfactant and a promoter of Fe‐Nx active sites. After carbonization in the presence of urea as a nitrogen precursor, this organic tannin‐Fe(III) framework produces Fe3C nanoparticles encapsulated on a Fe‐N‐C single‐atom catalyst with hierarchical porosity. The optimal catalyst, with a Pluronic F127/mimosa tannin mass ratio of 0.5, exhibits high ORR performance in both alkaline and acidic electrolytes, with half‐wave potentials of 0.87 and 0.74 V versus RHE, respectively. In addition, good performance is achieved in practical hydrogen polymer‐electrolyte membrane fuel cells using OH−‐ or H+‐conducting membranes with peak power densities of 242 and 200 mW cm−2 at cell voltages of 0.43 and 0.3 V, respectively. The synthetic approach can be explored to design new renewable M‐N‐C electrodes for electrochemical energy conversion or storage devices due to tannin's exceptional ability to coordinate metals.
Soft carbon has been recognized as a promising anode material for potassium-ion batteries (PIBs), due to low cost, high conductivity and low voltage platform. However, their practical application is hampered by slow storage kinetics and unsatisfactory cycle life. In this work, pitch-derived needle coke, a typical soft carbon, was incorporated with oxygenated functional groups through liquid phase oxidation by using H2O2 oxidant. When used as anode materials for PIBs, the oxidized needle coke delivers a high reversible capacity of 322.7 mAh g−1, significantly superior to that of the needle coke (237.9 mAh g−1). The enhanced electrochemical performance can be attributed to the abundant oxygenated functional groups and resultant defects on the surface of oxidized needle coke, which not only serve as extra active sites for potassium storage, but also provide sufficient pathways for K+ migration across the adjacent carbon layers. Moreover, the expanded interlayer spacing derived from H2O2 oxidation facilitates rapid K+ intercalation and deintercalation. This work offers an effective modification strategy for the fabrication of high-performance pitch-based soft carbon anodes for PIBs. Graphical Abstract
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