Construction of durable superhydrophilic activated carbon fibers based material for highly-efficient oil/water separation and aqueous contaminants degradation.

Developing filtering materials with high permeation flux and contaminant removal rate is of great importance for oily wastewater remediation. Herein, a robust three-dimensional (3D) activated carbon fibers (ACFs) based composite with uniformly grown layered double hydroxide (LDH) on the surface was successfully constructed through a feasible hydrothermal strategy. The LDH with a high surface energy and vertically aligned structure could provide superhydrophilicity to ACFs. Systematic investigation confirmed that the 3D material could overcome the size mismatch between the ACFs macropores and tiny emulsified droplets through the combination of size-sieving filtration on the surface and oil droplet coalescence in the fiber network. This process efficiently separated the intractable surfactant-stabilized oil-in-water emulsions with high permeation flux (up to 4.16 × 106 L m-2 h-1 bar-1). Notably, the LDH also had well-dispersed catalytic active sites, which could initiate advanced oxidation processes (AOPs) to efficiently eliminate various types of water-soluble organic pollutants (e.g., pharmaceuticals, phenolic compounds and organic dyes). The resulting modified ACFs exhibited exceptional removal rates for both oil and organic pollutants in the complex sewage during the continuous filtration process. These versatile abilities integrated with the facile preparation method reported herein provide outstanding prospects for the large-scale treatment of oily wastewater.

A polymer tethering strategy to achieve high metal loading on catalysts for Fenton reactions.

The development of heterogenous catalysts based on the synthesis of 2D carbon-supported metal nanocatalysts with high metal loading and dispersion is important. However, such practices remain challenging to develop. Here, we report a self-polymerization confinement strategy to fabricate a series of ultrafine metal embedded N-doped carbon nanosheets (M@N-C) with loadings of up to 30 wt%. Systematic investigation confirms that abundant catechol groups for anchoring metal ions and entangled polymer networks with the stable coordinate environment are essential for realizing high-loading M@N-C catalysts. As a demonstration, Fe@N-C exhibits the dual high-efficiency performance in Fenton reaction with both impressive catalytic activity (0.818 min-1) and H2O2 utilization efficiency (84.1%) using sulfamethoxazole as the probe, which has not yet been achieved simultaneously. Theoretical calculations reveal that the abundant Fe nanocrystals increase the electron density of the N-doped carbon frameworks, thereby facilitating the continuous generation of long-lasting surface-bound •OH through lowering the energy barrier for H2O2 activation. This facile and universal strategy paves the way for the fabrication of diverse high-loading heterogeneous catalysts for broad applications.

Well-dispersed iron and nitrogen co-doped hollow carbon microsphere anchoring by g-C3N4 for efficient peroxymonosulfate activation.

Developing single-atom Fenton-like catalysts with the maximum utilization of active sites present an attractive potential in environmental remediation. Herein, the single-atom Fe and N co-doped hollow carbon microsphere loaded g-C3N4 catalyst (HFeNC-g-C3N4) was prepared by an innovative cascade anchoring strategy using polystyrene as the hard template, iron phthalocyanine, polydopamine and urea as the Fe, N and C precursor, in which the in-situ generated g-C3N4 could not only effectively anchor Fe atom to create the well-dispersed Fe-Nx active sites, but also accelerate the electron transfer in peroxymonosulfate (PMS) activation. Taking advantages of such sequential protecting strategy, the as-synthesized HFeNC-g-C3N4 catalyst with single-atom Fe-Nx active sites, verified by XRD, XPS and HAADF-STEM, could work as an efficient Fenton-like catalyst for PMS activation, which achieved almost 100% removal of 4-chlorophenol (4-CP) in 5 min with the turnover frequency calculated to be 34.6 times higher than that of the homogeneous Fe2+ catalyst. The mechanism of O2•- dominated radical combined with nonradical 1O2 pathway was confirmed by quenching experiments and ESR analysis, which might be interrelated to the improvement of pH adaptability and interference immunity of HFeNC-g-C3N4/PMS system. Overall, the present findings provided an innovation strategy for the synthesis of excellent single-atom Fe based catalyst in wastewater purification.