Single Atom Catalyst in Persulfate Oxidation Reaction: From Atom Species to Substance.

With maximum utilization of active metal sites, more and more researchers have reported using single atom catalysts (SACs) to activate persulfate (PS) for organic pollutants removal. In SACs, single metal atoms (Fe, Co, Cu, Mn, etc.) and different substrates (porous carbon, biochar, graphene oxide, carbon nitride, MOF, MoS2 , and others) are the basic structural. Metal single atoms, substances, and connected chemical bonds all have a great influence on the electronic structures that directly affect the activation process of PS and degradation efficiency to organic pollutants. However, there are few relevant reviews about the interaction between metal single atoms and substances during PS activation process. In this review, the SACs with different metal species and substrates are summarized to investigate the metal-support interaction and evaluate their effects on PS oxidation reaction process. Furthermore, how metal atoms and substrates affect the reactive species and degradation pathways are also discussed. Finally, the challenges and prospects of SACs in PS-AOPs are proposed.

Coupling of kenaf Biochar and Magnetic BiFeO3 onto Cross-linked Chitosan for Enhancing Separation Performance and Cr(VI) Ions Removal Efficiency.

Cr(VI) contamination has posed great threat to both the ecosystem and human health for its carcinogenic and mutagenic nature. A highly effective adsorbent for the removal of Cr(VI) was prepared and its adsorption mechanism was thoroughly discussed in this study. In detail, magnetic BiFeO3 and kenaf biochar were loaded on cross-linked chitosan to obtain chitosan-kenaf biochar@BiFeO3 (CKB) for improving adsorption capacity towards Cr(VI). The adsorption process of Cr(VI) onto CKB was evaluated as a function of the pH, the existence of competing ions, the initial concentration of Cr(VI) and contact time. The results show that CKB exhibits the highest adsorption capacity under the optimal pH 2.0. The presence of competing ions such as Ca2+, NO3-, SO42-, and Cl- decreases the adsorption capacity; among them, Ca2+ and NO3- show the greatest hindrance. By studying the effect of initial Cr(VI) concentration on the adsorption capacity, it was found that CKB in the solution was enough to remove Cr(VI) for all treatments (10-200 mg/L). The adsorption experimental data were well fitted with pseudo-first-order model, suggesting that chemisorption is not the dominant rate-limiting step. Freundlich isotherm model can better explain the adsorption process, indicating a non-ideal adsorption towards Cr(VI) on a heterogeneous surface of CKB. A 25-1 Fractional Factorial Design (FFD) showed that pH and initial concentration of Cr(VI) have significant influence on Cr(VI) adsorption in our reaction system. In general, excellent adsorption efficiency of CKB indicates that it may be a good candidate for the remediation of Cr(VI)-contaminating wastewater.

Three-dimensional microspheric g-C3N4 coupled by Broussonetia papyrifera biochar: facile sodium alginate immobilization and excellent photocatalytic Cr(iv) reduction.

Photocatalysts comprising Broussonetia papyrifera biochar and g-C3N4 loaded on sodium alginate were prepared and characterized in terms of reusability and photocatalytic Cr(vi) reduction performance. The observed photocurrent responses as well as photoluminescence and UV-visible diffuse reflectance spectra showed that the best-performing catalyst featured the benefits of efficient photogenerated charge separation, superior electron conductance/transfer, and excellent light adsorption ability, which resulted in a higher photocatalytic Cr(vi) reduction performance compared to that of pure g-C3N4 powder. The prepared composite was shown to be reusable and well separable from the reaction mixture, thus being a promising material for the practical photocatalytic removal of Cr(vi) from wastewater. The trapping experiment and XPS spectra of catalysts after reactions confirm that the decontamination of Cr(vi) lies in the photocatalytic reduction of this species into low-toxicity Cr(iii) by photoinduced electrons generated from g-C3N4, followed by the adsorption of Cr(iii) on biochar or alginate with large specific areas.

Synergy of Photocatalysis and Adsorption for Simultaneous Removal of Hexavalent Chromium and Methylene Blue by g-C3N4/BiFeO3/Carbon Nanotubes Ternary Composites.

A novel graphite-phase carbon nitride (g-C3N4)/bismuth ferrite (BiFeO3)/carbon nanotubes (CNTs) ternary magnetic composite (CNBT) was prepared by a hydrothermal synthesis. Using this material, Cr(VI) and methylene blue (MB) were removed from wastewater through synergistic adsorption and photocatalysis. The effects of pH, time, and pollutant concentration on the photocatalytic performance of CNBT, as well as possible interactions between Cr(VI) and MB species were analyzed. The obtained results showed that CNTs could effectively reduce the recombination rate of electron-hole pairs during the photocatalytic reaction of the g-C3N4/BiFeO3 composite, thereby improving its photocatalytic performance, while the presence of MB increased the reduction rate of Cr(VI). After 5 h of the simultaneous adsorption and photocatalysis by CNBT, the removal rates of Cr(VI) and MB were 93% and 98%, respectively. This study provides a new theoretical basis and technical guidance for the combined application of photocatalysis and adsorption in the treatment of wastewaters containing mixed pollutants.

Ternary assembly of g-C3N4/graphene oxide sheets /BiFeO3 heterojunction with enhanced photoreduction of Cr(VI) under visible-light irradiation.

A novel ternary composite of graphitic carbon nitride (g-C3N4)/graphene oxide (GO) sheets/BiFeO3 (CNGB) with highly enhanced visible-light photocatalytic activity toward Cr(VI) photoreduction is prepared and characterized. The characterization and photocatalysis experiments corroborate its reasonable band gap, efficient charge separation and transfer, widened visible-light adsorption, easy solid-liquid separation, good stability and superior catalytic activity of CNGB. Three CNGB samples with different ratios of g-C3N4 and BiFeO3 (CNGB-1, -2, -3 with 2:4, 3:3, and 4:2, respectively), though possessing different adsorption ability, eventually remove all Cr(VI) ions via photocatalysis within 90 min. The catalytic efficiency of the composite is the highest at pH 2; increases in pH decrease the catalytic ability. The inorganic anions such as SO4-, Cl-, and NO3- only slightly affects the photocatalytic process. The matching of the band structure between BiFeO3 and g-C3N4 generates efficient photogenerated electron migration from the conduction band of g-C3N4 to that of BiFeO3, which is also facilitated by the electron bridging and collecting effects of GO, and holes transfer from the valence band of BiFeO3 to that of g-C3N4, yielding the efficient separation of photogenerated electron-hole pairs and the subsequent enhancement of photocatalytic activity. The research provides a theoretical basis and technical support for the development of photocatalytic technologies for effective application in wastewater treatment and Cr-contaminated water restoration.