Natural subsurface environment is a complex heterogeneous system. To investigate the effect of ionic strength (IS) and heterogeneity on the transport and remobilization of graphene oxide (GO)-facilitated uranium (U(VI)) in saturated porous media, column experiments were performed by the injection of U(VI) alone and U(VI)+GO mixtures into homogeneous and heterogeneous porous media under low and high ionic strength (1 and 50 mM) conditions, and then the columns were successively flushed with background solution and DI water. Results showed that when U(VI) only was introduced into the columns, IS had little effect on the migration of U(VI) alone in both media and the presence of preferential flow in heterogeneous media slightly enhanced the mobility of U(VI). As U(VI)+GO mixtures were injected into the columns, GO showed strong mobility at low IS and high released peak at high IS. The appearance of GO significantly enhanced U(VI) transport in both media. Under low IS condition, the mobility of U(VI) was significantly enhanced at the injection phase, and the medium heterogeneity further promoted the amount of GO-sorbed U(VI) transport. At high IS, less GO-sorbed U(VI) was observed during injection phase, and a large amount of retained GO-sorbed U(VI) were released with GO remobilization during water flushing phase, and the release showed the longer-tailing phenomenon and the release amount was more pronounced in heterogeneous media. The findings in this study showed that the coupled effect of solution chemistry and media heterogeneity played important roles on GO-facilitated U(VI) transport and release in soil and groundwater system.

Photocatalytic degradation is an attractive strategy to purify waste water contaminated by macromolecular organics. Compared with the single-component photocatalysts, heterostructures of different semiconductors have been widely used to improve the photocatalytic performance. In this work, we fabricate a hetero-structured photocatalyst consisting of two-dimensional graphitic carbon nitride (g-C3N4) nanosheets and commercial MoO3 microparticles through a simple mixing and annealing process. The photocatalytic performance was evaluated in various dye degradation reactions, especially Rhodamine (RhB) degradation. The MoO3/g-C3N4 composite shown a significant improvement compared with individual MoO3 or g-C3N4 as well as their physical mixture. By applying electron spin resonance (ESR) spin-trap spectra, radical scavenge experiments and electrochemical analysis, we find that a direct Z-scheme charge transfer between MoO3 and g-C3N4 not only causes an accumulation of electrons in g-C3N4 and holes in MoO3, but also boosts the formation of superoxide radical and hydroxyl radical. The superoxide radical and hole dominate the photocatalytic degradation, while the hydroxyl radical plays a negligible role and its production can be suppressed by lowering the pH value.

Degrading aquatic organic pollutants efficiently is very important but strongly relied on the design of photocatalysts. Porous graphene could increase photocatalytic performance of ZnO nanoparticles by promoting the effective charge separation of electron-hole pairs if they can be composited. Herein, porous graphene, ZnO nanoparticles and porous graphene/ZnO nanocomposite were prepared by fine tuning of partial combustion, which graphene oxide imperfectly covered by the layered Zn salt was combusted under muffle furnace within few minutes. Resulting ZnO nanoparticles (32–72 nm) are dispersed uniformly on the surface of graphene sheets, the pore sizes of porous graphene are in the range from ∼3 to ∼52 nm. The synthesized porous graphene/ZnO nanocomposite was confirmed to show enhanced efficiency under natural sunlight irradiation compared with pure ZnO nanoparticles. Using porous graphene/ZnO nanocomposite, 100% degradation of methyl orange can be achieved within 150 min. The synergetic effect of photocatalysis and adsorption is main reason for excellent MO degradation of PG/ZnO nanocomposite. This work may offer a new route to accurately prepare porous graphene-based nanocomposite and open a door of their applications.

One of the most important reasons for the controversy over the development of nuclear energy is the proper disposal of spent fuel. Separation of actinide and lanthanide ions is an important part of safe long-term storage of radioactive waste. Herein, a three-dimensional (3D) graphene-based macrostructure (GOCS) was utilized to remove actinide thorium and lanthanide europium ions from aqueous solutions. The adsorption of Eu(III) and Th(IV) on the GOCS was evaluated as a function of adsorption time, solution pH, initial ion concentrations, and ionic strength. The experimentally determined maximum adsorption capacities of this GOCS for Eu(III) (pH 6.0) and Th(IV) (pH 3.0) are as high as 150 and 220 mg/g, respectively. By using Fourier transformation infrared (FT-IR), X-ray photoelectron (XPS), and extended X-ray absorption fine structure (EXAFS) spectroscopy, we concluded that the Eu(III) and Th(IV) adsorption was predominantly attributed to the inner-sphere coordination with various oxygen- and nitrogen-containing functional groups on GOCS surfaces. Our selective adsorption results demonstrate that the actinide and lanthanide ions can be effectively separated from transition metal ions. This study provides new clues to the overall recycling of actinide and lanthanide ions in radioactive environmental pollution treatments.

The decontamination of U(VI) on graphene oxide/nano-alumina (GO/Al₂O₃) composites were investigated by batch, XRD, FT-IR and XPS techniques. The characterization results showed that GO/Al₂O₃ composites presented a variety of oxygen-containing functional groups, which provided the more surface reactive sites. The batch experiments indicated that sorption equilibrium of U(VI) on GO/Al₂O₃ composites was achieved within 30 min, and the maximum sorption capacity derived from Langmuir model was 142.8 mg/g at pH 6.5. In addition, the slight decrease of sorption capacity was observed even after fifth recycling times. These results indicated that GO/Al₂O₃ composites displayed the fast sorption rate, high sorption capacity and good regeneration performance. No effect of ionic strength revealed the inner-sphere surface complexation of U(VI) on GO/Al₂O₃ composites. FT-IR and XPS analysis demonstrated that the high adsorption of U(VI) on GO/Al₂O₃ was attributed to the various oxygen-bearing functional groups. In addition, the nano Al₂O₃ was transferred to amorphous AlO(OH) mineral phase by XRD pattern, which provided the additional reactive sorption sites. These observations indicated that GO-based composites can be regarded as a promising adsorbent for immobilization and pre-concentration of U(VI) from aqueous solutions in the environmental remediation.

The cobalt ferrite-reduced oxidized graphene (CoFe2O4/rGO) catalyst was synthesized by hydrothermal method and characterized by Powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Scanning electron microscope (SEM), Brunauere Emmette Teller (BET) and Hysteresis loop. For developing a new method of removing elemental mercury (Hg0) from flue gas, the effects of catalyst dosage, PMS concentration, solution pH and reaction temperature on the removal efficiency were investigated experimentally by using peroxymonosulfate (PMS) catalyzed by CoFe2O4/rGO at a self-made bubbling reactor. The average removal efficiency of Hg0 in a 30-min period reached 95.56%, when CoFe2O4/rGO dosage was 0.288 g/L, PMS concentration was 3.5 mmol/L, solution pH was 5.5 and reaction temperature was 55 °C. Meanwhile, based on the free radical quenching experiments, in which, ethyl alcohol and tert butyl alcohol were used as quenchers to prove indirectly the presence of •OH and SO4•−, the characterizations of catalysts and reaction products, and the existing results from other scholars. The reaction mechanism was proposed.

As a useful heavy metal ion, chromium has seen its applications in various fields. While it is also a toxic contaminant in water and may cause serious threats to the environment and human health. To develop a novel material with good adsorption capacity and easy solid-liquid separation strategy was necessary and significant. In this paper, the β-cyclodextrin (β-CD) functionalized three-dimensional structured graphene foam (CDGF) was successfully synthesized with the facile and one-step hydrothermal method. The SEM, BET, XRD, FT-IR and XPS analysis were carried out and the results confirmed the successfully grafting of β-CD onto GF. The batch adsorption of Cr(VI) was also taken out and the CDGF possessed good selectivity compared with other metal ions at pH = 3. The adsorption capacity reduced gradually as the initial pH of the Cr(VI) solution grew higher, which was because the anionic species of Cr(VI) were partial to the positively charged surface of CDGF. The easy separation strategy of the CDGF was also demonstrated and the CDGF could be taken out easily with a tweezer after the adsorption of Cr(VI), which significantly simplified the separation procedure and reduced time. By comparing the FT-IR and XPD analysis results, the adsorption mechanism was explored and the hydroxyl groups on CDGF played the main role in the adsorption process. This work brings a novel material for the adsorption of Cr(VI) from water and provides an innovative direction for the easy and fast solid-liquid separation strategy in the adsorption and other application fields.

Graphene oxide (GO), used in a wide variety of applications, is increasingly being introduced into aquatic environments; this situation calls for research on GO aggregation and sedimentation to regulate the environmental behaviors and risks. Many studies have investigated the aggregation and the mechanism of GO in water with a single background salt (monosalt system); however, this may not reflect real water environments where multiple salts coexist (multisalt system). A typical synthetic surface water (soft water) with representative multisalts was therefore used to study the aggregation and sedimentation of GO. The GO concentration-dependent aggregation (low concentration aggregation, high concentration stability) was observed in the soft water, and this concentration-dependent aggregation is opposite to the aggregation in monosalt systems (NaCl or CaCl2 solutions). The presence of GO sheets induced the formation of amorphous CaMg(CO3)2 nanoparticles on the GO surfaces in the soft water, and the formed nanoparticles promoted the aggregation and sedimentation of low concentrations of GO through bridging action. Neutral and alkaline conditions were favorable for the formation of CaMg(CO3)2 nanoparticles and the induced GO aggregation. These findings show a new mechanism of GO aggregation in environmentally relevant waters and help us to better evaluate the environmental fate of GO.

The efficient removal of mercury from aqueous media remains a severe challenge in ensuring environmental safety, especially for low-concentration mercury, which requires adsorbents with high mercury affinity. In this work, we reported a nanocomposite of β-cyclodextrin and three-dimensional graphene (3D CD@RGO) to enhance the adsorption affinity and capacity for mercury with low concentrations. Characterization of the nanocomposite revealed that cyclodextrin was well dispersed on the 3D graphene support structure to provide highly exposed hydroxyl groups. Adsorption experiments showed that CD@RGO exhibited different adsorption behaviors for mercury within different concentration ranges of 0.2–4.0 mg/L and 4.0–10.0 mg/L, and the adsorption affinity for the former range (KL = 10.05 L/mg) was 1.5 times higher than that for the latter range (KL = 6.69 L/mg). Moreover, CD@RGO had a high adsorption efficiency of 96.6% with a superb adsorption affinity (172.09 L/g) at Ce = 0.01 mg/L, which is 6.70 and 41.25 times higher than that of RGO and RCD (physical mixture of RGO and cyclodextrin), respectively, indicating a synergistic effect of CD@RGO for mercury adsorption. This enhancement can be attributed to the transformation of the adsorption mechanism from the outer-sphere force of electrostatic interaction in RGO to the inner-sphere surface complexation in CD@RGO.

Development of low-cost cathode materials for Plant-Sediment Microbial Fuel Cells (P-SMFCs) has gained increasing interest, due to improved performance levels in terms of power and pollutant removal. A novel low cost three-dimensional cathode prepared by simple three-step strategy with growth of Co₃O₄ in-situ biofilm was successfully prepared. Different cathodes were applied to the six parallel P-SMFCs systems (reactor: R1-R6), such as graphite felt (GF), Pt/C, GF@Co₃O₄ (non-bonding Co₃O₄ nanowires on GF), GF@SG-Co₃O₄ (using argon as shielding gas (SG)). Its performances (R1, R2: control groups) were evaluated by electricity generation and Cr(VI) reduction at initial cadmium concentrations (4.97, 10.29 and 21.16 mg L⁻¹). A significant Cr(VI) removal efficiency of 99.76%, maximum power density of 75.12 ± 2.90 mW m⁻² and Cr(VI) adsorption capacity of 1.67 mg g⁻¹ were obtained at initial Cr(VI) concentration of 21.16 mg L⁻¹ with non-bonding GF@Co₃O₄ and bio-GF@SG-Co₃O₄ as cathodes. This indicated that these two materials were better than others (GF, Pt/C and GF@Co₃O₄) as cathodes. Characterization analysis including scanning electron microscope (SEM), cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), Polarization curve, X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) showed that high current generation Cr(VI) removal mainly attributed to transportation of plants, adsorption of bio-cathode, formation of a relatively high concentration region and abundant oxygen vacancies of GF@SG-Co₃O₄. The results show that P-SMFCs with GF@SG-Co₃O₄ cathode may be a potentially novel approach for remediating Cr(VI) contaminated waster or soil.