Huaping Dong

Colloidal diatomite, radionickel, and humic substance interaction: a combined batch, XPS, and EXAFS investigation

This work determined the influence of humic acid (HA) and fulvic acid (FA) on the interaction mechanism and microstructure of Ni(II) onto diatomite by using batch experiments, X-ray photoelectron spectroscopy (XPS), and extended X-ray absorption fine structure (EXAFS) methods. Macroscopic and spectroscopic experiments have been combined to see the evolution of the interaction mechanism and microstructure of Ni(II) in the presence of HA/FA as compared with that in the absence of HA/FA. The results indicated that the interaction of Ni(II) with diatomite presents the expected solution pH edge at 7.0, which is modified by addition of HA/FA. In the presence of HA/FA, the interaction of Ni(II) with diatomite increased below solution pH 7.0, while Ni(II) interaction decreased above solution pH 7.0. XPS analysis suggested that the enrichment of Ni(II) onto diatomite may be due to the formation of (≡SO)2Ni. EXAFS results showed that binary surface complexes and ternary surface complexes of Ni(II) can be simultaneously formed in the presence of HA/FA, whereas only binary surface complexes of Ni(II) are formed in the absence of HA/FA, which contribute to the enhanced Ni(II) uptake at low pH values. The results observed in this work are important for the evaluation of Ni(II) and related radionuclide physicochemical behavior in the natural soil and water environment.

Enhanced Removal of Uranium(VI) by Nanoscale Zerovalent Iron Supported on Na-Bentonite and an Investigation of Mechanism

The reductive removal of U(VI) by nanoscale zerovalent iron (NZVI) was enhanced by using Na(+)-saturated bentonite (Na-bent) as the support, and the mechanism for the enhanced removal were investigated comprehensively. Under the same experimental conditions, NZVI supported on the negatively charged Na-bent showed much higher removal efficiency (99.2%) of cationic U(VI) than either bare NZVI (48.3%) or NZVI supported on the positively charged bentonite (Al-bent) did. Subsequent experimental investigations revealed the unique roles of bentonite on enhancing the reactivity and reusability of NZVI. First, Na-bent can buffer the pH in reaction media, besides preventing NZVI from aggregation. Second, Na-bent promoted the mass transfer of U(VI) from solution to NZVI surface, leading to the enhanced removal efficiency. Third, the bentonite may transfer some insoluble reduction products away from the iron surface according to X-ray absorption fine structure (XAFS) study. Finally, Na-bent as the adsorbent to Fe(II) makes it more reactive with U(VI), which enhanced stoichiometrically the reduction capacity of NZVI besides accelerating the reaction rate.

Characterization of diatomite and its application for the retention of radiocobalt: role of environmental parameters.

Clay minerals have been extensively studied because of their strong sorption and complexation ability. In this work, diatomite was characterized by using acid-base titration. Retention of radionuclide (60)Co(II) from aqueous solution by sorption onto diatomite was investigated by using batch technique under various environmental conditions such as pH, ionic strength, humic acid (HA), fulvic acid (FA), and temperature. The results indicated that the sorption of Co(II) onto diatomite was strongly dependent on pH. At low pH value, the sorption of Co(II) was dominated by outer-sphere surface complexation and ion exchange with Na(+)/H(+) on diatomite surfaces, whereas inner-sphere surface complexation was the main sorption mechanism at high pH value. The D-R model fitted the sorption isotherms better than the Langmuir and Freundlich models. The thermodynamic parameters (ΔH(0), ΔS(0) and ΔG(0)) calculated from the temperature-dependent sorption isotherms suggested that the sorption of Co(II) was an endothermic and spontaneous process. In addition, diatomite showed higher sorption capacity than that of lots of the sorbents reported in the literatures we surveyed. From the results of Co(II) removal by diatomite, the optimum reaction conditions can be obtained for the maximum removal of Co(II) from water. It is clear that the best pH values of the system to remove Co(II) from solution by using diatomite are 7-8. Considering the low cost and effective disposal of Co(II)-contaminated wastewaters, the best condition for Co(II) removal is at room temperature and solid content of 0.5 g/L. The results might be important for assessing the potential of practical application of diatomite in Co(II) and related radionuclide pollution management.

Environmental condition effects on radionuclide 64Cu(II) sequestration to a novel composite: polyaniline grafted multiwalled carbon nanotubes

This work examines the sequestration of 64Cu(II) by sorption process onto plasma-induced polyaniline (PANI)-grafted multiwalled carbon nanotubes (denoted as MWCNTs/PANI) prepared by an plasma-induced grafting technique. The role of a variety of environmental conditions such as pH, ionic strength, natural organic matter (NOM) in the sorption of 64Cu(II) onto MWCNTs/PANI is studied. The results indicate that the sorption is strongly dependent on pH but independent of ionic strength. A positive effect of NOM on 64Cu(II) sorption is found at pH <7.5, whereas a negative effect is observed at pH >7.5. The sorption isotherms in the absence and presence of NOM can be better described by Freundlich model than Langmuir model. Sorption isotherms of 64Cu(II) at higher initial NOM concentrations are higher than those at lower NOM concentrations. The thermodynamic data calculated from temperature-dependent sorption suggest that the sorption is spontaneous and enhanced at higher temperature. Results of this work suggest that MWCNTs/PANI may be a promising candidate for cost-effective treatments of 64Cu(II)-contaminated wastewaters.

The roles of a pillared bentonite on enhancing Se(VI) removal by ZVI and the influence of co-existing solutes in groundwater

The zero-valent iron permeable reactive barrier (ZVI-PRB) is a promising technology for in-situ groundwater remediation. However, its long-term performance often declined due to the blocked reactive sites by corrosion products and by interference of co-existing solutes. In order to address these issues, a pillared bentonite (Al-bent) was homogeneously mixed with ZVI for removing selenate (Se(VI)) from simulated groundwater in column experiments. The Se(VI) removal was enhanced because first Al-bent could facilitate the mass transfer of Se(VI) from solution to iron surface and accelerate Se(VI) reduction. XANES analysis indicated that Se(VI) was almost completely reduced to Se(0) and Se(-II) of less toxicity and solubility by the ZVI/Al-bent mixture, and the buffering effect of Al-bent could maintain the pH at a lower level that favored the Se(VI) removal. Besides, Al-bent could transfer the corrosion products away from iron surface, leading to the enhanced reactivity and longevity of ZVI. The inhibition on reactivity towards Se(VI) in both the single ZVI and the ZVI/Al-bent systems increased in the order of Cl(-)<NO3(-)<HCO3(-)<SO4(2-), and the removal efficiency decreased with the increasing HA concentration. However, the lower decrease of Se(VI) removal in the ZVI/Al-bent system indicates its resistance to the interference of these co-existing solutes in groundwater.

Enhanced removal of Ni(II) by nanoscale zero valent iron supported on Na-saturated bentonite

Nanoscale zero valent iron (NZVI) can remove Ni(II) from wastewater through surface adsorption and then reduction into lower-toxic Ni0, but the reduction is often blocked by the iron oxide shell of NZVI. In this study, the negatively charged Na-saturated bentonite (Na-bent) with high adsorption capacity to Ni(II) was used to support NZVI for improving the removal and reduction of Ni(II), and the functions of Na-bent were investigated by X-ray photoelectron micro-spectroscopy (XPS), transmission electron microscope (TEM) and Fe(II) determination. The results showed that Na-bent as a carrier could enrich Ni(II) on the reaction surface, protect the surface of NZVI from oxidation, prevent the aggregation of NZVI particles, and decrease the iron oxides products on NZVI surface by pH buffering. Therefore, NZVI/Na-bent not only showed much higher removal efficiency of Ni(II) (98.5%) than the sum (48.8%) of those by bare NZVI removal (41.9%) and by Na-bent adsorption (6.9%), but also greatly enhanced the reduction efficiency of Ni(II) into Ni0 by facilitating the electron transfer from Fe0 core to the surface-adsorbed Ni(II). In general, the unique property of bentonites will provide effective solutions to support NZVI for enhancing the removal and transformation of various environmental contaminants.

Effect of surfactants on the removal of nitrobenzene by Fe-bearing montmorillonite/Fe(II)

Nonionic and anionic surfactants often occur in anaerobic environments, but their roles in the removal of organic contaminants by Fe-bearing mineral/Fe(II) have not been determined. In this study, batch experiments were performed to investigate the effects of a nonionic surfactant (TX-100) and an anionic surfactant (SDBS) on the removal of nitrobenzene (NB) by Fe-bearing montmorillonite (FM)/Fe(II). Mössbauer spectrum and XPS were applied to analyze the edge surface bound Fe(II) and secondary minerals formed on FM. The contribution of surfactant to the enrichment of NB on FM was studied. The results showed that TX-100 and SDBS had opposite effects on the removal of NB by FM/Fe(II) at neutral pH. The presence of TX-100 improved the removal efficiency of NB from 36.4% to 70.0%, and increased the initial removal rate by 1.7 times. This enhancement effect was mainly attributed to the formation of more active edge surface bound Fe(II) that can reduce more NB to aniline. Formation of more magnetite on FM and selective enrichment of NB on the reactive surface also contributed to the removal of NB. In contrast, the presence of SDBS reduced the amount of edge surface bound Fe(II) via formation of SDBS-Fe(II) complex, which decreased the removal efficiency of NB.