Jiang-Shan Li

Fate of arsenic before and after chemical-enhanced washing of an arsenic-containing soil in Hong Kong

This study evaluated the feasibility of 2-h chemical-enhanced washing of As-containing soil resulting from geogenic sources in Hong Kong and the fate of As before and after remediation. The soil morphology and As speciation in soil was elucidated by scanning electron microscopy with energy dispersive X-ray spectroscopy, X-ray diffractometer, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy. Integrated analysis of the results suggests that the As (>90%) resides predominantly as arsenate bound to ferric iron oxides, with a minor contribution (<10%) from an AsIII-sulphide phase. This accounts for the marginal leachability, mobility, and bioaccessibility of geogenic As in the untreated soil despite its high concentration. Among the five types of reagents (organic ligands, reductants, alkaline solvents, inorganic acids, and chelants), only dithionite-citrate-bicarbonate method and alkaline solvents (NaOH and Na2CO3) extracted 37-78% and 26-42% of the As by mineral dissolution. However, these extraction methods notably increased the leachability, mobility, and bioaccessibility of remaining As after soil washing, suggesting that a significant proportion of newly released As is prone to re-adsorption onto the soil surface and becomes highly mobile and bioaccessible. While inorganic acids and chelating agents had marginal effects on the fate of remaining As, organic ligands (citrate, oxalate, or pyrophosphate) probably destabilized the bonding of geogenic As and increased its mobility/bioaccessibility despite marginal extraction. The applicability of chemical extraction of geogenic As is questionable regardless of chemical agents, thus proper management of the As-containing soil by containment or physical encapsulation may be considered before land development.

Arsenic-containing soil from geogenic source in Hong Kong: Leaching characteristics and stabilization/solidification

Geogenic sources of arsenic (As) have aroused extensive environmental concerns in many countries. This study evaluated the vertical profiles, leaching characteristics, and surface characteristics of As-containing soils in Hong Kong. The results indicated that elevated levels of As (486-1985xa0mgxa0kg-1) were mostly encountered in deeper layer (15-20xa0m below ground). Despite high concentrations, geogenic As displayed a high degree of chemical stability in the natural geochemical conditions, and there was minimal leaching of As in various leaching tests representing leachability, mobility, phytoavailability, and bioaccessibility. Microscopic/spectroscopic investigations suggested that As in the soils was predominantly present as As(V) in a coordination environment with Fe oxides. Sequential extraction indicated that the majority of As were strongly bound with crystalline Fe/Al oxides and residual phase. Yet, uncertainties may remain with potential As exposure through accidental ingestion and abiotic/biotic transformation due to changes in geochemical conditions. Hence, the effectiveness of stabilization/solidification (S/S) treatment was evaluated. Although the leached concentrations of As from the S/S treated soils increased to varying extent in different batch leaching tests due to the increase in alkalinity, the mobility of As was considered very low based on semi-dynamic leaching test. This suggested that As immobilization in the S/S treated soils was predominantly dependent on physical encapsulation by interlocking framework of hydration products, which could also prevent potential exposure and allow controlled utilization of S/S treated soils as monolithic materials. These results illustrate the importance of holistic assessment and treatment/management of As-containing soils for enabling flexible future land use.

Innovative solidification/stabilization of lead contaminated soil using incineration sewage sludge ash.

The proper treatment of lead (Pb) contaminated soils and incinerated sewage sludge ash (ISSA) has become an environmental concern. In this study, ordinary Portland cement (OPC) and blended OPC containing incinerated sewage sludge ash (ISSA) were used to solidify/stabilize (S/S) soils contaminated with different concentrations of Pb. After curing for 7 and 28xa0d, the S/S soils were subjected to a series of strength, leaching and microscopic tests. The results showed that replacement of OPC by ISSA significantly reduced the unconfined compressive strength (UCS) of S/S soils and leached Pb. In addition, the leaching of Pb from the monolithic samples was diffusion controlled, and increasing the ISSA addition in the samples led to a lower diffusion coefficient and thus an increase in the feasibility for controlled utilization of S/S soils. Furthermore, the proposed S/S method significantly decreased the amount of Pb associated with carbonates and increased the amount of organic and residual Pb in S/S soils, reflecting that the risk of Pb contaminated soils can be effectively mitigated by the incorporating of ISSA. Overall, the leachability of Pb was controlled by the combined effect of adsorption, encapsulation or precipitation in the S/S soils.

Speciation, mobilization, and bioaccessibility of arsenic in geogenic soil profile from Hong Kong

The behaviour of arsenic (As) from geogenic soil exposed to aerobic conditions is critical to predict the impact of As on the environment, which processes remain unresolved. The current study examined the depth profile of As in geologically derived subsoil cores from Hong Kong and investigated the mobilization, plant availability, and bioaccessibility of As in As-contaminated soil at different depths (0-45.8xa0m). Results indicated significant heterogeneity, with high levels of As in three layers of soil reaching up to 505xa0mg/kg at a depth of 5xa0m, 404xa0mg/kg at a depth of 15xa0m, and 1510xa0mg/kg at a depth of 27-32xa0m. Arsenic in porewater samples was <11.5xa0μg/L in the study site. X-ray absorption spectroscopy (XAS) indicated that main As species in soil was arsenate (As(V)), as adsorbed fraction to Fe oxides (41-69% on goethite and 0-8% on ferrihydrite) or the mineral form scorodite (30-57%). Sequential extraction procedure demonstrated that 0.5xa0±xa00.4% of As was exchangeable. Aerobic incubation experiments exhibited that a very small amount (0.14-0.48xa0mg/kg) of As was desorbed from the soil because of the stable As(V) complex structure on abundant Fe oxides (mainly goethite), where indigenous microbes partly (59xa0±xa018%) contributed to the release of As comparing with the sterilized control. Furthermore, no As toxicity in the soil was observed with the growth of ryegrass. The bioaccessibility of As was <27% in the surface soil using simplified bioaccessibility extraction test. Our systematic evaluation indicated that As in the geogenic soil profile from Hong Kong is relatively stable exposing to aerobic environment. Nevertheless, children and workers should avoid incidental contact with excavated soil, because high concentration of As was present in the digestive solution (<0.1-268xa0μg/L).

Characteristics and metal leachability of incinerated sewage sludge ash and air pollution control residues from Hong Kong evaluated by different methods

The improper disposal of incinerated sewage sludge ash (ISSA) and air pollution control residues (APCR) from sewage sludge incinerators has become an environmental concern. The physicochemical, morphological and mineralogical characteristics of ISSA and APCR from Hong Kong, and the leachability and risk of heavy metals, are presented in this paper. The results showed that a low hydraulic and pozzolanic potential was associated with the ISSA and APCR due to the presence of low contents of SiO2, Al2O3 and CaO and high contents of P, S and Cl (especially for APCR). Although high concentrations of Zn and Cu (especially for ISSA) followed by Ni, Pb and As, Se were detected, a low leaching rate of these metals (especially at neutral and alkaline pH) rendered them classifiable as non-hazardous according to the U.S. EPA and Chinese national regulatory limits. The leached metals concentrations from ISSA and APCR were mainly pH dependent, and metals solubilization occurred mainly at low pH. Different leaching tests should be adopted based on the simulated different environmental conditions and exposure scenarios for assessing the leachability as contrasting results could be obtained due to the differences in complexing abilities and final pH of the leaching solutions.

Fate of metals before and after chemical extraction of incinerated sewage sludge ash

Chemical extraction of incinerated sewage sludge ash (ISSA) can effectively recycle P, but it may change the speciation and mobility of the remaining metals. This study investigated the changes of the leaching potential and distribution of metals in the chemically extracted ISSA. Batch extraction experiments with different extractants, including inorganic acids, organic acids, and chelating agents, were conducted on the ISSA collected from a local sewage sludge incinerator. The extraction of Zn, Cu, Pb, Ni, Cd, Ba, Cr and As from the ISSA and the corresponding changes of the mobility and speciation were examined. The results showed that the metals in ISSA were naturally stable because large portions of metals were associated with the residual fraction. The inorganic (HNO3 and H2SO4) and organic acids (citric acid and oxalic acid) significantly co-dissolved the metals through acid dissolution, but the reduction in the total concentrations did not tally the leaching potential of the residual metals. The increase in the exchangeable fraction due to destabilization by the extractants significantly enhanced the mobility and leachability of the metals in the residual ISSA. Chelating agents (EDTA and EDTMP) only extracted a small quantity of metals and had a marginal effect on the fate of the residual metals, but they significantly reduced the Fe/Mn oxide-bound fraction. In comparison, the bioaccessibility of residual metals were reduced to varying extent. Therefore, the disposal or reuse of chemically extracted ISSA should be carefully evaluated in view of possible increase in mobility of residual metals in the environment.

Dynamic leaching behavior of geogenic As in soils after cement-based stabilization/solidification

Cement-based stabilization/solidification (S/S) is a practical treatment approach for hazardous waste with anthropogenic As sources; however, its applicability for geogenic As-containing soil and the long-term leaching potential remain uncertain. In this study, semi-dynamic leaching test was performed to investigate the influence of S/S binders (cement blended with fuel ash (FA), furnace bottom ash (FBA), or ground granulated blast furnace slag (GGBS)) on the long-term leaching characteristics of geogenic As. The results showed that mineral admixtures with higher Ca content and pozzolanic activity were more effective in reducing the leached As concentrations. Thus, cement blended with FBA was inferior to other binders in suppressing the As leaching, while 20% replacement of ordinary Portland cement by GGBS was considered most feasible for the S/S treatment of As-containing soils. The leachability of geogenic As was suppressed by the encapsulation effect of solidified matrix and interlocking network of hydration products that were supported by scanning electron microscopy (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) results. The long-term leaching of geogenic As from the monolithic samples was diffusion-controlled. Increasing the Ca content in the samples led to a decrease in diffusion coefficient and an increase in feasibility for “controlled utilization” of the S/S-treated soils.

Green remediation of contaminated sediment by stabilization/solidification with industrial by-products and CO 2 utilization

Navigational dredging is an excavation of marine/freshwater sediment to maintain channels of sufficient depth for shipping safety. Due to historical inputs of anthropogenic contaminants, sediments are often contaminated by metals/metalloids, polycyclic aromatic hydrocarbons, polychlorinated biphenyls, and other contaminants. Its disposal can present significant environmental and financial burdens. This study developed a novel and green remediation method for contaminated sediment using stabilization/solidification with calcium-rich/low-calcium industrial by-products and CO2 utilization. The hydration products were evaluated by quantitative X-ray diffraction analysis and thermogravimetric analysis. The incorporation of calcium carbide residue (CCR) facilitated hydration reaction and provided relatively high 7-d strength. In contrast, the addition of Class-F pulverized fly ash (PFA) and ground granulated blast furnace slag (GGBS) was beneficial to the 28-d strength development due to supplementary pozzolanic and hydration reactions. The employment of 1-d CO2 curing was found to promote strength development (98%) and carbon sequestration (4.3wt%), while additional 7-d air curing facilitated cement rehydration and further carbonation in the sediment blocks. The leachability tests indicated that all studied binders, especially CCR binder, effectively immobilized contaminants in the sediments. The calcium-rich CCR and GGBS were regarded as promising candidates for augmenting the efficacy of CO2 curing, whereas GGBS samples could be applicable as eco-paving blocks in view of their superior 28-d strength. This study presents a new and sustainable way to transform contaminated sediment into value-added materials.

Phosphorus recovery and leaching of trace elements from incinerated sewage sludge ash (ISSA)

Chemical extraction of phosphorus (P) from incinerated sewage sludge ash (ISSA) is adversely influenced by co-dissolution of metals and metalloids. This study investigated P recovery and leaching of Zn, Cu, Pb, As and Ni from ISSA using inorganic acids (sulphuric acid and nitric acid), organic acids (oxalic acid and citric acid), and chelating agents (ethylenediaminetetraacetic acid (EDTA) and ethylene diamine tetramethylene phosphonate (EDTMP)). The aim of this study was to optimize a leaching process to recover P-leachate with high purity for P fertilizer production. The results show that both organic and inorganic acids extract P-containing phases but organic acids leach more trace elements, particularly Cu, Zn, Pb and As. Sulphuric acid was the most efficient for P recovery and achieved 94% of total extraction under the optimal conditions, which were 2-h reaction with 0.2xa0mol/L H2SO4 at a liquid-to-solid ratio of 20:1. EDTA extracted only 20% of the available P, but the leachates were contaminated with high levels of trace elements under optimum conditions (3-h reaction with EDTA at 0.02xa0mol/L, pH 2, and liquid-to-solid ratio of 20:1). Therefore, EDTA was considered an appropriate pre-treatment agent for reducing the total metal/metalloid content in ISSA, which produced negligible changes in the structure of ISSA and reduced contamination during subsequent P extraction using sulphuric acid.

Change in re-use value of incinerated sewage sludge ash due to chemical extraction of phosphorus

The potential of six different extractants to recover phosphorus (P) from incinerated sewage sludge ash (ISSA) was evaluated. Secondary effects such as the co-dissolution of Zn and Cu were also considered. The residual ISSA from each study was assessed in particular detail, focusing on the leachability of remaining Zn and Cu, major element composition, crystalline phases and overall degree of crystallinity and particle size distribution. The residual ISSA was also evaluated as a pozzolanic material using a Strength Activity Index (SAI) test with mortars containing Portland cement with a 20% substitution by ISSA. All results were compared to tests with untreated ISSA. Overall, the use of 3 of the 6 extractants could be ruled out due to poor P recovery potential and/or a serious compromise of the potential reuse of residual ISSA in Portland cement-based materials. The results highlight the added value of considering the potential reuse of residual ISSA when trying to optimize P recovery from ISSA by wet methods.