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Creators/Authors contains: "Lee, Cheng-Shiuan"

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  1. A novel composite hydrogel bead composed of sodium alginate (SA) and aldehyde cellulose nanocrystal (DCNC) was developed for antibiotic remediation through a one-step cross-linking process in a calcium chloride bath. Structural and physical properties of the hydrogel bead, with varying composition ratios, were analyzed using techniques such as BET analysis, SEM imaging, tensile testing, and rheology measurement. The optimal composition ratio was found to be 40% (SA) and 60% (DCNC) by weight. The performance of the SA–DCNC hydrogel bead for antibiotic remediation was evaluated using doxycycline (DOXY) and three other tetracyclines in both single- and multidrug systems, yielding a maximum adsorption capacity of 421.5 mg g−1 at pH 7 and 649.9 mg g−1 at pH 11 for DOXY. The adsorption mechanisms were investigated through adsorption studies focusing on the effects of contact time, pH, concentration, and competitive contaminants, along with X-ray photoelectron spectroscopy analysis of samples. The adsorption of DOXY was confirmed to be the synergetic effects of chemical reaction, electrostatic interaction, hydrogen bonding, and pore diffusion/surface deposition. The SA–DCNC composite hydrogel demonstrated high reusability, with more than 80% of its adsorption efficiency remaining after five cycles of the adsorption–desorption test. The SA–DCNC composite hydrogel bead could be a promising biomaterial for future antibiotic remediation applications in both pilot and industrial scales because of its high adsorption efficiency and ease of recycling. 
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  2. Although most manufacturers stopped using long-chain per- and polyfluoroalkyl substances (PFASs), including perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS), short-chain PFASs are still widely employed. Short-chain PFASs are less known in terms of toxicity and have different adsorption behavior from long-chain PFASs. Previous studies have shown electrostatic interaction with the adsorbent to be the dominant mechanism for the removal of short-chain PFASs. In this study, we designed a high charge density cationic quaternized nanocellulose (QNC) to enhance the removal of both short- and long-chain PFASs from contaminated water. Systematic batch adsorption tests were conducted using the QNC adsorbent to compare its efficiency against PFASs with varying chain lengths and functional groups. From the kinetic study, PFBA (perfluorobutanoic acid), PFBS (perfluorobutanesulfonic acid) and PFOS showed rapid adsorption rates, which reached near equilibrium values (>95% of removal) between 1 min to 15 min, while PFOA required a relatively longer equilibration time of 2 h (it obtained 90% of removal within 15 min). According to the isotherm results, the maximum adsorption capacity ( Q m ) of the QNC adsorbent exhibited the following trend: PFOS ( Q m = 559 mg g −1 or 1.12 mmol g −1 ) > PFOA ( Q m = 405 mg g −1 or 0.98 mmol g −1 ) > PFBS ( Q m = 319 mg g −1 or 1.06 mmol g −1 ) > PFBA ( Q m = 121 mg g −1 or 0.57 mmol g −1 ). This adsorption order generally matches the hydrophobicity trend among four PFASs associated with both PFAS chain length and functional group. In competitive studies, pre-adsorbed short-chain PFASs were quickly desorbed by long-chain PFASs, suggesting that the hydrophobicity of the molecule played an important role in the adsorption process on to QNC. Finally, the developed QNC adsorbent was tested to treat PFAS-contaminated groundwater, which showed excellent removal efficiency (>95%) for long-chain PFASs (C7–C9) even at a low adsorbent dose of 32 mg L −1 . However, short-chain PFASs ( i.e. , PFBA and perfluoropentanoic acid (PFPeA)) were poorly removed by the QNC adsorbent (0% and 10% removal, respectively) due to competing constituents in the groundwater matrix. This was further confirmed by controlled experiments that revealed a drop in the performance of QNC to remove short-chain PFASs at elevated ionic strength (NaCl), but not for long-chain PFASs, likely due to charge neutralization of the anionic functional group of PFASs by inorganic cations. Overall, the QNC adsorbent featured improved PFAS adsorption capacity at almost two-fold of PFAS removal by granular activated carbons, especially for short-chain PFASs. We believe, QNC can complement the use of common treatment methods such as activated carbon or ionic exchange resin to remove a wide range of PFAS pollutants, heading towards the complete remediation of PFAS contamination. 
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  3. Abstract Elemental mercury (Hg0) formation from other mercury species in seawater results from photoreduction and microbial activity, leading to possible evasion from seawater to overlying air. Microbial conversion of monomethylmercury (MeHg) to Hg0in seawater remains unquantified. A rapid radioassay method was developed using gamma‐emitting203Hg as a tracer to evaluate Hg0production from Hg(II) and MeHg in the low pM range. Bacterioplankton assemblages in Atlantic surface seawater and Long Island Sound water were found to rapidly produce Hg0, with production rate constants being directly related to bacterial biomass and independent of dissolved Hg(II) and MeHg concentrations. About 32% of Hg(II) and 19% of MeHg were converted to Hg0in 4 d in Atlantic surface seawater containing low‐bacterial biomass, and in Long Island Sound water with higher bacterial biomass, 54% of Hg(II) and 8% of MeHg were transformed to Hg0. Decreasing temperatures from 24°C to 4°C reduced Hg0production rates cell−1from Hg(II) 3.3 times as much as from a MeHg source. Because Hg0production rates were linearly related to microbial biomass and temperature, and microbial mercuric reductase was detected in our field samples, we inferred that microbial metabolic activities and enzymatic reactions primarily govern Hg0formation in subsurface waters where light penetration is diminished. 
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  4. Abstract Methylmercury (MeHg) is known to biomagnify in marine food chains, resulting in higher concentrations in upper trophic level animals than their prey. To better understand how marine copepods, an important intermediate between phytoplankton and forage fish at the bottom of the food chain, assimilate and release MeHg, the authors performed a series of laboratory experiments using the gamma‐emitting radiotracer203Hg2+and Me203Hg with the calanoid copepodAcartia tonsa. Assimilation efficiencies of Hg2+and MeHg ranged from 25% to 31% and 58% to 79%, respectively, depending on algal diets. Assimilation efficiencies were positively related to the fraction of Hg in the cytoplasm of the algal cells that comprised their diet. Efflux rates of Hg2+(0.29/d) and MeHg (0.21/d) following aqueous uptake were similar, but efflux rates following dietary uptake were significantly lower for MeHg (0.11–0.22/d) than Hg2+(0.47–0.66/d). The calculated trophic transfer factors in copepods were >1 for MeHg and consistently low (≤0.2) for Hg2+. The authors used the parameters measured to quantitatively model the relative importance of MeHg sources (water or diet) for copepods and to predict the overall MeHg concentrations in copepods in different marine environments. In general, MeHg uptake from the diet accounted for most of the body burden in copepods (>50%). For an algal diet with a MeHg dry weight bioconcentration factor ≥106, >90% of a copepod's MeHg body burden can be shown to derive from the diet. The model‐predicted MeHg concentrations in the copepods were comparable to independent measurements for copepods in coastal and open‐ocean regions, implying that the measured parameters and model are applicable to natural waters.Environ Toxicol Chem2017;36:1287–1293. © 2016 SETAC 
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