科研成果

Microbial desalination cells (MDCs) extract organic energy from wastewater for in situ desalination of saline water. However, to desalinate salt water, traditional MDCs often require an anolyte (wastewater) and a catholyte (other synthetic water) to produce electricity. Correspondingly, the traditional MDCs also produced anode effluent and cathode effluent, and may produce a concentrate solution, resulting in a low production of diluate. In this study, nitrogen-doped carbon nanotube membranes and Pt carbon cloths were utilized as filtration material and cathode to fabricate a modularized filtration air cathode MDC (F-MDC). With real wastewater flowing from anode to cathode, and finally to the middle membrane stack, the diluate volume production reached 82.4%, with the removal efficiency of salinity and chemical oxygen demand (COD) reached 93.6% and 97.3% respectively. The final diluate conductivity was 68 +/- 12 mu S/cm, and the turbidity was 0.41 NTU, which were sufficient for boiler supplementary or industrial cooling. The concentrate production was only 17.6%, and almost all the phosphorus and salt, and most of the nitrogen were recovered, potentially allowing the recovery of nutrients and other chemicals. These results show the potential utility of the modularized F-MDC in the application of municipal wastewater advanced treatment and self-driven desalination.

Nitryl chloride (ClNO2) is a dominant source of chlorine radical in polluted environment, and can significantly affect the atmospheric oxidative chemistry. However, the abundance of ClNO2 and its exact role are not fully understood under different environmental conditions. During the summer of 2014, we deployed a chemical ionization mass spectrometer to measure ClNO2 and dinitrogen pentoxide (N2O5) at a rural site in the polluted North China Plain. Elevated mixing ratios of ClNO2 (> 350 pptv) were observed at most of the nights with low levels of N2O5 (< 200 pptv). The highest ClNO2 mixing ratio of 2070 pptv (1 min average) was observed in a plume from a megacity (Tianjin), and was characterized with a faster N2O5 heterogeneous loss rate and ClNO2 production rate compared to average conditions. The abundant ClNO2 concentration kept increasing even after sunrise, and reached a peak 4 h later. Such highly sustained ClNO2 peaks after sunrise are discrepant from the previously observed typical diurnal pattern. Meteorological and chemical analysis shows that the sustained ClNO2 morning peaks are caused by significant ClNO2 production in the residual layer at night followed by downward mixing after breakup of the nocturnal inversion layer in the morning. We estimated that similar to 1.7-4.0 ppbv of ClNO2 would exist in the residual layer in order to maintain the observed morning ClNO2 peaks at the surface site. Observation-based box model analysis show that photolysis of ClNO2 produced chlorine radical with a rate up to 1.12 ppbv h(-1), accounting for 10-30% of primary ROx production in the morning hours. The perturbation in total radical production leads to an increase of integrated daytime net ozone production by 3% (4.3 ppbv) on average, and with a larger increase of 13% (11 ppbv) in megacity outflow that was characterized with higher ClNO2 and a relatively lower oxygenated hydrocarbon (OVOC) to non-methane hydrocarbon (NMHC) ratio.

Although efficient aerobic denitrification has received increasing attention, few studies have been made on simultaneous denitrification and phosphorus removal (SDPR) under aerobic condition. In this study, SDPR by an efficient aerobic denitrifier, Agrobacterium sp. LAD9, was firstly demonstrated. High nitrate and phosphorus removal rates of 7.50 and 1.02 mg L-1 h(-1) were achieved in wide range of O-2 concentration from 5.92 to 20.02 mg L-1. The N2O production would be inhibited as O-2 concentration exceeded 11.06 mg L-1, while the phosphorus removal efficiency would be generally improved with increasing O-2 concentration. N-15 mass spectrometry revealed that nitrogen removal accorded with the typical aerobic denitrification pathway, while P-31 nuclear magnetic resonance spectroscopy (P-31 NMR) indicated the fate of phosphorus to cells, extracellular polymeric substances (EPS), and polyphosphate (poly-P) of the denitrifier. EPS acted as a reservoir of phosphorus and the transformation of poly-P was dynamic and depended on initial orthophosphate (ortho-P) content. The aerobic SDPR would greatly simplify the conventional wastewater treatment processes which required separated considerations of nitrogen and phosphorus removal.

In the present investigation, we reported the fabrication of host networks formed by two newly prepared phenanthrene-butadiynylene macrocycles (PBMs) at the liquid-solid interface. Size, shape and concentration controlled experiments have been performed to investigate the PBMs/coronene (COR) host-guest system with the structural polymorphism phenomenon. Initially, PBM1 could form a regular linear network structure and PBM2 form a well-ordered nanoporous network structure. When the COR molecules were introduced, the self-assembled structure of PBM1 remained unchanged, while COR could be entrapped into the cavities of the PBM2 nanoporous network, and the co-assembly of the PBM2/COR host-guest systems underwent a structural transformation with the increase of concentration of COR. Scanning tunneling microscopy (STM) measurements and density functional theory (DFT) calculations are utilized to reveal the formation mechanism of the molecular nanoarrays controlled by the solution concentration.

Atmospheric size-fractionated particles were collected at different heights in an e-waste recycling zone (QY) and urban Guangzhou (GZ), China and analyzed for organophosphate flame retardants (OPFRs). The total air concentrations of eight OPFRs were 130 +/- 130 and 138 +/- 127 ng m(-3) in QY and GZ, respectively. Compositional profiles of chlorinated OPFRs were different between QY and GZ, but the size distribution patterns of all OPFRs were not significantly different at different heights. Estimated atmospheric deposition fluxes of OPFRs were 51 +/- 67 and 55 +/- 13 mu gm(-2) d(-1) in QY and GZ, respectively, and the coarse particles (D-p > 1.8 mu m) dominated both the dry and wet deposition fluxes. Moreover, not all particle-bound OPFRs were inhalable and deposited in the human respiratory tract. The calculated inhalation doses of OPFRs were much lower than the reference doses, suggesting that potential health risk due to inhalation exposure to particle-bound OPFRs in the e-waste recycling zone and urban site was low. (C) 2015 Elsevier B.V. All rights reserved.