•Methamphetamine and amphetamine sources were traced via concentration and enantiomeric profiling.•Methamphetamine in Chinese wastewater was found to predominantly arise from abuse.•Amphetamine was abused considerably in a significant number of major cities in China.•Combined concentration and enantiomeric profiling revealed direct methamphetamine disposal into receiving waters.Wastewater analysis is a promising approach to monitor illicit drug abuse of a community. However, drug use estimation via wastewater analysis may be biased by sources other than abuse. This is especially true for methamphetamine and amphetamine as their presence in wastewater may come from many sources, such as direct disposal or excretion following administration of prescription drugs. Here we traced methamphetamine and amphetamine sources via concentration and enantiomeric profiling of the two compounds from black market to receiving waters. Methamphetamine in wastewater was found to predominantly arise from abuse, proving the feasibility of using wastewater analysis for estimating its consumption in China. Amphetamine abuse was previously considered negligible in East and Southeast Asia. However, we found that amphetamine was abused considerably (up to 90.7 mg/1000 inh/day) in a significant number (> 20%) of major cities in China. Combined concentration and enantiomeric profiling also revealed direct disposal into receiving waters of methamphetamine manufactured by different processes. These findings have important implications for monitoring of and law enforcement against methamphetamine/amphetamine abuse and related crimes in China and abroad.

•First large scale wastewater-based investigation on heroin abuse in major Chinese cities•Morphine and codeine in wastewater were predominantly from street heroin.•Codeine abuse was evident in cities in Guangdong province.•Heroin consumption was estimated based on morphine loads in wastewater.•Heroin consumption in Northwest and Southwest was much higher than in other regions.Heroin consumption in major cities across China was estimated for the first time via wastewater-based epidemiology. Influent and effluent wastewater samples were collected from 49 wastewater treatment plants (WWTPs) in 24 major cities that cover all the geographic regions of the country. Concentrations of morphine, 6-acetylmorphine, and codeine were measured. Near complete removal of morphine by wastewater treatment processes was observed, whereas removal rates of codeine were slightly lower. Morphine loads were much higher than codeine loads at most WWTPs in China, a trend opposite to that in many European countries. In addition, morphine and codeine loads were strongly correlated at most WWTPs, indicating morphine and codeine in wastewater were predominantly from the same source, street heroin. At WWTPs in Guangzhou and Shenzhen, codeine loads were considerably higher than morphine loads, consistent with previous reports of codeine abuse (e.g., as cough syrup) among middle and high school students in Guangdong province. Heroin consumption was derived based on morphine loads and taking into account therapeutic use of morphine and codeine, as well as contribution of codeine and acetylcodeine in street heroin. Highest heroin consumption was observed in northwestern and southwestern China. The average heroin consumption of the sampled cities was 64.6 ± 78.7 mg/1000 inh/d. The nation-wide average heroin consumption was much lower than that of methamphetamine, consistent with seizure data and numbers of registered heroin and methamphetamine users in China.Download high-res image (115KB)Download full-size image

•First nationwide reconnaissance on occurrence of NPS in wastewater in China•Mephedrone, TFMPP, mCPP not detected wastewater across China•MDPV detected at about 40% of the sampled cities with low concentrations•BZP quantified in all the wastewater samples but showed no geographic pattern•Apparent removal of MDPV was low, whereas removal of BZP was nearly complete.New psychoactive substances have become increasingly popular across the globe in recent years, which may cause certain public health issues. In this work, sewage-based epidemiology was applied to examine the use of two synthetic cathinones, mephedrone and methylenedioxypyrovalerone (MDPV), and three piperazines, benzylpiperazine (BZP), trifluoromethylphenylpiperazine (TFMPP), and 1-(3-Chlorophenyl)piperazine (mCPP), across China. Influent wastewater samples were collected from 36 sewage treatment plants (STPs) in 18 major cities that cover all the geographic regions of the country. Effluent samples were also collected from selected STPs to determine removal rates. Mephedrone, TFMPP, and mCPP were below detection limits in all the wastewater samples collected, indicating negligible use of these substances in China. MDPV was detected in wastewater at 13 STPs. However, its loads were < 1 mg/1000 inh/d at most of these STPs, indicating low use of this substance. BZP was detected at all the STPs examined, with loads typically falling within the range of 3–10 mg/1000 inh/d. No clear geographic pattern in BZP occurrence in wastewater was identified. Since BZP in wastewater may also come from its legal sources, whether widespread occurrence of BZP means widespread abuse is yet to be confirmed. Apparent removal of MDPV by wastewater treatment was low (< 25%), whereas removal of BZP was nearly complete (typically > 95%).Download high-res image (157KB)Download full-size image

In this work, a simple, cost-effective, and label-free biosensor was constructed for methamphetamine (METH) detection. The biosensor consists of a G-quadruplex–hemin DNAzyme molecular beacon (DNAzyme MB), a METH aptamer, and a colorimetric substrate. The DNAzyme MB loses peroxidase activity when it hybridizes with the METH aptamer. In the presence of METH, DNAzyme MB dissociates from the inactive hybrid due to preferable hybridization of METH with the aptamer. This process recovers the activity of DNAzyme MB, which catalyzes a reaction with the colorimetric substrate to yield measurable signals. Under optimized conditions, a detection limit as low as 0.5 nM (74.6 ng L−1) was achieved. Common illicit drugs were found to have little interference on detection of METH. Recoveries of METH spiked in urines of addicts were greater than 85%. Good agreement was observed between METH concentrations in urines determined by the sensor and by liquid chromatography-tandem mass spectrometer. These results indicate that the G-quadruplex–hemin DNAzyme MB probe holds promise to detect METH not only in biological samples, but also in environmental matrices.

To examine the relevance of low flow zones and flow vortices to colloid transport in real porous media, lattice-Boltzmann (LB) simulations were combined with X-ray microtomography (XMT) to simulate flow fields in glass beads and quartz sand. Backward flow zones were demonstrated to be widely present in both porous media, with a greater volume fraction in the former relative to the latter porous media. Glass beads in the XMT images were approximated as spheres and their coordinates and radii were extracted to allow reconstruction of pore structures. LB simulations were again performed and the simulated flow fields in the reconstructed pore structures were coupled to a three-dimensional particle tracking algorithm. Particle tracking simulations demonstrated that significant amounts of colloids stayed in the simulated domains for long periods (up to 50 pore volumes). The percentages of colloids with long residence time increased as the depth of the secondary energy minimum increased. The majority of the colloids with long residence time were translated to low flow zones while being associated with grain surfaces via secondary minima. A small fraction of colloids entered low flow zones without being associated with the grains surfaces. Backward flow zones were also found to trap a small fraction of colloids for significantly long time (up to 10 pore volumes). In overall, however, backward flow zones trapped fewer colloids for shorter durations than low flow zones. In summary, this work demonstrates the importance of temporary trapping of colloids by the low flow and backward flow zones in real porous media. This trapping process can explain a number of intriguing experimental observations.