科研成果 by Year: 2018

Peracetic acid (PAA) is a sanitizer with increasing use in food, medical and water treatment industries. Amino acids are important components in targeted foods for PAA treatment and ubiquitous in natural waterbodies and wastewater effluents as the primary form of dissolved organic nitrogen. To better understand the possible reactions, this work investigated the reaction kinetics and transformation pathways of selected amino acids towards PAA. Experimental results demonstrated that most amino acids showed sluggish reactivity to PAA except cysteine (CYS), methionine (MET), and histidine (HIS). CYS showed the highest reactivity with a very rapid reaction rate. Reactions of MET and HIS with PAA followed second-order kinetics with rate constants of 4.6 ± 0.2, and 1.8 ± 0.1 M−1⋅s−1 at pH 7, respectively. The reactions were faster at pH 5 and 7 than at pH 9 due to PAA speciation. Low concentrations of H2O2 coexistent with PAA contributed little to the oxidation of amino acids. The primary oxidation products of amino acids with PAA were [O] addition compounds on the reactive sites at thiol, thioether and imidazole groups. Theoretical calculations were applied to predict the reactivity and regioselectivity of PAA electrophilic attacks on amino acids and improved mechanistic understanding. As an oxidative disinfectant, the reaction of PAA with organics to form byproducts is inevitable; however, this study shows that PAA exhibits lower and more selective reactivity towards biomolecules such as amino acids than other common disinfectants, causing less concern of toxic disinfection byproducts. This attribute may allow greater stability and more targeted actions of PAA in various applications.

Volatile organic compounds play an important role in air quality and climate change, largely because they contribute to the formation of oxidizing compounds and secondary organic aerosol (SOA). In this study, a series of products, including peroxides and carbonyl compounds in both gaseous and particulate phases, were simultaneously detected to investigate the oxidation regime and SOA composition in limonene ozonolysis. The roles of different double bonds (DBs), radicals, and water were also examined. In our first investigation, we focused on representative oxidizing compounds produced in limonene ozonolysis, including stabilized Criegee intermediates (SCIs), OH radicals, and peroxides. The dependence of H2O2 and hydroxymethyl hydroperoxide (HMHP) formation on RH demonstrates that the reaction with water is an important reaction pathway for limonene SCIs, and the lower-limit SCI yields of endocyclic and exocyclic DBs were estimated to be ~0.24 and ~0.43, respectively. The OH yield was determined by adding sufficient amounts of an OH scavenger, and the OH yields of endocyclic and exocyclic DBs were ~0.65 and ~0.24, respectively. These results indicate that in limonene ozonolysis the endocyclic DB is inclined to generate OH radicals through hydroperoxide channel, while the exocyclic DB has a higher fraction of forming SCIs. Besides, other gas-phase and particle-phase peroxides were also studied in this work. The formation of peroxyformic acid (PFA) and peroxyacetic acid (PAA) was promoted significantly by increasing RH and the degree of oxidation, and the discrepancy between the experimental and model results suggested some missing formation pathways. Considerable generation of H2O2 from SOA in the aqueous phase was observed, especially at high [O3]/[limonene], which was mainly attributed to the hydration and decomposition of unstable peroxides in SOA such as peroxycarboxylic acids and peroxyhemiacetals. Different DBs and OH scavengers had a large impact on the particulate peroxides, and their stability indicated that the types of peroxides in SOA changed under different conditions. As for the contribution of peroxides to SOA, the results demonstrated that the mass fraction of particulate peroxides in limonene SOA was less than 0.2 at low [O3]/[limonene], while the mass fraction was 0.4–0.6 at high [O3]/[limonene]. The partitioning behavior of peroxides showed that multi-generation oxidation helped produce more low-volatility peroxides, which partially explained the higher SOA yield. The partitioning behavior of carbonyls was also examined and the experimental partitioning coefficients (Kp) were found to be typically several orders of magnitude higher than the theoretical values. This study provided new insights into the oxidation regime and SOA composition in limonene ozonolysis, and limonene showed its specificity in many aspects when both endocyclic and exocyclic DBs were ozonated. We suggest that the atmospheric implications of terpenes containing more than one DB and the SOA composition, especially particulate peroxides, need further study.

Background & aims: The 4 genotypes of hepatitis E virus (HEV) that infect humans (genotypes 1-4) vary in geographical distribution, transmission, and pathogenesis. Little is known about the properties of HEV or its hosts that contribute to these variations. Primary isolates grow poorly in cell culture; most studies have relied on variants adapted to cancer cell lines, which likely alter virus biology. We investigated the infection and replication of primary isolates of HEV in hepatocyte-like cells (HLCs) derived from human embryonic and induced pluripotent stem cells. Methods: Using a cell culture-adapted genotype 3 strain and primary isolates of genotypes 1 to 4, we compared viral replication kinetics, sensitivity to drugs, and ability of HEV to activate the innate immune response. We studied HLCs using quantitative reverse-transcriptase polymerase chain reaction and immunofluorescence assay and enzyme-linked immunosorbent assays. We used an embryonic stem cell line that can be induced to express the CRISPR-Cas9 machinery to disrupt the peptidylprolyl isomerase A gene, encoding cyclophilin A (CYPA), a protein reported to inhibit replication of cell culture-adapted HEV. We further modified this line to rescue expression of CYPA before terminal differentiation to HLCs and performed HEV infection studies. Results: HLCs were permissive for infection by nonadapted, primary isolates of HEV genotypes 1 to 4. HEV infection of HLCs induced a replication-dependent type III interferon response. Replication of primary HEV isolates, unlike the cell culture-adapted strain, was not affected by disruption of the peptidylprolyl isomerase A gene or exposure to the CYPA inhibitor cyclosporine A. Conclusions: Cell culture adaptations alter the replicative capacities of HEV. HLCs offer an improved, physiologically relevant, and genetically tractable system for studying the replication of primary HEV isolates. HLCs could provide a model to aid development of HEV drugs and a system to guide personalized regimens, especially for patients with chronic hepatitis E who have developed resistance to ribavirin. Keywords: Antiviral; HLCs; Personalized Medicine; Primary Isolates.

Biomass burning (BB) activities have a great impact on the particle number size distribution (PNSD) in the upper troposphere of the Tibetan Plateau, which could affect regional and global climate. An intensive campaign focused on the measurement of the PNSD, gaseous pollutants, and meteorological parameters was conducted at Mt. Yulong, a high-altitude site (3410ma.s.l.) on the southeastern Tibetan Plateau during the pre-monsoon season (22 March to 15 April). During this period, intensive BB activities in southern Asia were detected by fire maps. The long-range transport of BB pollutants can increase the accumulation mode particles in the background atmosphere at Mt. Yulong. As a consequence, the cloud condensation nuclei (CCN) concentration was found to be 2-8 times higher during BB periods than during clean periods. Apart from BB, variations of the planet boundary layer (PBL) and new particle formation (NPF) were other factors that influenced the PNSD. However, only three NPF events (with a frequency of 14 %) were observed at Mt. Yulong. The occurrence of NPF events during clean episodes corresponded to an elevated PBL or transported BB pollutants. Due to the lack of condensable vapors including sulfuric acid and organic compounds, the newly formed particles were not able to grow to CCN size. Our study emphasizes the influences of BB on the aerosol and CCN concentration in the atmosphere of the Tibetan Plateau. These results also have the potential to improve our understanding of the variation of the particle concentration in the upper troposphere, and provide information for regional and global climate models.

The study of strongly frustrated magnetic systems has drawn great attentions from both theoretical and experimental physics. Efficient simulations of these models are essential for understanding their exotic properties. Here we present PEPS++, a novel computational paradigm for simulating frustrated magnetic systems and other strongly correlated quantum many-body systems. PEPS++ can accurately solve these models at the extreme scale with low cost and high scalability on modern heterogeneous supercomputers. We implement PEPS++ on Sunway TaihuLight based on a carefully designed tensor computation library for manipulating high-rank tensors and optimize it by invoking various high-performance matrix and tensor operations. By solving a 2D strongly frustrated \textlessformula\textgreater\textlesstex\textgreater\$J\_1-J\_2\$\textless/tex\textgreater\textless/formula\textgreater model with over ten million cores, PEPS++ demonstrates the capability of simulating strongly correlated quantum many-body problems at unprecedented scales with accuracy and time-to-solution far beyond the previous state of the art.

BACKGROUND AND AIMS: Considerable attention is given nowadays to the presence of cardiovascular diseases risk factors in children. The current blood lipid classification system for Chinese children was based on the United States National Cholesterol Education Program (NCEP) cutpoints, which did not take the age, gender and race differences into consideration. This study aimed to develop gender- and age-specific lipid cutpoints for dyslipidemia screening in Chinese children and compare the ability of new cutpoints and NCEP pediatric cutpoints to predict obesity and unfavorable blood pressure (BP) levels. METHODS: Data were obtained from a nationwide multicenter cross-sectional study: The China Child and Adolescent Cardiovascular Health Study, comprising 12,875 Chinese children aged 6-18 years. We calculated cutpoints for abnormal levels of total cholesterol (TC), low-density lipoprotein cholesterol (LDL-C), high-density lipoprotein cholesterol (HDL-C), and triglycerides (TG) that were linked to Chinese adult abnormal lipid thresholds using the General Additive Model for Location Scale and Shape method. RESULTS: Borderline-high and high cutpoints (TC, LDL-C and TG) as well as low cutpoints (HDL-C) were developed to classify the abnormal blood lipid levels in Chinese children. Better performance for prediction of obesity, elevated BP, and hypertension were found with the proposed cutpoints in comparison with the NCEP pediatric cutpoints (AUC for obesity: 0.612 vs. 0.597, p=0.017; AUC for elevated BP: 0.529 vs. 0.521, p=0.017; AUC for hypertension: 0.536 vs. 0.527, p=0.016). CONCLUSIONS: The gender- and age-specific cutpoints should improve the accuracy of dyslipidemia screening in China and be more reasonable in practice.

Two kinds of hybrid two-step multi-soil-layering (MSL) systems loaded with different filter medias (zeolite-ceramsite MSL-1 and ceramsite-red clay MSL-2) were set-up for the low-(C/N)-ratio polluted river water treatment. A long-term pollutant removal performance of these two kinds of MSL systems was evaluated for 214 days. By-pass was employed in MSL systems to evaluate its effect on nitrogen removal enhancement. Zeolite-ceramsite single-pass MSL-1 system owns outstanding ammonia removal capability (24 g NH4+-Nm(-2)d(-1)), 3 times higher than MSL-2 without zeolite under low aeration rate condition (0.8 x 10(4) L m(-2).h(-1)). Aeration rate up to 1.6 x 10(4) L m(-2).h(-1) well satisfied the requirement of complete nitrification in first unit of both two MSLs. However, weak denitrification in second unit was commonly observed. By-pass of 50% influent into second unit can improve about 20% TN removal rate for both MSL-1 and MSL-2. Complete nitrification and denitrification was achieved in by-pass MSL systems after addition of carbon source with the resulting C/N ratio up to 2.5. The characters of biofilms distributed in different sections inside MSL-1 system well illustrated the nitrogen removal mechanism inside MSL systems. Two kinds of MSLs are both promising as an appealing nitrifying biofilm reactor. Recirculation can be considered further for by-pass MSL-2 system to ensure a complete ammonia removal. (C) 2018 Elsevier Ltd. All rights reserved.

With the deterioration of the environment across the globe, environmental problems have attracted much attention from the public, academia, and governments. This study contributes to the understanding of environmental policy implementation by empirically testing the policy feedback theory and official ranking tournament theory in the Chinese context. In particular, it focuses on how prior environmental performance ranking transitions into future policy performance through the mandatory target system (MTS) in China. The results from this study show that provincial environmental performance ranking serves as an effective incentive for strengthening environmental governance. Low‐ranking provinces will improve their environmental policy performances in future years because of competition in the official tournament. Policy implications are drawn to improve the administrative design of environmental management.