The high efficiency of perovskite solar cells benefits from the high density of photoinduced free carriers. We studied how exciton and free carriers, as the two major photoproducts, coexist inside the CH3NH3PbI3 perovskite. A new density-resolved spectroscopic method was developed for this purpose. The density-dependent coexistence of excitons and free carriers over a wide density range was experimentally observed. The quantitative analysis on the density-resolved spectra revealed a moderate exciton binding energy of 24 +/- 2 meV. The results effectively proved that the strong ionic polarization inside the perovskite has a negligible contribution to exciton formation. The spectra also efficiently uncovered the effective mass of electron-hole pairs. Our spectroscopic method and the results profoundly enrich the understanding of the photophysics in perovskite materials for photovoltaic applications.
Particulate pollution is a major air pollution problem in Chinese mega-cities. Under such conditions, the atmospheric gas-phase chemistry is strongly influenced by heterogeneous reactions, of which to quantify the heterogeneous reaction processes of N2O5 is essential for the understanding of the nighttime oxidation capacity, regional NOx budget, photochemical ozone prodution, etc. In this paper, we extensively review the research progress of the N2O5 heterogeneous reaction processes such as its reaction mechanism, measurement techniques of the corresponding uptake coefficient (gamma(N2O5)) and the measurement results on different aerosol substrates. The heterogeneous reaction processes of N2O5 is a typical reactive uptake process which can be ideally studied by the aerosol flow tube system. The corresponding laboratory kinetic studies are started from model aerosols (sulfate), and evolved to be more realistic aerosols according to the accumulated knowledges on the aerosol properties obtained in field studies. It is found that the gamma(N2O5) varied from 0. 001 to 0. 2 on different aerosol substrates, more than two orders of magnitude. The variation is influenced by the ambient temperature, relative humidity, mixing state, phase state, aerosol chemical compositions like NO3-, Cl-, SO42-, liquid water content (LWC), organics, etc., of which the uptake coefficient is higher with higher LWC, Cl-, SO42- while lower with higher NO3- and organics. The avaiable field studies in the United States and Europe showed that, to describe gamma(N2O5), these impact factors can' t be independently expressed; and the dependence seems to be very complicated and cross correlated. Therefore the state of art parameterization methods of gamma(N2O5) developed from lab kinetic studies are still not able to describe the field observations. Since high aerosol loading and high N2O5 are always co-located at urban aeras, more field observations and sucessful parameterization of gamma(N2O5) is proposed to be conducted in typical urban conditions including Chinese megacity regions.
The treatment efficiency of constructed wetlands (CWs) is highly dependent on the stability of the hydraulic flow patterns. To date, general technologies used to study hydraulic flow patterns of CWs mainly include tracer method, model simulation and velocity measurement, which are either expensive, empirical, or having secondary pollution. In this study, a new technology, which was based on the isotopic composition variation in CWs, was applied to detect the hydraulic flow patterns of two different CWs. Results showed that the hydraulic flow patterns of the two studied wetlands could be detected effectively by using hydrogen and oxygen isotopes. Furthermore, the locations of stagnant areas (SAS) and preferential flow areas (PFAs) were also determined. Significant regional difference in isotopic composition existed inside each CW, and two wetland design suggestions are proposed after hydraulic analysis. One is that the influent of CWs is supposed to be distributed uniformly, and another piece of advice is that the vegetation in the direction perpendicular to water flow should be maintained at the same types and density. (C) 2016 Elsevier B.V. All rights reserved.
Heavy-atom-free triplet photosensitizers are developed by harnessing the thermally active triplet state of carbazolyl dicyanobenzene (CDCB) derivatives and applied to realize visible-to-ultraviolet photon upconversion (UC) via triplet-triplet annihilation (TTA). Demonstrating an annihilator-appending strategy, the designed sensitizers effectively realize TTA UC in polyurethane films with 2,7-di-tert-butylpyrene (DBP) as the annihilator/emitter. The covalently tethered DBP to CDCB is proven critical for achieving the superior sensitizing and UC performance in the solid matrix, essentially by suppressing the reverse ISC and more effectively transferring triplet excitons to free emitters.
Dietary intake is one of the major exposure pathways of polycyclic aromatic hydrocarbons (PAHs), especially in Chinese people because foods are often prepared with grilling and/or frying that would produce high levels of PAHs. In this paper, we assessed daily dietary intakes (DDI) of PAHs, using a "duplicate plate method", among 100 Chinese urban residents. The DDI of benzo(a)pyrene ranged from 0.06 mu g per day to 13.5 mu g per day with a median of 0.69 mu g per day, varying largely across subjects. The median Incremental Lifetime Cancer Risk (ILCR) attributable to PAH dietary intake was 6.65 x 10(-5) (4.41 x 10(-5) to 1.02 x 10(-4) as inter-quartile range). The contribution of several high-PAH containing foods like barbecued, smoked or deep-fried meats to the overall DDIs was about 13%. The use of raw foods may underestimate dietary intake of PAHs and associated exposure risk considerably. Results from foods sampled in different seasons suggested that seasonal variability within an individual may contribute notably to overall variability measured in a population and more future studies with longer-term investigation on food ingestion and pollutant exposure are needed. The study indicates that measuring actually consumed foods is more appropriate for dietary intake exposure assessment, and intra-individual variance should be taken into account during study design and data analysis. (C) 2015 Elsevier Ltd. All rights reserved.
Contradictory results were reported for the prognostic role of CpG island methylator phenotype (CIMP) among colorectal cancer (CRC) patients. Differences in the definitions of CIMP were the most common explanation for these discrepancies. The aim of this systematic review was to give an overview of the published studies on CRC prognosis according to the different definitions of CIMP. A systematic literature search was performed in MEDLINE and ISI Web of Science for articles published until 3 April 2015. Data extraction included information about the study population, the definition of CIMP, and investigated outcomes. Thirty-six studies were included in this systematic review. Among them, 30 studies reported the association of CIMP and CRC prognosis and 11 studies reported the association of CIMP with survival after CRC therapy. Overall, 16 different definitions of CIMP were identified. The majority of studies reported a poorer prognosis for patients with CIMP-positive (CIMP+)/CIMP-high (CIMP-H) CRC than with CIMP-negative (CIMP-)/CIMP-low (CIMP-L) CRC. Inconsistent results or varying effect strengths could not be explained by different CIMP definitions used. No consistent variation in response to specific therapies according to CIMP status was found. Comparative analyses of different CIMP panels in the same large study populations are needed to further clarify the role of CIMP definitions and to find out how methylation information can best be used to predict CRC prognosis and response to specific CRC therapies.