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We report a template-free and easy solvent evaporation method during carbonizing a metal–organic framework (MOF) for the construction of large-scale meso- and macropore. While the direct thermal evaporation method of non-volatile solvent captured in micropore of a MOF is believed to reduce overall porosity of the resultant MOF, this method unprecedentedly directs the reorganization of MOFs toward the production of ultrahigh porous carbon materials. The obtained porous carbon materials possess a unique interconnected three-dimensional wormhole-like structure, high specific surface area (3000 m2 g−1), and exceptionally high pore volume (5.45 cm3 g−1). The micropores, along with accessible meso- and macropores, provide ion storage site and ion transport channel, respectively, that contributes to a rapid elimination of large amounts of salt within a very short period of time.  相似文献   
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Single-atom photocatalysts have shown their fascinating strengths in enhancing charge transfer dynamics; however, rationally designing coordination sites by metal doping to stabilize isolated atoms is still challenging. Here, a one-unit-cell ZnIn2S4 (ZIS) nanosheet with abundant Cu dopants serving as the suitable support to achieve a single atom Pt catalyst (Pt1/Cu–ZIS) is reported, and hence the metal single atom–metal dopant interaction at an atomic level is disclosed. Experimental results and density functional theory calculations highlight the unique stabilizing effect (Pt–Cu interaction) of single Pt atoms in Cu-doped ZIS, while apparent Pt clusters are observed in pristine ZIS. Specifically, Pt–Cu interaction provides an extra coordination site except three S sites on the surface, which induces a higher diffusion barrier and makes the single atom more stable on the surface. Apart from stabilizing Pt single atoms, Pt–Cu interaction also serves as the efficient channel to transfer electrons from Cu trap states to Pt active sites, thereby enhancing the charge separation and transfer efficiency. Remarkably, the Pt1/Cu–ZIS exhibits a superb activity, giving a photocatalytic hydrogen evolution rate of 5.02 mmol g−1 h−1, nearly 49 times higher than that of pristine ZIS.  相似文献   
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Excessive nitrogen loads and subsequent eutrophication risk have led to a series of critical water quality problems in Chinese watersheds. To address this issue, a modeling approach is useful for quantifying nitrogen sources, assessing source apportionment, and guiding management responses. In this study, we modeled the main hydrochemical processes of the Lian River watershed located in the south of China using the Regional Nutrient Management (ReNuMa) model, a model derived from the Generalized Watershed Loading Function (GWLF) model and incorporating Net Anthropogenic Nitrogen Inputs (NANI) to estimate runoff nitrogen concentrations. An informal Bayesian method, the Generalized Likelihood Uncertainty Estimation (GLUE) procedure, was applied for model calibration and uncertainty analysis. The resulting modeled monthly total nitrogen fluxes have high Nash-Sutcliff coefficients (>0.85) for the calibration (2005–2009) and verification (2003, 2004 and 2010) periods, representing an acceptable goodness-of-fit. The model outputs were further processed using multivariate statistical analysis to determine latent rules of nitrogen source apportionment under different circumstances, including different water regimes, seasonal patterns, and loading levels. The main nitrogen contributions in different natural and management-driven conditions have been identified, and appear to be significant for supporting decision-making priorities. We find that the ReNuMa model, with its Bayesian procedure and the linkage of subsequent multivariate statistical analysis, represents a useful approach with applicability within China and a great potential to be extended elsewhere.  相似文献   
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通过磷释放动力学实验,研究了天津滨海盐碱地区水库15个沉积物的磷释放动力学特征,并探讨了沉积物组成对磷释放的影响.结果表明:0~2 h内磷快速解吸,2~12 h内磷出现反复吸附、解吸,12 ~24 h内磷的解吸逐渐达到平衡,达最大磷释放量,15个沉积物对于磷的最大解吸量在8.01~ 12.62 mg/kg之间,不同沉积物之间具有较大差异.拟二级动力学模型可以很好地拟合沉积物磷释放动力学特征.沉积物磷释放动力学参数与沉积物全磷、全铁含量呈极显著正相关,与粘粒含量呈显著正相关,而与全盐量呈显著负相关.因此,天津滨海盐碱地区沉积物磷的释放与沉积物磷含量密切相关,并受全铁、全盐量和粘粒含量等因素的共同影响.  相似文献   
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Carbon materials have been widely used as cathodes in lithium oxygen batteries but the detailed influence of the structure of these materials on their performance is not very clear yet. In this study, the same starting pristine commercial carbon black (N330) was treated under different atmospheres and the resultant carbons were employed as cathode materials for lithium oxygen batteries. It was demonstrated that the porosity and surface topology of these carbons tremendously changed as their treating time increased. The parameters that influenced the battery performance were identified. It was found that the main factor determining the battery performance is the specific surface area of the carbon mesopores, while nitrogen- or oxygen-bearing functionalities, introduced in these carbons during their heat-treatment or by contact with air after their pyrolysis, had little or no influence on the battery performance.  相似文献   
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Trichloroethylene (TCE) is a common groundwater contaminant of toxic and carcinogenic concern. Aerobic co-metabolic processes are the predominant pathways for TCE complete degradation. In this study, Pseudomonas fluorescens was studied as the active microorganism to degrade TCE under aerobic condition by co-metabolic degradation using phenol and gasoline as growth substrates. Operating conditions influencing TCE degradation efficiency were optimized. TCE co-metabolic degradation rate reached the maximum of 80% under the optimized conditions of degradation time of 3 days, initial OD600 of microorganism culture of 0.14 (1.26 × 107 cell/mL), initial phenol concentration of 100 mg/L, initial TCE concentration of 0.1 mg/L, pH of 6.0, and salinity of 0.1%. The modified transformation capacity and transformation yield were 20 μg (TCE)/mg (biomass) and 5.1 μg (TCE)/mg (phenol), respectively. Addition of nutrient broth promoted TCE degradation with phenol as growth substrate. It was revealed that catechol 1,2-dioxygenase played an important role in TCE co-metabolism. The dechlorination of TCE was complete, and less chlorinated products were not detected at the end of the experiment. TCE could also be co-metabolized in the presence of gasoline; however, the degradation rate was not high (28%). When phenol was introduced into the system of TCE and gasoline, TCE and gasoline could be removed at substantial rates (up to 59% and 69%, respectively). This study provides a promising approach for the removal of combined pollution of TCE and gasoline.  相似文献   
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Seventy water samples, including wastewaters, tap waters, fresh surface waters, coastal waters, groundwaters, and precipitation samples, from Tianjin, China, were analyzed for seven commonly used artificial sweeteners (ASs). The concentrations of the investigated ASs were generally in the order of wastewater treatment plant (WWTP) influent > WWTP effluent > surface water > tap water > groundwater ≈ precipitation, while the composition profiles of ASs varied in different waters. Acesulfame, sucralose, cyclamate, and saccharin were consistently detected in surface waters and ranged from 50 ng/L to 0.12 mg/L, while acesulfame was the dominant AS in surface and tap waters. Aspartame was found in all of the surface waters at a concentration up to 0.21 μg/L, but was not found in groundwaters and tap waters. Neotame and neohesperidin dihydrochalcone were less frequently detected and the concentrations were low. The concentrations of the ASs in some of the surface waters were of the same order with those in the WWTP influents, but not with the effluents, indicating there are probably untreated discharges into the surface waters. The ASs were detected in precipitation samples with high frequency, and acesulfame, saccharin, and cyclamate were the predominant ASs, with concentrations ranging from 3.5 ng/L to 1.3 μg/L. A gross estimation revealed that precipitation may act as a source for saccharin and cyclamate in the surface environment of Tianjin city. Moreover, the presence of ASs in the atmosphere was primarily assessed by taking 4 air samples to evaluate their potential source in precipitation.  相似文献   
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