Plasmonic silver/silver oxide nanoparticles anchored bismuth vanadate as a novel visible-light ternary photocatalyst for degrading pharmaceutical micropollutants

The degradation of pharmaceutical micropollutants is an intensifying environmental problem and synthesis of efficient photocatalysts for this purpose is one of the foremost challenges worldwide. Therefore, this study was conducted to develop novel plasmonic Ag/Ag₂O/BiVO₄ nanocomposite photocatalysts by simple precipitation and thermal decomposition methods, which could exhibit higher photocatalytic activity for mineralized pharmaceutical micropollutants. Among the different treatments, the best performance was observed for the Ag/Ag₂O/BiVO₄ nanocomposites (5 wt.%; 10 min's visible light irradiation) which exhibited 6.57 times higher photodegradation rate than the pure BiVO₄. Further, the effects of different influencing factors on the photodegradation system of tetracycline hydrochloride (TC-HCl) were investigated and the feasibility for its practical application was explored through the specific light sources, water source and cycle experiments. The mechanistic study demonstrated that the photogenerated holes (h⁺), superoxide radicals (?O₂^?) and hydroxyl radicals (?OH) participated in TC-HCl removal process, which is different from the pure BiVO₄ reaction system. Hence, the present work can provide a new approach for the formation of novel plasmonic photocatalysts with high photoactivity and can act as effective practical application for environmental remediation.     

Morphology-dependent interfacial interactions of Fe2O3 with Ag nanoparticles for determining the catalytic reduction of p-nitrophenol

In this work,we fabricated three kinds of Ag/Fe_2O_3 model catalysts with different morphologies to study the interfacial interactions between Ag and Fe_2O_3,and how they affected the catalytic activity in hydrogenation of p-nitrophenol was explored.The hydrothermal method was used to synthesize the metal oxide supported silver catalyst,with various morphologies including nanoplates(NPs),nanospheres(NSs),and nanocubes(NCs).The crystal structure,morphology and surface elements of the composite were investigated by various measurements,such as X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM) and X-ray photoelectron spectroscopy(XPS).The catalytic activity was also evaluated by the reduction of p-nitrophenol to p-aminophenol.It was found that the activities of the above catalysts varied with the morphology of the support.Among them,Ag/Fe_2O_3 NPs promoted the highest performance,Ag/Fe_2O_3 NSs were slightly inferior,and Ag/Fe_2O_3 NCs were the worst.At last,we ascribed the remarkable activity of Ag/Fe_2O_3 NPs to the strong metal-support interactions between Ag and Fe_2O_3.     

Synergistic effects of Cu species and acidity of Cu-ZSM-5 on catalytic performance for selective catalytic oxidation of n-butylamine

In this work, a series of Cu-ZSM-5 catalysts with different SiO₂/Al₂O₃ ratios (25, 50, 100 and 200) were synthesized and investigated in n-butylamine catalytic degradation. The n-butylamine can be completely catalytic degradation at 350°C over all Cu-ZSM-5 catalysts. Moreover, Cu-ZSM-5 (25) exhibited the highest selectivity to N₂, exceeding 90% at 350°C. These samples were investigated in detail by several characterizations to illuminate the dependence of the catalytic performance on redox properties, Cu species, and acidity. The characterization results proved that the redox properties and chemisorption oxygen primarily affect n-butylamine conversion. N₂ selectivity was impacted by the Brønsted acidity and the isolated Cu²⁺ species. Meanwhile, the surface acid sites over Cu-ZSM-5 catalysts could influence the formation of Cu species. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra was adopted to explore the reaction mechanism. The Cu-ZSM-5 catalysts are the most prospective catalysts for nitrogen-containing volatile organic compounds removal, and the results in this study could provide new insights into catalysts design for VOC catalytic oxidation.     

UV/H2O2 oxidation of tri(2-chloroethyl) phosphate: Intermediate products, degradation pathway and toxicity evaluation

Tri(2-chloroethyl) phosphate (TCEP) with the initial concentration of 5 mg/L was degraded by UV/H₂O₂ oxidation process. The removal rate of TCEP in the UV/H₂O₂ system was 89.1% with the production of Cl^? and PO₄^3? of 0.23 and 0.64 mg/L. The removal rate of total organic carbon of the reaction was 48.8% and the pH reached 3.3 after the reaction. The oxidative degradation process of TCEP in the UV/H₂O₂ system obeyed the first order kinetic reaction with the apparent rate constant of 0.0025 min^?1 (R²=0.9788). The intermediate products were isolated and identified by gas chromatography-mass spectrometer. The addition reaction of HO? and H₂O and the oxidation reaction with H₂O₂ were found during the degradation pathway of 5 mg/L TCEP in the UV/H₂O₂ system. For the first time, environment risk was estimated via the “ecological structure activity relationships” program and acute and chronic toxicity changes of intermediate products were pointed out. The luminescence inhibition rate of photobacterium was used to evaluate the acute toxicity of intermediate products. The results showed that the toxicity of the intermediate products increased with the increase of reaction time, which may be due to the production of chlorine compounds. Some measures should be introduced to the UV/H₂O₂ system to remove the highly toxic Cl-containing compounds, such as a nanofiltration or reverse osmosis unit.     

Photodegradation of Hexafluoropropylene Oxide Trimer Acid under UV Irradiation

As a novel alternative to traditional perfluoroalkyl substances (PFASs), including perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS), hexafluoroproplyene oxide trimer acid (HFPO-TA) has been detected worldwide in surface water. Moreover, recent researches have demonstrated that HFPO-TA has stronger bioaccumulation potential and higher hepatotoxicity than PFOA. To treat these contaminants e.g. PFOA and PFOS, some photochemical techniques by adding exogenous substances had been reported. However, there is still no report for the behavior of HFPO-TA itself under direct UV irradiation. The current study investigated the photo-transformation of HFPO-TA under UV irradiation in aqueous solution. After 72 hr photoreaction, 75% degradation ratio and 25% defluorination ratio were achieved under ambient condition. Reducing active species, i.e., hydrated electrons and active hydrogen atoms, generated from water splitting played dominant roles in degradation of HFPO-TA, which was confirmed by different effects of reaction atmospheres and quenching experiments. A possible degradation pathway was proposed based on the products identification and theoretical calculations. In general, HFPO-TA would be transformed into shorter-chain PFASs, including hexafluoropropylene oxide dimer acid (HFPO-DA), perfluoropropionic acid (PFA) and trifluoroacetate (TFA). This research provides basic information for HFPO-TA photodegradation process and is essential to develop novel remediation techniques for HFPO-TA and other alternatives with similar structures.     

Can a low-carbon development path achieve win-win development: evidence from China’s low-carbon pilot policy

Mitigation and Adaptation Strategies for Global Change - Low-carbon pilot (LCP) policy aims to not only achieve economic development but also address climate change problems in China. With a...     

Regionalization based on spatial and seasonal variation in ground-level ozone concentrations across China

Owing to the vast territory of China and strong regional characteristic of ozone pollution,it's desirable for policy makers to have a targeted and prioritized regulation and ozone pollution control strategy in China based on scientific evidences. It's important to assess its current pollution status as well as spatial and temporal variation patterns across China.Recent advances of national monitoring networks provide an opportunity to insight the actions of ozone pollution. Here, we present rotated empirical orthogonal function(REOF)analysis that was used on studying the spatiotemporal characteristics of daily ozone concentrations. Based on results of REOF analysis in pollution seasons for 3 years' observations, twelve regions with clear patterns were identified in China. The patterns of temporal variation of ozone in each region were separated well and different from each other, reflecting local meteorological, photochemical or pollution features. A rising trend in annual averaged Eight-hour Average Ozone Concentrations(O_3-8 hr) from 2014 to 2016 was observed for all regions, except for the Tibetan Plateau. The mean values of annual and 90 percentile concentrations for all 338 cities were 82.6 ± 14.6 and 133.9 ± 25.8 μg/m~3,respectively, in 2015. The regionalization results of ozone were found to be influenced greatly by terrain features, indicating significant terrain and landform effects on ozone spatial correlations. Among 12 regions, North China Plain, Huanghuai Plain, Central Yangtze River Plain, Pearl River Delta and Sichuan Basin were realized as priority regions for mitigation strategies, due to their higher ozone concentrations and dense population.     

基于短时傅里叶变换的干扰信号识别方法

目的提高无线电引信识别欺骗式干扰的能力。方法根据炮弹弹体自旋的特点,使得采用连续波线极化天线的无线电引信所收到的干扰信号呈现出有别于地面回波的周期性幅度调制特征,通过对此特征进行短时傅里叶变换后进行识别,可以作为无线电引信是否受到欺骗式干扰的判断依据。结果通过仿真和试验对方法的可行性进行了验证,表明该识别方法可以很好地提高连续波无线电引信的识别欺骗式干扰的能力。结论基于短时傅里叶变换检测旋转调制的对地旋转弹无线电引信欺骗干扰识别的方法可以对干扰信号特征进行识别,算法处理时间短,能够作为引信是否受到干扰的一种判断依据。     

基于环境保护大数据的监测与智能诊断研究

为了提高环境保护的智能监测能力,采用大数据分析方法进行环境监测和诊断分析,提出一种基于环保大数据关联特征挖掘的环境保护智能监测与诊断技术。构建环境监测的约束参量模型,以土壤监测数据、空间污染排放量以及水资源监测数据为原始统计数据,采用关联规则特征提取方法进行环保大数据的有用信息挖掘,结合模糊C均值聚类算法实现对环保大数据的分类处理,根据分类结果进行环保监测和智能诊断分析。仿真结果表明,采用该方法进行环保大数据挖掘的准确性较好,对各种污染信息的分类精度较高,提高了环保监测和诊断的有效性与实时性。     

Methane emissions from natural wetlands

Methane is considered one of the most important greenhouse gases in the atmosphere. Because of the strict anaerobic conditions required by CH₄-generating microorganisms, natural wetland ecosystems are one of the main sources of biogenic CH₄. The total natural wetland area is estimated to be 5.3 to 5.7 × 10¹² m², making up less than 5% of the Earth's land surface. However, natural wetland plays a disproportionately large role in CH₄ emissions. Wetlands are likely the largest natural sources of CH₄ to the atmosphere, accounting for about 20% of the current global annual emission. Out of the total amount of CH₄ emitted, northern wetlands contribute 34%, temperate wetlands 5%, and tropical systems about 60%.Because of the unique characteristics and high productivity, wetland ecosystems are important in the global carbon cycle. Natural wetlands are permanently or temporarily saturated. Strict anaerobic conditions consequently develop, which allows methanogenesis to occur. But the thin oxic layer and the oxic plant rhizophere promote activity of CH₄-oxidizing bacteria or methanotrophs. Thus, both CH₄ formation and consumption in wetland systems are microbiological processes and are controlled by many factors. Eight of the controlling factors, including carbon supply, soil oxidation-reduction status, pH, temperature, vegetation, salinity and sulfate content, soil hydrological conditions and CH₄ oxidation are discussed in this paper.