Enhancement of solar-driven photocatalytic activity of oxygen vacancy-rich Bi/BiOBr/Sr2LaF7:Yb3+,Er3+ composites through synergetic strategy of upconversion function and plasmonic effect

For better use of solar energy, the development of efficient broadband photocatalyst has attracted extraordinary attention. In this study, a ternary composite consisting of Sr₂LaF₇:Yb³⁺,Er³⁺ upconversion (UC) nanocrystals and Bi nanoparticles loaded BiOBr nanosheets with oxygen vacancies (OVs, SLFBB) was designed and synthesized by multistep solvent-thermal method. Mechanisms of in-situ formation of Bi nanoparticles and OVs in BiOBr/Sr₂LaF₇:Yb³⁺,Er³⁺ composites (SFLB) are clarified. The Bi metal and OVs enhanced the light-harvesting capacity in the region of visible-near-infrared (Vis-NIR), and promoted the separation of electron–hole (e⁻/h⁺) pairs. Furthermore, the surface plasmon resonance (SPR) effect of Bi metal can improve the energy transfer from Sr₂LaF₇:Yb³⁺,Er³⁺ to BiOBr via nonradiative energy transfer process, resulting in enhancing the light utilization from upconverting NIR into Vis light. Due to the synergistic effects of UC function, SPR and OVs, the SFLBB exhibited obviously enhanced photocatalytic ability for the degradation of BPA with a rate of 8.9 × 10⁻³ min⁻¹, which is about 2.78 times higher than 3.2 × 10⁻³ min⁻¹ of BiOBr (BOB) under UV–Vis-NIR light irradiation. This work provides a novel strategy for the project of high-efficiency Bismuth-based broadband photocatalysts, which is helpful to further understand the mechanism of enhanced photocatalysis by UC function and plasmonic effect.     

Response of PM2.5-bound elemental species to emission variations and associated health risk assessment during the COVID-19 pandemic in a coastal megacity

The coronavirus (COVID-19) pandemic is disrupting the world from many aspects. In this study, the impact of emission variations on PM_2.5-bound elemental species and health risks associated to inhalation exposure has been analyzed based on real-time measurements at a remote coastal site in Shanghai during the pandemic. Most trace elemental species decreased significantly and displayed almost no diel peaks during the lockdown. After the lockdown, they rebounded rapidly, of which V and Ni even exceeded the levels before the lockdown, suggesting the recovery of both inland and shipping activities. Five sources were identified based on receptor modeling. Coal combustion accounted for more than 70% of the measured elemental concentrations before and during the lockdown. Shipping emissions, fugitive/mineral dust, and waste incineration all showed elevated contributions after the lockdown. The total non-carcinogenic risk (HQ) for the target elements exceeded the risk threshold for both children and adults with chloride as the predominant species contributing to HQ. Whereas, the total carcinogenic risk (TR) for adults was above the acceptable level and much higher than that for children. Waste incineration was the largest contributor to HQ, while manufacture processing and coal combustion were the main sources of TR. Lockdown control measures were beneficial for lowering the carcinogenic risk while unexpectedly increased the non-carcinogenic risk. From the perspective of health effects, priorities of control measures should be given to waste incineration, manufacture processing, and coal combustion. A balanced way should be reached between both lowering the levels of air pollutants and their health risks.     

Ce改性钒磷氧催化剂的制备及其脱硝性能研究

采用Ce调控负载型钒磷氧（VPO/TiO₂）催化剂的表面酸性并与之形成密切相关的微观结构,研究催化剂VPO-Ce/TiO₂的脱硝性能.结果表明,当P/V为1/3、Ce/V为1/4、活性组分负载量10%、催化剂焙烧温度为400℃时,催化剂的脱硝活性最好,反应温度250~350℃范围内的脱硝率高于96.0%.BET测试结果表明,催化剂0.1VP（0.33）O-Ce（0.25）/TiO₂的比表面积为10.74m²/g,较0.1VP（0.33）O/TiO₂提高了约58.6%.0.1VP（0.33）O/TiO₂表面化学吸附氧（O_α）和晶格氧（O_β）的比例O_α/O_β为72%,掺杂Ce后O_α/O_β升高至85%,Ce掺杂还能促进相邻V⁵⁺和V⁴⁺的形成,提高催化剂的氧化还原性能.Ce掺杂对催化剂的表面酸性影响较大,当Ce/V为1/4时催化剂表面Brønsted酸最强,这与活性测试相吻合.控制烟气中SO₂和水蒸气的体积浓度分别为200×10^-6和4vol.%,催化剂的脱硝活性在150~300℃温度范围内最高下降约15.8%,当温度高于300℃时催化剂的脱硝活性几乎不下降,且反应后的催化剂表面无硫酸根生成,催化剂呈现出较强的抗SO₂和水蒸汽的性能.     

Monitoring biofouling based on aerobic respiration in reverse osmosis system

A monitoring method of biofouling in reverse osmosis (RO) system was proposed based on the fluorescent signal of resorufin, which is reduced by nicotinamide adenine dinucleotide released from viable cells during aerobic respiration. The fluorescent signal of resorufin reduced by planktonic cells and microorganisms of biofilm showed linearity, indicating its feasibility to monitor biofouling in a RO system. For the application of the method to the lab-scale RO system, the injection concentration of resazurin and the injection flow rate were optimized. Biofilm on RO membranes continuously operated in a lab-scale RO system was estimated by resorufin fluorescence under optimized detection condition. As a result, resorufin fluorescence on RO membrane showed a significant increase in which the permeability of RO system decreased by 30.48%. Moreover, it represented the development of biofilm as much as conventional biofilm parameters such as adenosine triphosphate, extracellular polymeric substances, and biofilm thickness. The proposed method could be used as a sensitive and low-cost technology to monitor biofouling without autopsy of membranes.     

Understanding the electrode reaction process of dechlorination of 2,4-dichlorophenol over Ni/Fe nanoparticles: Effect of pH and 2,4-dichlorophenol concentration

Herein,with the exploitation of iron and nickel electrodes,the 2,4-dichlorophenol(2,4-DCP)dechlorinating processes at the anode and cathode,respectively,were separately studied via various electrochemical techniques(e.g.,Tafel polarization,linear polarization,electrochemical impedance spectroscopy).With this in mind,Ni/Fe nanoparticles were prepared by chemical solution deposition,and utilized to test the dechlorination activities of 2,4-DCP over a bimetallic system.For the iron anode,the results showed that higher 2,4-DCP concentration and solution acidity aggravated the corrosion within the electrode.The charge transfer resistance(R_(ct))values of the iron electrode were 703,473,444,and 437Ω·cm~2 for the initial 2,4-DCP concentrations of0,20,50,and 80 mg/L,respectively.When the bulk pH of the 2,4-DCP solution varied from 3.0,5.0to 7.0,the corresponding R_(ct) values were 315,376,and 444Ω·cm~2,respectively.For the nickel cathode,the reduction current densities on the electrode at-0.75 V(vs.saturated calomel electrode)were 80,106,and 111μA/cm~2,for initial 2,4-DCP concentrations of 40,80,and125 mg/L.The dechlorination experiments demonstrated that when the initial pH of the solution was 7.0,5.0,and 3.0,the dechlorination percentage of 2,4-DCP by Ni/Fe nanoparticles was 62%,69%,and 74%,respectively,which was in line with the electrochemical experiments.10 wt.%Ni loading into Ni/Fe bimetal was affordable and gave a good dechlorination efficiency of 2,4-DCP,and fortunately the Ni/Fe nanoparticles remained comparatively stable in the dechlorination processes at pH 3.0.     

上海市专项化学品制造行业VOCs排放特征及臭氧生成潜势研究

选取上海市某工业区内专项化学品制造行业中有代表性的10家企业,使用苏玛罐对各企业有组织排放废气进行采样,通过GC-MS（气相色谱-质谱联用仪）对106种VOCs进行分析,研究了专项化学品制造行业的VOCs排放特征,并使用MIR（最大增量反应活性）法计算了各企业排放VOCs对臭氧生成的贡献.结果表明:OVOCs（含氧挥发性有机物）和芳香烃是专项化学品制造行业的VOCs特征组分,OVOCs与芳香烃质量分数之和为65.0%~100.0%;8家企业排放的VOCs中质量分数最高的物种均为OVOCs,w（OVOCs）为55.8%~99.9%.异丙醇、四氢呋喃、丙酮、乙酸乙酯等OVOCs及苯、甲苯等芳香烃是专项化学品制造行业的特征物种.10家企业排放VOCs的OFP（臭氧生成潜势）为1.9~933.5 mg/m 3,OVOCs和芳香烃是专项化学品制造企业的主要活性组分,累计对OFP的贡献率在80.1%~100.0%之间.异丙醇、四氢呋喃、丙酮、乙酸乙酯、甲基异丁基酮、苯和甲苯等是专项化学品制造行业的关键活性物种.研究显示,专项化学品制造行业VOCs污染治理应重点控制OVOCs和芳香烃.      

多级串联表面流库塘-湿地净化农田径流效果评价

农田径流已成为湖泊流域非点源污染治理的主要制约因素.为研究多级串联表面流库塘-湿地中各级表面流湿地对洱海流域农田径流水体的净化效果,以大理市喜洲镇美坝村新建的多级串联表面流库塘-湿地为研究对象,跟踪监测其各级表面流湿地进、出水中ρ（TN）、ρ（NO₃--N）和ρ（TP）,分析水质净化效果及营养盐质量浓度沿程变化规律.结果表明:①多级串联表面流库塘-湿地出水ρ（TN）、ρ（NO₃--N）和ρ（TP）平均值分别为1.77、1.18和0.05 mg/L,低于GB 3838—2002《地表水环境质量标准》中Ⅴ类标准限值,TN、NO₃--N和TP去除率分别为57.75%、65.54%和67.43%.②农田径流在经过沉淀池、一级和二级表面流湿地后,对TN、NO₃--N和TP的去除率已分别达45.35%、52.21%和50.59%,且二级表面流湿地中出水ρ（TN）、ρ（NO₃--N）和ρ（TP）分别为2.36、1.69和0.06 mg/L,已达到较好的出水水质.③氮、磷营养盐质量浓度沿程削减模型拟合结果表明,指数削减模型较适宜表征TN、NO₃--N在多级串联表面流库塘-湿地中的沿程削减过程,而TP的最佳削减模型为线性削减模型.研究显示,多级串联表面流库塘-湿地对农田径流具有较好的净化效果,其对营养盐净化作用主要体现在前两级表面流湿地.      

Thiocyanate-induced labilization of schwertmannite: Impacts and mechanisms

Schwertmannite is an amorphous iron(III)-oxyhydroxysulfate that forms in acid mine drainage(AMD) environments. The characteristic of high heavy metal adsorption capability makes schwertmannite a potentially useful, environmentally friendly material in wastewater treatment. Unstable schwertmannite is prone to recrystallization.Understanding the mechanisms that induce schwertmannite labilization and affect its capacity to remove heavy metals are of great environmental and geochemical significance.Thiocyanate(SCNˉ) is a hazardous pseudohalide that is also normally found in AMD.However, little is known about the impact of Fe(III)-binding ligand SCNˉ on schwertmannite stability and its subsequent capacity to bind trace elements. Here, we investigated the adsorption of SCNˉ on schwertmannite and subsequent mineral transformation to characterize this little-known process. The appearance of Fe2+indicated that the interactions between schwertmannite and SCNˉ may involve complexation and reduction reactions. Results showed that the majority of the adsorbed-SCNˉ was immobilized on schwertmannite during the 60-days transformation. The transformation rates of schwertmannite increased with increasing concentrations of SCNˉ. Goethite was detected as the dominant transformation product with or without SCNˉ. The mechanisms of SCNˉ-promoted dissolution of schwertmannite can be described as follows:(1) formation of Fe(III)–NCS complexes on the schwertmannite surface and in solution, a process which increases the reactivity of solid phase Fe(III);(2) the extraction of Fe(III) from schwertmannite by SCNˉ and subsequent schwertmannite dissolution; and(3) the formation of secondary minerals from extracted Fe(III). These findings may improve AMD treatment strategies and provide insight into the use and potential reuse of schwertmannite as a trace element sorbent.     

Facile synthesis of graphitic carbon-nitride supported antimony-doped tin oxide nanocomposite and its application for the adsorption of volatile organic compounds

Antimony-doped tin oxide(ATO) nanoparticles with an average size of ～ 6 nm were prepared by co-precipitation and subsequent heat treatment. Graphitic carbon nitride(g-CN)/ATO hybrid nanocomposite was designed by the combination of thermally synthesized g-CN and ATO nanoparticles by ultrasonication. The materials were characterized using N2 adsorption/desorption(BET), X-ray diffraction(XRD), scanning electron microscopy(SEM), energy dispersive spectroscopy(EDS), transmission electron microscopy(TEM) and Fourier transform infrared spectroscopy(FTIR). A mixture of five volatile organic compounds(VOCs, chloroform, benzene, toluene, xylene and styrene) was used to compare the adsorption capacity of the samples. The adsorption capacity of ATO nanoparticles was improved by the addition of g-CN. Experimental data showed that, among the five VOCs,chloroform was the least adsorbed, regardless of the samples. The g-CN/ATO showed nearly three times greater adsorption capacity for the VOC mixture than pure ATO. The unchanged efficiency of VOC adsorption during cyclic use demonstrated the completely reversible adsorption and desorption behavior of the nanocomposite at room conditions. This economically and environmentally friendly material can be a practical solution for outdoor and indoor VOC removal.     

Vertical response of microbial community and degrading genes to petroleum hydrocarbon contamination in saline alkaline soil

A column microcosm was conducted by amending crude oil into Dagang Oilfield soil to simulate the bioremediation process. The dynamic change of microbial communities and metabolic genes in vertical depth soil from 0 to 80 cm were characterized to evaluate the petroleum degradation potential of indigenous microorganism. The influence of environmental variables on the microbial responds to petroleum contamination were analyzed. Degradation extent of 42.45% of n-alkanes(C8–C40) and 34.61% of 16ΣPAH were reached after 22 weeks. Relative abundance of alkB, nah, and phe gene showed about 10-fold increment in different depth of soil layers. Result of HTS profiles demonstrated that Pseudomonas, Marinobacter and Lactococcus were the major petroleum-degrading bacteria in0–30 and 30–60 cm depth of soils. Fusarium and Aspergillus were the dominant oil-degrading fungi in the 0–60 cm depth of soils. In 60–80 cm deep soil, anaerobic bacteria such as Bacteroidetes, Lactococcus, and Alcanivorax played important roles in petroleum degradation.Redundancy analysis(RDA) and correlation analysis demonstrated that petroleum hydrocarbons(PHs) as well as soil salinity, clay content, and anaerobic conditions were the dominant effect factors on microbial community compositions in 0–30, 30–60, and 60–80 cm depth of soils, respectively.