SO2-4/TiO2对SO2-C7H16-TiO2复相光化学反应的影响

研究了TiO2与SO2,C7H16复相光化学反应的光催化活性.在SO2-C7H16-O2-TiO2光催化反应过程中,TiO2表面可形成SO2-4/TiO2结构,它的存在可提高庚烷的光催化氧化速率,利用IR和XPS研究了反应过程中TiO2表面形成的SO2-4/TiO2结构.     

KMnO4/H2SO4引发制备淀粉改性絮凝剂的研究

以高锰酸钾为引发剂,制备淀粉-丙烯酰胺接枝共聚物.研究酸浓度、引发剂浓度、单体浓度、温度和加料方式对接枝反应的影响.结果表明,少量KMnO4(0.45mmol·l-1)和H2SO4(0.8mmol·l-1)可有效引发淀粉-丙烯酰胺接枝共聚反应,接枝效率达到90%以上,分子量大大提高,对高岭土的絮凝效果较好.     

Heterostructuring noble-metal-free 1T' phase MoS2 with g-C3N4 hollow nanocages to improve the photocatalytic H2 evolution activity

In this work,we report the preparation of 1T’-MoS₂/g-C₃N₄ nanocage(NC) heterostructure by loading 2D semi-metal noble-metal-free 1T’-MoS₂ on the g-C₃N₄ nanocages(NCs).DFT calculation and experimental data have shown that the 1T’-MoS₂/g-C₃N₄ NC heterostructure has a stronger light absorption capacity and larger specific surface area than pure g-C₃N₄ NCs and g-C₃N     

3D flower-like mesoporous Bi4O5I2/MoS2 Z-scheme heterojunction with optimized photothermal-photocatalytic performance

3D flower-like hierarchical mesoporous Bi₄O₅I₂/MoS₂ Z-scheme layered heterojunction photocatalyst was fabricated by oil bath and hydrothermal methods. The heterojunction with narrow band gap of ～1.95 eV extended the photoresponse to near-infrared region, which showed obvious photothermal effect due to the introduction of MoS₂ with broad spectrum response. MoS₂ nanosheets were anchored onto the surface of flower-like hierarchical m...     

Sunlight-controlled CO2 separation resulting from a biomass-based CO2 absorber

Renewable solid sorbents for CO₂ capture and storage have shown great potentials for the sake of gaseous separation, tail gas treatment,environmental regulation and climate governance. However, current existed preparation and reusability of solid sorbents are generally subject to high energy consumption and complicated procedure. Herein, a light-controlled CO₂ separation system with high working temperature resulting from natural sawdust combined with polyethyleneimine is f...     

大气CO2、CH4、CO高精度观测混合标气配制方法

高精度、高准确度的大气CO2、CH4、CO浓度观测需使用以干洁大气为底气的标气.标气中水汽含量及CO2的δ13C对基于光学原理的观测系统有不可忽视的影响.本研究利用自组装的混合标气配制系统,以环境大气为底气,并通过添加高浓度气体或利用吸附剂吸附,调节目标物种浓度.CO2和CO吸附效率分别达99.7%和99.8%,标气水汽含量小于3.7×10-6(物质的量分数,下同),可配制不同浓度范围的CO2、CH4、CO混合标气.在青海瓦里关全球大气本底站配制环境大气浓度范围的标气,CO2、CH4、CO实际配制浓度同目标浓度的偏差小于10×10-6、30×10-9、30×10-9,CO2中δ13C同实际大气接近.本方法配制的标气已应用于我国本底站大气CO2、CH4、CO高精度观测,符合世界气象组织/全球大气观测(WMO/GAW)质量要求.     

Simultaneous removal of NOx and chlorobenzene on V2O5/TiO2 granular catalyst: Kinetic study and performance prediction

• A V₂O₅/TiO₂ granular catalyst for simultaneous removal of NO and chlorobenzene. • Catalyst synthesized by vanadyl acetylacetonate showed good activity and stability. • The kinetic model was established and the synergetic activity was predicted. • Both chlorobenzene oxidation and SCR of NO follow pseudo-first-order kinetics. • The work is of much value to design of multi-pollutants emission control system. The synergetic abatement of multi-pollutants is one of the development trends of flue gas pollution control technology, which is still in the initial stage and facing many challenges. We developed a V₂O₅/TiO₂ granular catalyst and established the kinetic model for the simultaneous removal of NO and chlorobenzene (i.e., an important precursor of dioxins). The granular catalyst synthesized using vanadyl acetylacetonate precursor showed good synergistic catalytic performance and stability. Although the SCR reaction of NO and the oxidation reaction of chlorobenzene mutually inhibited, the reaction order of each reaction was not considerably affected, and the pseudo-first-order reaction kinetics was still followed. The performance prediction of this work is of much value to the understanding and reasonable design of a catalytic system for multi-pollutants (i.e., NO and dioxins) emission control.     

包膜尿素对水田土壤排放NH3、NOx、CO2影响的研究

为了研究包膜尿素对水田土壤排放NH3、NOx和CO2的影响,采用水稻盆栽的方法,探讨了在水稻不同生育期内不同种类包膜尿素对水田土壤排放NH3、NOx和CO2的影响。结果表明,包膜尿素处理对水田土壤排放NH3、NOx和CO2均具有抑制作用,与普通尿素相比,包膜尿素LP40、LPSS、BB、SC60 NH3的挥发总量降低了5.4%~19.3%,NOx的挥发总量降低了8.1%~23.4%,CO2的挥发总量降低了1.6%~13.0%;施用包膜尿素能够抑制水田土壤NH3、NOx和CO2的排放。     

Mass concentrations and temporal profiles of PM10, PM2.5 and PM1 near major urban roads in Beijing

Mass concentrations of PM₁₀, PM_2.5 and PM₁ were measured near major roads in Beijing during six periods: summer and winter of 2001, winter of 2007, and periods before, during and after the 2008 Beijing Olympic Games. Since the control efforts for motor vehicles helped offset the increase of emissions from the rapid growth of vehicles, the averaged PM_2.5 concentrations at roadsides during the sampling period between 2001 and 2008 fluctuated over a relatively small range. With the implementation of temporary traffic control measures during the Olympics, a clear “V” shaped curve showing the concentrations of particulate matter and other gaseous air pollutants at roadsides over time was identified. The average concentrations of PM₁₀, PM_2.5, CO and NO decreased by 31.2%, 46.3%, 32.3% and 35.4%, respectively, from June to August; this was followed by a rebound of all air pollutants in December 2008. Daily PM₁₀ concentrations near major roads exceeded the National Ambient Air Quality Standard (Grade II) for 61.2% of the days in the non-Olympic periods, while only for 12.5% during the Olympics. The mean ratio of PM_2.5/PM₁₀ near major roads remained relatively stable at 0.55 (±0.108) on non-Olympic days. The ratio decreased to 0.48 (±0.099) during the Olympics due to a greater decline in fine particles than in coarse-mode PM. The ratios PM₁/PM_2.5 fluctuated over a wide range and were statistically different from each other during the sampling periods. The average ratios of PM₁/PM_2.5 on non-Olympic days were 0.71.     

Catalytic ozonation of organic compounds in water over the catalyst of RuO2/ZrO2-CeO2

This research investigates the performances of RuO₂/ZrO₂-CeO₂ in catalytic ozonation for water treatment. The results show that RuO₂/ZrO₂-CeO₂ was active for the catalytic ozonation of oxalic acid and possessed higher stability than RuO₂/Al₂O₃ and Ru/AC. In the catalytic ozonation of dimethyl phthalate (DMP), RuO₂/ZrO₂-CeO₂ did not enhance the DMP degradation rate but significantly improved the total organic carbon (TOC) removal rate. The TOC removal in catalytic ozonation was 56% more than that in noncatalytic ozonation. However this does not mean the catalyst was very active because the contribution of catalysis to the overall TOC removal was only 30%. The adsorption of the intermediates on RuO₂/ZrO₂-CeO₂ played an important role on the overall TOC removal while the adsorption of DMP on it was negligible. This adsorption difference was due to their different ozonation rates. In the catalytic ozonation of disinfection byproduct precursors with RuO₂/ZrO₂-CeO₂, the reductions of the haloacetic acid and trihalomethane formation potentials (HAAFPs and THMFPs) for the natural water samples were 38%–57% and 50%–64%, respectively. The catalyst significantly promoted the reduction of HAAFPs but insignificantly improved the reduction of THMFPs as ozone reacts fast with the THMs precursors. These results illustrate the good promise of RuO₂/ZrO₂-CeO₂ in catalytic ozonation for water treatment.     

Self-assembly synthesis of phosphorus-doped tubular g-C3N4/Ti3C2 MXene Schottky junction for boosting photocatalytic hydrogen evolution

Establishing highly effective charge transfer channels in carbon nitride(g-C₃N₄) to enhance its photocatalytic activity is still a challenging issue. Herein, the delaminated 2D Ti₃C₂ MXene nanosheets were employed to decorate the P-doped tubular g-C₃N₄(PTCN)for engineering 1D/2D Schottky heterojunction(PTCN/TC) through electrostatic self-assembly. The optimized PTCN/TC exhibited the highest hydrogen evolution rate(565 μmol h^-...     

Catalytic oxidation of CO over Pt/Fe3O4 catalysts: Tuning O2 activation and CO adsorption

• Strong metal-support interaction exists on Pt/Fe₃O₄ catalysts. • Pt metal particles facilitate the formation of oxygen vacancies on Fe₃O₄. • Fe₃O₄ supports enhance the strength of CO adsorption on Pt metal particles. The self-inhibition behavior due to CO poisoning on Pt metal particles strongly impairs the performance of CO oxidation. It is an effective method to use reducible metal oxides for supporting Pt metal particles to avoid self-inhibition and to improve catalytic performance. In this work, we used in situ reductions of chloroplatinic acid on commercial Fe₃O₄ powder to prepare heterogeneous-structured Pt/Fe₃O₄ catalysts in the solution of ethylene glycol. The heterogeneous Pt/Fe₃O₄ catalysts achieved a better catalytic performance of CO oxidation compared with the Fe₃O₄ powder. The temperatures of 50% and 90% CO conversion were achieved above 260°C and 290°C at Pt/Fe₃O₄, respectively. However, they are accomplished on Fe₃O₄ at temperatures higher than 310°C. XRD, XPS, and H₂-TPR results confirmed that the metallic Pt atoms have a strong synergistic interaction with the Fe₃O₄ supports. TGA results and transient DRIFTS results proved that the Pt metal particles facilitate the release of lattice oxygen and the formation of oxygen vacancies on Fe₃O₄. The combined results of O₂-TPD and DRIFTS indicated that the activation step of oxygen molecules at surface oxygen vacancies could potentially be the rate-determining step of the catalytic CO oxidation at Pt/Fe₃O₄ catalysts. The reaction pathway involves a Pt-assisted Mars-van Krevelen (MvK) mechanism.     

Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation over an urchin-like oxygen-doped MoS2/ZnIn2S4 composite

● An urchin-like OMS/ZIS composite was fabricated by a facile solvothermal method. ● The OMS/ZIS exhibits superior photocatalytic H₂ evolution for organics degradation. ● A probable mechanism of dual-functional photocatalysis was proposed in detail. ● This work provides an inspiration for rational design of dual-functional catalysts. Achieving hydrogen production and simultaneous decomposition of organic pollutants through dual-functional photocatalytic reactions has received increasing attention due to the environmentally friendly and cost-effective characteristics of this approach. In this work, an urchin-like oxygen-doped MoS₂/ZnIn₂S₄ (OMS/ZIS) composite was fabricated for the first time using a simple solvothermal method. The unique microstructure with abundant active sites and fast charge transfer channels further shortened the charge migration distance and compressed carrier recombination. The obtained composite exhibited an efficient H₂ evolution reaction rate of 12.8 mmol/g/h under visible light, which was nearly times higher than pristine ZnIn₂S₄, and the apparent quantum efficiency was 14.9% (420 nm). The results of the simultaneous photocatalytic H₂ evolution and organic pollutant decomposition test were satisfactory, resulting in decomposition efficiencies of resorcinol, tetracycline, and bisphenol A that reached 41.5%, 63.5%, and 53.0% after 4 h, respectively, and the highest H₂ evolution rate was 672.7 μmol/g/h for bisphenol A. Furthermore, natural organic matter (NOM) abundantly found in actual water was adopted as an electron donor for H production under simulated sunlight irradiation, indicating the promising practicability of simultaneous hydrogen evolution and NOM decomposition. Moreover, the mechanisms of the dual-purpose photocatalytic reactions, as well as the synergistic effect between the molecular structures of the organic pollutants and the corresponding adsorption behavior on the photocatalyst surface were illustrated in detail. These obtained results may serve as an inspiration for the rational design of highly efficient, dual-functional photocatalysts in the future.     

Visible-light-driven heterostructured g-C3N4/Bi-TiO2 floating photocatalyst with enhanced charge carrier separation for photocatalytic inactivation of Microcystis aeruginosa

• Bi doping in TiO₂ enhanced the separation of photo-generated electron-hole. • The performance of photocatalytic degradation of MC-LR was improved. • Coexisting substances have no influence on algal removal performance. • The key reactive oxygen species were h⁺ and ^•OH in the photocatalytic process. The increase in occurrence and severity of cyanobacteria blooms is causing increasing concern; moreover, human and animal health is affected by the toxic effects of Microcystin-LR released into the water. In this paper, a floating photocatalyst for the photocatalytic inactivation of the harmful algae Microcystis aeruginosa (M. aeruginosa) was prepared using a simple sol-gel method, i.e., coating g-C₃N₄ coupled with Bi-doped TiO₂ on Al₂O₃-modified expanded perlite (CBTA for short). The impact of different molar ratios of Bi/Ti on CBTA was considered. The results indicated that Bi doping in TiO₂ inhibited photogenerated electron-hole pair recombination. With 6 h of visible light illumination, 75.9% of M. aeruginosa (initial concentration= 2.7 × 10⁶ cells/L) and 83.7% of Microcystin-LR (initial concentration= 100 μg/L) could be removed with the addition of 2 g/L CBTA-1% (i.e., Bi/Ti molar ratio= 1%). The key reactive oxygen species (ROSs) in the photocatalytic inactivation process are h⁺ and ^•OH. The induction of the Bi⁴⁺/Bi³⁺ species by the incorporation of Bi could narrow the bandgap of TiO₂, trap electrons, and enhance the stability of CBTA-1% in the solutions with coexisting environmental substances.     

Oxidation and biotoxicity assessment of microcystin-LR using different AOPs based on UV,O3 and H2O2

MC-LR removal performances under different AOPs were compared systematically. Higher removal efficiency and synergistic effects were obtained by combined process. The acute biotoxicity raised in different degrees after oxidation. Microcystin-LR attracts attention due to its high toxicity, high concentration and high frequency. The removal characteristics of UV/H₂O₂ and O₃/H₂O₂ advanced oxidation processes and their individual process for MC-LR were investigated and compared in this study. Both the removal efficiencies and rates of MC-LR as well as the biotoxicity of degradation products was analyzed. Results showed that the UV/H₂O₂ process and O₃/H₂O₂ were effective methods to remove MC-LR from water, and they two performed better than UV-, O₃-, H₂O₂-alone processes under the same conditions. The effects of UV intensity, H₂O₂ concentration and O₃ concentration on the removal performance were explored. The synergistic effects between UV and H₂O₂, O₃ and H₂O₂ were observed. UV dosage of 1800 mJ·cm⁻² was required to remove 90% of 100 mg·L⁻¹ MC-LR, which amount significantly decreased to 500 mJ·cm⁻² when 1.7 mg·L⁻¹ H₂O₂ was added. 0.25 mg·L⁻¹ O₃, or 0.125 mg·L⁻¹ O₃ with 1.7 mg·L⁻¹ H₂O₂ was needed to reach 90% removal efficiency. Furthermore, the biotoxicity results about these UV/H₂O₂, O₃/H₂O₂ and O₃-alone processes all present rising trends with oxidation degree of MC-LR. Biotoxicity of solution, equivalent to 0.01 mg·L⁻¹ Zn²⁺, raised to 0.05 mg·L⁻¹ Zn²⁺ after UV/H₂O₂ or O₃/H₂O₂ reaction. This phenomenon may be attributed to the aldehydes and ketones with small molecular weight generated during reaction. Advice about the selection of MC-LR removal methods in real cases was provided.     

One-pot hydrothermal fabrication of BiVO4/Fe3O4/rGO composite photocatalyst for the simulated solar light-driven degradation of Rhodamine B

• BiVO₄/Fe₃O₄/rGO has excellent photocatalytic activity under solar light radiation. • It can be easily separated and collected from water in an external magnetic field. • BiVO₄/Fe₃O₄/0.5% rGO exhibited the highest RhB removal efficiency of over 99%. • Hole (h⁺) and superoxide radical (O₂^•−) dominate RhB photo-decomposition process. • The reusability of this composite was confirmed by five successive recycling runs. Fabrication of easily recyclable photocatalyst with excellent photocatalytic activity for degradation of organic pollutants in wastewater is highly desirable for practical application. In this study, a novel ternary magnetic photocatalyst BiVO₄/Fe₃O₄/reduced graphene oxide (BiVO₄/Fe₃O₄/rGO) was synthesized via a facile hydrothermal strategy. The BiVO₄/Fe₃O₄ with 0.5 wt% of rGO (BiVO₄/Fe₃O₄/0.5% rGO) exhibited superior activity, degrading greater than 99% Rhodamine B (RhB) after 120 min solar light radiation. The surface morphology and chemical composition of BiVO₄/Fe₃O₄/rGO were studied by scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, UV–visible diffuse reflectance spectroscopy, Fourier transform infrared spectroscopy, and Raman spectroscopy. The free radicals scavenging experiments demonstrated that hole (h⁺) and superoxide radical (O₂^•−) were the dominant species for RhB degradation over BiVO₄/Fe₃O₄/rGO under solar light. The reusability of this composite catalyst was also investigated after five successive runs under an external magnetic field. The BiVO₄/Fe₃O₄/rGO composite was easily separated, and the recycled catalyst retained high photocatalytic activity. This study demonstrates that catalyst BiVO₄/Fe₃O₄/rGO possessed high dye removal efficiency in water treatment with excellent recyclability from water after use. The current study provides a possibility for more practical and sustainable photocatalytic process.     

A2型高粱细胞质雄性不育系与其保持系的胞质DNA和核DNA差异

以高粱细胞质雄性不育系A2V4（A）及其保持系V4（B）的总DNA为模板,对184个随机引物进行筛选,找到6个其RAPD扩增产物在A／B间存在稳定差异的引物,将该6个引物同时扩增A／B的总DNA、线粒线DNA（mtDNA）及叶绿体DNA（cpDNA）,以总DNA为模板时得到12个扩增片段,以mtDNA为模板时得到4个,以cpDNA为板时得到11个,结果分析表明,在这些扩增片段中,有7个仅仅出现在以胞质DNA为模板的扩增中,有5个在以总NDA和胞质DNA为模板时同时出现,即认为这12个片段来自胞质DNA,另有7个片段,在以胞质DNA为模板时未出现,而是仅仅出现在以总DNA为模板的扩增中,认为是来自核DNA,来自核DNA的7个扩增片段中,有5个来自保持系,有2个来自不育系,这表明,不育系与保持系在核DNA上存在差异,对A／B核DNA在CMS中的重要性及研究对策进行了讨论。     

六铝酸盐负载CuO催化还原NO性能

采用共沉淀法制备了LaAl12O19六铝酸盐载体,采用等体积浸渍法制备了不同负载量的CuO/LaAl12O19催化剂,并对其进行了XRD、H2-TPR和BET表征,考察了催化剂对CH4选择催化还原NO的性能.结果表明,CuO的负载并未改变六铝酸盐载体的结构,Cu在载体上以Cu2+的形式存在,活性组分CuO与载体LaAl12O19之间存在协同作用;CuO/LaAl12O19催化剂对CH4选择催化还原NO表现出良好活性,所制备的催化剂均能使NO的转化率达到99%;其中负载量为1.0 wt%的CuO/LaAl12O19催化剂的活性最好,完全反应温度T99%为560℃,且在80 h稳定性试验中表现出了良好的高温活性和热稳定性.     

Fe2O3-CeO2-Bi2O3/γ-Al2O3 catalyst in the catalytic wet air oxidation (CWAO) of cationic red GTL under mild reaction conditions

Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃, an environmental friendly material, was investigated. The catalyst exhibited good catalytic performance in the CWAO of cationic red GTL. The apparent activation energy for the reaction was 79 kJ·mol⁻¹. HO₂· and O₂·⁻ appeared as the main reactive species in the reaction. The Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃ catalyst, a novel environmental-friendly material, was used to investigate the catalytic wet air oxidation (CWAO) of cationic red GTL under mild operating conditions in a batch reactor. The catalyst was prepared by wet impregnation, and characterized by special surface area (BET measurement), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃ catalyst exhibited good catalytic activity and stability in the CWAO under atmosphere pressure. The effect of the reaction conditions (catalyst loading, degradation temperature, solution concentration and initial solution pH value) was studied. The result showed that the decolorization efficiency of cationic red GTL was improved with increasing the initial solution pH value and the degradation temperature. The apparent activation energy for the reaction was 79 kJ·mol⁻¹. Hydroperoxy radicals (HO₂·) and superoxide radicals (O₂⁻·) appeared as the main reactive species upon the CWAO of cationic red GTL.     

Influence of MnOx deposition on TiO2 nanotube arrays for electrooxidation

TiO₂ has demonstrated outstanding performance in electrochemical advanced oxidation processes(EAOPs) due to its structural stability and high oxygen overpotential.However,there is still much room for improving its electrochemical activity.Herein,narrow bandgap manganese oxide(MnOx) was composited with TiO₂ nanotube arrays(TiO₂ NTAs) that in-situ oxidized on porous Ti sponge,forming the MnO_x-TiO₂ NTAs anode.XANES and XPS analysis further prov...