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.     

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.     

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.     

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...     

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.     

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。     

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     

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.     

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...     

SO_2与CeO_2超细颗粒非均相反应产物的细胞毒性效应

大气二次细颗粒物(secondary fine particulate matters,SFPMs)是我国城市大气PM_(2.5)的主要组成部分。然而由于PM_(2.5)组成成份复杂,其毒性产生的来源并不明确。在本研究中,我们以二氧化铈(CeO_2)超细颗粒物(UFPs)为大气细矿物质颗粒模型,研究了SO_2气体在模拟大气环境中,如湿度(RH)、紫外光照(UV)和NO_2存在条件下,在CeO_2UFPs界面经多相反应生成的二次无机细颗粒物的性质及与细胞毒性的构效关系。实验通过实时高通量细胞分析系统,实时观察了CeO_2-SFPMs暴露对小鼠单核巨噬细胞(RAW264.7)增殖的影响;并进一步检测了CeO_2-SFPMs对细胞膜通透性和细胞凋亡的影响。结果表明,SO_2与CeO_2UFPs作用后可转化为硫酸盐,在有NO_2存在下转化更为明显。CeO_2-SFPMs对细胞毒性效应与其生成的环境条件相关,并具有时间效应性。RAW264.7细胞暴露于CeO_2-SFPMs 8 h,细胞增殖无明显变化;暴露8~25 h后,CeO_2-SFPMs对细胞增殖的抑制率随CeO_2@CeO_2+SO_2@CeO_2+SO_2+RH≈@CeO_2+SO_2+RH+UV@CeO_2+SO_2+RH+NO_2的顺序显著升高。CeO_2-SFPMs对Raw264.7细胞膜通透性和细胞凋亡的影响研究也证明CeO_2-SFPMs@CeO_2+SO_2+RH+NO_2产生的细胞毒性最明显。     

SO2和NO2胁迫对红花荷等植物光合生理影响及抗性评价

为探讨红花荷(Rhodoleia championii)等12种园林植物抗SO2和NO2污染能力,以1～2年生实生苗为材料,通过人工气候室的盆栽实验,研究不同SO2和NO2混合气体胁迫对园林植物苗木光合参数和相对叶绿素含量的影响,并利用隶属函数法及系统聚类分析法对其抗SO2和NO2污染能力进行了综合评价。结果表明,植物叶片净光合速率、气孔导度、蒸腾速率和相对叶绿素含量基本上随着SO2和NO2胁迫的加剧而逐渐降低,但水分利用效率受净光合速率和蒸腾速率变化的影响规律不明显。综合隶属函数和聚类分析可知,红花荷和红千层(Callistemon rigidus)抗污染能力强,杜鹃红山茶(Camellia azalea)和粉红羊蹄甲(Bauhinia blakeana)抗污染能力较强,红花银桦(Grevillea robusta)和无忧树(Saraca divespierre)抗污染能力中等,大叶紫薇(Lagerstroemia speciosa)、金花风铃木(Tabebuia chrysantha)和腊肠树(Cassia fistula)抗污染能力较弱,而本地火焰木(Spathodea nilotica)、复羽叶栾树(Koelreuteria bipinnata)和樱花(Prunus serrulata)抗污染能力弱。研究结果为火电厂、陶瓷厂、钢铁厂、石化厂等重度酸污染地区植物选择提供参考。     

Utilizing transparent and conductive SnO2 as electron mediator to enhance the photocatalytic performance of Z-scheme Si-SnO2-TiOx

• A novel Z-scheme Si-SnO₂-TiO_x with SnO₂ as electron mediator is first constructed. • Transparent and conductive SnO₂ can pass light through and promote charge transport. • V_O from SnO₂ and TiO_x improve photoelectrochemical performances. • Efficient photocatalytic degradations originate from the Z scheme construction. Z-scheme photocatalysts, with strong redox ability, have a great potential for pollutants degradation. However, it is challenging to construct efficient Z-scheme photocatalysts because of their poor interfacial charge separation. Herein, by employing transparent and conductive SnO₂ as electron mediator to pass light through and promote interfacial charge transportation, a novel Z-scheme photocatalyst Si-SnO₂-TiO_{x (1<x<2)} was constructed. The Z-scheme photocatalyst displayed an order of magnitude higher photocurrent density and a 4-fold increase in open-circuit potential compared to those of Si. Moreover, the onset potential shifted negatively for approximately 2.2 V. Benefiting from these advantages, this Z-scheme Si-SnO₂-TiO_x exhibited efficient photocatalytic performance toward phenol degradation and mineralization. 75% of the phenol was degraded without bias potential and 70% of the TOC was removed during phenol degradation. Other typical pollutants such as bisphenol A and atrazine could also be degraded without bias potential. Introducing a transparent and conductive electron mediator to construct Z-scheme photocatalyst gives a new sight to the improvement of photocatalytic performance in Z scheme.     

Ultra-small UiO-66-NH2 nanoparticles immobilized on g-C3N4 nanosheets for enhanced catalytic activity

UiO-66-NH₂,an important metal-organic framework,is usually synthesized by solvothermal method and the particle size is generally larger than 200 nm,which limits its catalytic applications in chemical reactions.It is very meaningful to produce UiO-66-NH₂ nanoparticles with ultrasmall size,but remains challenging.Herein,we synthesized UiO-66-NH₂ nanoparticles in size of 8-15 nm that are immobilized on g-C₃N₄ nanosheets.Compared with the UiO-66...     

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...     

过氧化氢和一氧化氮在小球藻抗阿特拉津胁迫中的作用

过氧化氢(H_2O_2)和一氧化氮(NO)作为信号分子,可调节植物生长、发育以及应对外源性胁迫。利用过氧化氢酶(CAT)以及NO清除剂(PTIO),研究了除草剂阿特拉津(atrazine,100μg·L~(-1))影响小球藻生长的机理,并分析内源性H_2O_2和NO在小球藻抗除草剂胁迫中的作用。研究结果表明,阿特拉津在诱发小球藻细胞死亡的过程中,不同程度促发了H_2O_2和NO生成;外源CAT可通过清除H_2O_2和诱导NO来缓解阿特拉津对小球藻的生长抑制;PTIO与阿特拉津的联合实验进一步证实,小球藻体内的NO诱导与H_2O_2的爆发无关,它们之间的合成没有相关性。因此,除草剂阿特拉津主要通过诱导小球藻体内的H_2O_2爆发来破坏藻细胞,抑制其生长,与NO的信号传递无关。     

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.     

Enhancing O2 electroreduction to H2O on Ag/MnO2-CHNTs by boosting a four-electron catalytic pathway

A fundamental question in the oxygen reduction reaction(ORR)is how to rationally control the electrocatalytic selectivity for opening a four-electron reaction pathway. However, it still lacks direct experimental evidence to understand the reaction mechanism. This work unravels that Ag nanoparticles and carbonizing halloysite nanotubes(CHNTs) can trigger the construction of oxygen defects in the MnO₂, which contribute to the generation of active sites. The Ag/MnO₂-CHNTs deli...     

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.     

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.     

Zn-TiO2纳米管的光催化活性

采用水热合成-浸渍法制备锌掺杂TiO2纳米管(Zn-TiO2纳米管),透射电镜照片显示Zn-TiO2纳米管为两端开口形貌均一的中空管状结构,管径约6～8 nm,壁厚约1 nm,长度约50～200 nm。研究了Zn-TiO2纳米管对甲基橙的光催化性能,结果表明:掺杂适量锌提高了TiO2纳米管对甲基橙的光催化降解性能,0.4%Zn-TiO2纳米管的光催化性能最佳。同时还探讨了Zn-TiO2纳米管用量和初始pH值等因素对光催化降解甲基橙的影响,结果显示Zn-TiO2纳米管能有效地降解甲基橙。随着光催化反应进行,CODCr去除率和脱色率变化规律不完全相同,可能是由于芳基和烷基降解速率不同所致。