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.     

Chemical poison and regeneration of SCR catalysts for NOx removal from stationary sources

Selective catalytic reduction (SCR) of NO_x with NH₃ is an effective technique to remove NO_x from stationary sources, such as coal-fired power plant and industrial boilers. Some of elements in the fly ash deactivate the catalyst due to strong chemisorptions on the active sites. The poisons may act by simply blocking active sites or alter the adsorption behaviors of reactants and products by an electronic interaction. This review is mainly focused on the chemical poisoning on V₂O₅-based catalysts, environmental-benign catalysts and low temperature catalysts. Several common poisons including alkali/alkaline earth metals, SO₂ and heavy metals etc. are referred and their poisoning mechanisms on catalysts are discussed. The regeneration methods of poisoned catalysts and the development of poison-resistance catalysts are also compared and analyzed. Finally, future research directions in developing poisoning resistance catalysts and facile efficient regeneration methods for SCR catalysts are proposed.     

Improvement of water resistance by Fe2O3/TiO2 photoelectrocatalysts for formaldehyde removal: experimental and theoretical investigation

Environmental Science and Pollution Research - TiO2-based photocatalysts are a potential technology for removing indoor formaldehyde (CHOH) owing to their strong photooxidation ability. However,...     

共存钙离子对镧铝改性稻壳生物炭除磷性能的影响

本研究利用稻壳制备高介孔率生物炭,然后用共沉淀法负载金属La、Al,制得镧铝改性稻壳基生物炭吸附剂.通过控制反应时间、磷浓度、共存阴离子、初始pH等条件,研究共存钙离子时对吸附剂除磷性能的影响.结果表明,La、Al在稻壳基生物炭上负载后呈无定型态;吸附剂的除磷过程符合伪二阶动力学模型和Langmuir模型,且Ca~(2+)的加入有利于提高磷的去除率,含Ca~(2+)体系的最终除磷效果是无Ca~(2+)时的2.6倍;含竞争阴离子时,Ca~(2+)的加入会使F~-对磷吸附的抑制作用减弱,使HCO_3~-对磷吸附的抑制作用略微增强;在pH值为2.0—8.0时,Ca~(2+)能提高改性生物炭的吸附容量,而pH8.0时主要是钙离子与磷酸盐的沉淀作用使体系中磷大量被去除.     

Chemical poison and regeneration of SCR catalysts for NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript> removal from stationary sources

Selective catalytic reduction (SCR) of NO _x with NH₃ is an effective technique to remove NO _x from stationary sources, such as coal-fired power plant and industrial boilers. Some of elements in the fly ash deactivate the catalyst due to strong chemisorptions on the active sites. The poisons may act by simply blocking active sites or alter the adsorption behaviors of reactants and products by an electronic interaction. This review is mainly focused on the chemical poisoning on V₂O₅-based catalysts, environmental-benign catalysts and low temperature catalysts. Several common poisons including alkali/alkaline earth metals, SO₂ and heavy metals etc. are referred and their poisoning mechanisms on catalysts are discussed. The regeneration methods of poisoned catalysts and the development of poison-resistance catalysts are also compared and analyzed. Finally, future research directions in developing poisoning resistance catalysts and facile efficient regeneration methods for SCR catalysts are proposed.     

营养盐与盐双重胁迫下水体中浮游细菌的响应

为阐释干旱地区内陆湖泊微生物群落对营养盐和盐双重胁迫的响应机制,针对干旱、半干旱地区许多湖泊水体受咸化与富营养化双重影响的特点,通过454高通量测序16S rRNA基因和多元统计分析,研究水体营养盐和盐的添加对细菌群落结构、多样性变化的影响. 结果表明,盐与营养盐的输入引起了水体中细菌群落组成和多样性的显著变化, 具体表现为:①随着盐度(以w计)的升高,α-变形菌纲(Alphaproteobacteria)的相对丰度显著增加,从对照处理的16.0%±4.6%增至SO(贫营养-盐水)处理的39.8%±18.1%;但会受到水体营养水平的制约. ②富营养水平下,微咸条件(盐度为1.5‰)有利于细菌类群丰富度的增加,BE-30(微咸-富营养处理培养30 d样品)的Shannon-Wiener多样性指数(4.62)显著高于FE-30(淡水-富营养处理培养30 d样品,2.08)和SE-30(高盐-富营养处理培养30 d样品,1.69);③高盐(盐度为3.0‰)条件下,随着水体中营养盐含量的增加,喜营养的嗜盐细菌类群大量繁殖(SE-30中无法分类的Comamonadaceae科的相对丰度达到69.3%),因而降低了水体中细菌群落的多样性. 研究显示,α-变形菌纲和无法分类的Comamonadaceae科对盐与营养盐的变化较为敏感,可作为干旱区湖泊咸化和富营养化过程的参考类群.      

模拟酸雨对土壤-辣椒系统中Hg的化学行为的影响

以桂林市典型的河流沉积沙土(穿山)和砂岩风化土(尧山)为供试土壤,在盆栽条件下种植辣椒(Capsicum annuum L.),设置不同土壤Hg水平,配制不同pH的模拟酸雨,研究土壤-蔬菜系统中Hg的化学行为.结果表明:不同浓度的土壤Hg处理对地上部分没有表现出明显的毒害作用,植株各部位Hg含量随土壤Hg含量的增加而升高,与对照相比,10 mg·kg-1 Hg处理的辣椒可食部位Hg含量是对照的2.4倍(0.031 mg·kg-1),是食品卫生质量标准(0.01 mg·kg-1)的3倍多.相同条件下穿山土壤处理的辣椒各部位Hg含量大于尧山土壤的处理.模拟酸雨与Hg的复合污染环境效应大于这两种污染物的单因素效应.模拟酸雨主要影响水溶态Hg、交换态Hg、腐殖酸络合态Hg,表现为随处理pH值的降低其分配系数增高.在处理pH = 3.5时影响到碳酸盐铁锰氧化物态Hg,有机物结合态Hg随酸雨pH降低略有减少趋势,对残渣态Hg没有明显影响.     

Chemical fingerprint and source apportionment of PM 2.5 in highly polluted events of southern Taiwan

To investigate the spatial distribution and diurnal variation of the chemical composition of PM2.5 pollution in an industrial city of southern Taiwan, 12-h PM2.5 was diurnally continuously collected simultaneously at the Kaoping Air Quality Zone (KAQZ) during one highly PM2.5-polluted episode. Water-soluble ions, metallic elements, carbonaceous contents, dicarboxylic acids, and anhydrosugars were analyzed to characterize the chemical fingerprint of PM2.5. Backward trajectory simulation and chemical mass balance (CMB) receptor modeling were applied to identify the potential sources of PM2.5 and their contributions. It showed that Chaozhou (rural area) accompanying the highest SORs and NORs suffered from the most severe PM2.5 pollution during the episode. Sulfate (SO42−) was probably formed by the atmospheric chemical reaction in the daytime, while NO3− processed at nighttime at the KAQZ. A homogeneous formation of NO3− occurred at Chaozhou. The concentrations of Zn, Pb, Fe, Cu, V, and Al, mainly emitted from anthropogenic sources, increased significantly at the KAQZ. The highest OC, SOC/OC, and DA/OCs at Daliao (industrial area) were attributed to the transformation of primary VOCs to secondary OC via photo-oxidation during the episode. Oxalic acid was mainly produced through photochemical reactions since a high correlation between oxalic acid and Ca2+ was observed at Nanzi (urban area) and Daliao during the episode. During the episode, PM2.5 mostly originated from local primary or secondary aerosol than long-range overseas transport. The dominant source was anthropogenic emissions, accounting for 67.1% and 70.4% of PM2.5 at Nanzi and Daliao, respectively. At Chaozhou, the contribution of anthropogenic emissions was the lowest (42.4%), but secondary aerosols had the highest contribution of 38.3% of PM2.5 among the three areas during the episode.     

浸渍活性炭脱除含硫气体研究进展

介绍了近年来国内外浸渍活性炭脱除含硫气体的研究进展。讨论了活性炭表面特性对脱硫的影响,并从改变孔径分布、孔容积,引入杂原子,改变表面pH和增大硫容量等方面进行了探讨。通过浸渍可以改善活性炭的孔径分布和表面化学环境,增大硫容量,提高催化性能和转化效率。目前研究的热点是新的制备活性炭的原料和新浸渍剂,指出目前该领域存在的问题是活性炭再生困难,再生后脱硫能力恢复较少。     

不锈钢酸洗过程中NOx的产生机制及控制

为降低奥氏体不锈钢混酸(HNO_3+HF)酸洗过程中产生的NO_x量,利用自制的酸洗-吸收装置研究了HNO_3和HF质量浓度及抑制剂和促进剂加入量对NO_x生成量的影响,探讨了NO_x的产生机制。结果表明,奥氏体不锈钢酸洗的优化工艺条件为:酸洗温度20～50℃,HNO_3质量浓度90～110 g/L,HF质量浓度40 g/L,抑制剂加入量30 g/L,促进剂加入量1～2 g/L。抑制剂的加入降低了NO_x的生成量,促进剂的加入减少了氧化皮酸洗时间,提高了酸洗效率。酸洗产生的NO_x来源于两部分:一是氧化皮与酸洗液反应,约占NO_x生成量的70%,二是裸露基体与酸洗液反应,约占NO_x生成量的30%。