NOx分解还原催化研究进展

介绍和评价了ＮＯ_ｘ分解还原的３类催化剂：贵金属催化剂、氧化物催化剂、金属离子置换的分子筛。在ＮＯ_ｘ的碳氢化合物选择性催化还原反应（ＨＣ－ＳＣＲ反应）中，同样有３类催化剂，即金属氧化物、贵金属和分子筛。由于Ｃｕ－ＺＳＭ－５是目前最有希望投入实际使用的一种，故本文重点介绍了它对ＮＯ_ｘ的ＨＣ－ＳＣＲ反应的催化机理，以及温度、Ｏ_２含量、Ｃｕ~（２＋）的置换度、不同种类ＨＣ及ＨＣ含量等各种因素对Ｃｕ－ＺＳＭ－５的影响，并对其工作台试验进行了评价，指出了其存在的问题及当前的研究热点。     

Arsenic release from arsenic-bearing Fe-Mn binary oxide: effects of E(h) condition

Ferric and manganese binary oxide (FMBO) has been successfully used to remediate arsenic-polluted river, but there still lacks sufficient data to evaluate its effects on environments. The release behaviors of iron (Fe), manganese (Mn), and arsenic (As) in different E_h ranges were investigated for As-bearing FMBO sediment after remediating As-polluted DaSha River by FMBO. Under high E_h range (+550 to +400 mV), slight dissolution of Fe and Mn, which corresponded to 12.2% and 25.6%, and less than 5% of As release were observed in 336 h. Under lower E_h range (+50 to −100 mV), elevated extent of the dissolution of Mn and Fe were observed, which corresponded to as high as 61.3% and 70.1%. Under such conditions, the dissolution rate of Mn was higher than that of Fe. Furthermore, from the established relationship of As release and the dissolution of Fe and Mn, the release of As seemed dominated by the dissolution of Fe. X-ray photoelectron spectroscopy (XPS) analysis demonstrated the release of Fe, Mn, As(III), and As(V) after sodium ascorbate-treatment, and the re-adsorption of As(V), as indicated from the increased binding energy of As 3d from 44.78 to 45.83 eV. Surface element composition analysis indicated significant decrease of Mn from 3.22% to 0.54%, slight increase of Fe from 12.45% to 13.67%, and elevated ratio of As from 0.11% to 0.32% accordingly. The main reactions of Fe and Mn dissolution and the pathways of As release under different E_h ranges were also proposed.     

Zero-valent iron nanoparticles in treatment of acid mine water from in situ uranium leaching

Acid mine water from in situ chemical leaching of uranium (Straz pod Ralskem, Czech Republic) was treated in laboratory scale experiments by zero-valent iron nanoparticles (nZVI). For the first time, nZVI were applied for the treatment of the real acid water system containing the miscellaneous mixture of pollutants, where the various removal mechanisms occur simultaneously. Toxicity of the treated saline acid water is caused by major contaminants represented by aluminum and sulphates in a high concentration, as well as by microcontaminants like As, Be, Cd, Cr, Cu, Ni, U, V, and Zn. Laboratory batch experiments proved a significant decrease in concentrations of all the monitored pollutants due to an increase in pH and a decrease in oxidation-reduction potential related to an application of nZVI. The assumed mechanisms of contaminants removal include precipitation of cations in a lower oxidation state, precipitation caused by a simple pH increase and co-precipitation with the formed iron oxyhydroxides. The possibility to control the reaction kinetics through the nature of the surface stabilizing shell (polymer vs. FeO nanolayer) is discussed as an important practical aspect.     

氧化物催化剂对非热等离子体催化降解甲苯的影响

考察了在干燥气氛下不同氧化物催化剂对非热等离子体催化降解甲苯的影响。从甲苯降解率、碳平衡、CO2选择性和O3去除4个方面,对比了氧化物催化剂的介电性能、表面供氧能力和比表面积与多孔结构对反应产生影响的强弱。结果表明,催化剂的介电性能有利于甲苯降解率、碳平衡和O3产量的提高,但对CO2选择性和O3去除的影响极小;一定能量密度下,催化剂比表面积与多孔结构对CO2选择性和O3去除所产生的影响要强于介电性能;催化剂表面供氧能力可明显促进反应的进行,其对反应所产生的影响要强于比表面积与多孔结构。     

Transport of copper as affected by titania nanoparticles in soil columns

The effects of TiO₂ nanoparticles on the transport of Cu through four different soil columns were studied. For two soils (HB and DX), TiO₂ nanoparticles acted as a Cu carrier and facilitated the transport of Cu. For a third soil (BJ) TiO₂ nanoparticles also facilitated Cu transport but to a much lesser degree, but for a fourth soil (HLJ) TiO₂ nanoparticles retarded the transport of Cu. Linear correlation analysis indicated that soil properties rather than sorption capacities for Cu primary governed whether TiO₂ nanoparticles-facilitated Cu transport. The TiO₂-associated Cu of outflow in the Cu-contaminated soil columns was significantly positively correlated with soil pH and negatively correlated with CEC and DOC. During passage through the soil columns 46.6-99.9% of Cu initially adsorbed onto TiO₂ could be “stripped” from nanoparticles depending on soil, where Cu desorption from TiO₂ nanoparticles increased with decreasing flow velocity and soil pH.     

NiO-CuO/ZSM-5催化剂对催化裂化烟气的脱硫脱硝性能

采用浸渍法制备了不同NiO和CuO质量分数的NiO-CuO/ZSM-5催化剂，并以CH4为还原剂研究了NiO-CuO/ZSM-5催化剂对催化裂化烟气的脱硫脱硝活性。XRD分析结果表明，NiO质量分数为4%、CuO质量分数为6%的催化剂4%NiO-6%CuO/ZSM-5中的ZSM-5结构完好，CuO和NiO高度分散在ZSM-5骨架中，表明具有较好的催化活性。4%NiO-6%CuO/ZSM-5的脱硫脱硝起活温度均较低，无氧条件下最高NO转化率和SO2转化率分别为94.7%和95.9%，O2体积分数为1.0%时的NO转化率和SO2转化率分别为97.7%和89.0%。     

堇青石负载Pd和过渡金属氧化物催化剂的表征及其对CO的催化氧化活性

以堇青石蜂窝陶瓷(CC)为载体，采用浸渍法制备了堇青石负载Pd和过渡金属混合氧化物催化剂，记作Pd-M-Mn(M=Cu，Co，Fe，Ni)/CC。实验结果表明:Pd-Co-Mn/CC催化剂的催化活性最高;随着Pd负载量的增加，CO转化率提高;当Pd负载量为1.00%时，反应温度为150℃时CO转化率达到98%，200℃时CO转化率达到100%;在反应温度150℃条件下，Pd-Co-Mn/CC催化剂(Pd负载量1.00%)的CO转化率在前30h内小幅度下降，随后稳定在90%以上，反应100h后，催化剂表面颜色由黑色变为棕褐色。     

用碳化法从制碱废渣一次盐泥中制取轻质氧化镁的研究

本研究是用制碱废渣一次盐泥作原料，采用二氧化碳碳化法制取轻质氧化镁。同时分析了提取轻质氧化镁后的残渣用于制造水泥或其它胶凝材料的原料的可行性。     

Differences in nitrous oxide fluxes from red soil under different land uses in mid-subtropical China

Red soil may play an important role in nitrous oxide (N₂O) emissions due to its recent land use change pattern. To predict the land use change effect on N₂O emissions, we examined the relationship between soil N₂O flux and environmental determinants in four different types of land uses in subtropical red soil. During two years of study (January 2005-January 2007), biweekly N₂O fluxes were measured from 09:00 to 11:00 a.m. using static closed chamber method. Objectives were to estimate the seasonal and annual N₂O flux differences from land use change and, reveal the controlling factors of soil N₂O emission by studying the relationship of dissolved organic carbon (DOC), microbial biomass carbon (MBC), water filled pore space (WFPS) and soil temperature with soil N₂O flux. Nitrous oxide fluxes were significantly higher in hot-humid season than in the cool-dry season. Significant differences in soil N₂O fluxes were observed among four land uses; 2.9, 1.9 and 1.7 times increased N₂O emissions were observed after conventional land use conversion from woodland to paddy, orchard and upland, respectively. The mean annual budgets of N₂O emission were 0.71-2.21 kg N₂O-N ha⁻¹ year⁻¹ from four land use types. The differences were partly attributed to increased fertilizer use in agriculture land uses. In all land uses, N₂O fluxes were positively related to soil temperature and DOC accounting for 22-48% and 30-46% of the seasonal N₂O flux variability, respectively. Nitrous oxide fluxes did significantly correlate with WFPS in orchard and upland only. Nitrous oxide fluxes responded positively to MBC in all land use types except orchard which had the lowest WFPS. We conclude that (1) land use conversion from woodland to agriculture land uses leads to increased soil N₂O fluxes, partly due increased fertilizer use, and (2) irrespective of land use, soil N₂O fluxes are under environmental controls, the main variables being soil temperature and DOC, both of which control the supply of nitrification and denitrification substrates.