Density functional theory (DFT) studies of vanadium-titanium based selective catalytic reduction (SCR) catalysts

Based on density functional theory (DFT) and basic structure models, the chemical reactions on the surface of vanadium-titanium based selective catalytic reduction (SCR) denitrification catalysts were summarized. Reasonable structural models (non-periodic and periodic structural models) are the basis of density functional calculations. A periodic structure model was more appropriate to represent the catalyst surface, and its theoretical calculation results were more comparable with the experimental results than a non-periodic model. It is generally believed that the SCR mechanism where NH₃ and NO react to produce N₂ and H₂O follows an Eley-Rideal type mechanism. NH₂NO was found to be an important intermediate in the SCR reaction, with multiple production routes. Simultaneously, the effects of H₂O, SO₂ and metal on SCR catalysts were also summarized.     

Effects of calcination temperature on physicochemical property and activity of CuSO4/TiO2 ammonia-selective catalytic reduction catalysts

CuSO_4/TiO_2 catalysts with high catalytic activity and excellent resistant to SO_2 and H_2 O,were thought to be promising catalysts used in Selective catalytic reduction of nitrogen oxides by NH_3.The performance of catalysts is largely affected by calcination temperature.Here,effects of calcination temperature on physicochemical property and catalytic activity of CuSO_4/TiO_2 catalysts were investigated in depth.Catalyst samples calcined at different temperatures were prepared first and then physicochemical properties of the catalyst were characterized by N2 adsorption-desorption,X-ray diffraction,thermogravimetric analysis,Raman spectra,Fourier-transform infrared spectroscopy,X-ray photoelectron spectroscopy,temperature-pro grammed desorption of NH_3,temperature-programmed reduction of H_2 and in situ diffuse reflectance infrared Fourier transform spectroscopy.Results revealed that high calcination temperature had three main effects on the catalyst.First,sintering and anatase transform into rutile with increase of calcination temperature,causing a decrement of specific surface area.Second,decomposition of CuSO_4 under higher calcination temperature,resulting in disappears of Br(?)nsted acid sites(S-OH),which had an adverse effect on surface acidity.Third,CuO from the decomposition of CuSO_4 changed surface reducibility of the catalyst and favored the process of NH_3 oxidation to nitrogen oxides(NO_x).Thus,catalytic activity of the catalyst calcined under high temperatures(≥600℃) decreased largely.     

Responses of nitrification performance, triclosan resistome and diversity of microbes to continuous triclosan stress in activated sludge system

Triclosan(TCS) is commonly found in wastewater treatment plants,which often affects biological treatment processes.The responses of nitrification,antibiotic resistome and microbial community under different TCS concentrations in activated sludge system were evaluated in this study.The experiment was conducted in a sequencing batch reactor(SBR)for 240 days.Quantitative PCR results demonstrated that the abundance of ammonium oxidizing bacteria could be temporarily inhibited by 1 mg/L TCS and then gradually recovered.And the abundances of nitrite oxidizing bacteria(NOB) under 2.5 and 4 mg/L TCS were three orders of magnitude lower than that of seed sludge,which accounted for partial nitrification.When the addition of TCS was stopped,the abundance of NOB increased.The mass balance experiments of TCS demonstrated that the primary removal pathway of TCS changed from adsorption to biodegradation as TCS was continuously added into the SBR system.Moreover,TCS increased the abundance of mexB,indicating the efflux pump might be the main TCS-resistance mechanism.As a response to TCS,bacteria could secrete more protein(PN) than polysaccharide.Three-dimensional excitation-emission matrix revealed that tryptophan PN-like substances might be the main component in PN to resist TCS.High-throughput sequencing found that the relative abundances of Paracoccus,Pseudoxanthomonas and Thauera increased,which could secrete extracellular polymeric substances(EPS).And Sphingopyxis might be the main TCS-degrading bacteria.Overall,TCS could cause partial nitrification and increase the relative abundances of EPS-secreting bacteria and TCS-degrading bacteria.     

生物气溶胶的吸湿性

归纳了有关气溶胶吸湿性的测量方法以及过去近30a来文献中报道的生物气溶胶吸湿性的主要研究成果,总结了不同种类生物气溶胶之间吸湿性的差异.已有研究表明,绝大部分的生物气溶胶粒子都具有一定的吸湿性,当相对湿度为90%时,吸湿增长因子约为1.04（真菌孢子）~1.22（细菌）,花粉颗粒物吸湿后的质量与之前的比值为1.30~1.55.最后,提出了目前关于生物气溶胶吸湿性研究中尚未解决的科学问题及该领域的主要发展方向.     

2019年10~12月京津冀及周边“2+26”城市重污染减排效果评估

为评估京津冀及周边区域重污染过程期间应急减排措施的效果,基于情景模拟的方法,采用NAQPMS模式和多种观测资料,分析了2019年10~12月期间京津冀及周边区域环境空气质量、重污染过程和气象条件概况,评估了模式24、72和144 h的PM_2.5预报效果,并对应急减排措施的效果和不确定性进行了讨论.结果表明,2019年10~12月京津冀及周边"2+26"城市PM_2.5平均浓度64 μg ·m^-3,同比降低了10 μg ·m^-3;区域性重污染过程4次,受影响城市重污染过程期间PM_2.5平均浓度156 μg ·m^-3."2+26"城市PM_2.5气象条件评估指数（EMI）变化值范围为-15.6%~16.8%,EMI显示北京、天津和石家庄等12个城市气象条件与同期相比变差,变差程度范围为3.2%~16.8%.减排情景模拟分析显示应急减排措施有效减少了区域性重污染过程的发生,污染物峰值浓度降幅明显,未出现区域性严重污染过程.典型重污染期间,北京、石家庄、保定和唐山等城市PM_2.5日均浓度削减2%~9%.区域应急减排措施促使"2+26"城市PM_2.5季度均值分别降低1~3 μg ·m^-3左右,区域性减排效果明显.     

三亚河红树林表层沉积物中好氧氨氧化微生物的分布特征及潜在硝化速率

氨氧化过程是硝化作用的限速步骤,氨氧化细菌(ammonia-oxidizing bacteria, AOB)和氨氧化古菌(ammonia-oxidizing archaea, AOA)是氨氧化作用的主要驱动者,其分布特征及其对硝化作用的相对贡献是氮素循环的研究热点.采用实时荧光定量PCR技术研究了三亚河红树林表层沉积物中好氧氨氧化微生物的分布特征,并通过测定潜在硝化速率分析了AOB和AOA对硝化作用的相对贡献率.结果表明,多数采样点中,AOA amoA基因丰度高于AOB amoA基因丰度; AOB丰度冬季较高,AOA丰度夏季较高,且冬季AOA和AOB丰度的比值较低;溶解氧、pH、总有机碳和硝态氮对AOB和AOA丰度影响较大; AOB和AOA在夏季的潜在硝化速率均高于冬季,冬季AOA对硝化作用的相对贡献率较高而夏季则是AOB在硝化作用中占主导地位,AOB和AOA的潜在硝化速率与amoA基因丰度均不存在显著相关性.     

德州市夏季臭氧敏感性特征及减排方案

近年来德州市臭氧污染频发,2018年夏季（6~8月）,德州市发生了严重臭氧污染事件,臭氧日最大8 h浓度值超标天数达60 d,超标率65%,3个月平均值为176 μg ·m^-3,最高达262 μg ·m^-3.本研究利用WRF-CAMx耦合的HDDM模块,分析期间德州臭氧敏感性特征及减排方案.结果表明,在空间上,德州市中心城区为VOCs控制区,而郊区为NO_x与VOCs协同控制区.在时间上,VOCs敏感值每日为正值,但dO₃_V₅₀在6月（城区18.7 μg ·m^-3,郊区19.7 μg ·m^-3）和8月（城区15.3 μg ·m^-3,郊区16.4 μg ·m^-3）高于7月（城区13.0 μg ·m^-3,郊区11.8 μg ·m^-3）,NO_x敏感值城区呈正负交错,郊区大部分为正值,并与VOCs敏感值接近.对于城区减排方案应考虑以仅VOCs削减为优先,而郊区由于NO_x和VOCs对臭氧减排效果相当,建议以NO_x：VOCs=1：1为优.     

UASB启动运行特征及互营丙酸氧化菌定量分析

为揭示升流式厌氧污泥床（UASB）反应器启动运行效能与互营丙酸降解菌群数量之间的关系,以稀释的玉米淀粉生产废水为底物,考察了UASB启动期的运行特征,并采用实时荧光定量PCR技术（qPCR）分析了互营丙酸降解菌群（丙酸氧化菌和产甲烷菌）的演替规律.结果表明,在进水COD 2000mg/L和水力停留时间（HRT）24h条件下,经过38d的连续运行,COD去除率达到了91.9%.当HRT分阶段缩短至8h时,比产甲烷速率达到了315LCH₄/（kg COD·d）,且形成了沉降性能良好的颗粒污泥.qPCR检测结果表明,至少有5种已鉴定的丙酸氧化菌存在于UASB反应器中.Pelotomaculum propionicum为接种污泥中的主要丙酸氧化菌,约占检测到丙酸氧化菌总数的45.7%.它的数量随着HRT缩短不断减少.而Syntrophobacter sulfatireducens和S.wolinii的数量随着HRT缩短不断增加,并在启动完成时达到最大值,分别为1.3×10³,5.5×10³个16S rRNA基因拷贝数/ng DNA,演替成为成熟颗粒污泥中的优势丙酸氧化菌群.Methanobacterium和Methanosarcina为接种污泥中的主要氢营养型产甲烷菌和乙酸营养型产甲烷菌,其数量随着HRT的缩短而逐渐减少,而Methanospirillum和Methanosaeta的数量随HRT的缩短逐渐增加,成为成熟颗粒污泥中的优势产甲烷菌群.     

高原湖泊沉积物中反硝化微生物的群落特征——以包头南海湖为例

为了探明内蒙古高原富营养化城市湖泊中nirS型反硝化细菌群落结构的特异性,利用特异性功能基因nirS对包头市南海湖的表层沉积物进行反硝化细菌多样性测定,在分析各采样点沉积物理化指标的基础上,对各样品中nirS型反硝化细菌群落和多样性进行研究.结果表明,南海湖沉积物Shannon指数变化为3.07~3.41,相比于其他研究,反硝化微生物多样性相对较低.参与反硝化的优势菌属与大多数湖泊保持一致,以假单胞菌属（Pseudomonas）和红杆菌属（Rhodobacter）为主.冗余分析（RDA）指出,城市湖泊中的各种类型的污染物对反硝化优势菌属有明显的促进作用,红杆菌属（Rhodobacter）与硝酸盐氮、亚硝酸盐氮呈正相关,假单胞菌属（Pseudomonas）除受硝酸盐氮、亚硝酸盐氮的影响外,还与总磷呈较强的正相关.南海湖nirS型反硝化细菌中的主要菌属促进了反硝化作用,加速了南海湖氮素的去除.     

水源水库贫营养好氧反硝化菌群脱氮特性研究

为削减微污染水库中氮素的浓度,通过对西安市李家河水库沉积物进行定向富集驯化,筛选出以Pseudomonas菌为主、具有高效好氧反硝化特性的混合菌群-A1.摇床实验表明,贫营养好氧反硝化菌群A1在15h时硝酸盐氮去除率可达93.39%,硝酸盐氮平均去除速率为0.2073mg/（L·h）;总氮去除率为52.11%,总氮平均去除速率为0.1153mg/（L·h）,无亚硝酸盐积累.氮平衡分析表明,约45%的初始氮被去除转化为气体产物.响应面法（RSM）结果表明,C/N比9.96,温度22.67℃,pH8.01,转速91r/min,溶解氧8.55mg/L是去除总氮（TN）的最优条件.