低温等离子体注入定向Hg氧化实验研究

燃煤烟气汞脱除的核心是单质汞(Hg~0)的高效氧化。本文基于低温等离子体技术,系统研究了放电电压、自由基源气体组成、烟气温度及烟气组分对氯自由基(Cl)注入强化氧化Hg~0的影响,结果发现降低注入点烟气温度、增加Cl注入量以及烟气中的NO均有利于Hg~0氧化,最佳放电电压的选取则与自由基源气体组成密切相关,一定条件下,注入极少量C_(12)(19 mg/m~3)即可获得97.9%的Hg~0氧化率。     

H2O/N2脉冲流光放电和介质阻挡放电发射光谱比较

本文采用脉冲流光放电和介质阻挡放电两种放电形式分别获得了H2O / N2等离子体的发射光谱。 OH荧光辐射在两种放电等离子体中均出现,而Ha荧光辐射仅存在于脉冲流光放电等离子体中。实验还对脉冲流光放电条件下H、OH 荧光信号进行了时间分辨测量,结果显示Ha荧光信号滞后OH荧光信号约10 ns。根据时间分辨测量结果以及水分子离解的相关文献,实验判断等离子体内水分子离解的主要产物是基电子态的H原子和OH自由基,Ha荧光辐射源于快电子对H原子的次级碰撞激发。介质阻挡放电等离子体的放电脉冲宽度较窄,不能对基态 原子进行有效地次级碰撞激发,所以H2O / N2介质阻挡放电等离子体发射光谱中没有出现Ha荧光辐射。实验结论证实放电脉冲宽度对放电等离子体内次级碰撞激发过程有影响。     

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进行了介质阻挡放电低温等离子体脱除伴有SO2的烟气中NO的研究,分别进行了直接等离子体脱硫脱硝和间接等离子体脱硫脱硝实验.在直接等离子体脱硫脱硝中,模拟烟气等混合气直接通入等离子体发生器,在反应器中电离分解NO以及和生成的高能电子、离子和自由基等离子体相互反应而进行脱除NO;间接等离子体脱硫脱硝中,模拟烟气连接在等离子体发生器出口与从反应器中产生出的等离子体发生氧化反应而进行脱除NO.结果表明,无论直接形式还是间接形式,脱硝效率都要比脱硫效率高,间接脱硫脱硝能够大大降低功率输入,节省能耗,具有重要的实际应用价值和意义.氨气的加入,有利于脱除效率的提升.     

介质阻挡放电低温等离子体脱硝性能研究

进行了介质阻挡放电低温等离子体脱除伴有SO₂的烟气中NO的研究,分别进行了直接等离子体脱硫脱硝和间接等离子体脱硫脱硝实验。在直接等离子体脱硫脱硝中,模拟烟气等混合气直接通入等离子体发生器,在反应器中电离分解NO以及和生成的高能电子、离子和自由基等离子体相互反应而进行脱除NO;间接等离子体脱硫脱硝中,模拟烟气连接在等离子体发生器出口与从反应器中产生出的等离子体发生氧化反应而进行脱除NO。结果表明,无论直接形式还是间接形式,脱硝效率都要比脱硫效率高,间接脱硫脱硝能够大大降低功率输入,节省能耗,具有重要的实际应用价值和意义。氨气的加入,有利于脱除效率的提升。     

硒化铜修饰海绵烟气脱汞研究

在气相元素汞(Hg0)吸附剂的设计和生产中,如何获得性能和经济性之间的平衡是最大的挑战.本文设计了一种化学镀偶联原位硒化方法,开发了硒化铜修饰商用聚氨酯海绵(Cu2Se/PUS)吸附材料,用于燃煤烟气脱汞.Cu2Se/PUS具有优异的Hg0吸附性能,海绵的物理结构特征以及Cu2Se前驱体用量对其吸附性能均没有明显影响;Cu2Se/PUS具有良好的抗H2O和SO2干扰能力,O2对Cu2Se/PUS的Hg0吸附能力具有一定的促进作用,NO存在时会与Hg0产生竞争吸附,抑制Hg0的吸附脱除.本研究不仅为燃煤烟气Hg0的脱除提供了有效的吸附材料,也为海绵在环境修复中的应用提供了通用的功能化策略.     

脉冲电晕放电脱除NO化学反应动力学过程

采用非接触的色散荧光发射光谱和时间分辨光谱方法,在大气压条件下,对脉冲电晕放电脱除NO的化学反应动力学过程进行了实验研究。在该研究中,首先利用色散荧光发射光谱方法,得到纯NO气体脉冲电晕放电中各活性粒子的色散荧光谱,并对其进行归属,确定了各活性粒子的灵敏指纹跃迁谱线;在此基础上,通过测量NO气体放电过程中所产生的N+,O,N₂及NO分子的灵敏指纹跃迁谱线的时间行为特性,研究脉冲电晕放电脱除NO的化学反应机理。实验结果表明：在脉冲电晕放电过程中,NO分子首先与高能电子发生非弹性电离碰撞,变成NO+离子,随后NO+离子发生解离反应,形成N+离子和O原子;N+离子在向阴极运动过程中与电子碰撞结合成激发态N原子,继而和其他激发态N原子结合成为激发态N₂;而O原子则应与其它O原子结合成为O₂。由此建立了大气压条件下纯NO气体脉冲电晕放电脱除NO的化学反应动力学模型。     

水蒸气／氨活化在脉冲电晕脱硫工业中试装置上的应用

脉冲放电等离子体烟气治理技术是利用高压脉冲电源产生的高能电子激活燃煤烟气中的氧气、水蒸气等生成活性物种OH，O，O3等，氧化烟气中的SO2和NOx，并加入氨作为中和剂，生成（NH4）2SO4和NH4NO3肥料的烟气综合治理技术。活化水蒸气／氨能有效地提高脱硫效率和降低能耗。     

气体NO/N2系统等离子体反应NO还原机理研究

首先建立了气体放电等离子体发射光谱测量系统,获得了NO/N2和纯N2气体放电的发射光谱,然后用自洽场分子轨道从头计算法得到了N2基态和激发态分子轨道模型.发现NO/N2气体放电等离子体脱除NO主要是通过包括反应速度非常快的N+NO→N2+O以及e+N2(A3∑u+)→2N+e和e+N2→N2(A3∑u+)+e在内的一系列基元反应进行的,活性N原子是NO还原的基础.     

SCR气氛下CuO-CeO_2/TiO_2催化剂对汞的催化氧化

采用溶胶一凝胶法合成了CuO-CeO_2/TiO_2(CuCeTi)催化剂,并采用BET,XRD,XPS等分析手段对催化剂进行了表征。在固定床实验装置上研究了低温SCR气氛下催化剂对单质汞(Hg~0)的催化氧化。结果表明;SCR气氛(NO+NH_3+4%O_2)下CuCeTi催化剂可以促进Hg~0的氧化。200℃,NO与NH_3体积分数均为0.1%,空塔气速(GHSV)高达54000 h~(-1)时,CuCeTi催化剂上Hg~0的氧化效率仍可高达99%;SCR气氛可以抑制CuCeTi催化剂上Hg~0的氧化,且NO与NH_3的浓度越高,抑制作用越强,但这种抑制作用随GHSV的降低可以得到缓解甚至消除。CuCeTi催化剂在SCR气氛下具有良好的汞氧化活性与稳定性,应用该SCR催化剂有望实现燃煤烟气中NO_x与Hg~0的协同控制。     

常压He气和N$lt;sub$gt;2$lt;/sub$gt;气均匀介质阻挡放电的伏安特性

对带有多电流峰的常压He气均匀介质阻挡放电与常压N₂气均匀介质阻挡放电的伏安特性进行了实验分析. 分析结果表明：实验结果与模拟结果相符. 在带有多电流峰的常压He均匀介质阻挡放电中,辉光放电模式和汤森放电模式可以共存于一个多电流放电序列内. 此外,在放电电流增长阶段,可以根据常压均匀介质阻挡放电的伏安特性曲线的微分电导来判断均匀介质阻挡放电的放电模式. 在放电电流增长阶段,如果电流脉冲的伏安特性曲线呈现负微分电导,则电流脉冲为辉光放电模式;如果呈现正微分电导,则为汤森放电模式. 由此可以判断,常压N₂气均匀介质阻挡放电为汤森放电模式. 关键词： 伏安特性 辉光放电模式 汤森放电模式 常压均匀介质阻挡放电     

Les phases Cd2Nb2-2xSn2xO7-2xF2x

The solid solution Cd₂Nb_2-2xSn_2xO_7-2xF_2x is studied by X-Ray diffraction and Mössbauer spectroscopy. Two phases I and II are observed; phase I presents a normal pyrochlore structure but phase II shows a local order around Sn⁴⁺. The difference between phases I and II is explained by the difference of electronic configuration between Sn⁴⁺ (4d¹⁰) and Nb⁵⁺ (4d⁰).     

Wing profile measurements of the Na-doublet lines in C2H2/O2/N2, H2/O2/N2 and H2/O2/Ar frames at 1 atm

Fluorescence-excitation (wing) profiles of the Na-D doublet lines were measured over a wavelength range extending from 0.3 to 200 Å from the line center for the red D₁ and blue D₂ wings and from 0.3 to 3 Å for the red D₂ and the blue D₁ wings, respectively. The line profiles were determined with the aid of a tunable CW dye-laser as a background source by measuring the total fluorescence intensity observed on detuning the laser wavelength. The flames were premixed, laminar, shielded flames at 1 atm, with temperatures ranging from 1860 to 2270 K; N₂ and Ar served as diluent gases. The line core and near-wing profiles (i.e. the region covering 0.3<Δλ<7 Å for the outer wings and 0.3<Δλ<3 Å for the inner ones) in all of the flames studied appeared to have the same frequency dependence, regardless of the nature and concentrations of the gases used. The blue D₂-line profile followed an unexpected (-2.2) law, while the other three profiles obeyed the theoretically expected (-2) law (the dispersion profile function). The line profile in the Δλ range between the impact and quasistatic regions was found to depend on the main perturbers involved. We found that the far blue D₂- and red D₁-wings in the Ar-diluted H₂/O₂ flame obeyed the (-$\text{5}\text{4}$) and (-$\text{3}\text{2}$) laws, respectively, as predicted by the quasi-static theory for the Lennard-Jones interaction. For the N₂-diluted C₂H₂/O₂ and H₂/O₂ flames, we did not find these wing dependences in the Δλ range investigated.     

Magnetic properties of NdCo2Ge2, ErCo2Ge2 and PrFe2Ge2 compounds

Magnetometric and neutron diffraction studies of polycrystalline NdCo₂GE₂, ErCo₂Ge₂ and PrFe₂Ge₂ compounds were carried out in the temperature range between 4.2 and 300 K. All samples are antiferromagnetic with Néel temperature 26.5, ～ 4.2 and 13 K, respectively. The RECo₂Ge₂ compounds have collinear antiferromagnetic order of +?+? type. For PrFe₂Ge₂ a sinusoidal magnetic structure is observed. Magnetic moment is localized on RE atoms only and is equal to that of RE³⁺ free ion value. In ErCo₂Ge₂ the magnetic moment of Er atoms is perpendicular to the c-axis, whereas for remaining compounds it is parallel to the c-axis.     

Orbital ordering in Mott-insulators La2O3Fe2Se2 and La2O3Co2Se2

The electronic structure and magnetic properties of new layered oxyselenide compounds La₂O₃Fe₂Se₂ and La₂O₃Co₂Se₂ are studied by first-principles calculations. Our results indicate that both compounds are Mott-insulators with orbital ordering. The ground states of both compounds are the checkerboard antiferromagnetic states, which are different from the iron pnictide superconductors, although their structures are similar to those of the Fe-As-based superconductors.     

Neutron diffraction study of magnetic ordering in PrCu2Si2, PrCu2Ge2, PrFe2Ge2 and NdFe2Ge2

A neutron diffraction study of polycrystalline PrCu₂Si₂ [1], PrCu₂Ge₂ [2], PrFe₂Ge₂ [3] and NdFe₂Ge₂ [4] intermetallics carried out at liquid helium temperature shows the presence of a collinear antiferromagnetic order below T_N = 19 ± 1 K [1], T_N = 16 ± 1 K [2], T_N = 9 ± 1 K [3] and 13 ± 1 K [4]. Magnetic moment, parallel to the c-axis is localized on RE ions only. The magnetic structure of these compounds consists of ferromagnetic layers perpendicular to the c-axis coupled antiferromagnetically with sequence +-+- for PrCu₂Si₂ and PrCu₂Ge₂ and +--+ for PrFe₂Ge₂ and NdFe₂Ge₂. The RE moments amount close to the free ion values for Fe containing compounds but are smaller in those containing Cu suggesting a fairly strong influence of crystal field.     

Structure, transport and magnetic properties in La2xSr2−2xCo2xRu2−2xO6

The perovskite solid solutions of the type La_2xSr_2−2xCo_2xRu_2−2xO₆ with 0.25≤x≤0.75 have been investigated for their structural, magnetic and transport properties. All the compounds crystallize in double perovskite structure. The magnetization measurements indicate a complex magnetic ground state with strong competition between ferromagnetic and antiferromagnetic interactions. Resistivity of the compounds is in confirmation with hopping conduction behaviour though differences are noted especially for x=0.4 and 0.6. Most importantly, low field (50 Oe) magnetization measurements display negative magnetization during the zero field cooled cycle. X-ray photoelectron spectroscopy measurements indicate the presence of Co²⁺/Co³⁺ and Ru⁴⁺/Ru⁵⁺ redox couples in all compositions except x=0.5. Presence of magnetic ions like Ru⁴⁺ and Co³⁺ gives rise to additional ferromagnetic (Ru-rich) and antiferromagnetic sublattices and also explains the observed negative magnetization.     

Structure and properties of Bi2Sr2CaCu2Ox/Bi2Sr2CuOx superlattices prepared by RF magnetron sputtering

We have prepared Bi₂Sr₂CaCu₂O_x/Bi₂Sr₂CuO_x (2212/2201) superlattices with various stacking periodicity by multitarget RF magnetron sputtering. Their crystal structure and electrical properties were investigated. The superlattice was found to be successfully constructed from the data of XRD patterns, AES, etc. The critical temperature increased almost linearly with increasing thickness of the 2212 phase up to a thickness of 6 unit cells. On the other hand, it did not decrease as the thickness of the 2201 layers was increased. The unit cell/unit cell superlattice showed T_{c zero} of 30 K.     

碱金属Li,Na,K,Rb,Cs,Fr的ns2S1/2,np2P1/2,3/2, nd2D3/2,5/2 和nf2F5/2,7/2 里德伯能级理论研究

本文在多通道量子数亏损理论(MQDT)框架下,利用相对论多通道理论(RMCT),分别在冻结实近似、 考虑Δl=-1的偶极极化效应、Δl=+1的偶极极化效应、Δl=± 1的偶极极化效应、伸缩模效应以及同时考虑偶极极化效应和伸缩模效应等不同层次近似下,系统地计算了碱金属Li, Na, K, Rb, Cs和Fr七个里德伯系列的能级,即ns²S_1/2, np²P_1/2, np²P_3/2, nd²D_3/2, nd²D_5/2, nf²F_5/2 和nf²F_7/2.计算结果表明,电子关联效应对碱金属原子的里德伯能级的影响很大.总的来说,偶极极化效应比伸缩模效应重要,而在偶极极化效应中, Δl = + 1的偶极极化效应比Δl = - 1的偶极极化效应重要.但对于Na的ns²S_1/2,(nd²D_3/2,nd²D_5/2)里德伯系列的能级,和Li的(np²P_1/2,np²P_3/2)里德伯系列的能级,是伸缩模效应比较重要.     

CO在MoS2/K2CO3/TiO2上的加H2反应

根据“盐类及氧化物等在高比表面载体上有自发分散倾向”的原理，制备了一种新型的用于由合成气（H2／CO）合成甲醇的催化剂MoS2/K2CO/TiO2(DSA),该催化剂具有较好的耐硫性和对甲醇有较高的选择性，通过对反应条件的教察得出结论：高压、低温、高空速有利于提高醇的选择性。     

Oscillator strengths and transition probabilities of the Be(I) isoelectronic sequence for 2p2-2s2p and 2s2p-2s2 transitions

Oscillator strengths and transition probabilities are obtained from an intermediate coupling scheme. The initial basis of the eigenstates is formed inLS-coupling. To obtain the resulting energy matrix,Z^-1 perturbation theory is applied. The values of oscillator strengths and transition probabilities for 1s²2p²?1s²2s2p and 1s²2s2p?1s²2s² transitions are calculated and the comparison is made with some recent results. The nuclear charges (Z) involved varied fromZ=4(Be(I)) toZ=35(Br(XXXII)).