烧结烟气脱硫脱硝用活性炭混合钢渣复合材料的光谱学分析

钢渣是冶金工业中产生的主要固体废弃物,其产量约为每年粗钢产量的15%~20%。由于技术的局限,导致我国钢渣利用率较低,仅为年钢渣产量的10%,同时加之管理制度的不健全,导致钢渣大量露天堆放,对土地资源、地下水源,以及空气质量形成严重影响。固体废弃物再利用是资源可持续发展的重要途径之一,钢渣的主要化学成分为CaO, SiO2, Al2O3, MgO, Fe2O3, MnO, f-CaO等。面对上述问题,利用冶金固体废弃物与活性炭开发一种价格低廉且性能优越的活性炭混合钢渣复合材料,既是冶金固体废弃物的高附加值利用与资源可持续发展的重要途径之一,也是大幅降低改性活性炭生产成本与提高经济效益的重要途径之一。该研究创新性以活性炭与钢渣为研究对象,利用钢渣中含有的金属氧化物对活性炭进行改性处理制备用于烧结烟气脱硫脱硝的活性炭混合钢渣复合材料,通过搭建实验反应装置对活性炭混合钢渣复合材料的脱硫脱硝性能进行测试。利用X射线荧光光谱仪(XRF)对钢渣的化学成分进行测试与分析,比表面积及孔径测定仪(BET)对活性炭混合钢渣复合材料的孔结构进行测试与分析,傅里叶变换红外光谱仪(FTIR)对钢渣的结构组成进行测试与分析,扫描电子显微镜(SEM)对活性炭混合钢渣复合材料的微观结构进行测试与分析,以揭示活性炭与钢渣制备活性炭混合钢渣复合材料的机理,以及活性炭混合钢渣复合材料对烧结烟气脱硫脱硝的机理。结果表明:当钢渣为电炉热泼渣、钢渣与活性炭质量比为2∶4、钢渣与活性炭细度为400目时,活性炭混合钢渣复合材料具有良好的脱硫脱硝性能与合理的经济性,即脱硫效率为100%、脱硝效率为58%。活性炭混合钢渣复合材料具有的多孔结构对SO2和NO进行有作用,钢渣中Fe2O3与MnO2促使活性炭官能团进行催化还原反应提高脱硫脱硝性能,其中吸附作用是主导与前提,催化还原反应是辅助与协同。以期为高附加值的钢渣利用提供新途径,实现钢铁企业以废治废、以废增效的目的。     

Yb3+掺杂稀土钽铌酸盐的晶体场从头计算研究

Yb³⁺掺杂晶体材料是重要的激光材料,在超短脉冲激光、大功率激光等领域有重要应用前景,但长期以来很难通过实验拟合确定Yb3+晶体场参数,尤其是低对称体系,从头计算是解决此问题的重要途经.本文介绍了适合计算稀土离子掺杂晶体的从头计算DV-Xα方法和有效哈密顿量模型,用该方法计算了Yb³⁺掺杂M型和M'型钽铌酸盐的晶场参数和旋轨耦合参数,得到的能级结构和实验能很好地符合,并发现了Yb³⁺掺杂钽铌酸盐的晶场强度参数随稀土原子序数呈现规律变化.表明结合DV-Xα计算和有效哈密顿量方法是计算Yb³⁺掺杂低对称钽铌酸盐晶体场的有效途径,结果显示Yb3+掺杂钽铌酸盐晶体有望成为新型全固态激光工作物质.     

Intertwined Detection and Recognition Roles of Tetrazine in Synergistic Anion-π and H-bond Based Anion Receptor

The intrinsic properties of tetrazine as a π-anion receptor and as an on/off recognition probe merged with H-bond ability of an urea motif into a single architecture constitutes a new generation of well-defined anion receptors. Complexation properties directly benefit from the dual and synergistic contribution of tetrazine and urea. In this study, we report on the synthesis and assessment of binding properties to anions of diverse geometries. Association constants have been predicted by theoretical calculations and evaluated by multiple and complementary experimental techniques including electrospray-mass tandem spectroscopy, NMR, UV-visible, steady state fluorescence spectroscopies and time resolved fluorescence. These results provide the basis for a better understanding of both the complexation and the anion-dependent quenching mechanism.     

Unravelling the Role of Water in Ultrafast Excited-State Relaxation Dynamics within Nano-Architectures of Chlorophyll a

Water plays a pivotal role in structural stability of supramolecular pigment assemblies designed for natural light harvesting (for example, chlorosome antenna complex) as well as their artificial analogs. However, the dynamic role of water in the context of excite-state relaxation has not been explored till date, which we report here. Using femtosecond transient absorption spectroscopy, we investigate the excited-state dynamics of two types of nano-scale assemblies of chlorophyll a with different structural motifs, rod-shaped and micellar assemblies, that depend on the water content. We show how water participates in excess energy dissipation by vibrational cooling of the non-thermally populated Q_y band at different rates in different types of clusters but exhibits no polar solvation dynamics. For the micelles, we observe a bifurcation of stimulated emission line shape, whereas a positive-to-negative switching of differential absorption is observed for the rods; both these observations are correlated with their specific structural aspects. Density functional theory calculations reveal two possible stable ground state geometries of dimers, accounting for the bifurcation of line shape in micelles. Thus, our study elucidates water-mediated structure–function relationship within these pigment assemblies.     

Non-Abelian gauge potentials driven localization transition in quasiperiodic optical lattices

Derived from quantum waves immersed in an Abelian gauge potential, the quasiperiodic Aubry-André-Harper (AAH) model is a simple yet powerful Hamiltonian to study the Anderson localization of ultracold atoms. Here, we investigate the localization properties of ultracold atoms in quasiperiodic optical lattices subject to a non-Abelian gauge potential, which are depicted by non-Abelian AAH models. We identify that the non-Abelian AAH models can bear the self-duality. We analyze the localization of such non-Abelian self-dual optical lattices, revealing a rich phase diagram driven by the non-Abelian gauge potential involved: a transition from a pure delocalization phase, then to coexistence phases, and finally to a pure localization phase. This is in stark contrast to the Abelian counterpart that does not support the coexistence phases. Our results establish the connection between localization and gauge symmetry, and thus comprise a new insight on the fundamental aspects of localization in quasiperiodic systems, from the perspective of non-Abelian gauge potential.     

第三族金属氧化物离子对二氧化碳转化的红外光谱研究

本文利用红外光解离光谱研究了第三族金属氧化物离子对二氧化碳分子的转化机制. 研究表明，对于[ScO(CO₂)_n]⁺体系，在n≤4时，形成了溶剂化结构；在n=5时，形成了碳酸盐结构，实现了二氧化碳的转化. 对于[YO(CO₂)_n]⁺体系，需要4个二氧化碳分子就可以实现二氧化碳的转化. 而在[YO(CO₂)_n]⁺体系中，只发现了溶剂化结构，没有观察到碳酸盐结构. 理论计算表明，[YO(CO₂)_n]⁺体系拥有最小的溶剂化结构向碳酸盐结构转化能垒，[LaO(CO₂)_n]⁺体系拥有最大的溶剂化结构向碳酸盐结构转化能垒. 本文从分子水平揭示了不同金属氧化物离子对二氧化碳分子转化的影响规律.     

光子晶体光纤温度压力传感器

提出了一种在高温环境下同时测量温度和气压的光子晶体光纤温度压力传感器.在普通单模光纤和光子晶体光纤之间熔接一段空心光纤构成干涉结构.空心光纤段构成非本征法布里-珀罗干涉仪,利用光子晶体光纤的微孔与外界相通,通过气体折射率变化来测量环境中的气压变化;光子晶体光纤段构成本征法布里-珀罗干涉仪,利用热膨胀效应和热光效应来测量环境中的温度.传感器的解调通过自制的白光干涉解调仪实现,实验通过测量腔长得到被测环境的温度和气压.在不同温度和气压环境下,对腔长分别为306μm和1535μm的温度压力光纤传感器进行连续测量.实验结果表明,传感器能够在28~800℃的温度下和0~10 MPa的气压下稳定工作,测量范围内温度灵敏度可达17.4 nm/℃,压力灵敏度随温度增加而降低,在28℃时可达1460.5 nm/MPa.     

考虑制动力影响的大型客车舒适性分析

利用有限元法和动力平衡原理,建立了具有层间接触的沥青路面和13个自由度的大型客车人体三维模型。以不平顺作为激励,随机模拟车流分布,在不同制动情况下,从时域和频域两方面分析人-车-路耦合振动下车辆和人体的动力响应。时域分析采用客观评价标准和主观烦恼率相结合的方法,频域分析考虑人体共振、人的心理和生理因素。结果表明:随着制动力增大,人体的竖向加速度幅值不变,俯仰、侧倾加速度幅值都增大,但是俯仰加速度增幅远大于侧倾加速度的情况,人的舒适性变差,烦恼率增高;在紧急制动时,主频段对人体共振、心理和生理产生的影响很小,但是次主频段与人体某些器官固有频段重合,对人体共振、心理和生理产生的影响是不容忽视的。     

Impact of the Oxygen Defects and the Hydrogen Concentration on the Surface of Tetragonal and Monoclinic ZrO2 on the Reduction Rates of Stearic Acid on Ni/ZrO2

The role of the specific physicochemical properties of ZrO₂ phases on Ni/ZrO₂ has been explored with respect to the reduction of stearic acid. Conversion on pure m‐ZrO₂ is 1.3 times more active than on t‐ZrO₂, whereas Ni/m‐ZrO₂ is three times more active than Ni/t‐ZrO₂. Although the hydrodeoxygenation of stearic acid can be catalyzed solely by Ni, the synergistic interaction between Ni and the ZrO₂ support causes the variations in the reaction rates. Adsorption of the carboxylic acid group on an oxygen vacancy of ZrO₂ and the abstraction of the α‐hydrogen atom with the elimination of the oxygen atom to produce a ketene is the key to enhance the overall rate. The hydrogenated intermediate 1‐octadecanol is in turn decarbonylated to heptadecane with identical rates on all catalysts. Decarbonylation of 1‐octadecanol is concluded to be limited by the competitive adsorption of reactants and intermediate. The substantially higher adsorption of propionic acid demonstrated by IR spectroscopy and the higher reactivity to O₂ exchange reactions with the more active catalyst indicate that the higher concentration of active oxygen defects on m‐ZrO₂ compared to t‐ZrO₂ causes the higher activity of Ni/m‐ZrO₂.