Infrared-to-visible upconversion luminescence of Er doped barium-natrium-yttrium-fluoride phosphor

Infrared-to-visible upconversion luminescence has been investigated in Er³⁺-doped barium-natrium-yttrium-fluoride phosphor (Ba_xNa_yY_zF_2x+y+3z+3m:Er_m) with different cation concentrations. Intense upconversion emissions around 530, 550, and 660 nm corresponding to the ²H_11/2, ⁴S_3/2, and ⁴F_9/2 transitions, respectively to the ⁴I_15/2 ground state were observed when excited by CW laser radiation at 1550 nm. We adopted the low-temperature combustion synthesis (LCS) method to decrease the phosphor particle size to 40-70 nm in order to couple to the photosensitive surface of CCD. The effect of the amount of carbamide on the particle size and the upconversion luminescence intensity was analyzed. The upconversion luminescence mechanism was studied by the log-log plot of intensity-power.     

纳米铁的低温热容和热力学性质研究

用扫描电子显微镜(SEM)测定了纳米铁试样的粒径, SEM结果表明Fe试样平均粒径d为25 nm. 在84～350 K温区, 用精密低温绝热量热计测定了该纳米铁试样的等压摩尔热容, 拟合出其等压摩尔热容与热力学温度的函数关系式: Cp=36.831+14.772x−5.4968x2−0.7099x3−1.3188x4, 其中x=(T−234)/156. 根据热容与热力学函数关系, 计算了以298.15 K为基准的纳米Fe(d=25 nm)热力学函数, 并与文献报导的粗晶Fe及粒径87 nm Fe的热容进行了比较, 从能量角度分析了不同粒径Fe热容曲线差别产生的原因.     

改性钒钛基SCR催化剂的研究进展

钒钛基选择性催化还原催化剂是目前燃煤电厂应用最为广泛的脱硝催化剂. 由于传统钒钛基催化剂存在低温脱硝效率低?热稳定性差?单质汞氧化效率低?二氧化硫氧化?氨逃逸?碱金属中毒等问题, 人们开始尝试通过对传统 SCR 催化剂进行改性, 以期改善其综合性能. 本文从 (1) 拓宽催化剂的反应温度窗口, 尤其是向低温区扩展, (2) 提高催化剂的热稳定性, (3) 协同氧化单质汞, (4) 控制氨逃逸, (5) 降低 SO2至 SO3的转化率和 (6) 提高催化剂抗碱金属中毒性能等方面综述了改性钒钛基 SCR 催化剂的研究进展, 总结了其催化性能和相关影响机理.研究表明, 某些金属及非金属的改性可以增加钒钛基 SCR 催化剂的表面酸度?活性位点及氧化还原性能, 非金属的掺杂还可以抑制 TiO2载体由锐钛矿向金红石型转化?增加表面氧空位, 从而改善了钒钛基催化剂的低温脱硝性能; 硅?钨?钡和稀土金属等的添加也可抑制 TiO2的金红石化过程, 锆?钾则改变了钒氧化物的存在形态, 抑制其高温聚合, 提高了钒钛基催化剂的热稳定性; 贵金属?过渡金属?金属氯化物及非金属的改性改变了钒钛基催化剂的汞氧化机制, 均可有效促进低氯甚至无氯条件下钒钛基催化剂对单质汞的氧化; 贵金属钌及助剂钼添加的钒钛基催化剂可在维持较高脱硝效率的同时, 实现单质汞及逃逸氨的高效去除, 在 SCR 尾部将逃逸氨选择性氧化生成无害的氮气和水; 被铜?氧化钡?氧化硅等物质改性后, 更多的钒以低价态存在, 使催化剂的氧化还原性能降低, 并抑制了二氧化硫的吸附, 从而减少了三氧化硫的生成;由于具有高储氧能力和氧化还原特性, 还可降低碱金属的吸附量, 铈的掺杂可提高钒钛基催化剂的抗碱金属中毒性能. 此外, 本文还汇总了包括贵金属 (如银?钌)?过渡金属 (如锰?铁?铜?锆等)?稀土金属 (铈?镨) 等金属?金属氯化物 (如氯化铜?氯化钙) 及非金属 (氟?硫?硅等) 改性钒钛基 SCR 催化剂的优缺点. 基于前人研究及作者观点, 改性组分的掺杂有利于进一步提高钒钛基催化剂的综合性能, 具有巨大的发展潜力, 也是在现有基础上实现多污染物控制的方法之一.     

Ag/SBA-15低温气相选择性催化氧化苯甲醇合成苯甲醛

以SBA-15为载体,采用浸渍法制备了不同Ag含量的Ag/SBA-15,通过N₂吸附-脱附、X射线衍射、扫描电子显微镜、高分辨透射电子显微镜、X射线光电子能谱和电感耦合等离子体质谱对催化剂进行了表征。将Ag/SBA-15用于苯甲醇气相选择性催化氧化合成苯甲醛,研究了反应条件对转化率和选择性的影响。结果表明,Ag/SBA-15具有均一的一维孔道结构、较厚的孔壁（3-5 nm）及较大的比表面积（411-541 m²/g）,其规整纳米空间的限域作用使一定负载量的Ag以纳米尺寸均匀分散于介孔SBA-15孔道内,增加了活性组分的比表面积。亲核性氧物种从Ag到SBA-15表面的氧溢流,提高了低温下Ag/SBA-15对苯甲醇气相选择性氧化合成苯甲醛的催化性能。5.3% Ag/SBA-15中的Ag粒径为5-6 nm,且均匀分散于载体孔道中,反应温度为220℃时,苯甲醇转化率为87%,苯甲醛选择性为95%;240℃时,苯甲醇转化率和苯甲醛选择性分别高达94%和97%;并在240-300℃范围内,其催化活性和选择性保持不变,表现出了良好的温度耐受能力。催化剂经活化再生可以连续使用40 h,选择性基本保持不变。     

腈基功能化有机硅电解液添加剂对LiFePO4电池低温性能的影响

合成了一种腈基功能化有机硅化合物3-氰乙基-二乙氧基-甲基硅烷(DESCN), 并对其化学结构和电化学窗口进行了表征. 采用恒流充放电、 扫描电子显微镜(SEM)、 X射线光电子能谱(XPS)及电化学阻抗谱(EIS)等方法研究了DESCN添加剂对LiFePO₄电池低温性能的影响. 结果表明, DESCN化合物能够在电极表面参与形成更薄、 更均匀且致密的固体电解质界面(SEI)膜, 抑制电解液副反应的发生, 减小界面膜阻抗, 有利于低温下电极/电解液界面的Li⁺扩散和电荷转移, 从而提高LiFePO₄电池的低温性能.     

光催化活性TiO2薄膜的低温制备

在低温下,将基材浸渍在含配合物,F－离子捕获剂H3BO3,及加有结晶诱导剂锐钛矿TiO2纳米晶的过饱和水溶液中,在基材上沉积锐钛矿型TiO2薄膜.研究了水溶液的浓度、反应物和H3BO3的摩尔比、沉积时间、反应温度等对沉积TiO2薄膜的结构和性能的影响.并用UV Vis、XRD和SEM等对TiO2薄膜的透明性、厚度、物相和形貌等进行了表征.用亚甲蓝的光催化降解,评价了TiO2薄膜的光催化活性.     

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基于介质阻挡放电(DBD)原理,研究设计了一种悬浮电极式的低温等离子体发生设备,产生的等离子体温度较低且对人体安全,可直接接触。用所研制的低温等离子体发生设备对大肠杆菌做了灭活实验,实验结果表明,该设备产生的低温等离子体对大肠杆菌作用10s 以上,在等离子体有效作用区内大肠杆菌杀灭率为100%,表明所研制的低温等离子体发生设备具有很好的杀菌消毒效果。     

Inelastic low-temperature transport through a quantum dot with a Mn ion

Using the nonequilibrium Hubbard operator Green's function technique, we study the inelastic low-temperature quantum transport through an artificial single-molecule magnet coupled to a single phonon mode. For a minimal model based on CdTe quantum dot doped with a single Mn²⁺ ion (S=5/2), the calculated results show that in the presence of hole–phonon coupling, in addition to main Kondo-like peaks associated with (2S+1) sublevels of spin pair states, satellite Kondo-like peaks originating from emitting phonons appear in the local density of states and differential conductance. Moreover, the number of these phonon-induced Kondo-like peaks depends on the parity of the local large spin, i.e., S=integer or half-integer. It is expected that the intrinsic properties of artificial single-molecule magnets can be obtained by detecting these transport characteristics.     

SBA-15表面改性及其对介孔La0.8Sr0.2CoO3钙钛矿型催化剂结构和性能的影响

Mesoporous SBA-15 with mesopore diameter up to 10.1 nm was prepared by a hydrothermal method, and was further functionalized to obtain different surface properties. Thus-prepared SBA-15 was employed as a template to synthesize rhombohedrally crystallized mesoporous La_0.8Sr_0.2CoO₃ perovskite via a nanocasting method. The surface properties of the SBA-15 were adjusted by treatment with concentrated hydrochloric acid, trimethylchlorosilane (TMCS), and 3-aminopropyltriethoxysilane (APTES). A series of characterization techniques verified that all the synthesized templates possessed ordered two-dimensional hexagonal mesoporous structure, and the surface was successfully modified with methyl and amino groups. The mesoporous perovskite structure was formed in the samples and the surface properties of SBA-15 significantly influenced the structure and properties of La_0.8Sr_0.2CoO₃ perovskite oxides. Wide-angle X-ray diffraction patterns suggested that the modified silica templates were conducive to the formation of pure perovskite frameworks with good crystallinity. The catalysts also possessed mesoporous structure, as confirmed by small-angle XRD patterns, high-resolution transmission electron microscopy images, and nitrogen adsorption analysis. Moreover, the La_0.8Sr_0.2CoO₃ materials synthesized using surface-functionalized templates exhibited relatively higher catalytic activity and stability in CO oxidation. Complete CO conversion could be achieved at 140℃ using the thus-prepared La_0.8Sr_0.2CoO₃ materials, and no significant loss in catalytic activity was observed after 100 h of on-stream reaction experiments. X-ray photoelectron spectroscopy, H₂ temperature-programmed reduction, and O₂ temperature-programmed desorption experiments revealed that the existence of Co⁴⁺, Sr enrichment in the perovskite structure, and high content of adsorbed oxygen species play a critical role in the enhanced catalytic activity of the catalysts. We also proposed the possible reasons for the effect of surface properties of the silica templates on the structure and properties of the La_0.8Sr_0.2CoO₃ nanomaterials.     

A low-temperature synthesis-induced defect formation strategy for stable hierarchical porous metal–organic frameworks

A stable hierarchical porous metal–organic framework PCN-56 with abundant Lewis acid sites (denoted as Defective-PCN-56) was synthesized by the low-temperature synthesis-induced defect formation method. The existence of mesopore in structure was confirmed by N₂ sorption isotherm and the successful encapsulation of large dye molecules. The Defective-PCN-56 has higher loading capacity toward anti-cancer drug Doxo compared with that of “nearly ideal-crystal” (denoted as Ideal-PCN-56) synthesized at high temperature, showing potential application as drug carrier. The low-temperature synthesis-induced defect formation strategy presented here provides a new and facile way to synthesize stable MOFs with the combination of intrinsic micropore and additional mesopore as well as abundant Lewis acid sites.