污泥基吸附剂对亚甲基蓝和环丙沙星的吸附性能研究

亚甲基蓝和环丙沙星是水体中2种污染物, 对生态环境有潜在危害. 本文以市政剩余活性污泥为原料, 氯化锌为活化剂热解制备污泥基吸附剂, 研究盐酸酸洗浓度、氯化锌浓度、热解温度、热解时间等对污泥基吸附剂吸附水中亚甲基蓝和环丙沙星性能的影响. 结果表明 (1)污泥基吸附剂对亚甲基蓝的吸附性能随盐酸酸洗浓度的增大而增加, 对环丙沙星的吸附性能则随盐酸酸洗浓度的增大呈先降后增趋势, 两者均在1.500mol·L-1盐酸浓度下取得最优值. (2)污泥基吸附剂对亚甲基蓝和环丙沙星的吸附性能随氯化锌浓度和热解温度的增加呈先升后降趋势, 在氯化锌浓度为4.0mol·L-1、热解温度为500℃时有最优值; 随着热解时间的延长, 污泥基吸附剂对亚甲基蓝和环丙沙星的吸附性能分别在500℃热解70min和80min时有最优值. (3)污泥基吸附剂的最佳制备条件为 氯化锌4.0mol·L-1活化2h、500℃热解70min和80min、1.500mol·L-1盐酸酸洗; 以此制得的污泥基吸附剂对亚甲基蓝和环丙沙星的去除率分别为97.7%和96.4%, 平衡吸附量分别为97.9mg·g-1和3.9mg·g-1, 且污泥基吸附剂对亚甲基蓝和环丙沙星的吸附过程均符合准二级动力学方程.     

Behavior and process of background signal formation of hydrogen,carbon, nitrogen,and oxygen in silicon wafers during depth profiling using dual-beam TOF-SIMS

The behavior and mechanism of background signals during depth profiling of atmospheric elements using dual-beam time-of-flight secondary ion mass spectrometry (TOF-SIMS) have been experimentally investigated for silicon wafers. The background signals of atmospheric elements were found to be inversely proportional to the sputtering rate. Most of the background signals are largely attributable to the accumulation of components through adsorption and ion bombardment in the pre-equilibrium state. On the other hand, the contribution of real-time adsorption during the instant after the last sputtering in the equilibrium state is negligible under the present experimental conditions. H₂O is dominant in the background formation process of hydrogen and oxygen, which is supported by the higher adsorption coefficients. The background levels of carbon and nitrogen are lower than those of hydrogen and oxygen. Furthermore, the background signal of carbon with respect to the sputtering rate shows a different trend than the other elements. This could be attributed to accumulation in the pre-equilibrium state. These results indicate that the background levels can be lowered close to those of dynamic-SIMS by using an extremely high sputtering rate in dual-beam TOF-SIMS.     

从化学视角剖析烫发、染发原理及顺序*

从头发的结构和组成出发分析头发形状和颜色改变的可能性,剖析烫发、染发的化学原理,阐释先烫发后染发的本质原因,从化学视角辨证地看待烫发、染发的利弊。     

Circularly polarized luminescence based on small organic fluorophores

Circularly polarized luminescence (CPL) has attracted attention as a next-generation light signal because of its carrying more information compared with normal and linearly polarized lights as well as its potential wide application in information fields. Recently, much attention has been paid to small organic molecules-based CPL emitters because of easy synthesis, fine structural modification at molecular level, and tunable wide range emission wavelength. This review highlights the development of small organic molecules-based CPL emitters in the past 5 years (2017–2021). The progress suggests that small organic molecules-based CPL emitters provide a simple and efficient way to generate CPL.     

The Decisive Role of Spin States and Spin Coupling in Dictating Selective O2 Adsorption in Chromium(II) Metal–Organic Frameworks**

The coordinatively unsaturated chromium(II)-based Cr₃[(Cr₄Cl)₃(BTT)₈]₂ (Cr−BTT; BTT³⁻=1,3,5-benzenetristetrazolate) metal–organic framework (MOF) has been shown to exhibit exceptional selectivity towards adsorption of O₂ over N₂/H₂. Using periodic density functional theory (DFT) calculations, we attempted to decipher the origin of this puzzling selectivity. By computing and analyzing the magnetic exchange coupling, binding energies, the partial density of states (pDOS), and adsorption isotherms for the pristine and gas-bound MOFs [(Cr₄(X)₄Cl)₃(BTT)₈]³⁻ (X=O₂, N₂, and H₂), we unequivocally established the role of spin states and spin coupling in controlling the gas selectivity. The computed geometries and gas adsorption isotherms are consistent with the earlier experiments. The binding of O₂ to the MOF follows an electron-transfer mechanism resulting in a Cr^III superoxo species (O₂^.−) with a very strong antiferromagnetic coupling between the two centers, whereas N₂/H₂ are found to weakly interact with the metal center and hence only slightly perturb the associated coupling constants. Although the gas-bound and unbound MOFs have an S=0 ground state (GS), the nature of spin the configurations and the associated magnetic exchanges are dramatically different. The binding energy and the number of oxygen molecules that can favorably bind to the Cr center were found to vary with respect to the spin state, with a significant energy margin (47.6 kJ mol⁻¹). This study offers a hitherto unknown strategy of using spin state/spin couplings to control gas adsorption selectivity in MOFs.     

Electronic structures of CO adsorbed Pt-skin surface on Pt–Co and Pt–Ni alloys

By using angle resolved photoemission spectroscopy, we investigate the electronic structures of Pt-skin layer of Pt–Co and Pt–Ni alloys with CO molecules on the surface. Measured Fermi surface maps and band dispersions reflect the signatures of chemical bonding between Pt-skin layer and CO molecules. Furthermore, the degree of chemical bonding strength of CO molecules, estimated from the energy shift of the participating bands, is found to be reduced on both Pt bimetallic alloys. Our results show how the surface band structure of Pt bimetallic alloys is modified with molecular orbitals of CO molecules on the surface, revealing the important role of the electronic structure in the determination of chemical properties of bimetallic alloys.     

低相对分子质量有机酸对α-FeO(OH)吸附As(Ⅲ)的影响

制备并表征了α-FeO(OH),探究了4种低相对分子质量有机酸(LMW)对α-FeO(OH)吸附As(Ⅲ)的影响,并阐明了机理。 单一和混合LMW对α-FeO(OH)吸附As(Ⅲ)均有抑制作用,4种LMW的影响大小顺序为:草酸(OA)>柠檬酸(CA)>乳酸(LA)、水杨酸(SA)。 混合LMW的影响为:OA会加剧CA对α-FeO(OH)吸附As(Ⅲ)的影响,而SA几乎不起作用。 当ρ(As(Ⅲ))较低,LMW通过与α-FeO(OH)的静电引力、与α-FeO(OH)表面的铁离子形成配合物、生成沉淀从而影响α-FeO(OH)对As(Ⅲ)的吸附;当ρ(As(Ⅲ))较高,LMW还通过阻碍As(Ⅲ)在α-FeO(OH)上的扩散和沉淀作用产生影响。 实验结果为土壤中As(Ⅲ)的迁移转化、污染治理提供技术支撑。     

Treatment of anionic dye aqueous solution using Ti,HDTMA and Al/Fe pillared bentonite. Essay to regenerate the adsorbent

In this study, the adsorption removal of an anionic dye (Congo red) by a local bentonite before and after modification was studied. The modification of the bentonite was made by organophilisation using surfactant (HDTMA) and by pillaring process to obtain a bentonite with Ti pillars and with mixed pillars of Fe/Al. The various synthesized materials are characterized by different techniques such as DRX, MET, N₂ adsorption-desorption, Zeta potential measurement. Results show the development of the texture and the structure of the bentonite after modification. The various adsorbents synthesized show an increase in the adsorption capacity of Congo Red compared to the initial bentonite. Adsorption isotherms are described by the Langmuir model in all cases except that for Ti pillared bentonite, the Freundlich model is more suitable. Pseudo-second order is better for describing the adsorption process. Also, regeneration of the adsorbent is approached in this study by photochemical way and the results show a total regeneration of the adsorbent.     

烯烃对噻吩在介孔分子筛Al-MCM-41活性位物种上吸附脱硫机制的影响

采用后嫁接法制备了不同铝负载量的Al-MCM-41分子筛。运用XRD、N₂吸附-脱附、NH₃-TPD、Py-FTIR等方法对分子筛进行物性表征，利用固定床评价其对噻吩的吸附性能。通过将分子筛吸附噻吩能力与分子筛的酸性质及织构性质进行关联，考察烯烃存在对Al-MCM-41活性位物种吸附脱硫机制的影响。结果表明，铝物种的引入即产生了B酸中心，也同时产生了两种类型的L酸中心L₁和L₂。引入低含量铝物种利于形成B酸中心和L₁型酸中心，引入高含量铝物种利于形成L₂型酸中心。其中，L₂型酸中心对噻吩的吸附效果最佳。烯烃和噻吩在B酸中心发生竞争吸附和催化转化反应，且催化转化反应占主导地位。L₂酸中心的存在促进了B酸中心上的催化转化反应，其所生成的大分子硫化物取代噻吩吸附在分子筛酸活性中心上提高了Al-MCM-41分子筛的饱和吸附硫容量。     

Protein interactions with negatively charged inorganic surfaces

Protein adsorption on charged inorganic solid materials has recently attracted enormous interest owing to its various possible applications, including drug delivery and biomaterial design. The need to combine experimental and computational approaches to get a detailed picture of the adsorbed protein properties is increasingly recognised and emphasised in this review. We discuss the methods frequently used to study protein adsorption and the information they can provide. We focus on model systems containing a silica surface, which is negatively charged and hydrophilic at physiological pH, and two contrasting proteins: bovine serum albumin (BSA) and lysozyme (LSZ) that are both water soluble. At pH 7, BSA has a net negative charge, whereas LSZ is positive. In addition, BSA is moderately sized and flexible, whereas LSZ is small and relatively rigid. These differences in charge and structural nature capture the role of electrostatics and hydrophobic interactions on the adsorption of these proteins, along with the impact of adsorption on protein orientation and function. Understanding these model systems will undoubtedly enhance the potential to extrapolate our knowledge to other systems of interest.