硅铝比对Cu/SSZ-13SCR活性位的影响

采用固态离子交换法制备了不同硅铝比（Si/Al=5,10,25）的Cu/SSZ-13分子筛催化剂,探究硅铝比对其NH₃选择性催化还原（NH₃-SCR）活性位的影响规律,并通过X射线衍射（XRD）,H₂程序升温还原（H₂-TPR）,NO_x程序升温脱附（NO_x-TPD）,NH₃程序升温脱附（NH₃-TPD）,原位红外实验（in situ DRIFTS）等手段进行物化性质表征.活性测试结果表明,当Cu负载量为4wt%时,不同硅铝比的Cu/SSZ-13具有显著差异的SCR活性;其中,Cu/SSZ-13（10）的SCR活性最佳,200~450℃温度范围内NO转化率均大于80%.XRD和H₂-TPR结果表明,硅铝比会影响Cu/SSZ-13的Cu物种的分布和氧化还原性.NO_x-TPD和NH₃-TPD结果表明,3种催化剂中Cu/SSZ-13（10）具有最多Cu²⁺离子,Cu²⁺离子可以为Cu/SSZ-13（10）提供更多的NO_x吸附位点和Lewis酸性位点,而Lewis酸性位是Cu/SSZ-13主要的低温SCR活性位点,因此有利于NH_3-SCR反应的进行.当硅铝比增加到25时,Cu/SSZ-13（25）的Lewis酸性位大量损失,导致其SCR活性明显下降.     

不同制备方法对Cu-SSZ-13催化性能的影响

为了考察制备方法对Cu-SSZ-13催化剂在氨选择性催化还原NO_x(NH_3-SCR)中催化性能的影响,使用不同的方法和载体,制备出理化性质有明显差异的3种催化剂(Cu_(3.9)-Na_(0.8)-SSZ-13、Cu_(5.1)-H-SSZ-13和Cu_(4.0)-Na_(4.0)-SSZ-13),并考察3种催化剂的水热稳定性和抗硫中毒性能.结果表明,由于具有适宜的Cu负载量,并且Cu物种的稳定性极高,一步合成法制备的Cu_(3.9)-Na_(0.8)-SSZ-13催化剂的水热稳定性优于液相离子交换法制备的两种催化剂.而以H-SSZ-13为载体,液相离子交换法负载Cu物种制备的Cu_(5.1)-H-SSZ-13催化剂具有最优的抗硫中毒能力,这与其较多的酸性位有关.因此,含有较多酸性位并且活性物种稳定性高是制备水热稳定性和抗硫中毒能力较优的Cu-SSZ-13催化剂的关键.     

资源型省份环境形势分析及“十三五”环境保护策略

在对历史环境问题进行梳理回顾的基础上,对新常态下作为典型资源型经济省份的山西省面临的环境保护形势进行了分析,并从实施绿色发展战略、改善环境质量、深化环境管理体制创新、加强环境监管、培育生态环保市场主体5个方面给出了基本的策略建议,以期为制定山西省"十三五"环境保护规划提供参考。     

济南市“十三五”环境保护所面临的形势研究

随着我国经济发展进入新常态,"十三五"期间的环境保护工作也进入新阶段,为准确制定济南市"十三五"环境保护规划,文章对济南市经济总体发展情况,农业、工业和服务业发展情况,以及能源消费情况等方面进行了全面分析和预测,对"十三五"期间济南市环境保护工作面临的问题进行了识别,以期对济南市"十三五"环境保护所面临的形式做出全面准确的研判。     

基于无线通讯技术的起重机抬吊同步控制系统改进

本文介绍了基于无线工业以太网通讯的可编程同步检测系统结构和设计方法、同步功能的检测原理及实现方法、调试和操作方法。通过在控制系统中加入信号反馈,将两台起重机的控制执行器信号和末端机械传动的差异值进行反馈跟踪,组成具有反馈功能的抬吊控制系统,在监測到执行器异步或末端传动异步现象时及时控制两车同步停止,从而避免吊物坠落等吊运事故的发生。     

Prenatal diagnosis of trisomy 4p: a new locus for holoprosencephaly?

Trisomy of the short arm of chromosome 4 is a well-known syndrome, and several observations have been made in the last 30 years. Herein, we report a new observation of trisomy 4p in a fetus with a semi-lobar holoprosencephaly (HPE), dysmorphic features and multiple malformations. The diagnosis of HPE was made, at 33 weeks' gestation, on the fetus of a healthy G1P0 woman. Amniocentesis was performed for chromosome analysis and additional material was found on a chromosome 22. The couple elected to terminate the pregnancy and fetal examination was realized. Conventional and molecular cytogenetic studies were performed on the fetus and the parents, which showed that the additional material found on one chromosome 22 corresponded to the short arm of chromosome 4 and therefore led us to establish a diagnosis of trisomy 4p inherited from the malsegregation of a paternal translocation t(4;22)(q12;q11.1). The etiology of HPE is very heterogeneous; it includes non-genetic factors such as maternal diabetes and genetic causes. HPE cases have been described in association with many chromosomal anomalies, trisomy 13 being the most frequent. However, to our knowledge, HPE has never been previously reported in association with a trisomy involving solely the short arm of chromosome 4. Copyright © 2005 John Wiley & Sons, Ltd.     

Decomposition of Al13 promoted by salicylic acid under acidic condition: Mechanism study by differential mass spectrometry method and DFT calculation

Decomposition of the polycation Al₁₃O₄(OH)₂₄(H₂O)₁₂⁷⁺ (Al₁₃) promoted by ligand is a vital subject to advance our understanding of natural and artificial occurrence and evolution of aluminum ions, especially in the case of acidic condition that dissolved Al³⁺ species can be released from the Al-bearing substances. However, the microscopic pathway of synchronous proton-promoted and ligand-promoted decomposition process for Al₁₃ is still in the status of ambiguity. Herein, we applied differential mass spectrometry method and DFT calculation to study the initial detailed process of Al₁₃ decomposition under the presence of proton and salicylic acid (H₂Sal). Mass results showed that the mononuclear Al³⁺-H₂Sal complexes dominated the resulting Al species, whereas the monodentate complex Al₁₃HSal⁶⁺ was not observed in the spectra. The difference of decomposition levels between the ligand/Al ratio 0.2 and 0.5 cases revealed that proton and ligand performed synergistic effect in initial Al₁₃ decomposition process, and the proton transfer determined the ring closure efficiency. The ring closure reaction is the prerequisite for the collapse of Al₁₃ structure and detachment of the mononuclear complex. DFT calculations reveal that hydrogen bond plays an important role in inducing the formation of chelated complex accompanying proton transfer. Attachment of protons at the bridging OH⁻ can elongate and weaken the critical bond between targeted Al³⁺ and µ₄-O^2- resulting from delocalization of electron pairs in the oxygen atom. These results demonstrate the detailed mechanism of Al₁₃ composition promoted by ligand and proton, and provide significant understanding for further application and control of Al₁₃.