低温等离子体协同分子筛净化甲苯的性能研究

本文开展了介质阻挡放电等离子体协同分子筛材料在常温常压下氧化甲苯的研究.结果表明,该系统对甲苯的去除效率与应用电压、分子筛种类有关.甲苯转化率随峰值电压的提高而提高,最高去除率可以达到48.1％.分子筛单位吸附量与该系统对甲苯转化率有关,吸附量越大的分子筛,甲苯转化率越高.     

Heterogeneous activation of persulfate by CuMgAl layered double oxide for catalytic degradation of sulfameter

In this study, a series of CuMgAl layered double oxides (CuMgAl-LDOs) were obtained via calcination of CuMgAl layered double hy-droxides (CuMgAl-LDHs) synthesised via a co-precipitation method. The results show that CuMgAl-LDO can be prepared using an optimal Cu:Mg:Al molar ratio of 3:3:2, NaOH:Na2CO3 molar ratio of 2:1, and calcination temperature of 600 °C. CuMgAl-LDO is a char-acteristic of mesoporous material with a lamellar structure and large specific surface area. The removal efficiency of sulfameter (SMD) based on CuMgAl-LDO/persulfate (PS) can reach>98％over a wide range of initial SMD concentrations (5–20 mg L-1). The best removal efficiency of 99.49％was achieved within 120 min using 10 mg L-1 SMD, 0.3 g L-1 CuMgAl-LDO, and 0.7 mmol L-1 PS. Kinetic analysis showed that the degradation of SMD was in accordance with a quasi-first-order kinetic model. The stability of the CuMgAl-LDO catalyst was verified by the high SMD removal efficiency (> 97％ within 120 min) observed after five recycling tests and low copper ion leaching concentration (0.89 mg L-1), which is below drinking water quality standard of 1.3 mg L-1 permittable in the U.S. Radical scavenging experiments suggest that SO·4- is the primary active species participating in the CuMgAl-LDO/PS system. Moreover, our mechanistic investigations based on the radical scavenging tests and X-ray photoelectron spectroscopy (XPS) results indicate that Cu(II)–Cu(III)–Cu(II) circulation is responsible for activating PS in the degradation of SMD and the degradation pathway for SMD was deduced. Accordingly, the results presented in this work demonstrate that CuMgAl-LDO may be an efficient and stable catalyst for the activation of PS during the degradation of organic pollutants. ? 2020, Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communi-cations Co., Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).     

非平衡等离子体治理有机含磷气体的实验研究

采用脉冲电晕放电产生的等离子体对沙林毒剂的模拟剂甲基磷酸二甲酯进行消除研究.着重进行了脉冲峰压、脉冲频率、初始质量浓度、气体流量等对消除率的影响实验.结果发现,消除率随脉冲峰压和脉冲频率的增加而提高,随气体流量和初始质量浓度的增大而降低.同时发现产物中含有C02、H2O、丙酸、甲基磷酸甲酯和磷酸(或P2O5)等物质.     

The formation of dithionate during the iron(III)-catalysed autoxidation of sulfur(IV)-oxides

The iron(III)-catalyzed autoxidation of sulfur(IV)-oxides results in the formation of two different oxidation products of sulfur(IV): dithionate, S₂O₆²⁻, and sulfate, SO₄²⁻. The yield of these reaction products depends on the experimental conditions. Under the studied conditions ([Fe(III)] : [SIV)] = 1:10, pH = 2–4) dithionate is the minor reaction product. The formation of dithionate is influenced by the initial pH but not by the initial O₂ concentration. The presence of CO²⁺, Mn²⁺, and Ni²⁺ have no influence on the yield of dithionate, whereas in the presence of Cr³⁺ less and, in the presence of Cu²⁺, no dithionate is formed.     

CuBr2分解缓释-膜催化对零价汞的氧化性能研究

以置于多孔陶瓷膜中的CuBr2受热分解所释放的Br2为氧化剂,利用膜催化装置对Hg0氧化效率进行研究,并设计反应-就地检测一体化装置,避免下游气体管壁效应对实验结果带来的影响.结果表明,MnO x/α-Al2O3催化膜对CuBr2分解所产生Br2的释放有较好的"缓释"作用.Hg0和Br2在催化膜表面的吸附和反应可用Langmuir-Hinshelwood机制描述.Hg0氧化效率随Br2浓度增大而升高,但在达到一定浓度后,Hg0和Br2的吸附速率及两者在催化膜表面的反应速率成为限速因素.473~573 K时Hg0氧化效率变化较稳定.烟气中SO2对Hg0氧化有一定抑制作用,NO无明显影响.     

Fe-MCM-41催化臭氧氧化间甲酚废水

首次应用Fe-MCM-41催化臭氧氧化间甲酚废水.研究了铁的掺杂质量分数、催化剂质量浓度和底物质量浓度对间甲酚转化率和TOC去除率的影响,并采用XRD、H2-TPR、穆斯堡尔谱、BET对催化剂的结构性质进行表征.结果表明,铁的掺杂质量分数对Fe-MCM-41在催化臭氧氧化间甲酚中的活性具有较大影响,最佳掺杂质量分数为4.4%.随着铁掺杂质量分数的提高,介孔分子筛的结晶度减弱,介孔结构晶面间距减小,比表面积、孔容、平均孔径整体上呈下降趋势,Fe在介孔分子筛表面仅以γ-Fe2O3形式存在,且催化剂具有良好的铁磁性和稳定性.臭氧在反应中既有直接氧化作用也有间接氧化作用,且二者比近似为1∶1.在模型废水原始p H值条件下,使用Fe掺杂质量分数为4.4%的催化剂,当间甲酚初始质量浓度为500mg·L-1,催化剂质量浓度为0.1 g·L-1时,30 min内间甲酚转化率为100%,TOC去除率为26.8%.     

硅铝比和NiO对ZSM-5协同低温等离子体降解甲苯的影响

研究了不同硅铝比的ZSM-5与Ni/ZSM-5分子筛协同低温等离子体技术对甲苯降解性能的影响.以Ni O(Nickel Oxide)为活性组分,采用浸渍法对ZSM-5分子筛进行改性,利用氮气吸附脱附(BET)、X射线衍射仪(XRD)、X射线光电子能谱分析(XPS)、H_2程序升温还原(H_2-TPR)、NH_3程序升温脱附(NH_3-TPD)、Toluene程序升温脱附(Toluene-TPD)等技术表征样品的物理化学性质.考察了硅铝比对ZSM-5与Ni/ZSM-5分子筛体系中甲苯的吸附性能,研究了不同放电电压下硅铝比对甲苯降解率、碳平衡及二氧化碳选择性的影响,并采用气相色谱-质谱联用仪(GC-MS)分析了催化剂表面的有机产物.结果表明:硅铝比不但影响分子筛本身的物理化学特性(比表面积、氧化还原性能、表面酸性、疏水性等),还会影响Ni的负载形态和方式,更高的硅铝比与Ni O的负载能促进甲苯深度氧化,减少副产物,提高碳平衡和二氧化碳选择性.     

N原子杂化石墨烯高效活化过一硫酸盐降解RBk5染料废水

过硫酸盐高级氧化技术使用过程中,活化剂的大量流失与其环境二次危害是影响该技术应用的主要限制因素.针对这一问题本研究采用改进的Hummers法结合水热法制备环境友好型的N原子掺杂石墨烯作为催化剂,活化过一硫酸盐(PMS)产生硫酸根自由基(SO4-·)和羟基自由基(·OH)降解活性黑5(RBk5)染料.利用傅立叶红外光谱,X-射线光电子能谱,拉曼光谱和透射电子显微镜对N原子掺杂石墨烯进行表征.对催化剂催化性能进行研究,考察了初始p H、催化剂投加量和PMS投加量等因素对降解过程的影响.结果表明,N元素掺杂能够有效提升石墨烯材料的PMS催化活性,且活性受N掺杂比例影响较大;废水的初始p H对降解效率无明显影响.催化剂投加量为1. 5 g·L-1,PMS投加量为0. 3 g·L-1的条件下,反应25min后RBk5染料废水的降解率可达到99%以上,反应过程符合一级反应动力学.自由基猝灭实验显示,N掺杂石墨烯/PMS体系降解RBk5为表面反应,SO4-·和·OH为降解RBk5的主要自由基.循环实验证明催化剂稳定性能良好.