Efficient degradation of Rhodamine B by magnetically recoverable Fe3O4-modified ternary CoFeCu-layered double hydroxides via activating peroxymonosulfate

Environment-friendly nano-catalysts capable of activating peroxymonosulfate (PMS) have received increasing attention recently. Nevertheless, traditional nano-catalysts are generally well dispersed and difficult to be separated from reaction system, so it is particularly important to develop nano-catalysts with both good catalytic activity and excellent recycling efficiency. In this work, magnetically recoverable Fe₃O₄-modified ternary CoFeCu-layered double hydroxides (Fe₃O₄/CoFeCu-LDHs) was prepared by a simple co-precipitation method and initially applied to activate PMS for the degradation of Rhodamine B (RhB). X-ray diffraction (XRD), fourier transform infrared spectrometer (FT-IR), scanning electron microscope (SEM), transmission electron microscopy (TEM), Brunauer-Emmett-Teller method (BET), and vibrating sample magnetometer (VSM) were applied to characterize morphology, structure, specific surface area and magnetism. In addition, the effects of several key parameters were evaluated. The Fe₃O₄/CoFeCu-LDHs exhibited high catalytic activity, and RhB degradation efficiency could reach 100% within 20 min by adding 0.2 g/L of catalyst and 1 mmol/L of PMS into 50 mg/L of RhB solution under a wide pH condition (3.0-7.0). Notably, the Fe₃O₄/CoFeCu-LDHs showed good super-paramagnetism and excellent stability, which could be effectively and quickly recovered under magnetic condition, and the degradation efficiency after ten cycles could still maintain 98.95%. Both radicals quenching tests and electron spin resonance (ESR) identified both HO? and SO₄^?? were involved and SO₄^?? played a dominant role on the RhB degradation. Finally, the chemical states of the sample's surface elements were measured by X-ray photoelectron spectroscopy (XPS), and the possible activation mechanism in Fe₃O₄/CoFeCu-LDHs/PMS system was proposed according to comprehensive analysis.     

碳化泡沫负载Co3O4活化过硫酸盐降解罗丹明B

Co₃O₄具有优良的活化过硫酸盐的性能而受到人们的重视,但Co₃O₄粉体易团聚、使用过程中难以分离、易流失和重复利用率差等问题严重制约了其实际应用．通过水热法制备碳化三聚氰胺泡沫负载Co₃O₄非均相催化剂．采用X-射线衍射仪（XRD）和扫描电子显微镜（SEM）对催化剂的结构和表面形貌进行分析．研究不同因素对催化剂活化过硫酸氢钾（PMS）降解罗丹明B（RhB）的性能．其最优催化工艺参数：催化剂投加量为35 mg·L^-1、PMS质量浓度为50 mg·L^-1和pH为7、RhB初始质量浓度为10 mg·L^-1,30 min反应后对RhB降解率为98%．结果表明,增大碳化泡沫负载Co₃O₄非均相催化剂投加量和PMS质量浓度能明显提高对RhB的降解率;而增加RhB初始质量浓度和提高pH值会明显抑制RhB的降解率．催化反应过程符合准一级动力学方程．温度对RhB降...     

废FCC催化剂对水中铅离子的连续吸附及脱附

通过测定吸附等温线，考察了Ｐｂ２＋在废ＦＣＣ（流化催化裂化）催化剂上的吸附性能及规律，结果表明，Ｐｂ２＋在废ＦＣＣ催化剂上的吸附规律可用Ｌａｎｇｍｕｉｒ和Ｆｒｕｎｄｌｉｃｈ模式描述，吸附呈单分子层形式且容易进行。又通过填充床吸附试验，对Ｐｂ２＋的连续吸附及脱附情形作了考察。结果表明，在温度为１５℃、ｐＨ为５．１３、过柱速率为３．０ｍＬ／ｍｉｎ、径高比为２．２５．０条件下，吸附柱具备适宜的生产周期，连续吸附操作可行，柱效率可达７５．９％；在温度为１５℃、采用２ｍｏｌ／Ｌ稀盐酸作脱附剂，过柱速率为５．０ｍＬ／ｍｉｎ的条件下，吸附剂易于脱附再生，脱附效率可达７８．１％     

Semi-closed synthesis of nitrogen and oxygen Co-doped mesoporous carbon for selective aqueous oxidation

Heteroatom-doped meso/micro-porous carbon materials are conventionally produced by harsh carbonization under an inert atmosphere involving specific precursors, hard/soft templates, and heteroatom-containing agents. Herein, we report a facile synthesis of N and O co-doped meso/micro-porous carbon (NOMC) by template-free carbonization of a small-molecule precursor in a semi-closed system. The semi-closed carbonizaiton process yields hydrophilic NOMCs with large surface area in a high yield. The porous structure as well as the elemental composition of NOMCs can be modulated by changing the holding time at a particular temperature. NOMCs as metal-free heterogeneous catalysts can selectively oxidize benzyl alcohol and its derivatives into aldehydes/ketones with>85％conversion in aqueous solution, which is much higher than that of the control sample obtained in tube furnace (21％conversion), mainly due to their high N content, high percentage of pyridinic N, and large surface area. The presence of O-containing moieties also helps to improve the hydrophilicity and dispersion ability of catalysts and thus facilitates the mass transfer process during aqueous oxidation. The NOMC catalysts also dispayed excellent activity for a wide range of substrates with a selectivity of>99％.     

MnOx/TiO2催化剂催化燃烧去除废气中的正己烷

采用溶胶-凝胶法制备了MnOx/TiO2催化剂,考察了n(Mn):n(Ti)、催化剂载体、气体流量对催化燃烧去除废气中正己烷效果的影响.实验结果表明:随着n(Mn):n(Ti)的增加,正己烷去除率先增加后减小,气体流量减小正己烷去除率增大;当n (Mn):n(Ti)为7.85％、气体流量为100 mL/min时,在240℃时正己烷的去除率为90％,MnOx/TiO2催化活性最大;MnOx/TiO2的催化活性优于MnOx/SiO2;SEM和XRD表征结果表明,所制备的MnOx/TiO2是一种活性物种MnOx高度分散的纳米结构催化剂.     

LSH-02G克劳斯尾气加氢催化剂的开发及应用

介绍了LSH-02G克劳斯尾气加氢催化剂的生产工艺及工业应用情况。LSH-02G催化剂具有一定的大孔,可减少CO在催化剂孔道中的停留时间,显著提高催化剂的COS水解率。LSH-02G催化剂工业应用结果表明：装置在80％、100％和110％负荷下运行,各项参数运行正常,急冷水pH稳定在7.8~8.0,急冷塔顶在线氢气含量（φ）维持在1.8%~2.2%,加氢反应器无SO₂穿透。加氢反应器中SO₂加氢转化率均为100％,COS水解率均在92%以上,符合普光天然气净化厂加氢催化剂技术规格书要求（SO₂加氢转化率100％,COS水解率达90%以上）。     

废SCR催化剂中钒和钨的有机酸浸出

在对废SCR催化剂组成进行分析的基础上,采用草酸和酒石酸两种有机酸浸取废SCR催化剂中的V和W。实验结果表明：草酸对V、W的浸出率均大于酒石酸;在草酸浓度为1.00 mol/L、浸取温度为80 ℃、液固比为10 mL/g、浸取时间为180 min时,V和W的浸出率分别为63.50%和13.12%;在酒石酸浓度为0.5 mol/L、浸取温度为100 ℃、液固比为10 mL/g、浸取时间为180 min时,V和W的浸出率分别为44.00%和9.00%。酸性浸出未改变SCR催化剂中TiO₂的晶型,剩余残渣中依然保留着TiO₂骨架,可继续作为催化剂载体使用。     

草酸浸取废SCR催化剂制备光催化剂

采用草酸浸取废SCR催化剂,得到钛钨粉,制备Bi₂WO₆/钛钨粉复合光催化剂,考察了其对罗丹明B的光催化降解性能。制备光催化剂的优化工艺条件为：采用聚乙烯吡咯烷酮为表面活性剂,n（Bi₂WO₆）∶n（钛钨粉）=2∶1,前驱液pH为5,水热反应时间为18 h。在此条件下制备的光催化剂在可见光下降解罗丹明B,反应 60 min,罗丹明B降解率达94.30%。表征结果显示：钛钨粉小颗粒散落在Bi₂WO₆片表面,为光催化反应提供了更多的活性位点;Bi₂WO₆和钛钨粉两者结合可提高光生电子和空穴的分离效率,进而提高催化剂的光催化活性。Bi₂WO₆/钛钨粉光催化剂对罗丹明 B 的降解符合一级反应动力学规律。     

废铜催化剂的综合利用

研究了以湿法回收利用废铜催化剂中的铜、锌制取氧化亚铜和氧化锌的原理以及最佳工艺条件。该工艺可同槽进行浸取、蒸氨、还原、中和水解等操作,生产成本低,产品质量好,工艺过程中无三废排放,具有很好的综合效益。     

Cracking styrene derivative polymers in decalin solvent with metal-supported carbon catalysts

The cracking of styrene derivative polymers dissolved in decalin was conducted with metal-supported carbon catalysts under an inert gas atmosphere to recover monosubstituted styrene or monosubstituted ethylbenzene in higher yields than is obtained by pyrolysis, and to elucidate the detailed reaction mechanisms in the solvent. Poly-(4-methylstyrene), poly-(4-t-butylstyrene), poly-(α-methylstyrene), and polystyrene were used. In decalin without a catalyst, each polymer was decomposed into the monomer, dimer, and trimer derived from the corresponding polymer except for poly-(α-methylstyrene), which was decomposed into the monomer and styrene. By using metal-supported carbon, the olefinic compounds derived from the corresponding polymer were thoroughly hydrogenated to the saturated form in a nitrogen atmosphere by a hydrogen transfer reaction from decalin, which was simultaneously dehydrogenated to tetralin and naphthalene with the evolution of hydrogen gas. In comparison with metal species, Pd- and Ru-supported carbon catalysts maintained the hydrogenation activity for a longer time and with a lower evolution of hydrogen than Pt or Rh. The dehydrogenation of decalin was mainly observed not on the metal surfaces, but on the carbon surfaces over Pd-supported carbon. Stabilization of the monomers will be able to suppress the coking which occurs with repolymerization in long running process. Received: July 19, 2000 / Accepted: March 16, 2001