Combined steam-dry reforming of toluene in syngas over CaNiRu/Al2O3 catalysts

Cracking, steam reforming, dry reforming, and combined steam and dry reforming of toluene in model syngas were performed using catalysts to simulate tar removal produced during biomass gasification. The catalysts were prepared by adding Ru, Ca, and Mn to Ni-based catalysts, and their properties were measured using BET, pulse CO chemisorption, XRD and TG. In steam and dry reforming of toluene, a high toluene conversion was observed with increasing Ca content in the catalyst and catalysts containing Ca showed a higher activity than those containing Mn. In combined steam-dry reforming with syngas, 1%CaNiRu/Al₂O₃ indicated a conversion of 93.9% at 800°C.     

Application of TiO2 nanoparticles for eco-friendly biodiesel production from waste olive oil

An environmentally benign, simple, and efficient process has been developed for biodiesel production from waste olive oil in the presence of a catalytic amount of TiO₂ nanoparticles at 120°C with a conversion of 91.2% within 4 h. The present method affords nontoxic and noncorrosive medium, high yield of biodiesel, clean reaction, and simple experimental and isolation procedures. The catalyst can be recycled by simple filtration and reused without any significant reduction in its activity.     

钙钛矿型催化剂催化燃烧VOCs的抗水蒸气性能研究

用柠檬酸溶胶-凝胶法制备了La0.8M0.2CoO(3M=Sr,Ce,Ba,Ca)4种钙钛矿型复合氧化物催化剂。通入相对湿度为70%的甲苯测试表明,相比较于没有水蒸气存在的情况,4种催化剂的催化活性都有所下降。同时还可发现,A位部分取代的离子不同,催化剂的催化活性下降程度不同,即抗水蒸气性能也不同。所制备的四种催化剂的抗水蒸气性能依次为La0.8Sr0.2CoO3>La0.8Ce0.2CoO3≈La0.8Ca0.2CoO3>La0.8Ba0.2CoO3,其ΔT50%分别为12℃、20℃、20℃和50℃左右,说明除La0.8Ba0.2CoO3外,其它3种对水蒸气具有一定的抗中毒性能。XRD、BET和SEM表征结果证实,水蒸气分子与甲苯分子竞争吸附占据催化剂表面部分活性位,使用于催化氧化甲苯的有效活性位相对减少;同时其与活性组分在高温下发生反应生成新物质,在催化剂表面形成一层致密的涂层,堵塞了原来的孔道结构,从而使催化剂比表面积减少而活性下降。     

负载型TiO2在印染废水降解中的失活及原因分析

研究了负载型TiO2光催化剂在印染废水降解中的失活及其产生的原因。实验结果说明，催化剂活性下降的主要原因有：废水中不溶于水的染料等悬浮物和催化反应中产生的无定形碳在催化剂表面的吸附；高含量的无机离子对催化剂活性位的占据或在表面的沉积；长时间的使用和反复冲洗使TiO2负载量减少。通过同时采用灼烧和酸洗的方法可以使TiO2的活性恢复到新催化剂的69．5％。     

Preparation of MnO2 decorated Co3Fe1Ox powder/monolithic catalyst with improved catalytic activity for toluene oxidation

In this paper, KMnO₄ was used to pre-treat Co₃Fe-layered double hydroxides (LDH) precursor to prepare MnO₂ decorated Co₃Fe₁O_x catalyst. The toluene oxidation performance of the catalyst was investigated systematically. The optimized 0.1MnCF-LDO catalyst exhibited the best catalytic performance, and the temperatures of 50% and 90% toluene conversion (T₅₀ and T₉₀) were 218 and 243°C, respectively. The apparent activation energy (E_a) was 31.6 kJ/mol. The characterization results showed that the pre-redox reaction by KMnO₄ could increase the specific surface area, Co³⁺ species amount and oxygen defect concentration of the catalyst, which are the main reason of the improved toluene catalytic activity. Besides, this method was also applied to enhance toluene oxidation of iron mesh based monolithic catalyst. The 0.1MnCF-LDO/Iron mesh (IM) catalyst showed a 90% toluene conversion at around 316°C which was much lower than that of without MnO₂ addition (359°C). In addition, the water resistant of all the catalysts was studied as well, all the samples showed relatively good water resistance. The toluene conversion still remained to be over >80% even in the presence of 10 vol.% water vapor.     

Na2SO4中毒SCR催化剂对SO3生成特性的影响

为研究Na₂SO₄中毒SCR催化剂（V₂O₅-WO₃/TiO₂催化剂）对SO₃生成特性的影响,采用湿式浸渍法制备w（Na）为3%的Na₂SO₄中毒SCR催化剂,并通过N₂物理吸附/脱附、XRD（X射线衍射）技术、SEM（扫描电镜）、XPS（X射线光电子能谱）分析技术对催化剂的物理化学特性进行表征.结果表明:①随着反应温度的升高,所有催化剂上的SO₃生成率逐渐增加.当温度升至490℃时,SCR催化剂上的SO₃生成率为0.85%,而3% Na₂SO₄中毒SCR催化剂上的SO₃生成率高达1.36%.SO₄2-的存在导致V-O-S增多,从而促进SO₃的生成.②随入口ρ（SO₂）的增加,SO₃生成率呈下降的趋势.当入口ρ（SO₂）为1 000 mg/m3时,3% Na₂SO₄中毒SCR催化剂上的SO₃生成率为1.02%,而SCR催化剂上仅为0.60%.ρ（SO₂）对SO₃生成率的影响主要依赖于温度和催化剂活性位点数等.③N₂物理吸附/脱附、XRD和SEM表征结果表明,与SCR催化剂相比,Na₂SO₄中毒SCR催化剂表面有Na₂SO₄的积聚,出现了裂纹和大孔隙,催化剂的比表面积和孔容下降,这些变化均不利于催化剂的催化性能;XPS结果表明,Na₂SO₄的加入提高了表面化学吸附氧含量,降低了活性组分中w（V4+）/w（V5+）的值.研究显示,相比于SCR催化剂,Na₂SO₄中毒SCR催化剂上的SO₃生成率大幅增加.      

Mesoporous cobalt monoxide-supported platinum nanoparticles: Superior catalysts for the oxidative removal of benzene

Mesoporous Co_3 O_4(meso-Co_3 O_4)-supported Pt(0.53 wt.% Pt/meso-Co304) was synthesized via the KIT-6-templating and polyvinyl alcohol(PVA)-assisted reduction routes.Mesoporous CoO(meso-CoO) was fabricated through in situ reduction of meso-Co304 with glycerol,and the 0.18-0.69 wt.% Pt/meso-CoO samples were generated by the PVA-assisted reduction method.Meso-Co_3 O_4 and meso-CoO were of cubic crystal structure and the Pt nanoparticles(NPs) with a uniform size of ca.2 nm were well distributed on the mesoCo_3 O_4 or meso-CoO surface.The 0.56 wt% Pt/meso-CoO(0.56 Pt/meso-CoO) sample performed the best in benzene combustion(T_(50%)=156℃and T_(90%)=186℃at a space velocity of 80,000 mL/(g h)).Introducing water vapor or C02 with a certain concentration led to partial deactivation of 0.56 Pt/meso-CoO and such a deactivation was reversible.We think that the superior catalytic activity of 0.56 Pt/meso-CoO was intimately related to its good oxygen activation and benzene adsorption ability.     

Fe改性原位Cu/SSZ-13催化剂柴油车尾气脱硝性能研究

以廉价的铜四乙烯五胺(Cu-TEPA)为模板剂,采用水热法原位合成Cu/SSZ-13分子筛,进一步经过浸渍铁对其改性制备Fe-Cu/SSZ-13催化剂.考察铁盐种类及浸渍铁量对其柴油车尾气脱硝活性及水热稳定性的影响.使用XRD、N_2吸附-脱附、H_2-TPR、NH_3-TPD对样品进行表征测试,并分析影响样品脱硝活性以及水热稳定性的原因.结果表明:浸渍量为1.0%时,以Fe(NO_3)_3为铁盐改性得到的Fe-Cu/SSZ-13分子筛催化剂柴油车尾气脱硝效果最佳,在160～530℃温度范围内,NO的转化率能到达90%以上,并且具有优异的N_2选择性和水热稳定性.由分析结果推测,以Fe(NO_3)_3为铁源时,负载在Cu/SSZ-13分子筛上的铁更为牢固,使其抗老化性能提高,且在脱硝过程中铁物种和铜物种同时起到对NO的还原作用.     

纳米Fe/Co催化降解土霉素效果及影响因素研究

为探究液相还原法制备的纳米Fe/Co催化剂的类芬顿催化效果,以单因素分析法研究了pH、OTC（土霉素）初始质量浓度、H₂O₂摩尔浓度和催化剂用量对纳米Fe/Co催化剂催化性能的影响,并通过SEM（扫描电子显微镜）和BET（比表面积测试仪）对纳米Fe/Co催化剂进行表征,进一步研究了纳米Fe/Co催化剂对OTC模拟废水的催化降解效果.结果表明:①纳米Fe/Co催化剂可以有效地改善催化体系的pH使用范围,在pH为3.0~11.0范围内,纳米Fe/Co催化剂对浓度为100 mg/L OTC的去除率（94.0%）高于纳米Fe催化剂（85.0%）;低浓度OTC有利于提高污染物的去除率,而高浓度的OTC有利于提高反应速率;H₂O₂摩尔浓度为200 mmol/L时,纳米Fe/Co催化剂对OTC的去除率最高（93.8%）;纳米Fe/Co催化剂用量为6 g/L时,其对OTC的去除率最高（92.8%）.②纳米Fe/Co催化剂粒径为20~30 nm,比表面积较高,为121.3 m2/g.③纳米Fe/Co催化剂在重复利用13次后OTC去除率仍在50.0%以上,其重复利用性能良好.研究显示,纳米Fe/Co催化剂对OTC废水具有较好的催化性能、重复利用性能以及较宽的pH使用范围,可为含抗生素废水处理提供理论支撑.      

贵阳公路周边尘土和土壤铂族元素特征分析

为降低温室效应气体一氧化碳、氮氧化物及碳氢化合物的排放,全球自上世纪80年代末期开始在汽车中引入铂族元素(PGE)催化剂,其释放的Pt、Pd和Rh等元素在城市道路尘土和路边土壤中聚积,对自然环境及人体健康产生危害。本文在贵州省贵阳市的主要交通路段采集了尘土和土壤样品,对样品中的铂族元素进行了同位素稀释-等离子体质谱法测定。结果表明,所有样品的铂族元素均高于未被污染土壤的背景值,而尘土样品中铂族元素含量明显高于土壤样品。其中Pt、Pd和Rh含量明显高于其它铂族元素(Ru和Ir等),并与Ru和Ir呈一定的正相关关系,表明汽车尾气催化剂的主要组成为Pt、Pd和Rh;高含量的Os具有低的~(187)Os/~(188)Os比值,表明Ru、Ir和Os也源于汽车尾气催化剂,可能是以杂质的形式存在于汽车尾气催化剂中。