CuYO/γ-Al_2O_3催化剂催化分解N_2O性能

通过等体积浸渍法制备了以γ-Al_2O_3为载体,CuO、Y_2O_3双组分CuYO/γ-Al_2O_3催化剂,通过CuYO/γ-Al_2O_3催化剂的XRD,BET,SEM等表征,分析发现,引入Y_2O_3组分,能够改变催化剂颗粒的结构与形态,提高了CuO在催化剂表面及孔道内的分散度.通过H2-TPR研究发现掺杂Y_2O_3大幅提高了CuO催化剂的还原性能,从而提高了CuYO/γ-Al_2O_3催化剂催化分解N_2O的活性.考察了CuYO/γ-Al_2O_3催化剂催化分解N_2O的活性,结果表明,当CuO和Y_2O_3负载量均为12%时,CuYO/γ-Al_2O_3催化剂催化分解N_2O的活性最高,完全分解N_2O温度为488℃.12Cu12YO/γ-Al_2O_3催化剂在有O2条件下,460℃连续反应100 h,活性仍能保持80%左右;还考察了体积分数为9.1%的水蒸气对12Cu12YO/γ-Al_2O_3催化剂活性的影响.     

金属掺杂的镧锰六铝酸盐催化还原NO

采用共沉淀法制备了以LaMnAl11O19-δ为基础的不同金属元素掺杂的六铝酸盐催化剂LaMnMAl10O19-δ（其中M分别为Fe、Co、Ni、Cu、Zn、Y、Ag、Ce）,对样品进行了XRD、H2-TPR和BET表征,在CH4存在下,考察了催化剂对NO的还原反应活性.实验结果表明,以（NH4）2CO3作沉淀剂制备的...     

LaCu_xZn_(1-x)Al_(11)O_(19-δ)六铝酸盐催化剂分解N_2O的催化性能

采用共沉淀法制备Cu和Zn取代的六铝酸盐(LaCuxZn1-xAl11O19-δ,0.2,0.4,O.5,0.6,0.8,1)催化剂,考察了催化剂对N2O的分解活性.结果表明,在1200℃焙烧4 h可以形成完整的六铝酸盐晶型,Cu和zn能够取代Al3+很好地促进六铝酸盐晶体结构的形成;LaCuxZn1-xAl11O19-δ催化剂对N2O分解有很好的催化活性,其中LaCu0.8Zn0 2Al11O19-δ活性最好.在LaCuxZn1-xAl11O19-δ六铝酸盐中,Cu为N2O催化分解的主要活性元素,Zn有助于提高催化剂的稳定性,但Zn在催化剂中的作用很小.     

以ZrO2为载体的金属氧化物催化剂对NO还原性能的研究

研究了负载于氧化锆载体上的多种金属氧化物在富氧条件下,以丙烯为还原剂,选择性还原NO的活性,考察了CuO和Ag的负载量与活性关系,CuO和Ag单独负载与共同负载时的催化性能,以及氧气浓度对催化剂活性影响.结果表明:在CuO,MgO,La2O3 ,CoO,Fe2O3 ,MoO3和WO3等七种金属氧化物中,CuO活性最好,NO转化率为47.5%,加入活性组分银可明显提高催化剂的NO还原能力,转化率提高到61%.单独负载银时,催化剂活性较差,NO转化率仅为22.1%.在对氧气浓度的考察中,确定在0.4%NO,0.4?H6的反应气中,氧气的最佳含量为2%.     

V2O5/ACF催化剂用于烟气低温脱硝的研究

采用等体积浸渍法制备V_2O_5/ACF,CuO/ACF和Fe_2O_3/ACF催化剂,在H_2O和SO_2存在下,三种催化剂选择性催化还原(SCR)NO_x的活性依次为V_2O_5/ACF>CuO/ACF>Fe_2O_3/ACF.对V_2O_5/ACF催化剂中V_2O_5担载量、反应温度和反应空速对脱硝活性的研究表明,当H_2O和SO_2存在时,V_2O_5的最佳负载量为0.5wt%,在反应温度为180℃,空速为2000 h~(-1)时,NO转化率可达84%,表明该催化剂具有良好的抗H_2O和SO_2毒化的能力.     

ZrO2掺杂的V2O5/TiO2催化剂表征及催化还原NOx

采用共沉淀法制备出不同锆掺杂量的钛锆复合载体(TiO2-ZrO2),运用XRD和BET研究其微观结构,结果显示钛锆物质的量之比1∶1时复合载体具有最大的比表面积,可达256.01 m.2g-1.以此为载体制备了V2O5/TiO2-ZrO2催化剂,并添加少量CeO2对其改性.采用XRD、BET、H2-TPR、原位FT-IR等手段研究其活性组分的表面分散状态、氧化还原特性和表面酸性.结果显示,V2O5高度分散在载体上;与纯V2O5相比,复合载体上V2O5的还原峰向低温方向发生了偏移;催化剂表面包含了大量的B酸和L酸.模拟氨气催化还原NO(NH3-SCR)的脱硝反应活性测试表明,V2O5/TiO2-ZrO2催化剂具有较好的热稳定性和较宽的活性窗口,少量CeO2的加入提高了催化剂的低温活性.     

TiO_2/CuO/Cu_2O(SeO_3)光催化去除水中腐殖酸

以Cu2Se为原料,用溶胶-凝胶法(Sol-Gel)合成了TiO2/CuO/Cu2O(SeO3)光催化剂,用XRD、FTIR和EDAX等方法进行了表征.探讨了催化剂制备过程中焙烧温度对催化剂组成、晶型结构和光催化去除水中腐殖酸性能的影响.当Cu2Se/TiO2焙烧温度为450℃,焙烧2h时,Cu2Se转化为CuO和Cu2O(SeO3).室温下当TiO2/CuO/Cu2O(SeO3)催化剂投加量为1.5g·l-1,溶液pH7.0时,水中腐殖酸的去除率可达到63.6%。     

凹凸棒石负载CuO催化剂脱除气态Hg~0

利用固定床反应器在模拟烟气条件下研究了凹凸棒石(PG)负载CuO催化剂(CuO/PG)对气态Hg~0的脱除.考察了CuO负载量、反应温度、烟气成分、SO_2浓度以及空速等对CuO/PG脱除Hg~0的影响,并利用逐级化学提取和程序升温脱附实验分析了CuO/PG上吸附Hg的形态.结果表明,CuO/PG对Hg~0具有较高的脱除能力,明显高于载体PG,且随CuO负载量的增加而增强(1%—8%);在150—250℃温度范围内,温度升高,CuO/PG对Hg~0的脱除能力降低;HCl对CuO/PG脱除Hg~0具有显著的促进作用,O2具有促进作用,H2O和SO_2具有抑制作用,NO的作用不明显;在6000—15000 h~(-1)空速范围内,空速降低,CuO/PG表现出了更好的脱除Hg~0的能力.逐级化学提取和程序升温脱附实验结果证实,CuO/PG对Hg~0的脱除是吸附和催化氧化的共同作用,Hg~0被氧化为Hg~(2+)的化合物并吸附在CuO/PG上.     

半焦负载Na-Fe催化还原NO的研究

在石英固定床反应器上于常压下研究了煤焦负载Na或Fe催化还原NO的反应，同时研究了Na-Fe复合催化剂的催化特性。研究结果表明：Na或Fe催化剂的催化行为差异较大，低温下Na的催化活性高于相同负载量的Fe，而温度较高时，二者的催化活性顺序与低温时相反。Na的催化活性随负载量的增加而迅速增大，而Fe的催化活性随温度的升高增加迅速。在保持相同的负载量下，一定配比的Na－Fe复合催化剂的催化活性高于其中任何单一催化剂的催化活性。在不加其他还原剂的条件下，负载于煤焦上的Na-Fe复合催化剂可有效地催化还原NO，得到了高的还原转化率。复合催化剂高的催化活性预示Na-Fe在制备过程中的相互作用以及催化半焦还原NO的反应中具有协同作用。     

CuO-ZnO催化剂的XRD和EXAFS研究

用XRD和EXAFS方法研究了CuO-ZnO(50:50)CO_2加氢合成甲醇催化剂的结构.XRD研究发现,在催化剂还原前后,分别存在CuO,ZnO和Cu-ZnO晶相.EXAFS研究发现,在CuO-ZnO中,Cu—O,Cu—Cu键长及Cu的氧配位数、Cu的Cu配位数与纯CuO的十分接近,在Cu-ZnO中,Cu—Wu键长、Cu的Cu配位数与纯Cu的十分接近,说明催化剂在还原前后,CU的近邻结构分别与CuO与Cu的十分接近.纯Cu的活性、选择性很低,而Cu-ZnO的活性、选择性较纯Cu的有很大提高,说明催化剂的性能与催化剂中Cu的近邻结构无关.     

稀土修饰的Co/Hβ催化剂催化分解N_2O

以Hβ分子筛为载体,采用浸渍法制备了一系列以钴为主活性组分,稀土元素为助剂的CoM/Hβ（M=La、Ce、Pr、Nd）催化剂,考察了在含氧条件下直接催化分解N2O的性能.采用X射线衍射、热重-质谱联用系统、H2-TPR、NH3-TPD等方法对催化剂进行了表征.XRD结果表明,Co物种主要以Co3O4尖晶石形态存在.NH3-TPD结果表明,催化剂活性与催化剂的酸性有关.活性评价结果显示,稀土助剂的添加使催化剂活性得到改善,其中以Pr为助剂的催化剂活性最好,N2O转化率达到95%时的反应温度为398℃.     

Ce0.7Zr0.3O2纳米棒的制备及其对柴油车尾气碳颗粒的催化净化性能

本研究以硝酸铈、硝酸锆为原料使用溶剂热合成法,制备了CeO₂-ZrO₂纳米棒催化剂(Ce_0.7Zr_0.3O₂(NR)),并用于柴油车尾气碳颗粒催化净化.催化活性检测证实:Ce_0.7Zr_0.3O₂(NR)纳米棒催化剂可有效净化柴油车尾气碳烟颗粒.在Ce_0.7Zr_0.3O₂(NR)存在下,碳颗粒净化率为10%、50%和90%时,所需温度分别仅为375℃、414℃和455℃,比商用Ce_0.7Zr_0.3O₂和Ce0.3Zr0.7O2催化剂性能更优.采用氮吸附-脱附、X射线光电子能谱(XPS)、H2程序升温还原(H₂-TPR)、X射线衍射(XRD)、拉曼光谱(Raman)、扫描电子显微镜(SEM)和透射电子显微镜(TEM)等技术对催化剂进行表征.XRD和Raman结果证实,Ce_0.7Zr_0.3O₂(NR)主要由立方相CeO₂构成,并掺杂了少量四方相氧化锆.SEM和TEM结果则显示,Ce_0.7Zr_0.3O₂(NR)催化剂颗粒明显由纳米棒堆积而成,特定的纳米形貌会影响其对碳颗粒的催化氧化活性.XPS结果证明Ce_0.7Zr_0.3O₂(NR)催化剂主要具有晶格氧、化学氧和表面吸附氧等氧物种;晶格氧是碳颗粒氧化的活性氧物种,其溢流到催化剂表面可与碳颗粒接触从而提高反应活性;化学氧和表面吸附氧均为表面氧物种,极易与表面固体碳颗粒直接接触,从而可在较低温度下促进碳颗粒的净化.H₂-TPR结果进一步证实了XPS结果,Ce_0.7Zr_0.3O₂(NR)催化剂的低温还原温度比商用Ce_0.7Zr_0.3O₂催化剂更低,且含有更多的易还原氧物种,这些低温易还原氧物种可以在较低温度下参与催化反应,促进柴油车尾气颗粒物的低温催化净化.     

Effect of Cu-ZSM-5 catalysts with different CuO particle size on selective catalytic oxidation of N,N-Dimethylformamide

● A series of Cu-ZSM-5 catalysts were tested for DMF selective catalytic oxidation. ● Cu-6 nm samples showed the best catalytic activity and N₂ selectivity. ● Redox properties and chemisorbed oxygen impact on DMF catalytic oxidation. ● Isolated Cu²⁺ species and weak acidity have effects on the generation of N₂. N, N-Dimethylformamide (DMF), a nitrogen-containing volatile organic compound (NVOC) with high emissions from the spray industry, has attracted increasing attention. In this study, Cu-ZSM-5 catalysts with different CuO particle sizes of 3, 6, 9 and 12 nm were synthesized and tested for DMF selective catalytic oxidation. The crystal structure and physicochemical properties of the catalyst were studied by various characterization methods. The catalytic activity increases with increasing CuO particle size, and complete conversion can be achieved at 300–350 °C. The Cu-12 nm catalyst has the highest catalytic activity and can achieve complete conversion at 300 °C. The Cu-6 nm sample has the highest N₂ selectivity at lower temperatures, reaching 95% at 300 °C. The activity of the catalysts is determined by the surface CuO cluster species, the bulk CuO species and the chemisorbed surface oxygen species. The high N₂ selectivity of the catalyst is attributed to the ratio of isolated Cu²⁺ and bulk CuO species, and weak acidity is beneficial to the formation of N₂. The results in this work will provide a new design of NVOC catalytic oxidation catalysts.     

含氮有机物在Pt／HM,Pd／HM和CuO／HM催化剂上的氧化降解

本文考虑了乙腈、硝基甲烷和乙二胺在Ｐｔ／ＨＭ，Ｐｄ／ＨＭ和ＣｕＯ／ＨＭ催化剂上氧化降解产物随反应温度的变化。在实验温度范围内，含氮产物在Ｎ２，Ｎ２Ｏ和ＮＯ２。随着反应温度的升高，硝基甲烷氧化降解的Ｎ２选择性呈单调下降；而乙腈和乙二胺的Ｎ２选择性出现极小值；高温时Ｎ２选择性升高可能是氧化生成的ＮＯ在高温时更在利于和ＣＮ基或ＮＨ２基相互反应生成Ｎ２的缘故。对于乙腈和乙二胺的催化氧化降解活性为：Ｐｔ／Ｈ     

ZrO2负载过渡金属氧化物催化剂对CO＋NO（O2）反应的影响

本文运用固定床微反技术考察了Ｃｕ,Ｆｅ,Ｍｎ,Ｃｒ,Ｃｏ和Ｎｉ负载（ＺｒＯ２载体）氧化物对ＣＯ＋ＮＯ（Ｏ２）反应的催化活性。研究了ＮＯ和ＣＯ在不同比例时,催化剂对Ｎ２Ｏ和Ｎ２生成的影响。结果表明,在ＮＯ＋ＣＯ反应中,ＮＯ和ＣＯ的比例对催化剂活性和Ｎ２Ｏ,Ｎ２生成均有明显的影响,ＣｕＯｘ／ＺｒＯ２催化剂的活性最高;Ｎ２Ｏ是ＮＯ＋ＣＯ反应的中间产物,低温或ＮＯ过量时有利于生成Ｎ２Ｏ,高温或ＮＯ不足时有     

活性炭催化剂上SO2转化活性中心的研究

研究了用不同原料及不同方法制备的活性炭催化剂物化性质变化及其与SO_2转化为SO_3的催化活性的关系。结果表明,催化剂的活性主要取决于其表面性质,而与其孔结构等物理性质无明显关系。XPS和TPD结果认为,催化剂表面上存在有五种数量不等的基团,即(酮基),(烯酮基),其中,含氧基团=C=O为SH_2转化为SO_3的活性中心,可以经改质手段使糠醛渣活性炭上该基团数量增加,从而可提高催化活性。     

NiB2O4 (B = Mn or Co) catalysts for NH3-SCR of NOx at low-temperature in microwave field

● Microwave-assisted catalytic NH₃-SCR reaction over spinel oxides is carried out. ● SCR reaction temperature is tremendously lowered in microwave field. ● NO conversion of NiMn₂O₄ is highly up to 90.6% at 70°C under microwave heating. Microwave-assisted selective catalytic reduction of nitrogen oxides (NO_x) was investigated over Ni-based metal oxides. The NiMn₂O₄ and NiCo₂O₄ catalysts were synthesized by the co-precipitation method and their activities were evaluated as potential candidate catalysts for low-temperature NH₃-SCR in a microwave field. The physicochemical properties and structures of the catalysts were characterized by X-ray diffraction (XRD), Scanning electron microscope (SEM), N₂-physisorption, NO adsorption-desorption in the microwave field, H₂-temperature programmed reduction (H₂-TPR) and NH₃-temperature programmed desorption (NH₃-TPD). The results verified that microwave radiation reduced the reaction temperature required for NH₃-SCR compared to conventional heating, which needed less energy. For the NiMn₂O₄ catalyst, the catalytic efficiency exceeded 90% at 70 °C and reached 96.8% at 110 °C in the microwave field. Meanwhile, the NiMn₂O₄ also exhibited excellent low-temperature NH₃-SCR reaction performance under conventional heating conditions, which is due to the high BET specific surface area, more suitable redox property, good NO adsorption-desorption in the microwave field and rich acidic sites.     

Catalytic oxidation of o-chlorophenol over Co2XAl (X= Co,Mg, Ca,Ni) hydrotalcite-derived mixed oxide catalysts

• Superior catalytic activity observed for o-chlorophenol oxidation on Co₂MgAlO. • The reducibility, oxygen species and basicity influenced catalytic activity. • The organic by-products were generated in o-chlorophenol catalytic oxidation. A cobalt-based hydrotalcite-like compound was prepared using a constant-pH coprecipitation method. Cobalt-transition metal oxides (Co₂XAlO, X= Co, Mg, Ca and Ni) were investigated for the deep catalytic oxidation of o-chlorophenol as a typical heteroatom contaminant containing chlorine atoms. The partial substitution of Co by Mg, Ca or Ni in the mixed oxide can promote the catalytic oxidation of o-chlorophenol. The Co₂MgAlO catalyst presented the best catalytic activity, and could maintain 90% o-chlorophenol conversion at 167.1°C, compared only 27% conversion for the Co₃AlO catalyst. The results demonstrated that the high activity could be attributed to its increased low-temperature reducibility, rich active oxygen species and excellent oxygen mobility. In the existence of acid and base sites, catalysts with strong basicity also showed preferred activity. The organic by-products generated during the o-chlorophenol catalytic oxidation over Co₂MgAlO catalyst included carbon tetrachloride, trichloroethylene, 2,4-dichlorophenol, and 2,6-dichloro-p-benzoquinon, et al. This work provides a facile method for the preparation of Co-based composite oxide catalysts, which represent promising candidates for typical chlorinated and oxygenated volatile organic compounds.