低温一氧化碳催化氧化研究进展

综述了贵金属 (Au、Pd、Pt)与非贵金属催化剂 (Co、Cu氧化物 )在低温CO氧化反应中的催化机理 ;阐述了催化剂的制备方法 (共沉淀法、细菌还原法、光沉积法、沉积沉淀法、化学气相沉积法、浸渍法等 )、制备条件 (pH值、焙烧温度、焙烧时间、沉淀剂种类等 )及载体种类 (金属氧化物、金属氢氧化物、沸石 )等对催化剂催化活性及稳定性的影响。指出了寻找一种活性、稳定性好且价廉的催化剂 ,以及通过助剂、载体的选择降低贵金属催化剂活性组分的含量 ,提高非贵金属的活性、稳定性的研究工作是今后的重要目标     

锰改性磁铁矿催化NH_3-SCR脱硝性能研究

采用水热法制备锰改性磁铁矿型催化剂用于烧结烟气选择性催化还原脱硝反应,研究水热反应温度对催化剂物理化学性能及脱硝性能的影响。结果表明,160℃水热反应制备的催化剂MnFe_2O_4-160表现出最佳的脱硝性能,在反应温度80℃即可达到90%的脱硝效率。提高锰的平均价态,促进表面吸附氧含量,增大比表面积,有利于提高锰改性磁铁矿催化剂的低温脱硝性能。     

工业MnOx颗粒催化剂的制备及其低温脱硝应用研究

以工业硫酸锰为前体,通过沉淀、洗涤、挤出、煅烧步骤批量制备了高活性颗粒状低温MnO_x脱硝催化剂（?5 mm×30 mm）。针对天然气冷热电三联供高含水低含硫烟气开展应用示范,研究催化剂在不同工况下的脱硝性能与长周期活性稳定性,结果表明：在入口NO_x浓度850~1000 mg/m3、床层温度145~175℃、空速4405 h^-1工况条件下,脱硝率达到87.88%～97.47%,连续运行1180 h后脱硝效率有约3%的微弱衰减。对长周期运行后催化剂进行取样,进行XRD、BET、SEM表征及活性测试结果表明：该催化剂在该高湿烟气长时间运行中发生了一定程度的晶型转变,颗粒烧结、尺寸变大以及比表面积降低,导致其脱硝活性降低。该研究结果将为高活性锰基催化剂的制备及其低温脱硝工业应用提供参考和借鉴。     

负载型锰铈复合氧化物SCR脱硝催化剂制备研究

采用复壁炭纳米管(CNTs)为载体,通过室温氧化还原法制备了锰铈复合氧化物低温NH_3-SCR脱硝催化剂Mn-CeO_x/CNTs。通过调节浸渍液的组成,考察了活性分锰铈配比对催化剂低温脱硝性能的影响。研究发现锰铈协同作用能够有效提高催化剂的低温脱硝性能,当Mn/(Ce+Mn)的摩尔比为0.6时,催化剂的低温活性最好,反应温度为160～180℃时脱硝率可达100%。该方法具有制备工艺简单、条件温和、低温脱硝效果好等优点。     

具有低温活性的高效脱硝催化体系研究进展

NH3选择性催化还原技术在烟气脱硝中应用广泛,但由于传统的氧化钒催化剂起活温度偏高,因此开发具有低温活性的高效脱硝体系成为当前国内外研究热点.介绍了该领域目前已经开发出的贵金属、分子筛、金属氧化物等低温脱硝体系和处于研究前沿的固体杂多酸催化脱硝新体系的最新研究进展.指出固体杂多酸催化体系具有耐硫、抗水抑制等优点,具有很好的研究和应用前景.     

氮氧化物选择性催化还原催化剂研究进展

氮氧化物是形成酸雨和光化学烟雾的主要物种和引发物,消除氮氧化物污染是环境保护中的重点和难点。选择性催化还原作为一种有效脱除氮氧化物的方法,在近年来得到了广泛深入的研究。本文对有关催化体系的文献进行了总结。     

新型铬钴复合氧化物中低温选择性催化NOx还原及原位机理研究

采用固相法合成系列铬钴复合氧化物催化剂,该催化体系在中低温[(180~300)℃]下具有优异的氨选择性催化氮氧化物还原活性,其中,Cr(0.5)-Cr Ox催化剂在空速50 000 h-1、反应温度200℃和220℃条件下,NOx转化率达100%。采用原位DRIFIS研究催化剂表面吸附物种以及催化机理,在反应温度220℃考察Cr(0.5)-Co Ox催化剂表面NH3与NO的吸附态形式和NH3-SCR反应过程中中间态及其反应机理。结果表明,Cr(0.5)-Cr Ox催化剂上NH3吸附在L酸位,也能吸附在B酸位,但只与气态的NOx反应,生成中间体NH2NO,再进一步反应,最终生成N2与H2O。吸附态的NOx不参与SCR反应,反应遵循Eley-Rideal机理。     

低温SCR锰系脱硝催化剂的研究进展

氮氧化物(NO_x)是大气环境的主要污染物之一,对人体健康和生态环境都会造成巨大的危害。选择性催化还原(SCR)是有效的烟气脱硝技术之一,而催化剂是脱硝技术的关键。近年来,锰系金属氧化物催化剂由于在低温SCR反应中表现出优良的催化活性得到了广泛的关注。综述了锰系低温SCR脱硝催化剂的的研究现状,按照非载体型和载体型催化剂进行了介绍,阐述了载体、元素掺杂等因素对锰系催化剂活性的影响,良好活性的催化剂须具有较高的比表面积、无定型的晶态结构。展望了锰系低温SCR脱硝催化剂的研究重点,为进一步研究和提高性能优良的低温锰系SCR脱硝催化剂提供参考信息。     

添加Pt的选择性催化还原催化剂低温去除NOx的研究

以锐钛矿型TiO2为载体,V5O2和WO3为活性组分,添加微量贵金属Pt,制备了选择性催化还原脱硝催化剂,并对催化剂样品进行表征和脱硝性能试验.结果表明,贵金属Pt的加入,使催化剂样品比表面积、起活温度和温度窗口均发生一定的改变,在低温段具有良好的催化活性.在温度160℃和氨氮体积比0.8～1.2时,催化剂的脱硝率较稳...     

用于一氧化碳低温氧化、性能稳定的负载型钠米金催化剂通过技术鉴定

由烟台大学应用催化研究所研制、开发的用于一氧化碳低温氧化、负载型钠米金催化剂近日通过山东省科技厅组织的专家组技术鉴定。采用专利技术制备的一氧化碳（CO）低温氧化催化剂为纳米分散的、负载型金催化剂，可在环境温度-10—50℃、相对湿度60％-100％的条件下清除空气中的有害气体CO，经防毒面具应用试验证明：催化剂对CO催化氧化性能优越，特别在不怕水汽中毒、催化活性高、使用稳定性好、可多次反复使用、耐储存等方面与国内外现用的Hopcalite催化剂相比，其性能有了显著提高，用该催化剂做成的防毒面具其重量和体积仅为原产品的四分之一，甚至更小，且可省去干燥罐。     

CO低温氧化霍加拉特催化剂的研究

综述了CO低温氧化霍加拉特（Hopcalite）催化剂的活性影响因素、催化机理、催化剂失活原因以及最新研究进展,并展望了以后的发展方向。     

催化CO氧化的铜系催化剂的研究进展

综述了近年来铜催化剂体系催化CO氧化反应的研究进展。阐述了催化剂的制备方法、制备条件及载体种类等对催化剂催化活性及稳定性的影响。通过加入添加剂、合适的制备方法和处理条件等手段是提高催化剂活性和选择性有效的途径。     

Alumina supported manganese oxides for the low-temperature selective catalytic reduction of nitric oxide with ammonia

Alumina supported manganese oxides exhibit a high and selective activity for the catalytic reduction of nitric oxide with ammonia (SCR) between 385 and 575 K. Samples with 3–15 wt.-% manganese were studied at space velocities between 22 000–116 000 h⁻¹ and at standard conditions of 500 ppm NO, 550 ppm NH₃ and 2% O₂. Manganese acetate results in a better dispersion of the manganese oxide on the support and a higher specific catalyst activity than manganese nitrate as precursor, for which crystalline structures could be detected. Temperature-programmed reduction revealed that acetate yields Mn₂O₃ and nitrate mainly MnO₂ on the γ-alumina support. The nitric oxide conversion per amount of manganese is fairly independent of the loading for the catalysts prepared from each precursor. The use of ¹⁵NH₃ reveals that it reacts in a 1:1 molar ratio with nitric oxide towards ¹⁵NN and/or ¹⁵NNO. The SCR activity (to nitrogen) is strongly dependent on the oxygen partial pressure, whereas water inhibits reversibly. Lattice oxygen of the catalyst is not able to maintain the SCR reaction in the absence of oxygen. The nitrous oxide formation is independent of the oxygen partial pressure, but increases with increasing manganese loading and with temperature, resulting in lower selectivities for nitrogen formation. The nitrogen and nitrous oxide formation probably occur at different sites. Above 525 K ¹⁵NH₃ oxidation occurs, yielding mainly ¹⁵N₂O and ¹⁵NO, depending on the temperature. The nitrous oxide is not further reduced by ammonia over this type of catalyst. The addition of tungsten to the catalyst increases the selectivity for nitrogen considerably. The stability of the ex-acetate catalyst is good, for at least 600 h the activity remained constant. The catalysts are sensitive towards sulphur dioxide, the ex-acetate catalysts the least, due to the strong interaction with the alumina support, as is revealed by TPR.     

Nitric oxide reduction and carbon monoxide oxidation over carbon-supported copper-chromium catalysts

Carbon supported copper-chromium catalysts are shown to be very active for both the reduction of nitric oxide with carbon monoxide and the oxidation of carbon monoxide with oxygen. Mixed copper-chromium oxide active phases have good activity in the simultaneous removal of nitric oxide and carbon monoxide from exhaust gases. The influence of several catalyst variables has been investigated. The activity per volume of catalyst increases with increasing loading, while the intrinsic activity shows a maximum around C/M=100−50. An optimum catalyst for nitric oxide reduction and carbon monoxide oxidation has a copper/chromium ratio of 2/1. The apparent activation energy for the carbon monoxide oxidation over carbon supported copper-chromium catalysts is 77 kJ/mol, suggesting that the Cu---O bond rupture is the rate-limiting process. The reduction of nitric oxide takes place at higher temperatures. Since all catalysts have a low selectivity for molecular nitrogen formation at lower temperatures, the dissociation of nitric oxide is probably rate determining, resulting in a slightly reduced catalyst system. In an excess of carbon monoxide the reaction is first-order in nitric oxide and zero-order in carbon monoxide. Moisture inhibits the reaction by reversible competitive adsorption, whereas carbon dioxide does not. Oxygen completely inhibits the reduction of nitric oxide due to the more rapid reoxidation of the catalytic sites compared to nitric oxide. Therefore, the reduction of nitric oxide takes place only when all oxygen has been converted and, hence, is shifted to higher temperatures. As a possible consequence, the production of nitrous oxide is reduced. Nitric oxide and molecular oxygen react preferentially with carbon monoxide, so, in an excess of oxidizing component, gasification of the carbon support occurs at higher temperatures after carbon monoxide has been completely consumed.     

La2O3对MnO2碳热还原的催化

研究了稀土氧化物La2O3作为添加剂对MnO2碳热还原的作用,通过还原实验,发现La2O3对MnO2碳热还原具有催化作用,对还原后试样进行SEM分析,认为其催化作用是通过催化试样中碳的气化反应而实现的.     

添加WO_3对铈钴催化剂CO氧化性能的影响

采用共沉淀法制备xWO_3-Ce O2-Co_3O_4复合型非贵金属CO低温催化剂,考察不同WO_3添加量和空速对催化剂催化活性的影响,并考察催化剂的抗硫性能。通过孔隙结构测试、H2-TPR、FT-IR和SEM等对催化剂进行表征。结果表明,WO_3添加质量分数1%时,催化剂具有最佳的低温活性。在CO进口体积分数0.12%、O2进口体积分数5%和空速15 000 h-1条件下,50℃时,CO转化率即可达到99.6%,60℃时,CO转化率达100%。添加WO_3,催化剂氧化能力增强,催化效率提高。随着空速升高,CO转化率下降。WO_3的加入可有效提高催化剂的比表面积,抑制硫酸盐在催化剂表面聚集,提高催化剂的抗硫性能。     

用于降低卷烟烟气中CO含量的Pd-Cu/活性炭催化剂

用浸渍法制备用于降低卷烟烟气中CO含量的Pd-Cu/活性炭催化剂,考察该催化剂对模拟卷烟烟气[4.4%CO-4.2%H2O-19.2%O2-72.2%N2(体积分数)]中的CO常温催化氧化性能,研究催化剂活性组分及其负载量、催化剂栽体、原料气中CO浓度和气体空速对催化剂的CO常温氧化活性的影响.研究表明,生产成本较低的...     

Ellipsometric study of a palladium catalyst during the oxidation of carbon monoxide and methane

Spectroscopic ellipsometry is used to monitor the surface of a thick Pd‐film catalyst during the oxidation of either carbon monoxide or methane. Dense PdO layers form under sufficiently lean conditions (excess oxygen) for both reactions. A stable metal surface exists in the case of CO, but a very porous PdO layer develops in the case of methane, under rich conditions. There is a large hysteresis in the conditions for PdO formation in the case of CO oxidation. Spontaneous oscillations in catalytic activity and Pd‐surface composition occur for both reactions, the higher activities corresponding to O‐atom‐rich or PdO‐rich surfaces for CO or methane oxidation, respectively. This revised version was published online in August 2006 with corrections to the Cover Date.     

一氧化碳还原硫酸镁制备氧化镁的工艺研究

应用热力学原理计算并分析了一氧化碳还原无水硫酸镁制备氧化镁反应的可能性;研究了反应温度、加热时间和样品粒径对无水硫酸镁分解率的影响; 并且通过正交设计与实验,给出了制备氧化镁的优化工艺条件：反应温度为973.15 K、加热时间为30 min、样品粒径为106 μm。采用此工艺,硫酸镁的分解率达到99.3%。得到的氧化镁晶型单一,呈多孔形貌,符合HG/T 2573-2006《工业轻质氧化镁》标准规定的I类优等品质量指标。