Pd/TiO2催化水体中四溴双酚A的电催化还原脱溴

以TiO₂、Al₂O₃、CeO₂和SiO₂为载体，采用浸渍法制备Pd基催化剂，并通过透射电镜(TEM)、X射线衍射(XRD)、X射线光电子能谱(XPS)和电感耦合等离子体发射光谱(ICP-OES)等手段对催化剂的结构进行了详细表征.以Pd/TiO₂为催化剂，研究四溴双酚A(TBBPA)在阴极池的电催化还原.结果表明，悬浮体系中Pd基催化剂的催化活性远高于固定体系；与其他载体相比，Pd/TiO₂的电催化还原活性最高；反应过程符合Langmuir-Hinshelwood模型，受控于TBBPA在催化剂表面的吸附过程；随着恒定电流和Pd负载量的增大，TBBPA电催化还原反应的初活性呈现火山型变化规律；经过5次循环使用，Pd/TiO₂催化剂仍能够完全去除TBBPA，具有良好的稳定性.     

Fe@CeO2/CN双空腔核壳磁性载金椭球催化剂及其催化还原对硝基苯酚和染料污染物

载金催化剂可在温和条件下还原性降解环境中某些有毒有害污染物,并转化为低毒性、高附加值的物质,从而促进水体污染物化学资源转化和综合利用.本文设计制备Fe@CeO₂/CN双空腔核壳磁性载金椭球催化剂,用于还原降解水体中对硝基苯酚和染料污染物.该催化剂先制备Fe₂O₃@CeO₂梭型微粒内核,采用乙二胺介导的Stober扩展法在其表面合成SiO₂@RF复合物,经过碳化-水热蚀刻得到具有介孔碳氮壳层的Fe₂O₃@CeO₂/CN椭球;采用[Au(en)₂]³⁺为金前驱体的沉积沉淀-还原气氛热处理法在上述椭球中构筑较好分散度超细纳米Au颗粒,同时Fe₂O₃转化为小体积Fe颗粒并形成内空腔,得到Fe@CeO₂-Au/CN双空腔核壳磁性椭球催化剂.该催化剂独特的结构特征和复合组分协同增强性效应使其在还原降解对硝基苯酚和染料...     

沉淀陈化对Ce0.7Mn0.3Ox催化净化柴油车尾气碳颗粒的影响

采用沉淀陈化法制备了Ce∶Mn摩尔比为7∶3的CeO_2-MnO_x复合氧化物(Ce_(0.7)Mn_(0.3)O_x-PR),并使用X射线多晶粉末衍射(XRD)、场发射扫描电子显微镜(SEM)、高分辨率透射电子显微镜(TEM)、N_2吸附-脱附、X射线光电子能谱(XPS)和拉曼光谱(Raman)对所制备复合氧化物催化剂进行表征.结果表明,沉淀陈化过程可有效促进Ce_(0.7)Mn_(0.3)O_x-PR催化剂晶粒的生长,稳定催化剂的织构性质,且明显有利于Mn离子进入CeO_2晶格,减少MnO_x物种在催化剂表面的聚集.Mn离子进入CeO_2晶格可有效增加Ce_(0.7)Mn_(0.3)O_x-PR催化剂的晶格氧和氧空位,从而有助于其表现出更优异的碳颗粒催化氧化性能.所制备的Ce_(0.7)Mn_(0.3)O_x-PR催化剂对碳颗粒催化氧化的起燃温度(T_(50))为362℃、完全转化温度(T_(90))为419℃,该性能明显优于传统共沉淀法所制备的Ce_(0.7)Mn_(0.3)O_x-CP催化剂的性能(T_(50)、T_(90)分别为376℃、457℃).     

改性FeCo2O4活化PMS降解水中2,4-二氯苯氧乙酸

以离子液体为氮源、磷源和氟源,采用一步水热法将N、P、F的3种元素掺杂到FeCo₂O₄中合成了NPF-FeCo₂O₄催化剂,用于活化过一硫酸氢钾(PMS)降解水中2,4-二氯苯氧乙酸(2,4-D).分别采用透射电子显微镜(TEM)、X射线光电子能谱(XPS)、傅立叶红外光谱(FTIR)、X射线衍射(XRD)对催化剂进行表征.实验结果表明,当催化剂投加量为0.1 g·L^-1、PMS浓度为1 mmol·L^-1时,反应30 min后2,4-D的去除率可达100%;初始pH值在3到9的范围内,体系对2,4-D的去除效果不受影响,水中低浓度的Cl^-、HCO₃^-和腐殖酸对反应有轻微的抑制.通过电子自旋共振波谱(EPR)测试结果显示,相较于FeCo₂O₄和NP-FeCo₂O₄催化剂,NPF-FeCo₂     

Ce(x)Mn/TiO2-y催化剂低温NH3-SCR脱硝性能

以锐钛矿TiO₂(P25)为载体采用原位生长法负载锰氧化物制备了Mn/TiO₂催化剂,再以等体积浸渍-煅烧法对该催化剂掺杂氧化铈制备Ce(x)Mn/TiO₂-y催化剂用以烟气低温SCR脱硝.在固定锰负载量(质量分数为8%)的基础上,考察了铈掺杂量(铈锰摩尔比)、煅烧温度对催化剂SCR脱硝性能的影响.采用TEM、BET、XRD和XPS等手段表征了催化剂的理化结构特性.结果发现,当Ce/Mn的摩尔比例为1.0,煅烧温度为300℃时,Ce(1.0)Mn/TiO₂-300催化剂在150—300℃温度范围内、10500—27000 h^-1的空速范围内,能够保持90%以上的NO转化率.理化性能分析结果表明,煅烧温度对催化剂的微观形貌影响显著,随着煅烧温度的升高,Ce(1.0)Mn/TiO₂-500催化剂活性物种颗粒集聚明显、比表面积降低,且锰氧化物价态分布偏向于低价态;铈的掺杂有助于Ce(1.0)Mn/TiO₂-300催化剂活性物种在载体表面的均匀分散,可以促进产生更多的Mn4+物种和更多的吸附氧,有利于催化剂低温SCR脱硝性能的提升.     

Fe3O4/MoS2强化过氧化单硫酸盐活化去除2,4-二氯苯氧乙酸

以MoS₂为载体,通过水热法合成Fe₃O₄/MoS₂催化剂,采用X射线衍射、透射电子显微镜和X射线光电子能谱分析对材料进行表征,研究了Fe₃O₄/MoS₂/PMS体系中2,4-二氯苯氧基乙酸（2,4-D）的降解效率并探究了其反应机理.结果表明,以Fe₃O₄、MoS₂和Fe₃O₄/MoS₂为催化剂,30 min内2,4-D的去除率分别为31%、 20%和89%.表征结果发现,在MoS₂的存在下,Fe₃O₄表面的Fe（Ⅲ）还原为Fe（Ⅱ）,Mo（Ⅳ）被氧化为Mo（Ⅵ）,Fe₃O₄和MoS₂间的协同作用加强了PMS分解,提高了2,4-D去除效率.自由基淬灭实验表明,·OH、 SO<...     

以NH2-MIL-53(Al)为前驱体制备多孔掺碳Al2O3吸附剂及其对水中Cr(Ⅵ)的吸附性能

铬是污染性金属元素,铬含量是水质污染控制的一项重要指标,其中Cr(Ⅵ)的毒性最大,且易被人体吸收.本研究以水中的Cr(Ⅵ)吸附传质分离为目标,利用以铝为金属源水热法合成的铝基MOFs为前驱体,600℃煅烧后制备了多孔掺碳Al₂O₃吸附材料,利用现代分析技术对其进行微观结构表征,探究了其吸附作用能力与机制.研究结果表明,XRD、SEM、BET等表征手段证明了NH₂-MIL-53(Al)与多孔掺碳Al₂O₃结构的成功合成.前驱体NH₂-MIL-53(Al)和煅烧后的衍生物多孔掺碳Al₂O₃,在形貌上相似,且多孔掺碳Al₂O₃材料(180.24 m²·g^-1)的比表面积要大于NH₂-MIL-53(Al)(116.73 m²·g^-1).多孔掺碳Al₂     

杂原子掺杂碳材料用于电合成过氧化氢的研究进展

过氧化氢(H₂O₂)可广泛应用于市政饮用水、工业废水和城市污水的处理.然而,过氧化氢在储存和运输方面的风险(如腐蚀和爆炸)限制了其在分散式水处理中的应用.以二电子氧还原反应(2eORR)原位合成H₂O₂用于分散式水处理具有良好的应用前景.然而,未被催化的2e^-ORR动力学缓慢、选择性差,不能满足大规模生产的要求.相比之下,杂原子掺杂碳材料具有良好的2e^-ORR活性、选择性和稳定性.本文回顾了2e^-ORR的反应机理和催化剂的改性原理,进一步描述了杂原子N、O、F掺杂碳材料的作用机理,并总结了几种具有优秀2e^-ORR催化活性和选择性的掺杂结构.最后,对杂原子掺杂碳材料合成H₂O₂应用于水处理的未来发展进行了展望.     

表面活性剂(十六烷基三甲基溴化铵)辅助合成Bi2MoO6光催化剂协同PMS降解AO7

采用CTAB辅助水热法合成钼酸铋(Bi₂MoO₆,BMO)微球,并将其用于活化过一硫酸盐(PMS),在可见光下降解废水中的偶氮染料金橙Ⅱ(AO7).利用X射线衍射(XRD),傅里叶红外光谱仪(FT-IR),扫描电子显微镜(SEM),X射线能谱(XPS),透射电子显微镜(TEM)和紫外-可见漫反射光谱(UV-vis)对催化剂进行了表征,并通过降解实验测试其催化性能.结果表明,合成的催化剂具有良好的吸附、催化降解AO7的性能.在中性条件下,催化剂投加量0.3 g·L^-1,AO7浓度0.1 mmol·L^-1,PMS浓度1 mmol·L^-1,可以在30 min内完全降解AO7.研究了催化剂含量、pH、共存阴离子等对AO7降解效果的影响.通过自由基消除实验,探索了0.10CTAB-BMO/光/PMS体系中存在的活性物种(h⁺、·O₂^-、¹O₂、·OH和SO₄...     

UV/H2O2对盐酸林可霉素的光催化降解及生物毒性分析

本文以盐酸林可霉素(LCM)为研究对象,探究其在UV/H₂O₂降解作用下的降解情况,探讨了H₂O₂浓度、初始pH值和有机物等影响因素对LCM的影响及机制.实验结果表明,当H₂O₂浓度为50 mg·L^-1,pH=7.3,LCM浓度为10 mg·L^-1,反应30 min后,LCM去除率达到98%,且反应过程遵循准一级动力学.利用高效液相色谱串联飞行时间质谱仪(LCMS-TOF 5600+)鉴别出其在UV/H₂O₂降解过程中主要产物的分子结构式,进而推导出可能的降解路径.利用TEST对降解过程中的产物进行毒性预测,结果表明,中间产物的毒性高于母体,对水质安全保障造成潜在风险.     

Fe2O3-CeO2-Bi2O3/γ-Al2O3 catalyst in the catalytic wet air oxidation (CWAO) of cationic red GTL under mild reaction conditions

Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃, an environmental friendly material, was investigated. The catalyst exhibited good catalytic performance in the CWAO of cationic red GTL. The apparent activation energy for the reaction was 79 kJ·mol⁻¹. HO₂· and O₂·⁻ appeared as the main reactive species in the reaction. The Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃ catalyst, a novel environmental-friendly material, was used to investigate the catalytic wet air oxidation (CWAO) of cationic red GTL under mild operating conditions in a batch reactor. The catalyst was prepared by wet impregnation, and characterized by special surface area (BET measurement), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The Fe₂O₃-CeO₂-Bi₂O₃/γ-Al₂O₃ catalyst exhibited good catalytic activity and stability in the CWAO under atmosphere pressure. The effect of the reaction conditions (catalyst loading, degradation temperature, solution concentration and initial solution pH value) was studied. The result showed that the decolorization efficiency of cationic red GTL was improved with increasing the initial solution pH value and the degradation temperature. The apparent activation energy for the reaction was 79 kJ·mol⁻¹. Hydroperoxy radicals (HO₂·) and superoxide radicals (O₂⁻·) appeared as the main reactive species upon the CWAO of cationic red GTL.     

Catalytic oxidation of CO over Pt/Fe3O4 catalysts: Tuning O2 activation and CO adsorption

• Strong metal-support interaction exists on Pt/Fe₃O₄ catalysts. • Pt metal particles facilitate the formation of oxygen vacancies on Fe₃O₄. • Fe₃O₄ supports enhance the strength of CO adsorption on Pt metal particles. The self-inhibition behavior due to CO poisoning on Pt metal particles strongly impairs the performance of CO oxidation. It is an effective method to use reducible metal oxides for supporting Pt metal particles to avoid self-inhibition and to improve catalytic performance. In this work, we used in situ reductions of chloroplatinic acid on commercial Fe₃O₄ powder to prepare heterogeneous-structured Pt/Fe₃O₄ catalysts in the solution of ethylene glycol. The heterogeneous Pt/Fe₃O₄ catalysts achieved a better catalytic performance of CO oxidation compared with the Fe₃O₄ powder. The temperatures of 50% and 90% CO conversion were achieved above 260°C and 290°C at Pt/Fe₃O₄, respectively. However, they are accomplished on Fe₃O₄ at temperatures higher than 310°C. XRD, XPS, and H₂-TPR results confirmed that the metallic Pt atoms have a strong synergistic interaction with the Fe₃O₄ supports. TGA results and transient DRIFTS results proved that the Pt metal particles facilitate the release of lattice oxygen and the formation of oxygen vacancies on Fe₃O₄. The combined results of O₂-TPD and DRIFTS indicated that the activation step of oxygen molecules at surface oxygen vacancies could potentially be the rate-determining step of the catalytic CO oxidation at Pt/Fe₃O₄ catalysts. The reaction pathway involves a Pt-assisted Mars-van Krevelen (MvK) mechanism.     

Enhanced catalytic oxidation of 2,4-dichlorophenol via singlet oxygen dominated peroxymonosulfate activation on CoOOH@Bi2O3 composite

• Bi₂O₃ cannot directly activate PMS. • Bi₂O₃ loading increased the specific surface area and conductivity of CoOOH. • Larger specific surface area provided more active sites for PMS activation. • Faster electron transfer rate promoted the generation of reactive oxygen species. • ¹O₂ was identified as dominant ROS in the CoOOH@Bi₂O₃/PMS system. Cobalt oxyhydroxide (CoOOH) has been turned out to be a high-efficiency catalyst for peroxymonosulfate (PMS) activation. In this study, CoOOH was loaded on bismuth oxide (Bi₂O₃) using a facile chemical precipitation process to improve its catalytic activity and stability. The result showed that the catalytic performance on the 2,4-dichlorophenol (2,4-DCP) degradation was significantly enhanced with only 11 wt% Bi₂O₃ loading. The degradation rate in the CoOOH@Bi₂O₃/PMS system (0.2011 min⁻¹) was nearly 6.0 times higher than that in the CoOOH/PMS system (0.0337 min⁻¹). Furthermore, CoOOH@Bi₂O₃ displayed better stability with less Co ions leaching (16.4% lower than CoOOH) in the PMS system. These phenomena were attributed to the Bi₂O₃ loading which significantly increased the conductivity and specific surface area of the CoOOH@Bi₂O₃ composite. Faster electron transfer facilitated the redox reaction of Co (III) / Co (II) and thus was more favorable for reactive oxygen species (ROS) generation. Meanwhile, larger specific surface area furnished more active sites for PMS activation. More importantly, there were both non-radical (¹O₂) and radicals (SO₄⁻•, O₂⁻•, and OH•) in the CoOOH@Bi₂O₃/PMS system and ¹O₂ was the dominant one. In general, this study provided a simple and practical strategy to enhance the catalytic activity and stability of cobalt oxyhydroxide in the PMS system.     

Size and shape effects of MnFe2O4 nanoparticles as catalysts for reductive degradation of dye pollutants

• Size and shape-dependent MnFe₂O₄ NPs were prepared via a facile method. • Ligand-exchange chemistry was used to prepare the hydrophilic MnFe₂O₄ NPs. • The catalytic properties of MnFe₂O₄ NPs toward dye degradation were fully studied. • The catalytic activities of MnFe₂O₄ NPs followed Michaelis–Menten behavior. • All the MnFe₂O₄ NPs exhibit selective degradation to different dyes. The magnetic nanoparticles that are easy to recycle have tremendous potential as a suitable catalyst for environmental toxic dye pollutant degradation. Rationally engineering shapes and tailoring the size of nanocatalysts are regarded as an effective manner for enhancing performances. Herein, we successfully synthesized three kinds of MnFe₂O₄ NPs with distinctive sizes and shapes as catalysts for reductive degradation of methylene blue, rhodamine 6G, rhodamine B, and methylene orange. It was found that the catalytic activities were dependent on the size and shape of the MnFe₂O₄ NPs and highly related to the surface-to-volume ratio and atom arrangements. Besides, all these nanocatalysts exhibit selectivity to different organic dyes, which is beneficial for their practical application in dye pollutant treatment. Furthermore, the MnFe₂O₄ NPs could be readily recovered by a magnet and reused more than ten times without appreciable loss of activity. The size and shape effects of MnFe₂O₄ nanoparticles demonstrated in this work not only accelerate further understanding the nature of nanocatalysts but also contribute to the precise design of nanoparticles catalyst for pollutant degradation.     

Catalytic activity of cerium-doped Ru/AlO during ozonation of dimethyl phthalate

In this paper, factors influencing the mineralization of dimethyl phthalate (DMP) during catalytic ozonation with a cerium-doped Ru/Al₂O₃ catalyst were studied. The catalytic contribution was calculated through the results of a comparison experiment. It showed that doping cerium significantly enhanced catalytic activity. The total organic carbon (TOC) removal over the doped catalyst at 100 min reached 75.1%, 61.3% using Ru/Al₂O₃ catalyst and only 14.0% using ozone alone. Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto Al₂O₃ support. Results of experiments on oxidation by ozone alone, adsorption of the catalyst, Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%, which showed the obvious effect of Ru–Ce/Al₂O₃ on catalytic activity.     

Simultaneous removal of NOx and chlorobenzene on V2O5/TiO2 granular catalyst: Kinetic study and performance prediction

• A V₂O₅/TiO₂ granular catalyst for simultaneous removal of NO and chlorobenzene. • Catalyst synthesized by vanadyl acetylacetonate showed good activity and stability. • The kinetic model was established and the synergetic activity was predicted. • Both chlorobenzene oxidation and SCR of NO follow pseudo-first-order kinetics. • The work is of much value to design of multi-pollutants emission control system. The synergetic abatement of multi-pollutants is one of the development trends of flue gas pollution control technology, which is still in the initial stage and facing many challenges. We developed a V₂O₅/TiO₂ granular catalyst and established the kinetic model for the simultaneous removal of NO and chlorobenzene (i.e., an important precursor of dioxins). The granular catalyst synthesized using vanadyl acetylacetonate precursor showed good synergistic catalytic performance and stability. Although the SCR reaction of NO and the oxidation reaction of chlorobenzene mutually inhibited, the reaction order of each reaction was not considerably affected, and the pseudo-first-order reaction kinetics was still followed. The performance prediction of this work is of much value to the understanding and reasonable design of a catalytic system for multi-pollutants (i.e., NO and dioxins) emission control.     

One-pot hydrothermal fabrication of BiVO4/Fe3O4/rGO composite photocatalyst for the simulated solar light-driven degradation of Rhodamine B

• BiVO₄/Fe₃O₄/rGO has excellent photocatalytic activity under solar light radiation. • It can be easily separated and collected from water in an external magnetic field. • BiVO₄/Fe₃O₄/0.5% rGO exhibited the highest RhB removal efficiency of over 99%. • Hole (h⁺) and superoxide radical (O₂^•−) dominate RhB photo-decomposition process. • The reusability of this composite was confirmed by five successive recycling runs. Fabrication of easily recyclable photocatalyst with excellent photocatalytic activity for degradation of organic pollutants in wastewater is highly desirable for practical application. In this study, a novel ternary magnetic photocatalyst BiVO₄/Fe₃O₄/reduced graphene oxide (BiVO₄/Fe₃O₄/rGO) was synthesized via a facile hydrothermal strategy. The BiVO₄/Fe₃O₄ with 0.5 wt% of rGO (BiVO₄/Fe₃O₄/0.5% rGO) exhibited superior activity, degrading greater than 99% Rhodamine B (RhB) after 120 min solar light radiation. The surface morphology and chemical composition of BiVO₄/Fe₃O₄/rGO were studied by scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, UV–visible diffuse reflectance spectroscopy, Fourier transform infrared spectroscopy, and Raman spectroscopy. The free radicals scavenging experiments demonstrated that hole (h⁺) and superoxide radical (O₂^•−) were the dominant species for RhB degradation over BiVO₄/Fe₃O₄/rGO under solar light. The reusability of this composite catalyst was also investigated after five successive runs under an external magnetic field. The BiVO₄/Fe₃O₄/rGO composite was easily separated, and the recycled catalyst retained high photocatalytic activity. This study demonstrates that catalyst BiVO₄/Fe₃O₄/rGO possessed high dye removal efficiency in water treatment with excellent recyclability from water after use. The current study provides a possibility for more practical and sustainable photocatalytic process.     

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 ozonation of organic compounds in water over the catalyst of RuO2/ZrO2-CeO2

This research investigates the performances of RuO₂/ZrO₂-CeO₂ in catalytic ozonation for water treatment. The results show that RuO₂/ZrO₂-CeO₂ was active for the catalytic ozonation of oxalic acid and possessed higher stability than RuO₂/Al₂O₃ and Ru/AC. In the catalytic ozonation of dimethyl phthalate (DMP), RuO₂/ZrO₂-CeO₂ did not enhance the DMP degradation rate but significantly improved the total organic carbon (TOC) removal rate. The TOC removal in catalytic ozonation was 56% more than that in noncatalytic ozonation. However this does not mean the catalyst was very active because the contribution of catalysis to the overall TOC removal was only 30%. The adsorption of the intermediates on RuO₂/ZrO₂-CeO₂ played an important role on the overall TOC removal while the adsorption of DMP on it was negligible. This adsorption difference was due to their different ozonation rates. In the catalytic ozonation of disinfection byproduct precursors with RuO₂/ZrO₂-CeO₂, the reductions of the haloacetic acid and trihalomethane formation potentials (HAAFPs and THMFPs) for the natural water samples were 38%–57% and 50%–64%, respectively. The catalyst significantly promoted the reduction of HAAFPs but insignificantly improved the reduction of THMFPs as ozone reacts fast with the THMs precursors. These results illustrate the good promise of RuO₂/ZrO₂-CeO₂ in catalytic ozonation for water treatment.     

CeO2 doping boosted low-temperature NH3-SCR activity of FeTiOx catalyst: A microstructure analysis and reaction mechanistic study

• CeO₂ doping significantly improved low-temperature NH₃-SCR activity on FeTiO_x. • The crystallinity of FeTiO_x was decreased dramatically after CeO₂ doping. • Unique Ce-O-Fe structure in FeCe_0.2TiO_x accounted for its superior redox property. • Facile activation of NH₃ to-NH₂ on FeCe_0.2TiO_x promoted the DeNO_x efficiency. FeTiO_x has been recognized as an environmental-friendly and cost-effective catalyst for selective catalytic reduction (SCR) of NO_x with NH₃. Aimed at further improving the low-temperature DeNO_x efficiency of FeTiO_x catalyst, a simple strategy of CeO₂ doping was proposed. The low-temperature (<250℃) NH₃-SCR activity of FeTiO_x catalyst could be dramatically enhanced by CeO₂ doping, and the optimal composition of the catalyst was confirmed as FeCe_0.2TiO_x, which performed a NO_x conversion of 90% at ca. 200℃. According to X-ray diffraction (XRD), Raman spectra and X-ray absorption fine structure spectroscopy (XAFS) analysis, FeCe_0.2TiO_x showed low crystallinity, with Fe and Ce species well mixed with each other. Based on the fitting results of extended X-ray absorption fine structure (EXAFS), a unique Ce-O-Fe structure was formed in FeCe_0.2TiO_x catalyst. The well improved specific surface area and the newly formed Ce-O-Fe structure dramatically contributed to the improvement of the redox property of FeCe_0.2TiO_x catalyst, which was well confirmed by H₂-temperature-programmed reduction (H₂-TPR) and in situ XAFS experiments. Such enhanced redox capability could benefit the activation of NO and NH₃ at low temperatures for NO_x removal. The detailed reaction mechanism study further suggested that the facile oxidative dehydrogenation of NH₃ to highly reactive-NH₂ played a key role in enhancing the low-temperature NH₃-SCR performance of FeCe_0.2TiO_x catalyst.