氮氧化物（NO_x）是主要的大气污染物之一，其排放会引起酸雨、光化学烟雾臭氧层破坏和许多其他环境问题，会在很大程度上对人类的健康及周边的环境造成危害。我国能源消耗中煤炭占主导地位，而近几年随着环保政策的变化，燃煤锅炉NO_x超低排放的政策已开始实施。为满足要求，采用高效的SCR烟气脱硝技术是行之有效的办法。市面上主流的SCR脱硝催化剂为商用钒基催化剂，该催化剂活性窗口窄（300~420℃），N₂选择性差，抗水抗SO₂能力差，当钒基催化剂长时间处在400℃以上的烟气环境中时，极易失活造成NO_x排放不达标、NH₃逃逸等一系列问题，并且活性元素V₂O₅含有剧毒，后期处理成本高。针对上述催化剂存在的问题，我们研发了绿色无毒的稀土基催化剂和抗砷稀土基催化剂来代替商用钒基催化剂，并对稀土基催化剂进行性能测试和高温活性机理分析。主要内容如下：

首先，由于Ce³⁺和Ce⁴⁺之间的氧化还原转化使CeO₂具有开发潜力，因此CeO₂在催化剂领域得到了广泛的应用，并且铈氧化物无生物毒性，所以它被认为是钒基催化剂有力的替代者。在此基础上，我们通过浸渍法制备Ce-La/TiO₂催化剂，测试其活性发现，Ce₁₀La₂/TiO₂稀土基催化剂在350~600℃内的NO转化效率始终保持在80%以上，N₂选择性在96~100％，抗300ppm的SO₂和5%H₂O，并且在高温下（550℃）具有良好的抗老化性能。通过分析Ce-La/TiO₂催化剂微观结构、化学元素价态变化、活性位点分布、表面酸性位分布及氧化还原性能等，阐明其保持高温活性的原因：La₂O₃的添加使催化剂的活性元素分布更加均匀，形成Ce-O-La短程化学键，为其提供了更多表面活性氧物种。原位红外表征的结果探明了反应过程中催化剂表面官能团的变化，推导出催化剂的反应路径及反应机理。在高温550℃的环境下，主要是Eley-Ridel机理占主导地位。经过对Ce-La/TiO₂稀土基催化剂的表征及分析结果，设计了Ce₁₀La₂/TiO₂稀土基催化剂与商用钒基催化剂在同等测试条件下进行性能对比，发现Ce₁₀La₂/TiO₂稀土基催化剂脱硝性能指标明显优于商用钒基催化剂。

其次，通过对催化剂的抗水、抗SO₂性能测试发现高温催化剂受水的影响脱硝温度会延后，但水对催化剂的影响是可逆的。基本不受SO₂的影响，原因可能是SO₂与水在高温环境下不易生成硫酸铵盐沉积，所以不会堵塞催化剂的孔道及活性位点；从活性表现及长时间的通水通SO₂实验中发现，催化剂活性始终保持在90%以上，也说明活性位点元素并未与SO₂发生反应造成催化剂中毒。并且催化剂在水通入后高温活性可以保持到更高温度窗口（600℃以上），说明H₂O在高温段参与了反应，使活性物种的Lewis酸性物种在H₂O的参与下转变为Brønsted酸性位点，为高温催化剂提供了更多酸性位点，最终促进催化剂在高温窗口活性的延续。测试也发现SO₂的平均转化率低于1%，这也符合催化剂设计的国家标准。

最后，针对高含砷煤燃烧的烟气环境，研发了抗砷中毒稀土基催化剂。通过抗砷性能分析及抗砷机理分析发现，Fe优先与As结合形成Fe-O-As的化学键以保护CeO₂的主要活性位，并且Fe的引入将改善CeO₂的分散性，并增加表面上Ce³⁺和不饱和活性氧的浓度，Ce-La-Fe/TiO₂稀土基催化剂表现出良好的抗砷性能。

综上所述，我们研发了高温稀土基SCR脱硝催化剂和抗砷稀土基SCR脱硝催化剂。基于不饱和氧物种的理论分析、催化剂表面活性位点的释放及表面酸性位点的分布，结合催化剂的反应路径分析，探明了E-R机理对催化剂保持高温活性起到的关键作用。基于理论分析，提出了高温SCR催化剂的设计依据，并通过Ce-La催化剂与商用钒基催化剂进行活性比较，最终验证了催化剂优异的抗高温性能。通过催化剂抗水抗SO₂实验结果分析，分析在高温阶段催化剂中SO₂和水对催化剂的影响。由于我国高砷煤分布广泛，为提高稀土基催化剂的抗砷中毒能力，我们通过添加活性助剂元素，制备了Ce-La-Fe/TiO₂催化剂，其具有优异的抗砷中毒、抗水和抗SO₂性能。使稀土基催化剂更加具有普适性，对其以后的工业化设计生产奠定了坚实的理论基础。

Nitrogen oxides (NO_x) are one of the main air pollutants, and their emissions can cause acid rain, photochemical smog, ozone layer destruction, and many other environmental problems, which can cause harm to human health and the surrounding environment to a large extent. Coal dominates in my country's energy consumption, and in recent years, with changes in environmental protection policies, the policy of ultra-low NOx emissions from coal-fired boilers has begun to be implemented. In order to meet the requirements, the use of high-efficiency SCR flue gas denitration technology is an effective method. The mainstream SCR denitration catalyst on the market is a commercial vanadium-based catalyst, which has a narrow active window (300~420℃), poor N₂ selectivity, and poor water and SO₂ resistance, when the vanadium-based catalyst is exposed to a flue gas environment above 400℃ for a long time, it is very easy to deactivate and run unstable, causing a series of problems such as substandard NO_x emissions and NH₃ escape. In addition, the active element V₂O₅ is highly toxic, high post-processing cost. In response to the problems of the above-mentioned catalysts, we have developed green and non-toxic rare earth-based catalysts and arsenic-resistant rare earth-based catalysts to replace V₂O₅/TiO₂, and conducted performance testing and high-temperature activity mechanism analysis of rare earth-based catalysts. The main contents are as follows:

First of all, CeO₂ has development potential due to the redox conversion between Ce³⁺ and Ce⁴⁺, CeO₂ has been widely used in the field of catalysts, and cerium oxide has no biological toxicity, so it is considered a powerful substitute for vanadium-based catalysts. On this basis, we prepared Ce-La/TiO₂ catalyst by impregnation method and tested its activity. It was found that the NO conversion efficiency of Ce₁₀La₂/TiO₂ rare earth-based catalyst at 350~600℃ always remained above 80%, and the N₂ selectivity was 96 ~100%, resistant to 300ppm SO₂ and 5% H₂O, and has good anti-aging properties at high temperatures (550°C). By analyzing Ce-La/TiO₂ catalyst microstructure, chemical element valence changes, active site distribution, surface acid site distribution and redox performance, etc., clarify the reason why it maintains high temperature activity: the addition of La₂O₃ makes the distribution of the active elements of the catalyst more uniform, forms Ce-O-La short-range chemical bonds, and provides it with more surface active oxygen species. The in-situ infrared characterization test is to study the functional group changes of the reactive species adsorbed on the catalyst surface during the reaction process of the catalyst by controlling the order of the introduction of the reaction gas, and deduce the reaction path and reaction mechanism of the catalyst. In a high temperature environment, the Eley-Ridel mechanism dominates. After characterizing and analyzing the results of the Ce-La/TiO₂ rare earth-based catalyst, the Ce₁₀La₂/TiO₂ rare earth-based catalyst was designed to compare the performance with the V₂O₅/TiO_2., the performance indicators of the Ce₁₀La₂/TiO₂ rare-earth-based catalyst are obviously superior for V₂O₅/TiO₂ under the same test conditions.

Secondly, after testing the water resistance and SO₂ resistance of the catalyst, it is found that the conversion rate temperature of the sample will be delayed after the sample is affected by water, but the effect of H₂O is recoverable. Not poisoned by SO₂, the reason may be that SO₂ and H₂O will not generate NH₃HSO₄ deposits at high temperatures, it will not block its micropores and the distributed CeO₂ points; it has been found from long-term experiments that the catalyst activity always remained above 90%, which also shows that the active site elements did not react with SO₂ to cause catalyst poisoning. In addition, the high temperature activity of the catalyst can be maintained above 600°C after H₂O is introduced, indicating that H₂O participates in the reaction in the high temperature section, and the Lewis acid species of the active species are transformed into Brønsted acid sites with the participation of H₂O. Provides more acidic sites for high temperature catalysts, and ultimately promotes the continuation of catalyst activity in the high temperature window. The test also found that the average conversion rate of SO₂ is less than 1%, which also meets the national standards for catalyst design.

Finally, for the flue gas environment of high-arsenic coal combustion, a rare earth-based catalyst against arsenic poisoning was developed. Through the anti-arsenic performance analysis and the anti-arsenic mechanism analysis, it is found that Fe preferentially combines with arsenic to form a Fe-O-As chemical bond to protect the main active sites of CeO₂, and the introduction of Fe will improve the dispersion of CeO₂ and increase Ce³⁺ and unsaturated active oxygen on the surface. The Ce-La-Fe/TiO₂ rare earth-based catalyst exhibits good arsenic resistance.

In summary, we have developed high-temperature rare earth-based SCR denitration catalysts and arsenic-resistant rare earth-based SCR denitration catalysts. Based on theoretical analysis and reaction path speculation, it is found that the high-temperature activity E-R mechanism of the catalyst is dominant. On this basis, the design basis for high-temperature SCR catalysts is proposed, and the activity of Ce-La catalysts and commercial vanadium-based catalysts were compared, and the excellent high-temperature resistance of the catalysts was finally verified. Through the results of Anti H₂O and SO₂ poisoning, the influence of SO₂ and H₂O on the catalyst is analyzed. Because of the widespread distribution of arsenic-containing coal in my country, in order to improve the ability of rare earth-based catalysts to resist arsenic poisoning, we prepared Ce-La-Fe/TiO₂ catalysts by adding active promoter elements, which have excellent resistance to arsenic poisoning, water resistance and resistance to arsenic poisoning. SO₂ performance. Make rare earth-based catalysts more universal, and lay a solid theoretical foundation for its future industrial design and production.

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