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高温SCR脱硝研究进展:从催化剂到反应机理

Research progress in high-temperature SCR denitration:from catalyst innovations to reaction mechanism exploration
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摘要 【目的】为应对燃气轮机、煤层气发电等行业烟气减排需求,急需开发高温(≥500℃)脱硝催化剂,以解决商用钒钛催化剂因高温烧结、氨氧化副反应加剧而带来的活性下降问题。【方法】系统综述了分子筛基和金属氧化物基两类高温催化剂,总结了催化剂制备方法与性能优化策略。结合文献报道,讨论了高温脱硝催化剂的NH_(3)-SCR反应机理以及抗中毒作用机制,包括抗(水)热稳定性和抗硫/碱金属中毒。【结果】在分子筛基催化剂中,Fe/SSZ-13和Cu-SSZ-13表现出优异高温活性,主要归因于孤立金属位点与酸性位点的协同作用。对于氧化物基催化剂,WO_(3)-FeO_(x)和硫酸化CeO_(2)通过增强表面酸性、氧空位及抑制NH_(3)氧化实现高效脱硝。抗中毒研究表明,ZrO_(2)掺杂可提升抗硫性能,而Ce掺杂能缓解碱金属中毒。【结论】分子筛基与氧化物基催化剂在高温脱硝领域展现出潜力,但需进一步优化抗失活机制。未来研究应聚焦高温微观失活机制解析、硫盐动态行为与碱金属捕获策略、多污染物协同控制及整体式催化剂的实际应用适配,推动高温脱硝技术的工业化应用。 [Objective]To meet the strict pollution control requirement for treating flue gas in scenarios like gas turbines and coalbed methane power generation,the development of efficient SCR catalysts that can perform well under high temperatures(>500℃)becomes very urgent,mainly due to the evident activity loss caused by serious sintering and aggravated NH3 over-oxidation for the commercial catalysts of V_(2)O_(5)-TiO_(2).[Methods]A systematic review was conducted on two categories of high-temperature catalysts:zeolite-based and metal oxide-based.Preparation methods,performance optimization strategies,and reaction mechanisms were analyzed.In-situ FTIR and poisoning resistance experiments were employed to investigate NH3-SCR pathways,hydrothermal stability,and resistance to sulfur/alkali metal poisoning under high temperatures.[Results]For zeolite-based catalysts,Fe/SSZ-13 and Cu-SSZ-13 exhibited outstanding performance due to isolated metal sites and synergistic acid-redox properties.Among oxide-based catalysts,WO_(3)-FeO_(x)and sulfated CeO_(2) achieved high efficiency by enhancing surface acidity,oxygen vacancies,and suppressing NH3 oxidation.Poisoning resistance studies revealed that ZrO_(2) doping improved sulfur tolerance,while Ce doping mitigated alkali metal poisoning.[Conclusion]Zeolite-and oxide-based catalysts demonstrate potential for hightemperature denitration,yet require further optimization in anti-deactivation mechanisms.Future research should focus on elucidating microstructural degradation under high temperatures;dynamic sulfur salt behavior and alkali metal trapping strategies;multi-pollutant synergistic control and practical adaptation of monolithic catalysts.
作者 王瑜 唐添发 周沁宇 许璐 汤常金 WANG Yu;TANG Tianfa;ZHOU Qinyu;XU Lu;TANG Changjin(School of Environment,Nanjing Normal University,Nanjing 210023,Jiangsu China)
出处 《电力科技与环保》 2025年第3期343-356,共14页 Electric Power Technology and Environmental Protection
基金 国家自然科学基金项目(22276097) 国家自然科学基金项目(52300132) 江苏省杰出青年基金项目(BK20230007) 低碳智能燃煤发电与超净排放全国重点实验室开放项目(D2023FK095) 江苏省研究生科研与实践创新计划项目(SJCX25_0690)。
关键词 烟气脱硝 高温催化剂 分子筛 金属氧化物 反应机理 抗中毒 NO_(x)removal high-temperature catalyst zeolite metal oxide reaction mechanism resistance to deactivation
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