Zian Liu , Qianwei Shu , Zhefei Li , Yang Liu , Shuya Rui , Binghui Wu , Zhiping Ye , Junhua Li
{"title":"揭示工业选择性催化还原(SCR)催化剂的历程:了解失活机制和创新再生技术","authors":"Zian Liu , Qianwei Shu , Zhefei Li , Yang Liu , Shuya Rui , Binghui Wu , Zhiping Ye , Junhua Li","doi":"10.1016/j.jclepro.2025.145475","DOIUrl":null,"url":null,"abstract":"<div><div>The selective catalytic reduction (SCR) of nitrogen oxides (NO<sub>x</sub>) using V<sub>2</sub>O<sub>5</sub>-WO<sub>3</sub>/TiO<sub>2</sub> catalysts is critical for mitigating emissions from coal-fired power plants. However, catalyst deactivation by arsenic (As) and alkali metals in flue gas poses a major operational challenge. This study focuses on industrial SCR catalysts poisoned under real-world coal combustion conditions, specifically addressing deactivation mechanisms and regeneration strategies tailored to this high-arsenic, high-sulfur environment. Through multi-scale characterization (XPS, TGA, NH<sub>3</sub>-TPD) and kinetic analyses, we demonstrate that arsenic (As<sub>2</sub>O<sub>3</sub>/As<sub>2</sub>O<sub>5</sub>) and sodium (Na) synergistically deactivate the catalyst by (i) blocking Brønsted acid sites, (ii) oxidizing V<sup>4+</sup> to V<sup>5+</sup> (reducing redox activity), and (iii) forming pore-clogging sulfates. To counteract this, we developed a novel two-step regeneration protocol combining ozone oxidation (0.5 wt% H<sub>2</sub>SO<sub>4</sub>, 120 min O<sub>3</sub> exposure) with ammonia alkaline washing (1.0 mol/L NH<sub>4</sub>OH). Regenerated catalysts were prepared as industrial-scale honeycomb monoliths to emulate real-world operating conditions, achieving 97.31 % As removal and restoring 98.7 % NO<sub>x</sub> conversion efficiency at 380 °C—performance comparable to fresh catalysts. Crucially, the regenerated catalyst exhibits sustained stability (>15 days, <em>GB/T 31,587–2015</em> compliance) under simulated flue gas (500 ppm SO<sub>2</sub>, 10 % H<sub>2</sub>O), with a 30 % cost reduction versus fresh catalyst procurement. This work provides actionable insights for SCR catalyst regeneration in coal power systems, emphasizing the interplay between contaminant-specific chemistries (As vs. alkali metals) and process-driven reactivation strategies.</div></div>","PeriodicalId":349,"journal":{"name":"Journal of Cleaner Production","volume":"506 ","pages":"Article 145475"},"PeriodicalIF":10.0000,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Unveiling the journey of industrial selective catalytic reduction (SCR) catalysts: Understanding deactivation mechanisms and innovating regeneration techniques\",\"authors\":\"Zian Liu , Qianwei Shu , Zhefei Li , Yang Liu , Shuya Rui , Binghui Wu , Zhiping Ye , Junhua Li\",\"doi\":\"10.1016/j.jclepro.2025.145475\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The selective catalytic reduction (SCR) of nitrogen oxides (NO<sub>x</sub>) using V<sub>2</sub>O<sub>5</sub>-WO<sub>3</sub>/TiO<sub>2</sub> catalysts is critical for mitigating emissions from coal-fired power plants. However, catalyst deactivation by arsenic (As) and alkali metals in flue gas poses a major operational challenge. This study focuses on industrial SCR catalysts poisoned under real-world coal combustion conditions, specifically addressing deactivation mechanisms and regeneration strategies tailored to this high-arsenic, high-sulfur environment. Through multi-scale characterization (XPS, TGA, NH<sub>3</sub>-TPD) and kinetic analyses, we demonstrate that arsenic (As<sub>2</sub>O<sub>3</sub>/As<sub>2</sub>O<sub>5</sub>) and sodium (Na) synergistically deactivate the catalyst by (i) blocking Brønsted acid sites, (ii) oxidizing V<sup>4+</sup> to V<sup>5+</sup> (reducing redox activity), and (iii) forming pore-clogging sulfates. To counteract this, we developed a novel two-step regeneration protocol combining ozone oxidation (0.5 wt% H<sub>2</sub>SO<sub>4</sub>, 120 min O<sub>3</sub> exposure) with ammonia alkaline washing (1.0 mol/L NH<sub>4</sub>OH). Regenerated catalysts were prepared as industrial-scale honeycomb monoliths to emulate real-world operating conditions, achieving 97.31 % As removal and restoring 98.7 % NO<sub>x</sub> conversion efficiency at 380 °C—performance comparable to fresh catalysts. Crucially, the regenerated catalyst exhibits sustained stability (>15 days, <em>GB/T 31,587–2015</em> compliance) under simulated flue gas (500 ppm SO<sub>2</sub>, 10 % H<sub>2</sub>O), with a 30 % cost reduction versus fresh catalyst procurement. 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Unveiling the journey of industrial selective catalytic reduction (SCR) catalysts: Understanding deactivation mechanisms and innovating regeneration techniques
The selective catalytic reduction (SCR) of nitrogen oxides (NOx) using V2O5-WO3/TiO2 catalysts is critical for mitigating emissions from coal-fired power plants. However, catalyst deactivation by arsenic (As) and alkali metals in flue gas poses a major operational challenge. This study focuses on industrial SCR catalysts poisoned under real-world coal combustion conditions, specifically addressing deactivation mechanisms and regeneration strategies tailored to this high-arsenic, high-sulfur environment. Through multi-scale characterization (XPS, TGA, NH3-TPD) and kinetic analyses, we demonstrate that arsenic (As2O3/As2O5) and sodium (Na) synergistically deactivate the catalyst by (i) blocking Brønsted acid sites, (ii) oxidizing V4+ to V5+ (reducing redox activity), and (iii) forming pore-clogging sulfates. To counteract this, we developed a novel two-step regeneration protocol combining ozone oxidation (0.5 wt% H2SO4, 120 min O3 exposure) with ammonia alkaline washing (1.0 mol/L NH4OH). Regenerated catalysts were prepared as industrial-scale honeycomb monoliths to emulate real-world operating conditions, achieving 97.31 % As removal and restoring 98.7 % NOx conversion efficiency at 380 °C—performance comparable to fresh catalysts. Crucially, the regenerated catalyst exhibits sustained stability (>15 days, GB/T 31,587–2015 compliance) under simulated flue gas (500 ppm SO2, 10 % H2O), with a 30 % cost reduction versus fresh catalyst procurement. This work provides actionable insights for SCR catalyst regeneration in coal power systems, emphasizing the interplay between contaminant-specific chemistries (As vs. alkali metals) and process-driven reactivation strategies.
期刊介绍:
The Journal of Cleaner Production is an international, transdisciplinary journal that addresses and discusses theoretical and practical Cleaner Production, Environmental, and Sustainability issues. It aims to help societies become more sustainable by focusing on the concept of 'Cleaner Production', which aims at preventing waste production and increasing efficiencies in energy, water, resources, and human capital use. The journal serves as a platform for corporations, governments, education institutions, regions, and societies to engage in discussions and research related to Cleaner Production, environmental, and sustainability practices.