生物质锅炉氯腐蚀的密度泛函理论研究(<sup>1</sup> 山东大学能源与动力工程学院，山东 济南 250061; <sup>2</sup> 山东丰源生物质发电股份公司,山东 枣庄 277300)

Zekang LYU; Shenwei LONG; Guanbing LI; Shengli NIU; Chunmei LU; Kuihua HAN; Yongzheng WANG

doi:10.11949/0438-1157.20190487

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生物质锅炉氯腐蚀的密度泛函理论研究(¹ 山东大学能源与动力工程学院，山东济南 250061; ² 山东丰源生物质发电股份公司,山东枣庄 277300)

能源和环境工程 | 更新时间：2020-06-24

- 生物质锅炉氯腐蚀的密度泛函理论研究(¹ 山东大学能源与动力工程学院，山东济南 250061; ² 山东丰源生物质发电股份公司,山东枣庄 277300)
- Density functional theory study on chlorine corrosion of biomass furnace
- 化工学报 2019年70卷第11期页码：4370-4376
- 作者机构：
  
  1.School of Energy and Power Engineering, Shandong University, Jinan 250061, Shandong, China
  2.Shandong Fengyuan Biomass Power Co., Ltd., Zaozhuang 277300, Shandong, China
- 作者简介：
- 基金信息：
  
  国家自然科学基金项目(51576117);山东省重点研发计划项目(2018GSF117034);山东大学青年学者未来计划资助项目(2015WLJH33)
- DOI：10.11949/0438-1157.20190487
  中图分类号： TK 6
- 收稿：2019-05-08，
  
  修回：2019-07-12，
  
  纸质出版：2019-11-05
- 稿件说明：
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吕泽康, 龙慎伟, 李冠兵, 牛胜利, 路春美, 韩奎华, 王永征. 生物质锅炉氯腐蚀的密度泛函理论研究[J]. 化工学报, 2019, 70(11): 4370-4376

LYU Zekang, LONG Shenwei, LI Guanbing, NIU Shengli, LU Chunmei, HAN Kuihua, WANG Yongzheng. Density functional theory study on chlorine corrosion of biomass furnace[J]. CIESC Journal, 2019, 70(11): 4370-4376
吕泽康, 龙慎伟, 李冠兵, 牛胜利, 路春美, 韩奎华, 王永征. 生物质锅炉氯腐蚀的密度泛函理论研究[J]. 化工学报, 2019, 70(11): 4370-4376 DOI： 10.11949/0438-1157.20190487.

LYU Zekang, LONG Shenwei, LI Guanbing, NIU Shengli, LU Chunmei, HAN Kuihua, WANG Yongzheng. Density functional theory study on chlorine corrosion of biomass furnace[J]. CIESC Journal, 2019, 70(11): 4370-4376 DOI： 10.11949/0438-1157.20190487.

摘要

氯气的活化氧化腐蚀是生物质锅炉过热器腐蚀的主要原因之一。为探究活化氧化腐蚀循环中FeCl

与O

的反应机理，本文利用Material Studio中的DMOl

模块，基于密度泛函和过渡态理论，优化了各反应物、产物、中间体和过渡态的几何构型。通过频率分析证实了中间体和过渡态的真实性。结果表明，FeCl

与O

反应生成Fe

的过程中逐次生成3个Cl

分子，其中第三个Cl

逸出生成Fe

需要吸收高达300.4 kJ/mol的能量，为反应路径的速率决定步骤。

Abstract

Activated oxidative corrosion of chlorine is one of the main causes of corrosion in biomass boiler superheaters. To investigate the reaction mechanism of FeCl

and O

in the activated oxidation corrosion cycle

the DMOl

module in Material Studio was used to optimize the geometry of each reactant

product

intermediate and transition state based on density functional theory and transition state theory. The authenticity of the intermediates and transition states was confirmed by frequency analysis. The results show that three Cl

molecules are successively formed during the reaction of FeCl

with O

to form Fe

. The third Cl

escaping to form Fe

needs to absorb up to 300.4 kJ/mol

which is the rate determining step of the reaction pathway.

关键词

Keywords

references

Khan A A , Jong W D , Jansens P J , et al . Biomass combustion in fluidized bed boilers: potential problems and remedies [J]. Fuel Processing Technology , 2009 , 90 ( 1 ): 21 - 50 .

Tillman D A . Biomass cofiring: the technology, the experience, the combustion consequences [J]. Biomass & Bioenergy , 2000 , 19 ( 6 ): 365 - 384 .

Dincer I . Renewable energy and sustainable development: a crucial review [J]. Renewable and Sustainable Energy Reviews , 2000 , 4 ( 2 ): 157 - 175 .

Vassilev S V , Baxter D , Andersen L K , et al . An overview of the chemical composition of biomass [J]. Fuel , 2010 , 89 ( 5 ): 913 - 933 .

Yu C , Qin J , Nie H , et al . Experimental research on agglomeration in straw-fired fluidized beds [J]. Applied Energy , 2011 , 88 ( 12 ): 4534 - 4543 .

Nielsen H P , Frandsen F J , Dam-Johansen K , et al . The implications of chlorine-associated corrosion on the operation of biomass-fired boilers [J]. Progress in Energy and Combustion Science , 2000 , 26 ( 3 ): 283 - 298 .

徐婧 . 生物质燃烧过程中碱金属析出的实验研究 [D]. 杭州 : 浙江大学 , 2006 .

Xu J . Experimental study on alkali metal precipitation during biomass combustion [D]. Hangzhou : Zhejiang University , 2006 .

Jensen P A , Frandsen F J , Dam-Johansen K , et al . Experimental investigation of the transformation and release to gas phase of potassium and chlorine during straw pyrolysis [J]. Energy&Fuel , 2000 , 14 ( 6 ): 1280 - 1285 .

Nielsen H P . The implications of chlorine-associated corrosion on the operation of biomass-fired boilers [J]. Progress in Energy & Combustion Science , 2000 , 26 ( 3 ): 283 - 298 .

岳茂振 . 秸秆类生物质与煤混燃过程中氯腐蚀规律研究 [D]. 济南 : 山东大学 , 2011 .

Yue M Z . Study on the corrosion law of chlorine in the process of straw-based biomass and coal co-firing [D]. Jinan : Shandong University , 2011 .

李至 . 生物质与煤混燃灰熔融特性及其影响研究 [D]. 武汉 : 华中科技大学 , 2015 .

Li Z . Study on melting characteristics and effects of biomass and coal mixed combustion ash [D]. Wuhan : Huazhong University of Science and Technology , 2015 .

Uusitalo M A , Vuoristo P M J , Mantyla T A . High temperature corrosion of coatings and boiler steels below chlorine-containing salt deposits [J]. Corrosion Science , 2004 , 46 ( 6 ): 1311 – 1331 .

Grahke H J . Reese E, Spiegel M. The effect of chlorides, hydrogen chloride, and sulthr dioxide in the oxidation of steels below deposits [J]. Corrosion Science , 1995 , 37 ( 7 ): 1023 - 1043 .

Berlanga C , Ruiz J A . Study of corrosion in a biomass boiler [J]. Journal of Chemistry , 2013 , 2013 ( 4 ): 1 - 8 .

Zahs A , Spiegel M , Grabke H J . Chloridation and oxidation of iron, chromium, nickel and their alloys in chloridizing and oxidizing atmospheres at 400–700℃ [J]. Corrosion Science , 2000 , 42 ( 6 ): 1093 - 1122 .

邹潺 , 王春波 , 邢佳颖 . 煤燃烧过程中砷与氮氧化物的反应机理 [J]. 燃料化学学报 , 2019 , 47 ( 2 ): 138 - 143 .

Zou C , Wang C B , Xing J Y . Reaction mechanism of arsenic and nitrogen oxides in coal combustion process [J]. Journal of Fuel Chemistry and Technology , 2019 , 47 ( 2 ): 138 - 143 .

贾建波 , 曾凡桂 , 李美芬 , 等 . 用密度泛函理论研究煤中甲基苯生成甲烷的反应机理 [J]. 化工学报 , 2010 , 61 ( 12 ): 3235 - 3242 .

Jia J B , Zeng F G , Li M F , et al . Study on the reaction mechanism of methylbenzene to methane in coal by density functional theory [J]. CIESC Journal , 2010 , 61 ( 12 ): 3235 - 3242 .

王荣杰 , 沈本贤 , 马健 , 等 . 基于密度泛函的硫黄S8开环裂解机理 [J]. 化工学报 , 2015 , 66 ( 10 ): 3919 - 3924 .

Wang R J , Shen B X , Ma J , et al . Mechanism of open-loop cracking of sulfur S8 based on density functional theory [J]. CIESC Journal , 2015 , 66 ( 10 ): 3919 - 3924 .

朱正和 , 阎世英 , 马美仲 . B 2 H 6 分子的几何构型 [J]. 物理学报 , 2005 , 54 ( 7 ): 3106 - 3110 .

Zhu Z H , Yan S Y , Ma M Z . Geometrical configuration of B 2 H 6 molecule [J]. Acta Physica Sinica , 2005 , 54 ( 7 ): 3106 - 3110 .

冯晓娜 , 杨冬花 , 武正簧 , 等 . B、Al、La 同晶取代 EU-1 分子筛酸性的密度泛函理论计算 [J]. 石油学报 , 2013 , 29 ( 4 ): 647 - 654 .

Feng X N , Yang D H , Wu Z H , et al . Density functional theory calculation of the acidity of B, Al and La isomorphous substituted EU-1 molecular sieves [J]. Acta Petrolei Sinica , 2013 , 29 ( 4 ): 647 - 654 .

田继权 , 王伯初 , 陈双扣 , 等 . HClO对TYR氧化的理论研究 [J]. 计算机与应用化学 , 2011 , 28 ( 2 ): 217 - 221 .

Tian J Q , Wang B C , Chen S K , et al . Theoretical study on oxidation of TYR by HClO [J]. Computers and Applied Chemistry , 2011 , 28 ( 2 ): 217 - 221 .

Zhang M , Wang W , Chen Y . Theoretical investigation of selective catalytic reduction of NO on MIL-100-Fe [J]. Physical Chemistry Chemical Physics , 2018 , 20 ( 4 ): 2211 - 2219 .

黄金保 , 刘朝 , 魏顺安 . 纤维素热解形成左旋葡聚糖机理的理论研究 [J]. 燃料化学学报 , 2011 , 39 ( 8 ): 590 - 594 .

Huang J B , Liu C , Wei S A . Theoretical study on the mechanism of cellulose pyrolysis to form L-glucan [J]. Journal of Fuel Chemistry and Technology , 2011 , 39 ( 8 ): 590 - 594 .

王小曼 , 苏亚欣 , 周皞 , 等 . Fe 2 与SO 2 反应的密度泛函理论研究 [J]. 原子与分子物理学报 , 2017 , 34 ( 4 ): 625 - 629 .

Wang X M , Su Y X , Zhou H , et al . Density functional theory study on the reaction of Fe 2 with SO 2 [J]. Journal of Atomic and Molecular Physics , 2017 , 34 ( 4 ): 625 - 629 .

侯封 , 金晶 , 王永贞 , 等 . 污泥热解中 HCN 与 CaO 的反应机理: 密度泛函理论研究 [J]. 燃料化学学报 , 2017 , 45 ( 1 ): 123 - 128 .

Hou F , Jin J , Wang Y Z , et al . Reaction mechanism of HCN and CaO in sludge pyrolysis: density functional theory study [J]. Journal of Fuel Chemistry and Technology , 2017 , 45 ( 1 ): 123 - 128 .

Reddy B V , Rasouli F , Hajaligol M R , et al . Novel pathway for CO oxidation on a Fe 2 O 3 cluster [J]. Chemical Physics Letters , 2004 , 384 ( 4/5/6 ): 242 - 245 .

迟绍明 , 王宁 , 马丽英 , 等 . NO 3 - +Cl 2 →ClONO 2 +Cl - 反应势能面和势能阱 [J]. 高等学校化学学报 , 2008 , 29 ( 6 ): 1228 - 1233 .

Chi S M , Wang N , Ma L Y , et al . Potential energy surface and potential energy well of NO 3 - +Cl 2 →ClONO 2 +Cl - [J]. Chemical Journal of Chinese Universities , 2008 , 29 ( 6 ): 1228 - 1233 .

Bojana G P , Camaioni D M , Michel D . About the barriers to reaction of CCl 4 with HFeOH and FeCl 2 [J]. Journal of Physical Chemistry A , 2011 , 115 ( 31 ): 8713 - 8720 .

Mejia-Olvera R , Reveles J U , Pacheco-Ortín S M , et al . Molecular dynamics and electronic structure study of neutral, cationic and anionic (Fe 3 O 4 ) 1–5, clusters [J]. Chemical Physics Letters , 2018 , 706 ( 3 ): 494 - 500 .

凌丽霞 , 赵俐娟 , 章日光 , 等 . 苯甲酸和苯甲醛热解机理的量子化学研究 [J]. 化工学报 , 2009 , 60 ( 5 ): 1224 - 1230 .

Ling L X , Zhao L J , Zhang R G , et al . Quantum chemistry study on the pyrolysis mechanism of benzoic acid and benzaldehyde [J]. CIESC Journal , 2009 , 60 ( 5 ): 1224 - 1230 .

徐建华 , 胡常伟 . FeCH 2 +H 2 →Fe+CH 4 反应机理的密度泛函理论研究 [J]. 原子与分子物理学报 , 2008 , 25 ( 2 ): 274 - 280 .

Xu J H , Hu C W . Density functional theory study on the reaction mechanism of FeCH 2 +H 2 →Fe+CH 4 [J]. Journal of Atomic and Molecular Physics , 2008 , 25 ( 2 ): 274 - 280 .

Qin W , Chen Q L , Wang Y , et al . Theoretical study of oxidation-reduction reaction of Fe 2 O 3 supported on MgO during chemical looping combustion [J]. Applied Surface Science , 2013 , 266 ( 2 ): 350 - 354 .

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生物质锅炉氯腐蚀的密度泛函理论研究(1 山东大学能源与动力工程学院，山东 济南 250061; 2 山东丰源生物质发电股份公司,山东 枣庄 277300)

Density functional theory study on chlorine corrosion of biomass furnace

DOI：10.11949/0438-1157.20190487

摘要

Abstract

关键词

Keywords

references

生物质锅炉氯腐蚀的密度泛函理论研究(¹ 山东大学能源与动力工程学院，山东济南 250061; ² 山东丰源生物质发电股份公司,山东枣庄 277300)