View in EDS PDF Full Text

低阶煤热解过程中硫氮元素迁移特性研究进展.

Saved in:
Bibliographic Details
Title: 低阶煤热解过程中硫氮元素迁移特性研究进展.
Alternate Title: Research progress on the migration characteristics of sulfur and nitrogen elements during the pyrolysis process of low rank coal.
Authors: 周安宁1,2 psu564@139.com, 惠 栋1, 白状伟1, 张 致1, 逯俊庆3, 陈福欣1, 赵 伟1,2, 刘向荣1,2
Source: Clean Coal Technology. Jan2026, Vol. 32 Issue 1, p403-420. 18p.
Subject Terms: *Pyrolysis, *Sulfuration, *Machine learning, *Air pollution potential, *Catalysis, *Thermolysis, *Lignite
Abstract (English): The sulfur and nitrogen elements in low-rank coal significantly impactits processing, conversion, and utilization. A clear understanding of the occurrence forms, structure, and migration patterns of sulfur and nitrogen during thermal conversion not only mitigates their potential environmental hazards but also enables the targeted conversion of these elements intosulfur- ornitrogencontaining chemicals and the development of sulfur-/nitrogen-doped novel carbon materials for high-value applications. To this end, this paper systematically summarizes the occurrence forms of sulfur and nitrogen in low-rank coal; analyzes the effects of pyrolysis atmosphere, pyrolysis temperature, catalysts, and other factors on the distribution characteristics and migration pathways of sulfur- and nitrogen-containing compounds in coal pyrolysis products; and explores the application of machine learning methods such as Random Forest and LightGBM in predicting pyrolysis products. Sulfur in low-rank coal primarily exists as organic sulfur, while nitrogen is predominantly present as four types of organic nitrogen: pyrrolic nitrogen, pyridinic nitrogen, quaternary nitrogen, andoxidized pyridinic nitrogen. Specifically, within vitrinite, the predominant sulfur-containing functional groups are thiophene, thiol, and thioether, while the nitrogen-containing functional groups are primarily pyridinic and benzonitrile derivatives. In contrast, within inertinite, the forms of sulfur-containing functional groups are similar to those in vitrinite, but the nitrogen is predominantly present as amine and pyrrolic structures.Increasing pyrolysis temperature promotes the decomposition of sulfur and nitrogen elements. Slower heating rates favor the removal of organic sulfur, whilefaster heating rates are more conducive to the migration of nitrogen to gaseous products. H2, water vapor, and CO2 atmospheres all promote the decomposition of sulfur- and nitrogen-containing compounds. Specifically, H2 and water vapor provide hydrogen radicals that attack sulfur and nitrogen atoms in heterocyclic aromatics, thereby accelerating their decomposition. The CO2 atmosphere promotes C—S, C—C, and C—N bond cleavage, accelerating the formation of gaseous sulfur- and nitrogen-containing compounds. Both calcium-based and iron-based catalysts exhibit sulfur fixationcapabilities while also influencing the conversion of nitrogen, typically promoting its release as gaseous species such as HCN and NH3. During pyrolysis, inorganic sulfur (primarily pyrite) is transformed into pyrrhotite, which further reacts with active hydrogen and CO to form gaseous products like H2S and COS; the undecomposed fraction remains in the char. Organic sulfur decomposition primarily occurs through C—S bond cleavage. The resulting sulfur-containing radicals react with hydrogen atoms or other hydrogen donors to form gaseous products like H2S and SO2. Other sulfurcontaining groups polymerize or combine with aromatic rings to form polycyclic sulfur-containing aromatics, migrating into tar and char. Nitrogen in pyrolysis gas originates from the ring-opening reactions of nitrogen-containing heterocycles like pyridine and quinoline. Nitrogen in tar derives from the elimination and reorganization of heterocyclic compounds such as pyridines and pyrroles, while highly stable organic nitrogen remains in the char. Using out-of-bag estimation for hyperparameter optimization of the random forest algorithm reduced the prediction deviation for naphthobenzothiopheneto 0.11%. The LightGBM model built on raw coal physical parameters achieved a prediction accuracy with a coefficient of determination (R²) of 0.91 for morphological forms of sulfur. Further hyperparameter optimization using Hyperopt not only reduced the computation time by 60% but alsoincreased model’s R² to 0.96. In summary, elucidating the migration and transformation characteristics and mechanisms of sulfur and nitrogen during the pyrolysis of low-rank coal, and constructing machine learning prediction models with multi-source feature parameter inputs, provide significant theoretical and practical guidancefor the targeted transformation of sulfur- and nitrogen-containing structural units in coal, their highvalue utilization, and the development of technologies for reducing pollutant emissions. [ABSTRACT FROM AUTHOR]
Abstract (Chinese): 低阶煤中硫、氮元素对其加工、转化和利用有重要影响, 清晰认识煤中硫、氮元素的赋存形态、 结构以及热转化过程的迁移与调变规律, 不仅能减少其对环境的潜在危害, 还有望实现将硫、氮元素定 向转化为含硫氮元素的化学品或硫氮掺改性的新型碳材料的高值化目标。为此, 系统归纳了低阶煤中 硫、氮元素的赋存形态, 分析了热解气氛、热解温度、催化剂等因素对煤热解产物中含硫、氮化合物的分 布特征和迁移路径的影响规律, 探讨了随机森林算法、LightGBM 等机器学习方法在热解产物预测中的 应用。低阶煤中硫元素以有机硫为主, 氮元素以吡咯型氮、吡啶型氮、季氮和氧化吡啶氮 4 类有机氮为 主。其中, 在镜质组分中含硫、氮官能团分别主要是噻吩、硫醇、硫醚, 吡啶、苯腈类; 在惰质组分中含硫 官能团的存在形态与镜质组相似, 含氮官能团则以胺、吡咯类为主。提高热解温度, 可促进硫、氮元素 分解; 升温速率越慢, 越有利于有机硫的脱除; 升温速率越快, 越有利于氮元素向气态产物迁移。H2、水 蒸气以及 CO2 气氛均有利于含硫、氮化合物的分解, 其中 H2 和水蒸气通过提供氢自由基, 以攻击杂环 芳烃上的硫、氮原子, 从而促进其分解; CO2 气氛促进了 C—S 、 C—C 、 C—N 键断裂, 加速气态含硫、含 氮化合物的生成。钙基和铁基催化剂均具有固硫效果, 同时能促进氮元素向气相氮转移。在热解过程 中, 无机硫分解为磁黄铁矿, 并进一步与活性氢、CO 反应生成 H2S 和 COS 等气相产物, 未分解部分残 留于半焦; 有机硫的分解主要是通过 C—S 键的断裂, 断裂后生成的含硫自由基与氢原子或其他供氢体 反应, 生成 H2S 和 SO2 等气相产物, 其他含硫基团则相互聚合或与芳香环结合形成多环含硫芳烃, 迁移 至焦油和半焦中。热解气中氮元素来源于吡啶、喹啉等含氮杂环的开环反应, 焦油中氮元素来源于吡 啶类、吡咯类等杂环化合物的脱除与重组, 而高稳定性的有机氮保留在半焦中。采用袋外估计方法对 随机森林算法超参数进行优化, 使得该模型对萘苯并噻吩的预测偏差低至 0.11% ;基于原煤物性参数构 建的 LightGBM 模型, 对形态硫的预测精度达到 0.91, 进一步引入 Hyperopt 进行超参数优化后, 不仅计 算耗时缩短 60%, 还将模型预测精度提升至 0.96。综上, 明晰低阶煤在热解过程中硫、氮的迁移转化特 性与机理, 采用机器学习方法构建多源特征参数输入的预测模型, 对于煤中含硫和含氮结构单元的定 向转化、高值利用和污染物减排技术发展具有重要理论和实际指导价值。 [ABSTRACT FROM AUTHOR]
Database: Energy & Power Source
FullText Links:
  – Type: pdflink
Text:
  Availability: 0
Header DbId: enr
DbLabel: Energy & Power Source
An: 191788677
AccessLevel: 6
PubType: Academic Journal
PubTypeId: academicJournal
PreciseRelevancyScore: 0
IllustrationInfo
Items – Name: Title
  Label: Title
  Group: Ti
  Data: 低阶煤热解过程中硫氮元素迁移特性研究进展.
– Name: TitleAlt
  Label: Alternate Title
  Group: TiAlt
  Data: Research progress on the migration characteristics of sulfur and nitrogen elements during the pyrolysis process of low rank coal.
– Name: Author
  Label: Authors
  Group: Au
  Data: <searchLink fieldCode="AR" term="%22周安宁%22">周安宁</searchLink><relatesTo>1,2</relatesTo><i> psu564@139.com</i><br /><searchLink fieldCode="AR" term="%22惠+栋%22">惠 栋</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22白状伟%22">白状伟</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22张+致%22">张 致</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22逯俊庆%22">逯俊庆</searchLink><relatesTo>3</relatesTo><br /><searchLink fieldCode="AR" term="%22陈福欣%22">陈福欣</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22赵+伟%22">赵 伟</searchLink><relatesTo>1,2</relatesTo><br /><searchLink fieldCode="AR" term="%22刘向荣%22">刘向荣</searchLink><relatesTo>1,2</relatesTo>
– Name: TitleSource
  Label: Source
  Group: Src
  Data: <searchLink fieldCode="JN" term="%22Clean+Coal+Technology%22">Clean Coal Technology</searchLink>. Jan2026, Vol. 32 Issue 1, p403-420. 18p.
– Name: Subject
  Label: Subject Terms
  Group: Su
  Data: *<searchLink fieldCode="DE" term="%22Pyrolysis%22">Pyrolysis</searchLink><br />*<searchLink fieldCode="DE" term="%22Sulfuration%22">Sulfuration</searchLink><br />*<searchLink fieldCode="DE" term="%22Machine+learning%22">Machine learning</searchLink><br />*<searchLink fieldCode="DE" term="%22Air+pollution+potential%22">Air pollution potential</searchLink><br />*<searchLink fieldCode="DE" term="%22Catalysis%22">Catalysis</searchLink><br />*<searchLink fieldCode="DE" term="%22Thermolysis%22">Thermolysis</searchLink><br />*<searchLink fieldCode="DE" term="%22Lignite%22">Lignite</searchLink>
– Name: Abstract
  Label: Abstract (English)
  Group: Ab
  Data: The sulfur and nitrogen elements in low-rank coal significantly impactits processing, conversion, and utilization. A clear understanding of the occurrence forms, structure, and migration patterns of sulfur and nitrogen during thermal conversion not only mitigates their potential environmental hazards but also enables the targeted conversion of these elements intosulfur- ornitrogencontaining chemicals and the development of sulfur-/nitrogen-doped novel carbon materials for high-value applications. To this end, this paper systematically summarizes the occurrence forms of sulfur and nitrogen in low-rank coal; analyzes the effects of pyrolysis atmosphere, pyrolysis temperature, catalysts, and other factors on the distribution characteristics and migration pathways of sulfur- and nitrogen-containing compounds in coal pyrolysis products; and explores the application of machine learning methods such as Random Forest and LightGBM in predicting pyrolysis products. Sulfur in low-rank coal primarily exists as organic sulfur, while nitrogen is predominantly present as four types of organic nitrogen: pyrrolic nitrogen, pyridinic nitrogen, quaternary nitrogen, andoxidized pyridinic nitrogen. Specifically, within vitrinite, the predominant sulfur-containing functional groups are thiophene, thiol, and thioether, while the nitrogen-containing functional groups are primarily pyridinic and benzonitrile derivatives. In contrast, within inertinite, the forms of sulfur-containing functional groups are similar to those in vitrinite, but the nitrogen is predominantly present as amine and pyrrolic structures.Increasing pyrolysis temperature promotes the decomposition of sulfur and nitrogen elements. Slower heating rates favor the removal of organic sulfur, whilefaster heating rates are more conducive to the migration of nitrogen to gaseous products. H2, water vapor, and CO2 atmospheres all promote the decomposition of sulfur- and nitrogen-containing compounds. Specifically, H2 and water vapor provide hydrogen radicals that attack sulfur and nitrogen atoms in heterocyclic aromatics, thereby accelerating their decomposition. The CO2 atmosphere promotes C—S, C—C, and C—N bond cleavage, accelerating the formation of gaseous sulfur- and nitrogen-containing compounds. Both calcium-based and iron-based catalysts exhibit sulfur fixationcapabilities while also influencing the conversion of nitrogen, typically promoting its release as gaseous species such as HCN and NH3. During pyrolysis, inorganic sulfur (primarily pyrite) is transformed into pyrrhotite, which further reacts with active hydrogen and CO to form gaseous products like H2S and COS; the undecomposed fraction remains in the char. Organic sulfur decomposition primarily occurs through C—S bond cleavage. The resulting sulfur-containing radicals react with hydrogen atoms or other hydrogen donors to form gaseous products like H2S and SO2. Other sulfurcontaining groups polymerize or combine with aromatic rings to form polycyclic sulfur-containing aromatics, migrating into tar and char. Nitrogen in pyrolysis gas originates from the ring-opening reactions of nitrogen-containing heterocycles like pyridine and quinoline. Nitrogen in tar derives from the elimination and reorganization of heterocyclic compounds such as pyridines and pyrroles, while highly stable organic nitrogen remains in the char. Using out-of-bag estimation for hyperparameter optimization of the random forest algorithm reduced the prediction deviation for naphthobenzothiopheneto 0.11%. The LightGBM model built on raw coal physical parameters achieved a prediction accuracy with a coefficient of determination (R²) of 0.91 for morphological forms of sulfur. Further hyperparameter optimization using Hyperopt not only reduced the computation time by 60% but alsoincreased model’s R² to 0.96. In summary, elucidating the migration and transformation characteristics and mechanisms of sulfur and nitrogen during the pyrolysis of low-rank coal, and constructing machine learning prediction models with multi-source feature parameter inputs, provide significant theoretical and practical guidancefor the targeted transformation of sulfur- and nitrogen-containing structural units in coal, their highvalue utilization, and the development of technologies for reducing pollutant emissions. [ABSTRACT FROM AUTHOR]
– Name: Abstract
  Label: Abstract (Chinese)
  Group: Ab
  Data: 低阶煤中硫、氮元素对其加工、转化和利用有重要影响, 清晰认识煤中硫、氮元素的赋存形态、 结构以及热转化过程的迁移与调变规律, 不仅能减少其对环境的潜在危害, 还有望实现将硫、氮元素定 向转化为含硫氮元素的化学品或硫氮掺改性的新型碳材料的高值化目标。为此, 系统归纳了低阶煤中 硫、氮元素的赋存形态, 分析了热解气氛、热解温度、催化剂等因素对煤热解产物中含硫、氮化合物的分 布特征和迁移路径的影响规律, 探讨了随机森林算法、LightGBM 等机器学习方法在热解产物预测中的 应用。低阶煤中硫元素以有机硫为主, 氮元素以吡咯型氮、吡啶型氮、季氮和氧化吡啶氮 4 类有机氮为 主。其中, 在镜质组分中含硫、氮官能团分别主要是噻吩、硫醇、硫醚, 吡啶、苯腈类; 在惰质组分中含硫 官能团的存在形态与镜质组相似, 含氮官能团则以胺、吡咯类为主。提高热解温度, 可促进硫、氮元素 分解; 升温速率越慢, 越有利于有机硫的脱除; 升温速率越快, 越有利于氮元素向气态产物迁移。H2、水 蒸气以及 CO2 气氛均有利于含硫、氮化合物的分解, 其中 H2 和水蒸气通过提供氢自由基, 以攻击杂环 芳烃上的硫、氮原子, 从而促进其分解; CO2 气氛促进了 C—S 、 C—C 、 C—N 键断裂, 加速气态含硫、含 氮化合物的生成。钙基和铁基催化剂均具有固硫效果, 同时能促进氮元素向气相氮转移。在热解过程 中, 无机硫分解为磁黄铁矿, 并进一步与活性氢、CO 反应生成 H2S 和 COS 等气相产物, 未分解部分残 留于半焦; 有机硫的分解主要是通过 C—S 键的断裂, 断裂后生成的含硫自由基与氢原子或其他供氢体 反应, 生成 H2S 和 SO2 等气相产物, 其他含硫基团则相互聚合或与芳香环结合形成多环含硫芳烃, 迁移 至焦油和半焦中。热解气中氮元素来源于吡啶、喹啉等含氮杂环的开环反应, 焦油中氮元素来源于吡 啶类、吡咯类等杂环化合物的脱除与重组, 而高稳定性的有机氮保留在半焦中。采用袋外估计方法对 随机森林算法超参数进行优化, 使得该模型对萘苯并噻吩的预测偏差低至 0.11% ;基于原煤物性参数构 建的 LightGBM 模型, 对形态硫的预测精度达到 0.91, 进一步引入 Hyperopt 进行超参数优化后, 不仅计 算耗时缩短 60%, 还将模型预测精度提升至 0.96。综上, 明晰低阶煤在热解过程中硫、氮的迁移转化特 性与机理, 采用机器学习方法构建多源特征参数输入的预测模型, 对于煤中含硫和含氮结构单元的定 向转化、高值利用和污染物减排技术发展具有重要理论和实际指导价值。 [ABSTRACT FROM AUTHOR]
PLink https://search.ebscohost.com/login.aspx?direct=true&site=eds-live&db=enr&AN=191788677
RecordInfo BibRecord:
  BibEntity:
    Identifiers:
      – Type: doi
        Value: 10.13226/j.issn.1006-6772.JJMJS25100801
    Languages:
      – Code: chi
        Text: Chinese
    PhysicalDescription:
      Pagination:
        PageCount: 18
        StartPage: 403
    Subjects:
      – SubjectFull: Pyrolysis
        Type: general
      – SubjectFull: Sulfuration
        Type: general
      – SubjectFull: Machine learning
        Type: general
      – SubjectFull: Air pollution potential
        Type: general
      – SubjectFull: Catalysis
        Type: general
      – SubjectFull: Thermolysis
        Type: general
      – SubjectFull: Lignite
        Type: general
    Titles:
      – TitleFull: 低阶煤热解过程中硫氮元素迁移特性研究进展.
        Type: main
  BibRelationships:
    HasContributorRelationships:
      – PersonEntity:
          Name:
            NameFull: 周安宁
      – PersonEntity:
          Name:
            NameFull: 惠 栋
      – PersonEntity:
          Name:
            NameFull: 白状伟
      – PersonEntity:
          Name:
            NameFull: 张 致
      – PersonEntity:
          Name:
            NameFull: 逯俊庆
      – PersonEntity:
          Name:
            NameFull: 陈福欣
      – PersonEntity:
          Name:
            NameFull: 赵 伟
      – PersonEntity:
          Name:
            NameFull: 刘向荣
    IsPartOfRelationships:
      – BibEntity:
          Dates:
            – D: 01
              M: 01
              Text: Jan2026
              Type: published
              Y: 2026
          Identifiers:
            – Type: issn-print
              Value: 10066772
          Numbering:
            – Type: volume
              Value: 32
            – Type: issue
              Value: 1
          Titles:
            – TitleFull: Clean Coal Technology
              Type: main
ResultId 1