Influence mechanism of H2S on reactivity of NiFe2O4 oxygen carriers for chemical looping combustion

DAI Jinxin; LIU Jing; LIU Feng

doi:10.11949/j.issn.0438-1157.20161223

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Influence mechanism of H₂S on reactivity of NiFe₂O₄ oxygen carriers for chemical looping combustion

更新时间：2025-12-10

- Influence mechanism of H₂S on reactivity of NiFe₂O₄ oxygen carriers for chemical looping combustion
- CIESC Journal Issue 3, Pages: 1163-1169(2017)
- 作者机构：
  
  华中科技大学煤燃烧国家重点实验室,湖北,武汉,430074
- 作者简介：
- 基金信息：
- DOI：10.11949/j.issn.0438-1157.20161223
  CLC： Q546
- Online First：05 March 2017，
  
  Published：05 March 2017
- 稿件说明：
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DAI Jinxin, LIU Jing, LIU Feng. Influence mechanism of H₂S on reactivity of NiFe₂O₄ oxygen carriers for chemical looping combustion[J]. CIESC Journal, 2017, (3): 1163-1169. DOI: 10.11949/j.issn.0438-1157.20161223.
DOI：

DAI Jinxin, LIU Jing, LIU Feng. Influence mechanism of H₂S on reactivity of NiFe₂O₄ oxygen carriers for chemical looping combustion[J]. CIESC Journal, 2017, (3): 1163-1169. DOI: 10.11949/j.issn.0438-1157.20161223. DOI：

摘要

采用密度泛函理论方法研究H2S与NiFe2O4（001）完整表面和氧缺陷表面的相互作用机理。结果表明，H2S在NiFe2O4氧载体表面Ni原子位的吸附能比其在Fe原子位的吸附能大。氧缺陷的形成会使H2S在氧载体表面金属原子位的吸附能增大，并且Ni原子位吸附H2S的吸附能增加更为明显。因而，NiFe2O4氧载体表面的Ni原子位是H2S的主要吸附位。同时采用热力学方法进一步研究含H2S的合成气与NiFe2O4氧载体之间的反应，发现H2S与氧载体的反应产物与氧载体的还原程度密切相关。由于铁氧化物的深度还原过程受到热力学限制，H2S与NiFe2O4氧载体反应的主要产物为Ni3S2。密度泛函理论方法与热力学方法研究结果均表明H2S倾向于与NiFe2O4氧载体中Ni发生相互作用，这将对NiFe2O4氧载体的反应性能产生不利影响。

Abstract

Chemical Looping Combustion (CLC) is a novel technology for its attractive advantage in the inherent separation of CO2. Due to the existence of sulfur contaminants in the fossil fuels

the interaction of the gaseous products of sulfur species with oxygen carrier is a great concern in the CLC operational aspect. Density Functional Theory (DFT) calculations were performed to investigate interaction mechanism between H2S and NiFe2O4 oxygen carrier at molecule level. The results show that H2S is easier to be adsorbed on NiFe2O4(001) defect surface than that on NiFe2O4(001) perfect surface. On both NiFe2O4(001) perfect surface and defect surface

the adsorption energies of H2S adsorbed on Ni site are greater than those of H2S adsorbed on Fe site

which infers that H2S is preferred to adsorb on Ni site of the oxygen carrier surface. Furthermore

the reduction reactions between NiFe2O4 oxygen carrier and H2S-containing synthesis gas were investigated by means of thermodynamic simulation. The result shows that generation of various sulfur-containing species are related to the reduction process of oxygen carrier. Mole percentage of Ni3S2 is higher than those of FeS due to thermodynamic limitation of reduction of iron oxides

indicating that nickel sulfides are easier to be generated than iron sulfides under equilibrium conditions. Both DFT calculations and thermodynamic simulations indicate that H2S is preferred to interact with Ni atom of the oxygen carrier

which may have adverse effects on the reactivity of NiFe2O4 oxygen carrier.

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