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

doi:10.11949/j.issn.0438-1157.20161223

Abstract

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.

Key words: CO₂ capture, chemical looping combustion, NiFe₂O₄, H₂S, DFT, adsorption, thermodynamics

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。

关键词: 二氧化碳捕集, 化学链燃烧, NiFe₂O₄, H₂S, 密度泛函理论, 吸附, 热力学

CLC Number:

TQ546

DAI Jinxin, LIU Jing, LIU Feng. Influence mechanism of H₂S on reactivity of NiFe₂O₄ oxygen carriers for chemical looping combustion[J]. CIESC Journal, 2017, 68(3): 1163-1169.

戴金鑫, 刘晶, 刘丰. 化学链燃烧中H₂S对NiFe₂O₄氧载体活性的影响机理[J]. 化工学报, 2017, 68(3): 1163-1169.

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

化学链燃烧中H₂S对NiFe₂O₄氧载体活性的影响机理

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