基于分子反应动力学揭示炭-H2O/CO2 气化过程中钙物种的催化机理

IF 5.6 2区 工程技术 Q2 ENERGY & FUELS Journal of The Energy Institute Pub Date : 2024-09-18 DOI:10.1016/j.joei.2024.101831
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引用次数: 0

摘要

钙在炭气化过程中具有一定的催化作用,并影响气化产物的分布和组成。因此,深入了解钙在气化过程中的反应特性和机理对气化过程具有重要意义。反应力场分子动力学(ReaxFF MD)作为一种探索复杂化学反应的方法,为深入研究煤气化过程中钙的反应特性提供了不可或缺的帮助。本研究采用 ReaxFF MD 构建了不同条件下的煤气化反应,通过统计不同条件下煤气化产物的分布以及钙物种的变化,研究了钙对煤气化过程中产物的影响。同时,通过计算气化剂和钙结合后气化剂的电荷和静电位,以及不同原子间的径向分布函数,进一步研究了钙在气化过程中对炭素的催化机理。研究表明,在气化过程中,炭中的钙与气化剂中的氧原子结合释放,导致 O-H 或 C=O 键能降低,从而促进了气化剂的裂解。值得注意的是,与 CO2 相比,钙在气化过程中很容易与 H2O 分子中的 O 形成离子键,从而导致 O-H 键更容易断裂。
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Insights into the catalytic mechanism of calcium species during char-H2O/CO2 gasification based on molecular reaction dynamics

Calcium has a definite catalytic effect in char gasification and affects the distribution and composition of gasification products. Therefore, a deep understanding of the reaction properties and mechanism of calcium in gasification is of great significance for the gasification process. Reactive Force Field Molecular Dynamics (ReaxFF MD), an approach for exploring complex chemical reactions, has provided an indispensable aid to the insightful study of the reaction properties of calcium in coal gasification processes. In this work, ReaxFF MD was adopted to construct gasification reactions with different conditions, and the effect of calcium on the products during the gasification was investigated by counting the distribution of the gasification products as well as the changes of calcium species in different conditions. At the same time, the catalytic mechanism of calcium in char during gasification was further investigated by calculating the charge and electrostatic potential of the gasification agent and the gasification agent after calcium binding, as well as the radial distribution function between different atoms. Research has shown that during gasification, the release of calcium from char combined with oxygen atoms in the gasifying agent leads to a decrease in the O–H or C=O bond energy, which promotes the cracking of the gasifying agent. It is worth noting that in comparison to CO2, Ca can easily form ionic bonds with O in the H2O molecule during the gasification process, which leads to easier breaking of the O–H bonds.

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来源期刊
Journal of The Energy Institute
Journal of The Energy Institute 工程技术-能源与燃料
CiteScore
10.60
自引率
5.30%
发文量
166
审稿时长
16 days
期刊介绍: The Journal of the Energy Institute provides peer reviewed coverage of original high quality research on energy, engineering and technology.The coverage is broad and the main areas of interest include: Combustion engineering and associated technologies; process heating; power generation; engines and propulsion; emissions and environmental pollution control; clean coal technologies; carbon abatement technologies Emissions and environmental pollution control; safety and hazards; Clean coal technologies; carbon abatement technologies, including carbon capture and storage, CCS; Petroleum engineering and fuel quality, including storage and transport Alternative energy sources; biomass utilisation and biomass conversion technologies; energy from waste, incineration and recycling Energy conversion, energy recovery and energy efficiency; space heating, fuel cells, heat pumps and cooling systems Energy storage The journal''s coverage reflects changes in energy technology that result from the transition to more efficient energy production and end use together with reduced carbon emission.
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