聚变堆材料钒合金和铍固体辐照效应的模拟研究
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摘要
相比传统能源,核聚变能具有原料储量丰富、反应可控和清洁无污染等优点,被认为是解决人类未来能源的终极方案。为了在聚变装置中成功实现核聚变能,聚变堆面向等离子体材料和结构材料必须能在长期高温和14MeV中子辐照下保持高的热机械稳定性、低的中子活化特性、优良的热力学性能,特别是抗中子辐照性能。微观上,中子与材料的作用包括弹性碰撞造成的离位损伤和核嬗变反应产生氢、氦杂质；宏观上则表现为材料的肿胀、蠕变、起泡、硬化和脆化。这就成为物理学、材料科学、化学等多个学科的研究热点。虽然国内外对聚变堆关键材料已经开展了大量的研究,积累了丰富的实验数据,但对于中子辐照损伤效应的微观机理仍存在许多亟待深入研究的问题。因此澄清聚变环境下中子辐照材料引起的各种物理过程和微观机理,并加以有效地控制,是未来核聚变能实现的重要环节之一。
目前,低活化钒合金和低原子序数铍分别被作为聚变堆候选结构材料和面向等离子体材料,对它们的深入研究有助于揭示材料从微观行为到宏观性能的演变规律,为高性能聚变材料的设计和改进提供科学依据。本论文主要选取聚变堆关键材料——体心立方钒和钒合金固体,密排六方铍固体作为研究对象,采用基于密度泛函理论的计算机模拟研究了在原子尺度下H、He、O和C杂质的滞留、扩散和偏聚行为；H/He杂质与空位缺陷的相互作用、氢-空位/氦-空位复合物的团簇化和解离机制；氢泡和氦泡形成的物理起源和微观机理。最后采用有限元方法宏观模拟了聚变堆第一壁材料服役行为。
对于结构材料钒合金,聚变环境下材料体内有大量的嬗变产物H和He杂质形成,对材料的性能和稳定性产生严重的影响。首先采用随机固溶体模型和第一性原理方法研究了聚变堆结构材料钒、V-4Cr-4Ti和V-5Cr-5Ti中点缺陷(H、He、自缺陷和空位)的优先占位和扩散行为,以及H-H、He-He、He-空位和自缺陷-自缺陷相互作用。He-空位存在很强的吸引作用,我们认为空位为H和He杂质聚集提供了场所。合金元素Ti和Cr对V-Cr-Ti合会中H和He的扩散起到抑制作用。其次,为了解释He-空位作用与氦泡形成之间的关系,采用第一性原理方法考察了He和空位的扩散行为,He、空位和He-空位团簇的稳定性。He的高扩散速率和He在空位处的低形成能解释了He杂质向空位聚集的根源。基于第一性原理结果,采用经验方法评估了He的扩散率。最后,为理解钒空位对H杂质的捕获行为,采用第一性原理方法研究了钒固体中H-空位和H-H的相互作用、H-空位团簇的结构和稳定性,给出了每捕获一个H对应H-空位复合团簇的稳定结构。空位处存在更低的电子密度解释了为什么H更容易被空位捕获。进而讨论了为什么空位能够捕获多个H杂质和氢泡形成的成核机理。
对于面向等离子体材料铍,聚变环境下H和He杂质将通过反应等离子体的直接轰击和核嬗变反应而引入,严重影响了材料的性能和稳定性。为了理解H/He与金属铍的相互作用和解释氢泡或氦泡形成的物理起源,通过第一性原理计算考察了密排六方铍中四种杂质(H、He、O和C)的热力学稳定性和动力学扩散行为、H-空位和He-空位相互作用和空位对H/He的捕获行为。能量热力学上,O原子的固溶是一个放热过程,而H、He和C的固溶都是吸热过程。我们发现空位的存在明显降低了氢或氦杂质的固溶能,为H和He聚集提供了场所,铍单空位最多能捕获5个H原子或12个He原子,这就为实验上观测到气泡通常会在空位型缺陷附近形成提供合理的解释。当前结果也为进一步理解这些杂质的聚集和辐照损伤过程中早期的气泡行为提供了初步的物理图像。
最后,为了评估正常国际热核聚变堆(ITER)运行下第一壁材料的宏观热力学行为,我们考虑到第一壁材料的热沉积来自等离子体面加热和中子体加热,采用有限元方法对等离子体和中子共同热负载下第一壁材料的响应进行了宏观模拟,通过温度场和应力场分析对第一壁材料的热力学性能进行了评估。模拟结果显示较高热应力存在于Be层与CuCrZr层的界面处,是导致材料失效的主要原因之一,我们建议在这两层之间加入一个有效过渡层,以降低热应力产生
Fusion energy compared to traditional energy sources, which has rich raw-materials, reaction safe and controlled, clean, economical energy with nearly infinite resource, is considered as a ultimate scheme to solve mankind's future energy. To successfully achieve fusion energy in fusion devices, plasma-facing materials and structural materials under long-term high temperature and14MeV neutron irradiation must be able to maintain high thermo-mechanical stability, low-activation properties, and excellent thermodynamic properties, especially resistance to neutron irradiation performance. For microcosmic behavior, the neutron-material interactions include dispacement damage caused by the elastic collision and H/He impurities produced by nuclear transmutation reactions. For macroscopic behavior, the materials appear swelling, creep, blistering, hardening and embrittlement phenomena. This is a comprensive and complicted issue of physics, materials science, and chemical. Until now large amounts of work have been carried out for key materials of fusion reator and accumulated a great number of experimental data; however, the microscopic mechanism of effect of neutron irradiation damage is still unclear and need intensive studies. Therefore, elucidating the physical process and microscopic mechanism during neutron irradiating ma terials is one of important steps to realize the use of fusion power in the future.
Low-activation vanadlium alloys have considered as structural materials of future fusion reactor, wihle low-Z beryllium has been used as plasma-facing materials in fusion reactor. Thus intensive studies for them are helpful for revealing the evolution laws of the materials from microscopic to macroscopic, privding the basis for design and improvement of fusion materials. In this thesis, we choose two key fusion materials, i.e., vanadium/vanadlium alloys, and beryllium solid, as research topics. Density functional theory caculations have studied (1) retention, diffusion and aggregation beahaior of H, He, O, C impurities;(2) interaction bewteen H/He impurities and vacancy defects, stability and dissociation mechanism of H-vacancy and He-vacancy complex clusters;(3) physical mechanism of H bubble and He bubble formations. In addition, we simulated macroscopic service behavior of first wall under operation of fusion reactor using finite element method.
Vanadium alloys as structural materials in fusion environment, large amounts of H and He impurities in bulk produced by transmutation reactions have a serious effect on the performance of the material. Using random solid solution model and first-principles methods we studied occpuaying and diffusion behavior of point defects (H, He, self-defect and vacancy) in vanadium, V-4Cr-4Ti and V-5Cr-5Ti alloys; H-H, He-He, He-vacancy and self-defects-self-defect interactions. Since He-vacancy exists a strong attractive interaction, we believe that vacancy privde a location for H and He aggregation, and the incorporation of Ti and Cr alloy elements can restrain H and He diffusion. Secondly, to explain the relationship between He-vacancy interactions and He bubble formation, first-principles calculations studied diffusion behavior of He and vacancy, stability of He, vacancies and of He-vacancy clusters. He high diffusion rate and low formation energy at vacancy is physical origin of He aggregating to vacancy. Based on first-principles results, we evaluate He diffusion rate in vanadium using empirical methods. Finally, to understand vacancy trapping for H in vanadium, we computed the interactions of H-vacancy and H-H, and the stability of H-vacancy clusters using first-principles methods. Lower electron density at vacancy explains why H is easier to be trapped by vacancy. And then we discuss why single vacancy can accommodate multiple H and nucleation mechanism of H bubble.
For plasma-facing materials beryllium in fusion environment, H and He impurities from direct plasma bombardment and transmutation reactions seriously influence on the performance of the material. To understand H/He-Be interactions and elucidate the physical origin of H bubble and He bubble formation, we investigated energetics and diffusion behavior of H, He, O, and C impurities in hcp beryllium, H-vacancy and He-vacancy interactions, and H or He trapping at vacancy using first-principles methods. Overall, the O solution in bulk is an exothermic process, while the solution of H, He and C is an endothermic process. We found that the presence of vacancy markedly decreased solution energy of H or He, and a momovacancy can trapp up to5H or12He atoms. This gives an explanation for why H and He bubbles were experimentally observed at vacancy defects in materials. Theoretical results provide an elementary physical picture for H/He aggregation and blister formation in the early stage of irradiation damage.
Finally, to assess the macroscopic thermodynamic behavior of first wall materials under normal operation for International Thermonuclear Experimental Reactor (ITER), we considered thermal deposition in first wall from plasma surface heating and neutron body heating, and simulated the combined effects of plasma heating and neutron heating loads in first wal by temperature and stress analysis using finite element method. The results show that high thermal stress exists in the interface of Be layer and CuCrZr layer, we suggest adding an effective buffer layer between two layers to reduce the thermal stress.
目前,低活化钒合金和低原子序数铍分别被作为聚变堆候选结构材料和面向等离子体材料,对它们的深入研究有助于揭示材料从微观行为到宏观性能的演变规律,为高性能聚变材料的设计和改进提供科学依据。本论文主要选取聚变堆关键材料——体心立方钒和钒合金固体,密排六方铍固体作为研究对象,采用基于密度泛函理论的计算机模拟研究了在原子尺度下H、He、O和C杂质的滞留、扩散和偏聚行为；H/He杂质与空位缺陷的相互作用、氢-空位/氦-空位复合物的团簇化和解离机制；氢泡和氦泡形成的物理起源和微观机理。最后采用有限元方法宏观模拟了聚变堆第一壁材料服役行为。
对于结构材料钒合金,聚变环境下材料体内有大量的嬗变产物H和He杂质形成,对材料的性能和稳定性产生严重的影响。首先采用随机固溶体模型和第一性原理方法研究了聚变堆结构材料钒、V-4Cr-4Ti和V-5Cr-5Ti中点缺陷(H、He、自缺陷和空位)的优先占位和扩散行为,以及H-H、He-He、He-空位和自缺陷-自缺陷相互作用。He-空位存在很强的吸引作用,我们认为空位为H和He杂质聚集提供了场所。合金元素Ti和Cr对V-Cr-Ti合会中H和He的扩散起到抑制作用。其次,为了解释He-空位作用与氦泡形成之间的关系,采用第一性原理方法考察了He和空位的扩散行为,He、空位和He-空位团簇的稳定性。He的高扩散速率和He在空位处的低形成能解释了He杂质向空位聚集的根源。基于第一性原理结果,采用经验方法评估了He的扩散率。最后,为理解钒空位对H杂质的捕获行为,采用第一性原理方法研究了钒固体中H-空位和H-H的相互作用、H-空位团簇的结构和稳定性,给出了每捕获一个H对应H-空位复合团簇的稳定结构。空位处存在更低的电子密度解释了为什么H更容易被空位捕获。进而讨论了为什么空位能够捕获多个H杂质和氢泡形成的成核机理。
对于面向等离子体材料铍,聚变环境下H和He杂质将通过反应等离子体的直接轰击和核嬗变反应而引入,严重影响了材料的性能和稳定性。为了理解H/He与金属铍的相互作用和解释氢泡或氦泡形成的物理起源,通过第一性原理计算考察了密排六方铍中四种杂质(H、He、O和C)的热力学稳定性和动力学扩散行为、H-空位和He-空位相互作用和空位对H/He的捕获行为。能量热力学上,O原子的固溶是一个放热过程,而H、He和C的固溶都是吸热过程。我们发现空位的存在明显降低了氢或氦杂质的固溶能,为H和He聚集提供了场所,铍单空位最多能捕获5个H原子或12个He原子,这就为实验上观测到气泡通常会在空位型缺陷附近形成提供合理的解释。当前结果也为进一步理解这些杂质的聚集和辐照损伤过程中早期的气泡行为提供了初步的物理图像。
最后,为了评估正常国际热核聚变堆(ITER)运行下第一壁材料的宏观热力学行为,我们考虑到第一壁材料的热沉积来自等离子体面加热和中子体加热,采用有限元方法对等离子体和中子共同热负载下第一壁材料的响应进行了宏观模拟,通过温度场和应力场分析对第一壁材料的热力学性能进行了评估。模拟结果显示较高热应力存在于Be层与CuCrZr层的界面处,是导致材料失效的主要原因之一,我们建议在这两层之间加入一个有效过渡层,以降低热应力产生
Fusion energy compared to traditional energy sources, which has rich raw-materials, reaction safe and controlled, clean, economical energy with nearly infinite resource, is considered as a ultimate scheme to solve mankind's future energy. To successfully achieve fusion energy in fusion devices, plasma-facing materials and structural materials under long-term high temperature and14MeV neutron irradiation must be able to maintain high thermo-mechanical stability, low-activation properties, and excellent thermodynamic properties, especially resistance to neutron irradiation performance. For microcosmic behavior, the neutron-material interactions include dispacement damage caused by the elastic collision and H/He impurities produced by nuclear transmutation reactions. For macroscopic behavior, the materials appear swelling, creep, blistering, hardening and embrittlement phenomena. This is a comprensive and complicted issue of physics, materials science, and chemical. Until now large amounts of work have been carried out for key materials of fusion reator and accumulated a great number of experimental data; however, the microscopic mechanism of effect of neutron irradiation damage is still unclear and need intensive studies. Therefore, elucidating the physical process and microscopic mechanism during neutron irradiating ma terials is one of important steps to realize the use of fusion power in the future.
Low-activation vanadlium alloys have considered as structural materials of future fusion reactor, wihle low-Z beryllium has been used as plasma-facing materials in fusion reactor. Thus intensive studies for them are helpful for revealing the evolution laws of the materials from microscopic to macroscopic, privding the basis for design and improvement of fusion materials. In this thesis, we choose two key fusion materials, i.e., vanadium/vanadlium alloys, and beryllium solid, as research topics. Density functional theory caculations have studied (1) retention, diffusion and aggregation beahaior of H, He, O, C impurities;(2) interaction bewteen H/He impurities and vacancy defects, stability and dissociation mechanism of H-vacancy and He-vacancy complex clusters;(3) physical mechanism of H bubble and He bubble formations. In addition, we simulated macroscopic service behavior of first wall under operation of fusion reactor using finite element method.
Vanadium alloys as structural materials in fusion environment, large amounts of H and He impurities in bulk produced by transmutation reactions have a serious effect on the performance of the material. Using random solid solution model and first-principles methods we studied occpuaying and diffusion behavior of point defects (H, He, self-defect and vacancy) in vanadium, V-4Cr-4Ti and V-5Cr-5Ti alloys; H-H, He-He, He-vacancy and self-defects-self-defect interactions. Since He-vacancy exists a strong attractive interaction, we believe that vacancy privde a location for H and He aggregation, and the incorporation of Ti and Cr alloy elements can restrain H and He diffusion. Secondly, to explain the relationship between He-vacancy interactions and He bubble formation, first-principles calculations studied diffusion behavior of He and vacancy, stability of He, vacancies and of He-vacancy clusters. He high diffusion rate and low formation energy at vacancy is physical origin of He aggregating to vacancy. Based on first-principles results, we evaluate He diffusion rate in vanadium using empirical methods. Finally, to understand vacancy trapping for H in vanadium, we computed the interactions of H-vacancy and H-H, and the stability of H-vacancy clusters using first-principles methods. Lower electron density at vacancy explains why H is easier to be trapped by vacancy. And then we discuss why single vacancy can accommodate multiple H and nucleation mechanism of H bubble.
For plasma-facing materials beryllium in fusion environment, H and He impurities from direct plasma bombardment and transmutation reactions seriously influence on the performance of the material. To understand H/He-Be interactions and elucidate the physical origin of H bubble and He bubble formation, we investigated energetics and diffusion behavior of H, He, O, and C impurities in hcp beryllium, H-vacancy and He-vacancy interactions, and H or He trapping at vacancy using first-principles methods. Overall, the O solution in bulk is an exothermic process, while the solution of H, He and C is an endothermic process. We found that the presence of vacancy markedly decreased solution energy of H or He, and a momovacancy can trapp up to5H or12He atoms. This gives an explanation for why H and He bubbles were experimentally observed at vacancy defects in materials. Theoretical results provide an elementary physical picture for H/He aggregation and blister formation in the early stage of irradiation damage.
Finally, to assess the macroscopic thermodynamic behavior of first wall materials under normal operation for International Thermonuclear Experimental Reactor (ITER), we considered thermal deposition in first wall from plasma surface heating and neutron body heating, and simulated the combined effects of plasma heating and neutron heating loads in first wal by temperature and stress analysis using finite element method. The results show that high thermal stress exists in the interface of Be layer and CuCrZr layer, we suggest adding an effective buffer layer between two layers to reduce the thermal stress.
引文
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