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基于电子结构理论筛选二维材料用于高性能能量存储及转化器件 被引量:1

Recent advances in screening two-dimensional materials for high-performance energy storage and conversion devices based on electronic structure theory
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摘要 在能源危机与环境污染问题日益严峻的背景下,探索新型的高性能能量存储和转化材料成为当今材料科学界研究的热点.近年来,有关新型能量存储和转化材料的预测、合成和性能研究取得了突飞猛进的进展;但同时如何提高能量的转化效率以及材料的循环性能和安全性能是制约其实际应用的瓶颈.另一方面,基于密度泛函方法的理论计算在揭示微观反应机理和筛选高性能的能量存储和转化材料方面发挥了重要的作用.通过理论计算能够从原子尺度上建立材料的本征属性与能量存储和转化性能之间的关系,为筛选高性能能量存储和转化材料提供重要的理论依据.本文首先从锂离子电池、燃料电池等能源器件所涉及的电化学反应出发,回顾二维材料在这些电化学反应中的应用,进一步探讨二维材料的电子结构与其化学反应性能之间的关系,并总结目前提出的用于化学反应性能的描述符并阐述其具体的应用领域,最后指出目前理论计算在研究能量存储及转化材料上存在的不足和未来的发展方向. With the ever-growing global energy demands and environmental pollution issues, developing high-performance energy storage and conversion materials has become a hot topic in the material science community. In this regard, substantial progress has been made in theoretically predicting new materials for energy-related fields, experimentally synthesizing these materials, and further improving their properties for high performance in energy storage and conversion devices. In particular, two-dimensional(2D) materials have shown great potential in the field of energy storage and conversion.However, it remains challenging to explore 2D materials that render high efficiency of energy storage and conversion while guarantee long-term stability and safety. Over the past decades, theoretical calculations based on density functional theory(DFT) have become a practical toolkit to address this issue by revealing the reaction mechanism at an atomic scale and screening high-performance energy storage and conversion materials on a large scale. In particular, DFT calculations enable us to establish the relationships between the intrinsic properties of materials and their performance for energy storage and conversion, and provide theoretical guidance for screening and experimentally synthesizing the promising materials.In this review, we summarize the DFT calculations’ applications in recent studies of developing high-performance and reliable energy-related 2D materials for Li-ion battery(LIB), water splitting, fuel cells, and electrochemical carbon dioxide reduction(CRR). First, we introduce the reaction mechanism of LIB, hydrogen evolution reaction(HER), oxygen evolution reaction/oxygen reduction reaction(OER/ORR), and CRR in detail and the application of 2D material in these fields. Then, we highlight the role of DFT calculations in unveiling the intrinsic relationships between the electronic structure and the performance of 2D materials by comprehensively discussing the descriptors in predicting the performance of 2D materials. For example, the occupancy of d orbital and energy required to fill empty states serve as descriptors to predict the electrochemical performance of the electrode in ion intercalation battery. The d orbital center, lowest unoccupied states, and oxygen vacancy formation energy serve as descriptors to predict the catalytic performance of electrode in HER. The energy difference between the lowest valance electron orbital center and Fermi level, occupancy of pzorbital, and the energy difference between pzand px/pyorbital center serve as descriptors to predict the catalytic performance of electrode in ORR. Even though these descriptors can help to further understand the relationships between the electronic structure and the performance of the electrochemical electrode, they are only reliable to specific materials and inapplicable to the electrode with a complex structure or complex reaction path, such as the electrode in CRR. Newly developed machine learning methods may bring a breakthrough to the exploration of a universal descriptor, which is a key factor in the large-scale screening of potential electrode materials with excellent performance and the dependable guidance to experimental synthesis. Finally, we summarize the disadvantage of DFT calculation, such as the underestimation of bandgap and incorrect description of van der Waals interaction, and give a perspective of DFT calculations in the study of new energy-related materials. The method to simulate the ambient environment of the electrode(including the electrolyte,external electric field, and non-cooperative transfer of proton and electron) based on DFT calculation is needed to be developed, which is vital to reflect the actual working condition of the electrode. The universal descriptor applicable to the electrode with a complex structure is also needed to explore to overcome the poor versatility of single intrinsic property of the material in predicting the performance of the electrochemical electrode.
作者 杨鑫 吴曦 李佳 Xin Yang;Xi Wu;Jia Li(Tsinghua Shenzhen International Graduate School,Tsinghua University,Shenzhen 518055,China)
出处 《科学通报》 EI CAS CSCD 北大核心 2021年第6期640-656,共17页 Chinese Science Bulletin
基金 国家重点研发计划(2017YFB0701600) 国家自然科学基金(11874036)资助。
关键词 二维材料 能量存储与转化 密度泛函理论 电子结构理论 电催化反应 two-dimensional materials energy storage and conversion density functional theory electronic structure theory electrochemical catalysis
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