单原子Co位点的CO2还原反应路径:局部配位环境的影响

doi:10.1016/S1872-2067(21)63893-7

催化学报 ›› 2022, Vol. 43 ›› Issue (3): 832-838.DOI: 10.1016/S1872-2067(21)63893-7

单原子Co位点的CO₂还原反应路径:局部配位环境的影响

高海峡^a^,^b, 刘康^b, 罗涛^b, 陈羽^b, 胡俊华^c, 傅俊伟^b^,^#(), 刘敏^b^,^*()

^a湖南科技学院理学院, 湖南永州 425100
^b中南大学物理与电子学院, 湖南长沙 410083
^c郑州大学材料科学与工程学院, 河南郑州 450002

收稿日期:2021-06-03 修回日期:2021-06-03 出版日期:2022-03-18 发布日期:2022-02-18
通讯作者: 傅俊伟,刘敏
基金资助:
国家自然科学基金项目(21872174);国家自然科学基金项目(22002189);国家自然科学基金项目(U1932148);国际科技合作项目(2017YFE0127800);国际科技合作项目(2018YFE0203402);湖南省科技项目(2017TP1001);湖南省科技项目(2017xk2026);湖南省自然科学基金项目(2020JJ2041);湖南省自然科学基金项目(2020JJ5691);湖南省自然科学基金项目(2020JJ4322);湖南省重点项目(2020WK2002);深圳市科技创新项目(JCYJ20180307151313532);中南大学中央高校科研专项资金;湖南省教育厅科研项目(19A193);湖南科技学院人才引进计划(111021804013);湖南科技学院应用特色学科建设重点项目

CO₂ reduction reaction pathways on single-atom Co sites: Impacts of local coordination environment

Haixia Gao^a^,^b, Kang Liu^b, Tao Luo^b, Yu Chen^b, Junhua Hu^c, Junwei Fu^b^,^#(), Min Liu^b^,^*()

^aCollege of Science, Hunan University of Science and Engineering, Yongzhou 425100, Hunan, China
^bSchool of Physics and Electronics, Central South University, Changsha 410083, Hunan, China
^cSchool of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450002, Henan, China

Received:2021-06-03 Revised:2021-06-03 Online:2022-03-18 Published:2022-02-18
Contact: Junwei Fu, Min Liu
Supported by:
National Natural Science Foundation of China(21872174);National Natural Science Foundation of China(22002189);National Natural Science Foundation of China(U1932148);International Science and Technology Cooperation Program(2017YFE0127800);International Science and Technology Cooperation Program(2018YFE0203402);Hunan Provincial Science and Technology Program(2017TP1001);Hunan Provincial Science and Technology Program(2017xk2026);Hunan Provincial Natural Science Foundation(2020JJ2041);Hunan Provincial Natural Science Foundation(2020JJ5691);Hunan Provincial Natural Science Foundation(2020JJ4322);Hunan Provincial Key Research and Development Program(2020WK2002);Shenzhen Science and Technology Innovation Project(JCYJ20180307151313532);Fundamental Research Funds for the Central Universities of Central South University;Scientific Research Project of Education Department of Hunan Province(19A193);Talent-Introduction Program of Hunan University of Science and Engineering(111021804013);Construct Program of Applied Characteristic Discipline in Hunan University of Science and Engineering

摘要/Abstract

摘要：

在CO₂还原反应(CO₂RR)应中, 单原子催化剂被认为是很有前途的电催化剂. Co-N₄活性位点因其优异的CO选择性和活性而受到广泛关注. 然而, Co位点的局部配位环境与CO₂RR途径之间的相关性尚不明确. 本文采用密度泛函理论(DFT)计算, 研究了含1,10-菲咯啉基底的N₄-大环配体(Co-N₄-CPY)负载的CoN₄位点上的CO₂RR路径. 该模型的平面空间构型使其具有高度离域的π电子轨道, 可以通过π-π相互作用更好地与底物相互作用. 在相对可逆氢电极(RHE)为‒0.70 V时, 最大CO的法拉第效率为96%, CO的转换频率为9.59 s^-1. 众所周知, 单原子位点的局部配位环境可以进一步优化电催化性能. 因此, 本文还研究了N被O(Co-N₃O-CPY)和C(Co-N₃C-CPY)取代的单原子Co位点的局部配位环境.
计算结果表明, Co-N₄, Co-N₃O和Co-N₃C位点的键长相差不大, 而且其结合能都较大, 意味着它们具有良好的稳定性. Co-N₃C-CPY, Co-N₃O-CPY和Co-N₄-CPY的投影态密度(PDOS)、电荷密度差分和晶体轨道哈密顿布居(COHP)显示, C和O配位均打破了初始CoN₄配体场的对称性, 并诱发了Co原子的电荷再分布. Co原子与配位原子间的相互作用由强到弱依次为Co‒C键、Co‒N键和Co‒O键, 这与电负性O > N > C相反. 通过分析CO₂RR过程的吉布斯自由能变化, 确定了Co-N₄-CPY的主要产物为CO. 当Co-N₄位点的局部配位环境改变后, Co-N₃O位点上有利于*COOH的形成, 而Co-N₃C位点对碳氢化合物(CH₃OH或CH₄)有更高的选择性. 这是由于CO₂在Co-N₃O位点上更容易质子化形成*OCHO, 从而有利于HCOOH的形成. 而在Co-N₃C位点上时, 由于*CO难以脱附, *CO将进一步质子化, 最终形成CH₃OH或CH₄. CO₂质子化形成*COOH或*OCHO的PDOS显示, 在Co位上吸附之前, *OCHO的自旋密度是对称的, 而*COOH的自旋密度是不对称的. 对于催化剂而言, 只有Co-N₃O-CPY的自旋密度是对称的, 因此容易形成*OCHO中间体. Co-3d轨道与*COOH的C-2p轨道和*OCHO的O-2p轨道的相互作用也体现了这一关系. 本工作为单原子位点的局部配位环境与CO₂RR途径之间的关系提供了一个新的视角.

关键词: 配位环境, 产品选择性, 单原子催化剂, CO₂还原反应, 密度泛函理论计算

Abstract:

Single-atom catalysts have been proposed as promising electrocatalysts for CO₂ reduction reactions (CO₂RR). Co-N₄ active sites have attracted wide attention owing to their excellent CO selectivity and activity. However, the effect of the local coordination environment of Co sites on CO₂ reduction reaction pathways is still unclear. In this study, we investigated the CO₂ reduction reaction pathways on Co-N₄ sites supported on conjugated N₄-macrocyclic ligands with 1,10-phenanthroline subunits (Co-N₄-CPY) by density functional theory calculations. The local coordination environment of single-atom Co sites with N substituted by O (Co-N₃O-CPY) and C (Co-N₃C-CPY) was studied for comparison. The calculation results revealed that both C and O coordination break the symmetry of the primary CoN₄ ligand field and induce charge redistribution of the Co atom. For Co-N₄-CPY, CO was confirmed to be the main product of CO₂RR. HCOOH is the primary product of Co-N₃O-CPY because of the greatly increased energy barrier of CO₂ to *COOH. Although the energy barrier of CO₂ to *COOH is reduced on Co-N₃C-CPY, the desorption process of *CO becomes more difficult. CH₃OH (or CH₄) are obtained by further *CO hydrogenation reduction when using Co-N₃C-CPY. This work provides new insight into the effect of the local coordination environment of single-atom sites on CO₂ reduction reaction pathways.

Key words: Coordination environment, Product selectivity, Single-atom catalyst, CO₂ reduction reaction, DFT calculation

高海峡, 刘康, 罗涛, 陈羽, 胡俊华, 傅俊伟, 刘敏. 单原子Co位点的CO₂还原反应路径:局部配位环境的影响[J]. 催化学报, 2022, 43(3): 832-838.

Haixia Gao, Kang Liu, Tao Luo, Yu Chen, Junhua Hu, Junwei Fu, Min Liu. CO₂ reduction reaction pathways on single-atom Co sites: Impacts of local coordination environment[J]. Chinese Journal of Catalysis, 2022, 43(3): 832-838.

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图/表 4

Fig. 1. Optimized structures of Co-N4-CPY (a), Co-N3O-CPY (b), and Co-N3C-CPY (c).

Fig. 2. Electronic structures. (a) Electronic projected densities of states (PDOS) of Co-N4-CPY, Co-N3O-CPY, and Co-N3C-CPY. (b) PDOS of Co atom in Co-N4-CPY, Co-N3O-CPY, and Co-N3C-CPY; (c) Charge density difference of Co-N4-CPY, Co-N3O-CPY, and Co-N3C-CPY, before and after Co is anchored onto the framework. Yellow and green regions represent positively and negatively charged regions, respectively, and the iso-surface value is 3 × 10-3 e/Bohr3.

Fig. 3. (a) Free energy diagrams of CO2 reduction pathway to CO and corresponding intermediates on Co-N4-CPY (at 0 V vs. RHE); (b) Free energy diagrams of CO2 reduction pathway to HCOOH and corresponding intermediates on Co-N3O-CPY (at 0 V vs. RHE); (c) Free energy diagrams of CO2 reduction pathway to CH4/CH3OH and corresponding intermediates on Co-N3C-CPY (at 0 V vs. RHE).

Fig. 4. (a) Electronic projected densities of states (PDOS) of C and O atoms; PDOS of Co, C-2p (bonded to Co on *COOH), and O-2p (bonded to Co on *OCHO) on Co-N4-CPY (b), Co-N3O-CPY (c), and Co-N3C-CPY (d).

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单原子Co位点的CO₂还原反应路径:局部配位环境的影响

CO₂ reduction reaction pathways on single-atom Co sites: Impacts of local coordination environment

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