高等学校化学学报 ›› 2022, Vol. 43 ›› Issue (5): 20220042.doi: 10.7503/cjcu20220042
收稿日期:
2022-02-21
出版日期:
2022-05-10
发布日期:
2022-03-20
通讯作者:
黄勃龙
E-mail:bhuang@polyu.edu.hk
基金资助:
WONG Honho, LU Qiuyang, SUN Mingzi, HUANG Bolong()
Received:
2022-02-21
Online:
2022-05-10
Published:
2022-03-20
Contact:
HUANG Bolong
E-mail:bhuang@polyu.edu.hk
Supported by:
摘要:
近年来, 原子催化剂(ACs)引起了广泛的研究关注. 目前该领域的长足发展受限于贵金属的使用和单原子催化剂(SACs)的性能有限. 本文总结了利用密度泛函理论(DFT)和机器学习(ML)方法筛选高效的基于石墨炔(GDY)的原子催化剂的工作. 研究表明, Pd, Co, Pt和Hg可以形成稳定的零价过渡金属-石墨炔组合(TM-GDY), 而镧系-过渡金属的双原子催化剂(Ln-TM DAC)组合通过f-d轨道耦合作用可以获得有效的催化性能提升. 进一步分析表明, 主族元素与过渡金属和镧系金属的结合可以通过p轨道耦合保持高电活性, 从而构成高度稳定的GDY-DAC系统, 机器学习算法也揭示了s,p轨道的作用. 此外, 理论算法技术在筛选催化水分解析氢反应(HER)的高效组合上也表现出了优越性, 创新性地预测了石墨炔-原子催化剂在实际催化反应中的潜能. 本综合评述可为未来设计新型原子催化剂提供新的思路与策略.
中图分类号:
TrendMD:
黄汉浩, 卢湫阳, 孙明子, 黄勃龙. 石墨炔原子催化剂的崭新道路:基于自验证机器学习方法的筛选策略. 高等学校化学学报, 2022, 43(5): 20220042.
WONG Honho, LU Qiuyang, SUN Mingzi, HUANG Bolong. Rational Design of Graphdiyne-based Atomic Electrocatalysts: DFT and Self-validated Machine Learning. Chem. J. Chinese Universities, 2022, 43(5): 20220042.
Fig.1 Redox energy diagrams, zero?valence anchoring ability and mapping of the electron transfer ability of metal on GDY[58](A—C) Summary of redox of 3d, 4d and 5d TMs; (D) the dependence of anchoring ability of TMs on d-electrons; (E) the mapping of zero-valence anchoring ability of TMs in periodic tables; (F) the decomposition of the mapping into oxidation; (G) the decomposition of the mapping into reduction reactions; (H) the mapping of the electron transfer ability of metal on GDY; (I) the mapping of the electron transfer stability on GDY.Copyright 2019, Elsevier.
Fig.2 Mapping of formation energy, stabilization energy, anchoring energy and d,f?band center energy of GDY?based DACs[60](A) The mappings of the formation energy for second metal of all the GDY-based DACs; (B) the mapping of stabilization energy for second metal of all the GDY-based DACs; (C) the mapping of anchoring energy for second metal of all the GDY-based DACs; (D) the mappings of the energy difference between the hetero-coupling DACs and homo-coupling DACs; (E) the mapping of d-band centers for all the combinations of GDY-based DACs; (F) the mapping of d-band center difference for all the combinations of GDY-based DACs which is obtained by the d-band center comparison between the DAC and the SAC of the left column metals; (G) the mapping of f-band for all the Ln-based DACs; (H) the mapping of f-band center difference for all the Ln-Ln-based DACs; (I) the mapping of f/d band center difference.Copyright 2021, Wiley-VCH.
Fig.3 Formation energies and band center mapping of GDY?based DACs[69](A) The formation energies of GDY-based DACs by combinations of AAEM and Ln metals; (B) the formation energies of GDY-based DACs by combinations of post-TMs and Ln metals; (C) the formation energies of GDY-based DACs by combinations of metalloid and Ln metals; (D) the formation energy mapping of all the combinations for TMs, Ln metals, AAEM, post-TMs, and metalloid elements; (E) the formation energy comparison between hetero- alkaline/alkaline earth, post-TMs, and metalloids based GDY-DACs and homo-TM DACs; (F) the formation energy comparison between hetero- and homo- alkaline/alkaline earth, post-TMs, and metalloids based GDY-DACs; (G) the formation energy comparison between hetero- alkaline/alkaline earth, post-TMs, and metalloids based GDY-DACs and TM-based GDY-SACs; (H) the p-band center of alkyl chain in the alkaline/alkaline earth, post-TMs, and metalloids based GDY-DACs; (I) the p-band center of alkyl chain in the post-TMs based GDY-DACs; (J) the p-band center of alkyl chain in the metalloid based GDY-DACs.Copyright 2021, Wiley-VCH.
Fig.4 Orbital coupling of GDY?based DACs[69](A) The p-band center difference between alkaline/alkaline earth metals and all the elements in the GDY-DACs; (B) the p-band center difference between post-TMs and all the elements in the GDY-DACs; (C) the p-band center difference between metalloids and all the elements in the GDY-DACs; (D) the difference between the p-band center of alkaline/alkaline earth metals and the d/f-band center of TMs and Ln metals in the GDY-DACs; (E) the p-band center of post-TMs and d/f-band center of TMs and Ln metals in the GDY-DACs; (F) the p-band center of metalloids and d/f-band center of TMs and Ln metals in the GDY-DACs.Copyright 2021, Wiley-VCH.
Fig.5 Adsorption of TMs based GDY ACs and their HER performances[70](A) The DFT calculated energy of initial adsorption and final desorption of 3d-TMs based GDY ACs; (B) the initial adsorption and final desorption of 4d-TMs based GDY ACs; (C) the initial adsorption and final desorption of 5d-TMs based GDY ACs; (D) the chemisorption trend of H on 3d-TMs based GDY ACs; (E) the chemisorption trend of H on 4d-TMs based GDY ACs; (F) the chemisorption trend of H on 5d-TMs based GDY ACs; (G) the volcano plot of the HER reaction energy of 3d-TMs; (H) the volcano plot of the HER reaction energy of 4d-TMs; (I) the volcano plot of the HER reaction energy of 5d-TMs; (J) the energy of initial adsorption and final desorption of HER on the Ln-based GDY ACs; (K) the volcano plot of the reaction energy of HER; (L, M) the free energy diagram of the HER process; (N) the DFT mapping of the preferable initial adsorption sites for H* in HER; (O) the DFT mapping of the final desorption sites for H2 in HER; (P) mapping of the chemisorption energies for GDY-TMs based ACs; (Q) the DFT mapping of the reaction energies of HER for 3d-GDY-TM based ACs; (R) the DFT mapping of the reaction energies of HER for 4d-GDY-TMs based ACs; (S) the DFT mapping of the reaction energies of HER for 5d-GDY-TMs based ACs.Copyright 2020, Wiley-VCH.
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