Computational screening of chemically active metal center in coordinated dipyridyl tetrazine network
Computational screening of chemically active metal center in coordinated dipyridyl tetrazine network
复制标题
配位联吡啶四嗪网络中化学活性金属中心的计算筛选
DOI：
10.1088/1361-648x/acb8f3
复制
发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Rahman, Talat S.
中科院分区：
文献类型：
--
作者：
Din, Naseem Ud;Le, Duy;Rahman, Talat S.
单个过渡金属（TM）原子的创造、稳定、表征和控制可能会导致下一代催化剂的重大进步。金属有机网络（MON）是一类极具发展前景的单原子催化剂，其中单个TM原子通过有机配体进行配位和分离。我们基于密度泛函理论计算了双吡啶基四嗪（DPTZ）配体与TM原子配位形成线性链的MONs，得到了两种类型的链。配位中心含有V、Cr、Mo、Fe、Co、Pt或Pd原子的分子是平面的，而含有Au、Ag、Cu或Ni原子的分子是非平面的。链的形成能很高（~ 2.0 ~ 7.9 eV），表明这些单晶硅可以稳定。此外，计算得到CO和o2在平面构型链中心金属原子对配位中心V、Cr、Mo、Fe和CO的吸附能在1.0 ~ 3.0 eV范围内，为进一步研究上述5个原子在配位中心的TM-DPTZ链上CO氧化铺平了道路。
Creation, stabilization, characterization, and control of single transition metal (TM) atoms may lead to significant advancement of the next-generation catalyst. Metal organic network (MON) in which single TM atoms are coordinated and separated by organic ligands is a promising class of material that may serve as a single atom catalyst. Our density functional theory-based calculations of MONs in which dipyridyl tetrazine (DPTZ) ligands coordinate with a TM atom to form linear chains leads to two types of geometries of the chains. Those with V, Cr, Mo, Fe, Co, Pt, or Pd atoms at the coordination center are planar while those with Au, Ag, Cu, or Ni are non-planar. The formation energies of the chains are high (∼ 2.0–7.9 eV), suggesting that these MON can be stabilized. Moreover, the calculated adsorption energies of CO and O 2 on the metal atom at center of the chains with the planar configuration lie in the range 1.0–3.0 eV for V, Cr, Mo, Fe, and Co at the coordination center, paving the way for future studies of CO oxidation on TM-DPTZ chains with the above five atoms at the coordination center.
通过配体设计对表面单点钒中心进行二电子和三电子氧化。
影响因子：
15
作者：
D. Skomski;Christopher D. Tempas;Brian J Cook;A. Polezhaev;Kevin A. Smith;K. G. Caulton;S. Tait
通讯作者：
S. Tait
影响因子：
21.8
作者：
Qiao, Botao;Wang, Aiqin;Zhang, Tao
通讯作者：
Zhang, Tao