Allangawi Abdulrahman, Kosar Naveen, Ayub Khurshid, Gilani Mazhar Amjad, Zainal Arfan Nur Hazimah Binti, Hamid Malai Haniti Sheikh Abdul, Imran Muhammad, Sheikh Nadeem S, Mahmood Tariq
Department of Chemistry, College of Science, University of Bahrain, Sakhir 32038, Bahrain.
Department of Chemistry, COMSATS University Islamabad, Lahore Campus, Lahore 54000, Pakistan.
ACS Omega. 2023 Oct 8;8(41):37820-37829. doi: 10.1021/acsomega.3c01794. eCollection 2023 Oct 17.
In the pursuit of sustainable clean energy sources, the hydrogen evolution reaction (HER) has attained significant interest from the scientific community. Single-atom catalysts (SACs) are among the most promising candidates for future electrocatalysis because they possess high thermal stability, effective electrical conductivity, and excellent percentage atom utilization. In the present study, the applicability of late first-row transition metals (Fe-Zn) decorated on the magnesium oxide nanocage (TM@MgO) as SACs for the HER has been studied, via density functional theory. The late first-row transition metals have been chosen as they have high abundance and are relatively low-cost. Among the studied systems, results show that the Fe@MgO SAC is the best candidate for catalyzing the HER reaction as it exhibits the lowest activation barrier for HER. Moreover, Fe@MgO shows high stability ( = -1.64 eV), which is essential in designing SACs to prevent aggregation of the metal. Furthermore, the results of the electronic properties' analysis showed that the HOMO-LUMO gap of the nanocage is decreased significantly upon doping of Fe (from 4.81 to 2.28 eV), indicating an increase in the conductivity of the system. This study highlights the potential application of the TM@nanocage SAC systems as effective HER catalysts.
在追求可持续清洁能源的过程中，析氢反应（HER）已引起科学界的极大关注。单原子催化剂（SACs）是未来电催化领域最有前途的候选材料之一，因为它们具有高热稳定性、有效的导电性和出色的原子利用率。在本研究中，通过密度泛函理论研究了负载在氧化镁纳米笼（TM@MgO）上的第一排晚期过渡金属（Fe-Zn）作为析氢反应单原子催化剂的适用性。选择第一排晚期过渡金属是因为它们储量丰富且成本相对较低。在所研究的体系中，结果表明Fe@MgO单原子催化剂是催化析氢反应的最佳候选材料，因为它对析氢反应表现出最低的活化能垒。此外，Fe@MgO表现出高稳定性（ = -1.64 eV），这对于设计防止金属聚集的单原子催化剂至关重要。此外，电子性质分析结果表明，掺杂Fe后纳米笼的HOMO-LUMO能隙显著降低（从4.81 eV降至2.28 eV），表明体系的导电性增加。本研究突出了TM@纳米笼单原子催化剂体系作为有效析氢催化剂的潜在应用。
