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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Unraveling Thermodynamic Stability, Catalytic Activity, and Electronic Structure of [TMxMgyOz](+/0/-) Clusters at Realistic Conditions: A Hybrid DFT and ab Initio Thermodynamics Study
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Unraveling Thermodynamic Stability, Catalytic Activity, and Electronic Structure of [TMxMgyOz](+/0/-) Clusters at Realistic Conditions: A Hybrid DFT and ab Initio Thermodynamics Study

机译：在现实条件下解开[TMXMGYOZ]（+ / 0 / - ）簇的热力学稳定性，催化活性和电子结构：Hybrid DFT和AB Initio热力学研究

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Aiming toward catalytic applications, a large data set is generated on [TMxMgyOz](+/0/-) clusters (TM = Cr, Fe, Co, Ni, x + y <= 5) using a massively parallel cascade genetic algorithm (cGA) approach at the hybrid density functional level of theory. The low-energy isomers are further analyzed via ab initio atomistic thermodynamics to estimate their free energy of formation at a realistic temperature T and partial pressure of oxygen p(O2). A thermodynamic phase diagram is drawn by minimizing Gibbs free energy of formation to identify the stable phases of neutral and charged [TMxMgyOz](+/0/-) clusters. From this analysis, we notice that neutral and negatively charged clusters are stable in the wide range of (T, p(O2)). The negatively charged clusters are more effective as a catalyst to lower the C-H bond activation barrier for oxidation of methane. We find that the nature of TM atoms toward controlling the activation barrier is less important. However, the TM gives rise to different structural motifs in the cluster, which may act as active centers for catalysis.
机译：针对催化应用，使用大规模平行级联遗传算法（CGA）在[TMXMGYOZ]（+ / 0 / - ）簇（TM = Cr，Fe，Co，Ni，X + Y <= 5）上产生大数据集）在混合密度函数理论水平的方法。通过AB Initio原子的热力学进一步分析低能量异构体，以估计其在氧气P（O2）的逼真温度T和部分压力下形成的自由能量。通过最小化Gibbs自由能量来鉴定中性和带电[TMXMGEDOZ]（+ / 0 / - ）簇的稳定相的热力学相图。根据该分析，我们注意到中性和带负电的簇在宽范围内稳定（T，P（O2））。带负电荷的簇作为催化剂更有效，以降低甲烷氧化的C-H键活化屏障。我们发现TM原子对控制激活屏障的性质不太重要。然而，TM在群体中产生不同的结构图案，这可能充当催化的活性中心。

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