Catalytic Properties Dominated by Electronic Structures in PdZn, NiZn, and PtZn Intermetallic Compounds
Catalytic Properties Dominated by Electronic Structures in PdZn, NiZn, and PtZn Intermetallic Compounds
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DOI：
10.1143/jpsj.80.064801
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发表时间：
2011-05
影响因子：
1.7
通讯作者：
K. Nozawa;Naruki Endo;S. Kameoka;A. Pang Tsai;Y. Ishii
中科院分区：
文献类型：
--
作者：
K. Nozawa;Naruki Endo;S. Kameoka;A. Pang Tsai;Y. Ishii
Pd 的催化功能通过与 Zn 合金化而完全改变，并且 PdZn 在甲醇蒸汽重整（SRM）中表现出与 Cu 相当的催化选择性。我们进行理论和实验研究来证实我们之前的论点，即 d 带的位置是决定催化性能的重要因素。 M-Zn（M = Pd、Ni、Pt）的第一性原理平板计算表明，表面的键断裂导致 d 带宽度有所减小，但稳定表面的 d 带位置与本体的位置基本保持不变。从理论上证明了合金化引起的电子结构剧烈变化的根源。我们之前的论点不仅在 SRM 中进行了实验检验，而且还在 CO 和 H 2 吸附等元素反应中进行了实验检验。磁测量还表明 d 带位置在 SRM 中的重要性。
The catalytic functions of Pd are completely modified by alloying with Zn, and PdZn exhibits comparable catalytic selectivity to Cu in the steam reforming of methanol (SRM). We perform theoretical and experimental studies to confirm our previous argument that the position of the d -band is a significant factor determining catalytic properties. First-principles slab calculations for M –Zn ( M = Pd, Ni, Pt) reveal that the bond breaking on the surface leads to some reduction in the d -bandwidth, but that the position of the d -band for stable surfaces remains essentially unchanged from that of the bulk. The origin of the dramatic change in the electronic structure caused by alloying is theoretically demonstrated. Our previous argument is experimentally examined not only in SRM, but also in elemental reactions such as CO and H 2 adsorptions. Magnetic measurements also indicate the importance of the d -band position in SRM.