Control of surface reactivity towards unsaturated C C bonds and H over Ni-based intermetallic compounds in semi-hydrogenation of acetylene
Control of surface reactivity towards unsaturated C C bonds and H over Ni-based intermetallic compounds in semi-hydrogenation of acetylene
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DOI：
10.1016/j.jcat.2019.02.018
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发表时间：
2019-04
影响因子：
7.3
通讯作者：
Yuanjun Song;Siris Laursen
中科院分区：
文献类型：
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作者：
Yuanjun Song;Siris Laursen
由过渡金属和半金属或后过渡金属组成的金属间化合物已被证明在烯烃和芳烃生产以及需要控制 C 双键 C 活化和官能化的其他反应中表现出较高的选择性。可用于金属间化合物生产的大量元素组合需要向下选择以隔离催化有用的组成空间。在这项研究中，我们研究了乙炔在由镍和硼族元素组成的等电子金属间化合物上以1:1的体积化学计量比进行的半氢化。我们已经分离出IMC组成元素之间的轨道重叠与其本体键合的性质、表面反应性以及乙炔半氢化成乙烯的催化偏好很好地吻合。孤立的趋势似乎是普遍的，并且标志着金属间化合物内的一个子空间，有望成为进一步研究的重点。结果还表明，有可能在金属间化合物的子空间上建立新布朗斯特-埃文斯-波兰尼关系。
Intermetallic compounds composed of transition metals and semimetals or post-transition metals have been shown to exhibit elevated selectivity in olefins and aromatics production and other reactions that require control of Cdouble bond C activation and functionalization. The vast number of element combinations available for intermetallic compound production necessitates down-selecting to isolate catalytically useful compositional spaces. In this study, we have investigated the semi-hydrogenation of acetylene over isoelectronic intermetallic compounds composed of nickel and the boron group elements at a bulk stoichiometry of 1: 1. We have isolated that orbital overlap between IMC constituent elements tracks well with the nature of their bulk bonding, surface reactivity, and catalytic preference for the semi-hydrogenation of acetylene to ethylene. The trend isolated appears to be universal and marks a subspace within intermetallic compounds that is promising to focus further studies upon. Results also suggest the possibility of accessing New Br ø nsted–Evans–Polanyi relationships over a subspace of intermetallic compounds.