Selective hydrogenation of 1,3-butadiene on platinum-copper alloys at the single-atom limit.
Selective hydrogenation of 1,3-butadiene on platinum-copper alloys at the single-atom limit.
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DOI：
10.1038/ncomms9550
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发表时间：
2015-10-09
影响因子：
16.6
通讯作者：
Sykes EC
中科院分区：
文献类型：
--
作者：
Lucci FR;Liu J;Marcinkowski MD;Yang M;Allard LF;Flytzani-Stephanopoulos M;Sykes EC
铂在化学品和燃料的生产部门中无处不在;然而，其稀缺性和高价格将限制铂催化反应的未来扩散。一种有希望的保存铂的方法是了解催化反应所需的最小数量的铂原子，然后设计具有最小铂集合的催化剂。在这里，我们设计并测试了新一代的铂-铜纳米颗粒催化剂，用于1，3-丁二烯的选择性氢化，这是一个工业上重要的反应。孤立的铂原子几何形状能够使氢活化和溢出，但不能导致选择性损失和催化剂失活的C-C键断裂。研究发现，每100个铜原子中铂原子数小于1的γ-氧化铝负载的单原子合金纳米颗粒催化剂在温和条件下表现出较高的丁二烯加氢活性和丁烯选择性，证明了模型研究到实际条件下催化反应的可移植性。 降低工业催化剂中的铂含量是一个重要的研究目标。在这里，作者提出了一种含有少于1%铂的纳米催化剂，其中孤立的铂原子有助于丁二烯氢化的催化剂活性和选择性。
Platinum is ubiquitous in the production sectors of chemicals and fuels; however, its scarcity in nature and high price will limit future proliferation of platinum-catalysed reactions. One promising approach to conserve platinum involves understanding the smallest number of platinum atoms needed to catalyse a reaction, then designing catalysts with the minimal platinum ensembles. Here we design and test a new generation of platinum–copper nanoparticle catalysts for the selective hydrogenation of 1,3-butadiene,, an industrially important reaction. Isolated platinum atom geometries enable hydrogen activation and spillover but are incapable of C–C bond scission that leads to loss of selectivity and catalyst deactivation. γ-Alumina-supported single-atom alloy nanoparticle catalysts with <1 platinum atom per 100 copper atoms are found to exhibit high activity and selectivity for butadiene hydrogenation to butenes under mild conditions, demonstrating transferability from the model study to the catalytic reaction under practical conditions. Reducing the platinum content of industrial catalysts is an important research target. Here, the authors present a nanocatalyst containing less than 1% platinum, where the isolated platinum atoms contribute to both the catalyst activity and selectivity for butadiene hydrogenation.