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在单原子极限条件下铂铜合金上1,3 - 丁二烯的选择性加氢反应

Selective hydrogenation of 1,3-butadiene on platinum-copper alloys at the single-atom limit.

作者信息

Lucci Felicia R, Liu Jilei, Marcinkowski Matthew D, Yang Ming, Allard Lawrence F, Flytzani-Stephanopoulos Maria, Sykes E Charles H

机构信息

Department of Chemistry, Tufts University, 62 Talbot Avenue, Medford, Massachusetts 02155, USA.

Department of Chemical and Biological Engineering, Tufts University, 4 Colby Street, Medford, Massachusetts 02155, USA.

出版信息

Nat Commun. 2015 Oct 9;6:8550. doi: 10.1038/ncomms9550.

Abstract

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.

摘要

铂在化工和燃料生产领域无处不在;然而,其在自然界中的稀缺性和高昂价格将限制未来铂催化反应的推广。一种有前景的铂节约方法是了解催化反应所需的最少铂原子数量,然后设计具有最小铂簇的催化剂。在此,我们设计并测试了用于1,3 - 丁二烯选择性加氢的新一代铂 - 铜纳米颗粒催化剂,这是一个具有工业重要性的反应。孤立的铂原子几何结构能够实现氢的活化和溢流,但无法进行导致选择性丧失和催化剂失活的碳 - 碳键断裂。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对丁二烯加氢生成丁烯表现出高活性和选择性,证明了从模型研究到实际条件下催化反应的可转移性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6c65/4633827/5a00cb132e15/ncomms9550-f1.jpg

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