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利用碳纳米管作为“氢高速公路”鉴定负载型金属催化剂的活性位。

Identification of active sites on supported metal catalysts with carbon nanotube hydrogen highways.

机构信息

School of Chemical, Biological and Materials Engineering, University of Oklahoma, Norman, OK, 73019, USA.

Davidson School of Chemical Engineering, Purdue University, 480 Stadium Mall Drive, West Lafayette, IN, 47907, USA.

出版信息

Nat Commun. 2018 Sep 20;9(1):3827. doi: 10.1038/s41467-018-06100-9.

Abstract

Catalysts consisting of metal particles supported on reducible oxides exhibit promising activity and selectivity for a variety of current and emerging industrial processes. Enhanced catalytic activity can arise from direct contact between the support and the metal or from metal-induced promoter effects on the oxide. Discovering the source of enhanced catalytic activity and selectivity is challenging, with conflicting arguments often presented based on indirect evidence. Here, we separate the metal from the support by a controlled distance while maintaining the ability to promote defects via the use of carbon nanotube hydrogen highways. As illustrative cases, we use this approach to show that the selective transformation of furfural to methylfuran over Pd/TiO occurs at the Pd-TiO interface while anisole conversion to phenol and cresol over Cu/TiO is facilitated by exposed Ti cations on the support. This approach can be used to clarify many conflicting arguments in the literature.

摘要

担载于可还原氧化物上的金属颗粒组成的催化剂在各种现有和新兴的工业过程中表现出有前途的活性和选择性。增强的催化活性可能源于载体和金属之间的直接接触,或者源于金属对氧化物的促进剂效应。发现增强的催化活性和选择性的来源具有挑战性,经常根据间接证据提出相互矛盾的论点。在这里,我们通过使用碳纳米管氢高速公路在保持通过金属促进缺陷能力的同时,将金属与载体分离到可控的距离。作为说明性的情况,我们使用这种方法表明,在 Pd/TiO 界面上发生糠醛到甲基呋喃的选择性转化,而在 Cu/TiO 上,苯甲醚转化为苯酚和间甲酚则由载体上暴露的 Ti 阳离子促进。这种方法可用于澄清文献中的许多相互矛盾的论点。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1ae3/6148247/51d83b57af3c/41467_2018_6100_Fig1_HTML.jpg

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