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纳米碳上的氧化脱氢:本征催化活性与结构-功能关系。

Oxidative Dehydrogenation on Nanocarbon: Intrinsic Catalytic Activity and Structure-Function Relationships.

机构信息

Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016 (China).

Fritz Haber Institute of the Max Planck Society, 14195 Berlin (Germany).

出版信息

Angew Chem Int Ed Engl. 2015 Nov 9;54(46):13682-5. doi: 10.1002/anie.201505818. Epub 2015 Sep 21.

Abstract

Physical and chemical insights into the nature and quantity of the active sites and the intrinsic catalytic activity of nanocarbon materials in alkane oxidative dehydrogenation (ODH) reactions are reported using a novel in situ chemical titration process. A study on the structure-function relationship reveals that the active sites are identical both in nature and function on various nanocarbon catalysts. Additionally, the quantity of the active sites could be used as a metric to normalize the reaction rates, and thus to evaluate the intrinsic activity of nanocarbon catalysts. The morphology of the nanocarbon catalysts at the microscopic scale exhibits a minor influence on their intrinsic ODH catalytic activity. The number of active sites calculated from the titration process indicates the number of catalytic centers that are active (that is, working) under the reaction conditions.

摘要

本文采用一种新颖的原位化学滴定法,深入研究了纳米碳材料在烷烃氧化脱氢(ODH)反应中活性位的本质、数量及其固有催化活性的理化性质。通过结构-功能关系研究发现,各种纳米碳催化剂的活性位在本质和功能上是相同的。此外,活性位的数量可作为归一化反应速率的指标,从而评估纳米碳催化剂的固有活性。在微观尺度上,纳米碳催化剂的形态对其固有 ODH 催化活性的影响较小。从滴定过程中计算出的活性位数量表明,在反应条件下,活性(即工作)的催化中心的数量。

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