4.7 Article

Neighboring Cu toward Mn site in confined mesopore to trigger strong interplay for boosting catalytic epoxidation of styrene

Journal

APPLIED SURFACE SCIENCE
Volume 537, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apsusc.2020.148100

Keywords

Synergy; Neighboring effect; Strong interplay; Mesopore; Styrene epoxidation

Funding

  1. National Natural Science Foundation of China [21908085, 21776129, 21706121]
  2. Natural Science Foundation of Jiangsu Province [BK20170995, BK20190961]
  3. General Program for University Natural Science Research of Jiangsu Province [16KJB530003]
  4. Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)

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This study developed an efficient controlled approach to create synergetic neighboring dual-metal active sites in confined mesopores of silica, by designing Mn-bearing mesoporous molecular sieve via a metal-assisted in-situ assembly route and further accommodating external Cu. The formed neighboring Cu-Mn species showed synergy in catalytic reactions, weakening and reinforcing chemical bonds in intermediates, providing a potential method for universal synergetic catalysts in industrial heterogeneous catalysis.
Herein, we report an efficient controlled approach to reach the synergetic neighboring dual-metal active sites in the confined mesopore of silica. In this approach, Mn-bearing mesoporous molecular sieve was designed in advance via a metal-assisted in-situ assembly route and further employed as a starting carrier to accommodate more extraneous Cu by impregnation. Controlling copper loading (Cu/Mn = 0.2, 0.4, and 0.6), comparative catalysts were attained and precisely characterized by key physicochemical methods. Impressively, in-situ formed highly-dispersed MnOx covered on the mesopore become the prerequisite for producing interplayed active species with neighboring dual Cu-Mn sites. Catalytic results concerning styrene epoxidation together with DRIFTS experiments and calculated bond energy variation in expected reaction intermediates demonstrated the existed synergy derived from formed neighboring Cu-Mn species via weakening and reinforcing appointed chemical bonds in intermediates. This study provides the foreseeable possibility for attaining universal synergetic catalysts in industrial heterogeneous catalysis.

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