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Open AccessArticle

Single-Atom Mn Active Site in a Triol-Stabilized β-Anderson Manganohexamolybdate for Enhanced Catalytic Activity towards Adipic Acid Production

by 1,2,†, 3,†, 1,2, 1,2, 1,2, 3,* and 3,*
1
Research Institute of Petroleum Exploration & Development (RIPED), Petro China, Beijing 100083, China
2
Key Laboratory of Nano Chemistry (KLNC), CNPC, Beijing 100083, China
3
Key Lab of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing 100084, China
*
Authors to whom correspondence should be addressed.
These authors contributed equally to this work.
Catalysts 2018, 8(3), 121; https://doi.org/10.3390/catal8030121
Received: 5 February 2018 / Revised: 10 March 2018 / Accepted: 14 March 2018 / Published: 19 March 2018
(This article belongs to the Special Issue Active Sites in Catalytic Reaction)
Adipic acid is an important raw chemical for the commercial production of polyamides and polyesters. The traditional industrial adipic acid production utilizes nitric acid to oxidize KA oil (mixtures of cyclohexanone and cyclohexanol), leading to the emission of N2O and thus causing ozone depletion, global warming, and acid rain. Herein, we reported an organically functionalized β-isomer of Anderson polyoxometalates (POMs) nanocluster with single-atom Mn, β-{[H3NC(CH2O)3]2MnMo6O18} (1), as a highly active catalyst to selectively catalyze the oxidation of cyclohexanone, cyclohexanol, or KA oil with atom economy use of 30% H2O2 for the eco-friendly synthesis of adipic acid. The catalyst has been characterized by single crystal and powder XRD, XPS, ESI-MS, FT-IR, and NMR. A cyclohexanone (cyclohexanol) conversion of >99.9% with an adipic acid selectivity of ~97.1% (~85.3%) could be achieved over catalyst 1 with high turnover frequency of 2427.5 h−1 (2132.5 h−1). It has been demonstrated that the existence of Mn3+ atom active site in catalyst 1 and the special butterfly-shaped topology of POMs both play vital roles in the enhancement of catalytic activity. View Full-Text
Keywords: polyoxometalates; catalytic oxidation; single-atom; active site engineering; KA oil; adipic acid polyoxometalates; catalytic oxidation; single-atom; active site engineering; KA oil; adipic acid
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MDPI and ACS Style

Luo, J.; Huang, Y.; Ding, B.; Wang, P.; Geng, X.; Zhang, J.; Wei, Y. Single-Atom Mn Active Site in a Triol-Stabilized β-Anderson Manganohexamolybdate for Enhanced Catalytic Activity towards Adipic Acid Production. Catalysts 2018, 8, 121.

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