PMID- 37092261
OWN - NLM
STAT- PubMed-not-MEDLINE
DCOM- 20230516
LR  - 20230516
IS  - 1477-9234 (Electronic)
IS  - 1477-9226 (Linking)
VI  - 52
IP  - 19
DP  - 2023 May 16
TI  - Solvent-free oxidation of benzyl C-H to ketone with Co-Ni layered double 
      hydroxide as the catalyst and O(2) as the sole oxidant.
PG  - 6398-6406
LID - 10.1039/d3dt00851g [doi]
AB  - The aerobic oxidation of ethylbenzene is an effective way to produce 
      acetophenone, in which solvent-free conditions and oxygen as the sole oxidant are 
      the best choice. At present, the catalytic activity and selectivity are still at 
      an unsatisfactory level, because efficient catalysts need to achieve both C-H 
      bond activation and O(2) activation. In this work, the 2-methylimidazole-induced 
      hydrolysis strategy was used to prepare a new class of CoNi-layered double 
      hydroxide (CoNi-LDH) materials with different metal ratios. High-Resolution 
      Transmission Electron Microscopy (HRTEM) showed that CoNi-LDH had obvious weak 
      crystallinity and a thin lamellar structure. X-ray Photoelectron Spectroscopy 
      (XPS) reveals the consistency between the content of the M-O component in the 
      host layer and the proportion of Co(3+), among which CoNi-LDH with a feed ratio 
      (Co : Ni) of 2 : 1 (Co(2)Ni-LDH) has the highest M-O content and Co(3+) ratio. 
      The formation of M-O is due to the H-vacancy generated by the breaking of the 
      hydroxyl group, which can be used for the H abstraction of C-H bonds. The redox 
      effect caused by M(2+)/M(3+) facilitates the transfer of electrons, which 
      promotes the activation of O(2) to the superoxide radical anion ( O(2)(-)). 
      Thereby, Co(2)Ni-LDH shows the highest catalytic activity for the oxidation of 
      ethylbenzene. Under solvent-free conditions and with oxygen as the sole oxidant, 
      97.8% conversion of ethylbenzene and 98.8% selectivity of acetophenone can be 
      obtained. The excellent catalytic performance is related to the structure of 
      CoNi-LDH, and is also the best when compared with the reported results. Various 
      types of aromatic hydrocarbons containing benzyl C-H bonds can be effectively 
      oxidized by CoNi-LDH to produce the corresponding ketone products.
FAU - Ren, Jiali
AU  - Ren J
AD  - Anhui Provincial Key Laboratory for Degradation and Monitoring of Pollution of 
      the Environment, School of Chemistry and Materials Engineering Fuyang Normal 
      University, Fuyang 236037, P. R. China. huimiao@mail.ahnu.edu.cn.
FAU - Zhou, Yan
AU  - Zhou Y
AD  - Key Laboratory of Functional Molecular Solids, Ministry of Education, College of 
      Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China. 
      chenzh07@mail.ahnu.edu.cn.
FAU - Miao, Hui
AU  - Miao H
AUID- ORCID: 0000-0001-7451-1311
AD  - Anhui Provincial Key Laboratory for Degradation and Monitoring of Pollution of 
      the Environment, School of Chemistry and Materials Engineering Fuyang Normal 
      University, Fuyang 236037, P. R. China. huimiao@mail.ahnu.edu.cn.
FAU - Wang, Chaoqun
AU  - Wang C
AD  - Anhui Provincial Key Laboratory for Degradation and Monitoring of Pollution of 
      the Environment, School of Chemistry and Materials Engineering Fuyang Normal 
      University, Fuyang 236037, P. R. China. huimiao@mail.ahnu.edu.cn.
FAU - Lv, Shanshan
AU  - Lv S
AD  - Key Laboratory of Functional Molecular Solids, Ministry of Education, College of 
      Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China. 
      chenzh07@mail.ahnu.edu.cn.
FAU - Song, Manman
AU  - Song M
AD  - Key Laboratory of Functional Molecular Solids, Ministry of Education, College of 
      Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China. 
      chenzh07@mail.ahnu.edu.cn.
FAU - Li, Feng
AU  - Li F
AD  - Key Laboratory of Functional Molecular Solids, Ministry of Education, College of 
      Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China. 
      chenzh07@mail.ahnu.edu.cn.
FAU - Feng, Mengmeng
AU  - Feng M
AD  - Key Laboratory of Functional Molecular Solids, Ministry of Education, College of 
      Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China. 
      chenzh07@mail.ahnu.edu.cn.
FAU - Chen, Zheng
AU  - Chen Z
AUID- ORCID: 0000-0002-4347-0235
AD  - Key Laboratory of Functional Molecular Solids, Ministry of Education, College of 
      Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China. 
      chenzh07@mail.ahnu.edu.cn.
LA  - eng
PT  - Journal Article
DEP - 20230516
PL  - England
TA  - Dalton Trans
JT  - Dalton transactions (Cambridge, England : 2003)
JID - 101176026
SB  - IM
EDAT- 2023/04/24 06:42
MHDA- 2023/04/24 06:43
CRDT- 2023/04/24 04:12
PHST- 2023/04/24 06:43 [medline]
PHST- 2023/04/24 06:42 [pubmed]
PHST- 2023/04/24 04:12 [entrez]
AID - 10.1039/d3dt00851g [doi]
PST - epublish
SO  - Dalton Trans. 2023 May 16;52(19):6398-6406. doi: 10.1039/d3dt00851g.