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Author:

Gu, Fubo (Gu, Fubo.) | Qin, Xuetao (Qin, Xuetao.) | Li, Mengwei (Li, Mengwei.) | Xu, Yao (Xu, Yao.) | Hong, Song (Hong, Song.) | Ouyang, Mengyao (Ouyang, Mengyao.) | Giannakakis, Georgios (Giannakakis, Georgios.) | Cao, Sufeng (Cao, Sufeng.) | Peng, Mi (Peng, Mi.) | Xie, Jinling (Xie, Jinling.) | Wang, Meng (Wang, Meng.) | Han, Dongmei (Han, Dongmei.) | Xiao, Dequan (Xiao, Dequan.) | Wang, Xiayan (Wang, Xiayan.) (Scholars:汪夏燕) | Wang, Zhihua (Wang, Zhihua.) | Ma, Ding (Ma, Ding.)

Indexed by:

EI Scopus SCIE

Abstract:

Direct conversion of methane into value-added chemicals, such as methanol under mild conditions, is a promising route for industrial applications. In this work, atomically dispersed Rh on TiO2 suspended in an aqueous solution was used for the oxidation of methane to methanol. Promoted by copper cations (as co-catalyst) in solution, the catalysts exhibited high activity and selectivity for the production of methanol using molecular oxygen with the presence of carbon monoxide at 150 degrees C with a reaction pressure of 31 bar. Millimole level yields of methanol were reached with the selectivity higher than 99 % using the Rh/TiO2 catalysts with the promotion of the copper cation. CO was the reductive agent to generate H-2 from H2O, which led to the formation of H2O2 through the reaction of H-2 and O-2. Atomically dispersed Rh activated the C-H bond in CH4 and catalyzed the oxidation using H2O2. Copper cations maintained the low-valence state of Rh. Moreover, copper acted as a scavenger for suppressing the overoxidation, thus leading to the high selectivity of methanol.

Keyword:

Atomic Dispersion Copper Cations Rhodium Methane Methanol

Author Community:

  • [ 1 ] [Gu, Fubo]Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
  • [ 2 ] [Hong, Song]Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
  • [ 3 ] [Han, Dongmei]Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
  • [ 4 ] [Wang, Zhihua]Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
  • [ 5 ] [Gu, Fubo]Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China
  • [ 6 ] [Hong, Song]Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China
  • [ 7 ] [Han, Dongmei]Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China
  • [ 8 ] [Wang, Zhihua]Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China
  • [ 9 ] [Qin, Xuetao]Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
  • [ 10 ] [Xu, Yao]Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
  • [ 11 ] [Peng, Mi]Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
  • [ 12 ] [Xie, Jinling]Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
  • [ 13 ] [Wang, Meng]Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
  • [ 14 ] [Ma, Ding]Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
  • [ 15 ] [Qin, Xuetao]Peking Univ, Coll Engn, Beijing 100871, Peoples R China
  • [ 16 ] [Xu, Yao]Peking Univ, Coll Engn, Beijing 100871, Peoples R China
  • [ 17 ] [Peng, Mi]Peking Univ, Coll Engn, Beijing 100871, Peoples R China
  • [ 18 ] [Xie, Jinling]Peking Univ, Coll Engn, Beijing 100871, Peoples R China
  • [ 19 ] [Wang, Meng]Peking Univ, Coll Engn, Beijing 100871, Peoples R China
  • [ 20 ] [Ma, Ding]Peking Univ, Coll Engn, Beijing 100871, Peoples R China
  • [ 21 ] [Qin, Xuetao]Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
  • [ 22 ] [Xu, Yao]Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
  • [ 23 ] [Peng, Mi]Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
  • [ 24 ] [Xie, Jinling]Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
  • [ 25 ] [Wang, Meng]Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
  • [ 26 ] [Ma, Ding]Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
  • [ 27 ] [Li, Mengwei]Tufts Univ, Dept Chem & Biol Engn, Medford, MA 02155 USA
  • [ 28 ] [Ouyang, Mengyao]Tufts Univ, Dept Chem & Biol Engn, Medford, MA 02155 USA
  • [ 29 ] [Giannakakis, Georgios]Tufts Univ, Dept Chem & Biol Engn, Medford, MA 02155 USA
  • [ 30 ] [Cao, Sufeng]Tufts Univ, Dept Chem & Biol Engn, Medford, MA 02155 USA
  • [ 31 ] [Xiao, Dequan]Univ New Haven, Ctr Integrat Mat Discovery, Dept Chem & Chem Engn, West Haven, CT 06516 USA
  • [ 32 ] [Wang, Xiayan]Beijing Univ Technol, Dept Chem & Biol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China

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Source :

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

ISSN: 1433-7851

Year: 2022

Issue: 18

Volume: 61

1 6 . 6

JCR@2022

1 6 . 6 0 0

JCR@2022

ESI Discipline: CHEMISTRY;

ESI HC Threshold:53

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 46

SCOPUS Cited Count: 51

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 11

Affiliated Colleges:

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