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author:

Wang, Sikai (Wang, Sikai.) [1] | Fung, Victor (Fung, Victor.) [2] | Hulsey, Max J. (Hulsey, Max J..) [3] | Liang, Xiaocong (Liang, Xiaocong.) [4] | Yu, Zhiyang (Yu, Zhiyang.) [5] (Scholars:喻志阳) | Chang, Jinquan (Chang, Jinquan.) [6] | Folli, Andrea (Folli, Andrea.) [7] | Lewis, Richard J. (Lewis, Richard J..) [8] | Hutchings, Graham J. (Hutchings, Graham J..) [9] | He, Qian (He, Qian.) [10] | Yan, Ning (Yan, Ning.) [11]

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EI Scopus SCIE

Abstract:

The selective partial oxidation of methane to methanol using molecular oxygen (O-2) represents a long-standing challenge, inspiring extensive study for many decades. However, considerable challenges still prevent low-temperature methane activation via the aerobic route. Here we report a precipitated Pd-containing phosphomolybdate, which, after activation by molecular hydrogen (H2), converts methane and O-2 almost exclusively to methanol at room temperature. The highest activity reaches 67.4 mu mol gcat(-1) h(-1). Pd enables rapid H-2 activation and H spillover to phosphomolybdate for Mo reduction, while facile O-2 activation and subsequent methane activation occur on the reduced phosphomolybdate sites. Continuous production of methanol from methane was also achieved by concurrently introducing H-2, O-2 and methane into the system, where H-2 assists in maintaining a moderately reduced state of phosphomolybdate. This work reveals the underexplored potential of such a Mo-based catalyst for aerobic methane oxidation and highlights the importance of regulating the chemical valence state to construct methane active sites.

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Community:

  • [ 1 ] [Wang, Sikai]Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou, Peoples R China
  • [ 2 ] [Chang, Jinquan]Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou, Peoples R China
  • [ 3 ] [Yan, Ning]Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou, Peoples R China
  • [ 4 ] [Wang, Sikai]Natl Univ Singapore, Dept Chem & Biomol Engn, Singapore, Singapore
  • [ 5 ] [Hulsey, Max J.]Natl Univ Singapore, Dept Chem & Biomol Engn, Singapore, Singapore
  • [ 6 ] [Chang, Jinquan]Natl Univ Singapore, Dept Chem & Biomol Engn, Singapore, Singapore
  • [ 7 ] [Yan, Ning]Natl Univ Singapore, Dept Chem & Biomol Engn, Singapore, Singapore
  • [ 8 ] [Fung, Victor]Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA
  • [ 9 ] [Fung, Victor]Georgia Inst Technol, Sch Computat Sci & Engn, Atlanta, GA USA
  • [ 10 ] [Liang, Xiaocong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou, Peoples R China
  • [ 11 ] [Yu, Zhiyang]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou, Peoples R China
  • [ 12 ] [Folli, Andrea]Cardiff Univ, Net Zero Innovat Inst, Cardiff Catalysis Inst, Sch Chem, Cardiff, Wales
  • [ 13 ] [Lewis, Richard J.]Cardiff Univ, Max Planck Cardiff Ctr Fundamentals Heterogeneous, Sch Chem, Cardiff Catalysis Inst, Cardiff, Wales
  • [ 14 ] [Hutchings, Graham J.]Cardiff Univ, Max Planck Cardiff Ctr Fundamentals Heterogeneous, Sch Chem, Cardiff Catalysis Inst, Cardiff, Wales
  • [ 15 ] [He, Qian]Natl Univ Singapore, Dept Mat Sci & Engn, Singapore, Singapore
  • [ 16 ] [Yan, Ning]Natl Univ Singapore, Ctr Hydrogen Innovat, Singapore, Singapore

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NATURE CATALYSIS

ISSN: 2520-1158

Year: 2023

4 2 . 9

JCR@2023

4 2 . 9 0 0

JCR@2023

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 0

SCOPUS Cited Count: 49

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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