High-performance photocatalytic nonoxidative conversion of methane to ethane and hydrogen by heteroatoms-engineered TiO2 View Full Text


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Article Info

DATE

2022-05-19

AUTHORS

Wenqing Zhang, Cenfeng Fu, Jingxiang Low, Delong Duan, Jun Ma, Wenbin Jiang, Yihong Chen, Hengjie Liu, Zeming Qi, Ran Long, Yingfang Yao, Xiaobao Li, Hui Zhang, Zhi Liu, Jinlong Yang, Zhigang Zou, Yujie Xiong

ABSTRACT

Nonoxidative coupling of methane (NOCM) is a highly important process to simultaneously produce multicarbons and hydrogen. Although oxide-based photocatalysis opens opportunities for NOCM at mild condition, it suffers from unsatisfying selectivity and durability, due to overoxidation of CH4 with lattice oxygen. Here, we propose a heteroatom engineering strategy for highly active, selective and durable photocatalytic NOCM. Demonstrated by commonly used TiO2 photocatalyst, construction of Pd–O4 in surface reduces contribution of O sites to valence band, overcoming the limitations. In contrast to state of the art, 94.3% selectivity is achieved for C2H6 production at 0.91 mmol g–1 h–1 along with stoichiometric H2 production, approaching the level of thermocatalysis at relatively mild condition. As a benchmark, apparent quantum efficiency reaches 3.05% at 350 nm. Further elemental doping can elevate durability over 24 h by stabilizing lattice oxygen. This work provides new insights for high-performance photocatalytic NOCM by atomic engineering. More... »

PAGES

2806

Identifiers

URI

http://scigraph.springernature.com/pub.10.1038/s41467-022-30532-z

DOI

http://dx.doi.org/10.1038/s41467-022-30532-z

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1147992154

PUBMED

https://www.ncbi.nlm.nih.gov/pubmed/35589743


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16 schema:description Nonoxidative coupling of methane (NOCM) is a highly important process to simultaneously produce multicarbons and hydrogen. Although oxide-based photocatalysis opens opportunities for NOCM at mild condition, it suffers from unsatisfying selectivity and durability, due to overoxidation of CH4 with lattice oxygen. Here, we propose a heteroatom engineering strategy for highly active, selective and durable photocatalytic NOCM. Demonstrated by commonly used TiO2 photocatalyst, construction of Pd–O4 in surface reduces contribution of O sites to valence band, overcoming the limitations. In contrast to state of the art, 94.3% selectivity is achieved for C2H6 production at 0.91 mmol g–1 h–1 along with stoichiometric H2 production, approaching the level of thermocatalysis at relatively mild condition. As a benchmark, apparent quantum efficiency reaches 3.05% at 350 nm. Further elemental doping can elevate durability over 24 h by stabilizing lattice oxygen. This work provides new insights for high-performance photocatalytic NOCM by atomic engineering.
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22 schema:keywords CH4
23 H2 production
24 NOCM
25 O sites
26 TiO2
27 TiO2 photocatalyst
28 apparent quantum efficiency
29 art
30 atomic engineering
31 band
32 conditions
33 construction
34 contrast
35 contribution
36 conversion
37 coupling
38 doping
39 durability
40 efficiency
41 elemental doping
42 engineering
43 engineering strategies
44 hydrogen
45 important process
46 insights
47 lattice oxygen
48 levels
49 limitations
50 methane
51 mild conditions
52 multicarbon
53 new insights
54 nonoxidative conversion
55 nonoxidative coupling
56 opportunities
57 overoxidation
58 oxygen
59 photocatalysis
60 photocatalyst
61 process
62 production
63 quantum efficiency
64 selectivity
65 sites
66 state
67 strategies
68 surface
69 thermocatalysis
70 valence band
71 work
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