In:
Angewandte Chemie International Edition, Wiley, Vol. 59, No. 47 ( 2020-11-16), p. 21216-21223
Abstract:
Photoassisted steam reforming and dry (CO 2 ) reforming of methane (SRM and DRM) at room temperature with high syngas selectivity have been achieved in the gas‐phase catalysis for the first time. The catalysts used are bimetallic rhodium–vanadium oxide cluster anions of Rh 2 VO 1–3 − . Both the oxidation of methane and reduction of H 2 O/CO 2 can take place efficiently in the dark while the pivotal step to govern syngas selectivity is photo‐excitation of the reaction intermediates Rh 2 VO 2,3 CH 2 − to specific electronically excited states that can selectively produce CO and H 2 . Electronic excitation over Rh 2 VO 2,3 CH 2 − to control the syngas selectivity is further confirmed from the comparison with the thermal excitation of Rh 2 VO 2,3 CH 2 − , which leads to diversity of products. The atomic‐level mechanism obtained from the well‐controlled cluster reactions provides insight into the process of selective syngas production from the photocatalytic SRM and DRM reactions over supported metal oxide catalysts.
Type of Medium:
Online Resource
ISSN:
1433-7851
,
1521-3773
DOI:
10.1002/anie.202010026
Language:
English
Publisher:
Wiley
Publication Date:
2020
detail.hit.zdb_id:
2011836-3
detail.hit.zdb_id:
123227-7