Photoassisted Selective Steam and Dry Reforming of Methane to Syngas Catalyzed by Rhodium–Vanadium Bimetallic Oxide Cluster Anions at Room Temperature
Dr. Yan-Xia Zhao
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorDr. Bin Yang
State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences, Beijing, 100049 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorDr. Hai-Fang Li
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorYan Zhang
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorYuan Yang
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences, Beijing, 100049 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorDr. Qing-Yu Liu
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorDr. Hong-Guang Xu
State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Wei-Jun Zheng
State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences, Beijing, 100049 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Sheng-Gui He
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences, Beijing, 100049 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorDr. Yan-Xia Zhao
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorDr. Bin Yang
State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences, Beijing, 100049 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorDr. Hai-Fang Li
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorYan Zhang
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorYuan Yang
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences, Beijing, 100049 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorDr. Qing-Yu Liu
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorDr. Hong-Guang Xu
State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Wei-Jun Zheng
State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences, Beijing, 100049 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Sheng-Gui He
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 P. R. China
University of Chinese Academy of Sciences, Beijing, 100049 P. R. China
Beijing National Laboratory for Molecular Sciences and CAS Research/Education Centre of Excellence in Molecular Sciences, Beijing, 100190 P. R. China
Search for more papers by this authorAbstract
Photoassisted steam reforming and dry (CO2) 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 Rh2VO1–3−. Both the oxidation of methane and reduction of H2O/CO2 can take place efficiently in the dark while the pivotal step to govern syngas selectivity is photo-excitation of the reaction intermediates Rh2VO2,3CH2− to specific electronically excited states that can selectively produce CO and H2. Electronic excitation over Rh2VO2,3CH2− to control the syngas selectivity is further confirmed from the comparison with the thermal excitation of Rh2VO2,3CH2−, 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.
Conflict of interest
The authors declare no conflict of interest.
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