Abstract
Gas flaring in oil/gas drilling and gas leakage in natural gas power plant lead to significant energy loss and environmental burden. Here, solar-driven efficient methane oxidation was demonstrated under high velocity continuous flow over the ZnO/La0.8Sr0.2CoO3 (ZnO/LSCO) heterojunctions. The ZnO/LSCO heterojunctions enable a unique epitaxial hetero-interface, which effectively regulates the electron transfer between Zn 3d-O 2p hybrid orbital in ZnO and Co eg orbital in LSCO and promotes the rapid generation and refill of oxygen vacancy with unpaired electron (Vo[rad]), thus enhancing the activity and mobility of surface lattice oxygen in ZnO/LSCO. Under solar illumination, the synergy of photothermal and photocatalytic effect boosts the reversible electron transfer in the interface, which further activates surface lattice oxygen, resulting in a ∼2 times higher methane oxidation activity. Such a solar-driven system not only enables a promising pathway for emitted methane utilization, but also provides an advanced catalyst design concept of epitaxial interface construction.
| Original language | English |
|---|---|
| Article number | 118469 |
| Journal | Applied Catalysis B: Environmental |
| Volume | 265 |
| DOIs | |
| State | Published - May 15 2020 |
Funding
Ji Yang and Wen Xiao contribute equally to this work. The authors are grateful for the financial support from the National Natural Science Foundation of China (No. 21777051 ), The Recruitment Program of Global Young Experts start-up funds , The Program of Introducing Talents of Discipline to Universities of China (111 program, B17019 ), the U.S. Department of Energy (DOE) (Award Nos. DE-EE0000210 and DE-EE0006854 ) and the U.S. National Science Foundation (Award No. CBET 1344792 ). Z. W. was supported by the U.S. DOE Office of Science , Office of Basic Energy Sciences , Chemical Sciences, Geosciences, and Biosciences Division . Part of the work including CO-TPR and O 2 isotope exchange experiments were conducted at the Center for Nanophase Materials Sciences at the Oak Ridge National Laboratory, a DOE Office of Science User Facility. The authors would like to acknowledge the Singapore Synchrotron Light Source (SSLS) for providing the facility necessary for conducting the research. The Laboratory is a National Research Infrastructure under the National Research Foundation Singapore. Appendix A Ji Yang and Wen Xiao contribute equally to this work. The authors are grateful for the financial support from the National Natural Science Foundation of China (No. 21777051), The Recruitment Program of Global Young Experts start-up funds, The Program of Introducing Talents of Discipline to Universities of China (111 program, B17019), the U.S. Department of Energy (DOE) (Award Nos. DE-EE0000210 and DE-EE0006854) and the U.S. National Science Foundation (Award No. CBET 1344792). Z. W. was supported by the U.S. DOE Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. Part of the work including CO-TPR and O2 isotope exchange experiments were conducted at the Center for Nanophase Materials Sciences at the Oak Ridge National Laboratory, a DOE Office of Science User Facility. The authors would like to acknowledge the Singapore Synchrotron Light Source (SSLS) for providing the facility necessary for conducting the research. The Laboratory is a National Research Infrastructure under the National Research Foundation Singapore.
Keywords
- Epitaxial hetero-interface
- Photo-excited electrons
- Photothermal effect
- Reversible electron transfer
- Solar-driven methane oxidation