| Title | Oxynitride-surface engineering of rhodium-decorated gallium nitride for efficient thermocatalytic hydrogenation of carbon dioxide to carbon monoxide |
| Authors | Li, Jinglin Sheng, Bowen Chen, Yiqing Sadaf, Sharif Md Yang, Jiajia Wang, Ping Pan, Hu Ma, Tao Zhu, Lei Song, Jun Lin, He Wang, Xinqiang Huang, Zhen Zhou, Baowen |
| Affiliation | Shanghai Jiao Tong Univ, Sch Mech Engn, Key Lab Power Machinery & Engn, Minist Educ, 800 Dongchuan Rd, Shanghai 200240, Peoples R China Peking Univ, State Key Lab Artificial Microstruct & Mesoscop P, Sch Phys, Nanooptoelect Frontier Ctr,Minist Educ NFC MOE, Beijing 10087, Peoples R China McGill Univ, Dept Min & Mat Engn, 3610 Univ St, Montreal, PQ H3A 0C9, Canada Univ Quebec, Ctr Energie Mat & Telecommun, Inst Natl Rech Sci INRS, 1650 Blvd Lionel Boulet, Varennes, PQ J3X 1S2, Canada Univ Michigan, Michigan Ctr Mat & Characterizat, 2800 Plymouth Rd, Ann Arbor, MI 48109 USA Peking Univ, Yangtze Delta Inst Optoelect, Nantong 226010, Jiangsu, Peoples R China Peking Univ, Collaborat Innovat Ctr Quantum Matter, Sch Phys, Beijing 100871, Peoples R China |
| Keywords | WATER-GAS SHIFT CO2 HYDROGENATION PREFERENTIAL OXIDATION INFRARED-SPECTROSCOPY CONVERTING CO2 REDUCTION ENERGY MECHANISM SELECTIVITY ACTIVATION |
| Issue Date | 6-Sep-2022 |
| Publisher | COMMUNICATIONS CHEMISTRY |
| Abstract | Upcycling of carbon dioxide towards fuels and value-added chemicals poses an opportunity to overcome challenges faced by depleting fossil fuels and climate change. Herein, combining highly controllable molecular beam epitaxy growth of gallium nitride (GaN) under a nitrogen-rich atmosphere with subsequent air annealing, a tunable platform of gallium oxynitride (GaN1-xOx) nanowires is built to anchor rhodium (Rh) nanoparticles for carbon dioxide hydrogenation. By correlatively employing various spectroscopic and microscopic characterizations, as well as density functional theory calculations, it is revealed that the engineered oxynitride surface of GaN works in synergy with Rh to achieve a dramatically reduced energy barrier. Meanwhile, the potential-determining step is switched from *COOH formation into *CO desorption. As a result, significantly improved CO activity of 127 mmol.g(cat)(-1).h(-1) is achieved with high selectivity of >94% at 290 degrees C under atmospheric pressure, which is three orders of magnitude higher than that of commercial Rh/Al2O3. Furthermore, capitalizing on the high dispersion of the Rh species, the architecture illustrates a decent turnover frequency of 270 mol CO per mol Rh per hour over 9 cycles of operation. This work presents a viable strategy for promoting CO2 refining via surface engineering of an advanced support, in collaboration with a suitable metal cocatalyst. |
| URI | http://hdl.handle.net/20.500.11897/654281 |
| ISSN | 2399-3669 |
| DOI | 10.1038/s42004-022-00728-x |
| Indexed | SCI(E) |
| Appears in Collections: | 物理学院 人工微结构和介观物理国家重点实验室 |
