作者: |
Rui Song1,2,3#, Guanshu Zhao2#, Juan Manuel Restrepo-Flórez4,5, Camilo J. Viasus Pérez2, Zhijie Chen1,3, Chaoqian Ai6, Andrew Wang2, Dengwei Jing6, Athanasios A. Tountas7, Jiuli Guo2, Chengliang Mao2, Chaoran Li1,8, Jiahui Shen1, Guangming Cai7, Chenyue Qiu9, Jessica Ye2, Yubin Fu10, Chistos T. Maravelias11,12, Lu Wang13, Junchuan Sun13, Yang-Fan Xu2, Zhao Li2, Joel Yi Yang Loh2, Nhat Truong Nguyen14, Le He1,3*, Xiaohong Zhang1,3* & Geoffrey A. Ozin2* |
单位: |
1Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou, P. R. China. 2Solar Fuels Group, Department of Chemistry, University of Toronto, Toronto, Ontario, Canada. 3Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, P. R. China. 4Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, WI, USA. 5Department of Chemical Engineering, University of Florida, Gainesville, FL, USA. 6International Research Center for Renewable Energy, StateKey Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, Xi’an, P. R. China. 7Department of Chemical Engineering and Applied Chemistry, University of Toronto, Toronto, Ontario, Canada. 8Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, P. R. China. 9Department of Materials Science and Engineering, University of Toronto, Toronto, Ontario, Canada. 10Max Planck Institute of Microstructure Physics, Halle, Germany. 11Department of Chemical and Biological Engineering, Princeton University, Princeton, NJ, USA. 12Andlinger Center for Energy and the Environment, Princeton University, Princeton, NJ, USA. 13School of Science and Engineering, The Chinese University of Hong Kong Shenzhen, Shenzhen, P. R. China. 14Department of Chemical and Material Engineering, Gina Cody School of Engineering and Computer Science, Concordia University, Montreal, Quebec, Canada. |
摘要: |
Industrial-scale ethylene production occurs primarily by fossil-powered steam cracking of ethane—a high-temperature, high-energy process. An alternative, photochemical, pathway powered by sunlight and operating under ambient conditions could potentially mitigate some of the associated greenhouse gas emissions. Here we report the photocatalytic dehydrogenation of ethane to ethylene and hydrogen using LaMn1−xCuxO3. This perovskite oxide possesses redox-active Lewis acid sites, comprising Mn(III) and Mn(IV), and Lewis base sites, comprising O(-II) and OH(-I), collectively dubbed surface-frustrated Lewis pairs. We fnd that tuning the relative proportions of these sites optimizes the activity, selectivity and yield for ethane dehydrogenation. The highest ethylene production rate and ethane conversion achieved were around 1.1mmol g−1h−1and 4.9%, respectively. We show a simple outdoor prototype to demonstrate the viability of a solar ethylene process. In addition, techno-economic analysis revealed the economic potential of an industrial-scale solar ethylene production from ethane. |