Ethylene production via photocatalytic dehydrogenation of ethane using LaMn1−xCuxO3

Rui Song; Guanshu Zhao; Juan Manuel Restrepo-Flórez; Camilo J. Viasus Pérez; Zhijie Chen; Chaoqian Ai; Andrew Wang; Dengwei Jing; Athanasios A. Tountas; Jiuli Guo; Chengliang Mao; Chaoran Li; Jiahui Shen; Guangming Cai; Chenyue Qiu; Jessica Ye; Yubin Fu; Chistos T. Maravelias; Lu Wang; Junchuan Sun; Yang Fan Xu; Zhao Li; Joel Yi Yang Loh; Nhat Truong Nguyen; Le He; Xiaohong Zhang; Geoffrey A. Ozin

doi:10.1038/s41560-024-01541-7

Ethylene production via photocatalytic dehydrogenation of ethane using LaMn₁₋_xCu_xO₃

Rui Song, Guanshu Zhao, Juan Manuel Restrepo-Flórez, Camilo J. Viasus Pérez, Zhijie Chen, Chaoqian Ai, Andrew Wang, Dengwei Jing, Athanasios A. Tountas, Jiuli Guo, Chengliang Mao, Chaoran Li, Jiahui Shen, Guangming Cai, Chenyue Qiu, Jessica Ye, Yubin Fu, Chistos T. Maravelias, Lu Wang, Junchuan SunYang Fan Xu, Zhao Li, Joel Yi Yang Loh, Nhat Truong Nguyen, Le He^*, Xiaohong Zhang^*, Geoffrey A. Ozin^*

^*Corresponding author for this work

EEE - Academic & Research

Research output: Contribution to journal › Article › peer-review

Abstract

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₋_xCu_xO₃. 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 find 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 1.1 mmol g⁻¹ h⁻¹ and 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.

Original language	English
Pages (from-to)	750-760
Number of pages	11
Journal	Nature Energy
Volume	9
Issue number	6
DOIs	https://doi.org/10.1038/s41560-024-01541-7
Publication status	Published - Jun 2024

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Song, R., Zhao, G., Restrepo-Flórez, J. M., Viasus Pérez, C. J., Chen, Z., Ai, C., Wang, A., Jing, D., Tountas, A. A., Guo, J., Mao, C., Li, C., Shen, J., Cai, G., Qiu, C., Ye, J., Fu, Y., Maravelias, C. T., Wang, L., ... Ozin, G. A. (2024). Ethylene production via photocatalytic dehydrogenation of ethane using LaMn₁₋_xCu_xO₃. Nature Energy, 9(6), 750-760. https://doi.org/10.1038/s41560-024-01541-7

@article{77caaba1df8a4f2395a71a9360e510c7,

title = "Ethylene production via photocatalytic dehydrogenation of ethane using LaMn1−xCuxO3",

abstract = "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 find 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 1.1 mmol g−1 h−1 and 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.",

author = "Rui Song and Guanshu Zhao and Restrepo-Fl{\'o}rez, {Juan Manuel} and {Viasus P{\'e}rez}, {Camilo J.} and Zhijie Chen and Chaoqian Ai and Andrew Wang and Dengwei Jing and Tountas, {Athanasios A.} and Jiuli Guo and Chengliang Mao and Chaoran Li and Jiahui Shen and Guangming Cai and Chenyue Qiu and Jessica Ye and Yubin Fu and Maravelias, {Chistos T.} and Lu Wang and Junchuan Sun and Xu, {Yang Fan} and Zhao Li and Loh, {Joel Yi Yang} and Nguyen, {Nhat Truong} and Le He and Xiaohong Zhang and Ozin, {Geoffrey A.}",

note = "Publisher Copyright: {\textcopyright} The Author(s), under exclusive licence to Springer Nature Limited 2024.",

year = "2024",

month = jun,

doi = "10.1038/s41560-024-01541-7",

language = "English",

volume = "9",

pages = "750--760",

journal = "Nature Energy",

issn = "2058-7546",

publisher = "Springer Nature",

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Song, R, Zhao, G, Restrepo-Flórez, JM, Viasus Pérez, CJ, Chen, Z, Ai, C, Wang, A, Jing, D, Tountas, AA, Guo, J, Mao, C, Li, C, Shen, J, Cai, G, Qiu, C, Ye, J, Fu, Y, Maravelias, CT, Wang, L, Sun, J, Xu, YF, Li, Z, Loh, JYY, Nguyen, NT, He, L, Zhang, X & Ozin, GA 2024, 'Ethylene production via photocatalytic dehydrogenation of ethane using LaMn₁₋_xCu_xO₃', Nature Energy, vol. 9, no. 6, pp. 750-760. https://doi.org/10.1038/s41560-024-01541-7

TY - JOUR

T1 - Ethylene production via photocatalytic dehydrogenation of ethane using LaMn1−xCuxO3

AU - Song, Rui

AU - Zhao, Guanshu

AU - Restrepo-Flórez, Juan Manuel

AU - Viasus Pérez, Camilo J.

AU - Chen, Zhijie

AU - Ai, Chaoqian

AU - Wang, Andrew

AU - Jing, Dengwei

AU - Tountas, Athanasios A.

AU - Guo, Jiuli

AU - Mao, Chengliang

AU - Li, Chaoran

AU - Shen, Jiahui

AU - Cai, Guangming

AU - Qiu, Chenyue

AU - Ye, Jessica

AU - Fu, Yubin

AU - Maravelias, Chistos T.

AU - Wang, Lu

AU - Sun, Junchuan

AU - Xu, Yang Fan

AU - Li, Zhao

AU - Loh, Joel Yi Yang

AU - Nguyen, Nhat Truong

AU - He, Le

AU - Zhang, Xiaohong

AU - Ozin, Geoffrey A.

PY - 2024/6

Y1 - 2024/6

N2 - 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 find 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 1.1 mmol g−1 h−1 and 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.

AB - 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 find 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 1.1 mmol g−1 h−1 and 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.

UR - http://www.scopus.com/inward/record.url?scp=85195296363&partnerID=8YFLogxK

U2 - 10.1038/s41560-024-01541-7

DO - 10.1038/s41560-024-01541-7

M3 - Article

AN - SCOPUS:85195296363

SN - 2058-7546

VL - 9

SP - 750

EP - 760

JO - Nature Energy

JF - Nature Energy

IS - 6

ER -

Ethylene production via photocatalytic dehydrogenation of ethane using LaMn₁₋_xCu_xO₃

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