Programmable heating and quenching for efficient thermochemical synthesis

Qi Dong, Yonggang Yao, Sichao Cheng, Konstantinos Alexopoulos, Jinlong Gao, Sanjana Srinivas, Yifan Wang, Yong Pei, Chaolun Zheng, Alexandra H. Brozena, Hao Zhao, Xizheng Wang, Hilal Ezgi Toraman, Bao Yang, Ioannis G. Kevrekidis, Yiguang Ju, Dionisios G. Vlachos (), Dongxia Liu () and Liangbing Hu ()
Additional contact information
Qi Dong: University of Maryland
Yonggang Yao: University of Maryland
Sichao Cheng: University of Maryland
Konstantinos Alexopoulos: University of Delaware
Jinlong Gao: University of Maryland
Sanjana Srinivas: University of Delaware
Yifan Wang: University of Delaware
Yong Pei: University of Maryland
Chaolun Zheng: University of Maryland
Alexandra H. Brozena: University of Maryland
Hao Zhao: Princeton University
Xizheng Wang: University of Maryland
Hilal Ezgi Toraman: University of Delaware
Bao Yang: University of Maryland
Ioannis G. Kevrekidis: Johns Hopkins University
Yiguang Ju: Princeton University
Dionisios G. Vlachos: University of Delaware
Dongxia Liu: University of Maryland
Liangbing Hu: University of Maryland

Nature, 2022, vol. 605, issue 7910, 470-476

Abstract: Abstract Conventional thermochemical syntheses by continuous heating under near-equilibrium conditions face critical challenges in improving the synthesis rate, selectivity, catalyst stability and energy efficiency, owing to the lack of temporal control over the reaction temperature and time, and thus the reaction pathways1–3. As an alternative, we present a non-equilibrium, continuous synthesis technique that uses pulsed heating and quenching (for example, 0.02 s on, 1.08 s off) using a programmable electric current to rapidly switch the reaction between high (for example, up to 2,400 K) and low temperatures. The rapid quenching ensures high selectivity and good catalyst stability, as well as lowers the average temperature to reduce the energy cost. Using CH4 pyrolysis as a model reaction, our programmable heating and quenching technique leads to high selectivity to value-added C2 products (>75% versus 100 h using a non-optimized catalyst. This study establishes a new model towards highly efficient non-equilibrium thermochemical synthesis.

Date: 2022
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DOI: 10.1038/s41586-022-04568-6

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