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; Liangbing Hu

doi:10.1038/s41586-022-04568-6

Programmable heating and quenching for efficient thermochemical synthesis

Nature. 2022 May;605(7910):470-476. doi: 10.1038/s41586-022-04568-6. Epub 2022 May 18.

Authors

Qi Dong^#¹, Yonggang Yao^#¹, Sichao Cheng^#², Konstantinos Alexopoulos^#^{3

4}, Jinlong Gao¹, Sanjana Srinivas³, Yifan Wang³, Yong Pei⁵, Chaolun Zheng⁵, Alexandra H Brozena¹, Hao Zhao⁶, Xizheng Wang¹, Hilal Ezgi Toraman^{3

7}, Bao Yang⁵, Ioannis G Kevrekidis⁸, Yiguang Ju⁶, Dionisios G Vlachos⁹, Dongxia Liu¹⁰, Liangbing Hu^{11

12}

Affiliations

¹ Department of Materials Science and Engineering, University of Maryland, College Park, MD, USA.
² Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA.
³ Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, USA.
⁴ Department of Chemical Engineering, The Pennsylvania State University, University Park, PA, USA.
⁵ Department of Mechanical Engineering, University of Maryland, College Park, MD, USA.
⁶ Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ, USA.
⁷ Department of Energy and Mineral Engineering, The Pennsylvania State University, University Park, PA, USA.
⁸ Department of Chemical and Biomolecular Engineering, Department of Applied Mathematics and Statistics, Johns Hopkins University, Baltimore, MD, USA.
⁹ Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, USA. vlachos@udel.edu.
¹⁰ Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA. liud@umd.edu.
¹¹ Department of Materials Science and Engineering, University of Maryland, College Park, MD, USA. binghu@umd.edu.
¹² Center for Materials Innovation, University of Maryland, College Park, MD, USA. binghu@umd.edu.

^# Contributed equally.

PMID: 35585339
DOI: 10.1038/s41586-022-04568-6

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 pathways^1-3. 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 <35% by the conventional non-catalytic method and versus <60% by most conventional methods using optimized catalysts). Our technique can be extended to a range of thermochemical reactions, such as NH₃ synthesis, for which we achieve a stable and high synthesis rate of about 6,000 μmol g_Fe^-1 h^-1 at ambient pressure for >100 h using a non-optimized catalyst. This study establishes a new model towards highly efficient non-equilibrium thermochemical synthesis.

Publication types

Research Support, U.S. Gov't, Non-P.H.S.
Research Support, Non-U.S. Gov't