Programmable heating and quenching for efficient thermochemical synthesis

Dong, Qi; Yao, Yonggang; Cheng, Sichao; Alexopoulos, Konstantinos; Gao, Jinlong; Srinivas, Sanjana; Wang, Yifan; Pei, Yong; Zheng, Chaolun; Brozena, Alexandra H.; Zhao, Hang; Wang, Xizheng; Toraman, Hilal Ezgi; Yang, Bao; Kevrekidis, Ioannis G.; Ju, Yiguang; Vlachos, Dionisios G.; Liu, Dongxia; Hu, Liangbing

doi:10.1038/s41586-022-04568-6

Cited by 109 publications

(68 citation statements)

References 40 publications

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“…The less severe sintering is also confirmed by the higher surface (Pt + Ni):Si ratio of the RPH1000 spent catalyst by X-ray photoelectron spectroscopy (XPS) in Table S2. This behavior is reminiscent of recent work on an Ru/C catalyst . Notably, peak temperatures higher than 1000 °C lead to significant particle sintering (XRD data in Figure S12b), leading to faster deactivation of the RPH1200 catalyst (Figure c).…”

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confidence: 65%

“…Electrification facilitates dynamic operation, which is promising to increase the reaction rate and selectivity, but the mechanisms remain poorly understood. , Early works on pulse heating catalysis have mainly focused on CO oxidation. Improved CO 2 yields were observed − that were postulated to be due to the transient surface coverages of CO on the catalyst during pulses. − More recently, Dong and colleagues discovered, using a programmable heating and quenching technique, that the selectivity of methane pyrolysis to C 2 products can be enhanced profoundly, likely due to limiting side reactions occurring over longer time scales . Ardagh et al predicted that the Sabatier maximum could be surpassed by the dynamic oscillation of the binding energy of a species on a catalytic surface between reaction-controlled and desorption-controlled regimes, bringing an order-of-magnitude higher turnover frequency (TOF), a phenomenon named “surface resonance” .…”

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confidence: 99%

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Dynamic Electrification of Dry Reforming of Methane with In Situ Catalyst Regeneration

Wang

Zheng

et al. 2023

ACS Energy Lett.

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We report the design and performance of a rapid pulse Joule heating (RPH) reactor with an in situ Raman spectrometer for highly endothermic, reversible reactions. We demonstrate it for methane dry reforming over a bimetallic PtNi/SiO2 catalyst that shows better performance than its monometallic counterparts. The catalyst temperature ramp rate can reach ∼14000 °C/s, mainly owing to the low thermal mass and resistivity of the heating element. Joule heating elements afford temperatures unachievable by conventional technology to enhance performance and more than double the energy efficiency. Dynamic electrification can increase syngas productivity and rate. Extensive characterizations suggest that pulse heating creates an in situ catalyst regeneration strategy that suppresses coke formation, sintering, and phase segregation, resulting in improved catalyst stability, under many conditions. Potentially driven by renewable electricity, the RPH can provide superb process advantages for high-temperature endothermic reactions and lead to negative carbon emissions.

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confidence: 65%

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confidence: 99%

Dynamic Electrification of Dry Reforming of Methane with In Situ Catalyst Regeneration

Wang

Zheng

et al. 2023

ACS Energy Lett.

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“…According to Arrhenius’ law, an exponential relationship exists between the reaction rate and temperature, and product distribution changes as chemical equilibrium is establishing or shifting. , Therefore, dynamic modulation of the temperature profile by tunable heating could be employed to control the reaction pathway for the selective and efficient formation of endo , exo -TCD. , However, it is difficult to realize temporal control over the reaction temperature on a traditional reactor using continuous heating . Recently, many dynamic heating techniques were developed and improved, , which can be adopted for selective production of endo , exo -TCD via effective control of the reaction pathway.…”

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confidence: 99%

Bayesian Optimized Oscillating Electric Heating of Dicyclopentadiene and Norbornene for Fuel Production

Zhao

Liu

Jing

et al. 2023

Ind. Eng. Chem. Res.

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Tetracyclo[6,2,1,01,7,13,6]dodecene (TCD) is conventionally synthesized by continuous heating of norbornene (NBE) and dicyclopentadiene (DCPD), in which the synthesis rate and isomer selectivity are hardly improved under such near equilibrium conditions. In this study, an alternative thermochemical synthesis technique using direct electric heating is present. Alternate heating and cooling of the reaction mixture can be rapidly realized by programmable electric current flowing in the reactor tube. The reaction has been switched in a timely fashion between high temperature and low temperature at a given speed. At a high temperature, the active intermediate of cyclopentadiene (CPD) quickly forms. Rapid cooling ensures the nonequilibrium kinetic control of CPD copolymerization for increasing the selectivity. The energy cost is reduced by lowering the average temperature. As optimized by the Bayesian method, the operating conditions of oscillating heating (e.g., amplitude, frequency, pressure, and so on) are determined to precisely match the time scales of fast generation and directed consumption of CPD. The oscillating heating method leads to a high yield of endo,exo-TCD (62.4% versus 11.6% by the conventional continuous-heating method). High-energy-density fuels with good low-temperature fluidity are prepared using hydrogenated TCD as the key component.

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“…However, catalyst deactivation as a result of high temperatures is often challenging. Now, writing in Nature, Dong et al 2 address the problems surrounding conventional high temperature synthesis. The findings pave the way for a process industry where temperatures are set by Joule heating resulting from an electric current imposed on reactor content and/or walls.…”

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confidence: 99%