Carbon-Assisted, Continuous Syngas Production in a Chemical Looping Scheme

Tian, Yuan; Benedict, Zoe; Li, Fanxing; Yang, Yingchao; Maiti, Debtanu; Wang, Yixiao; Fushimi, Rebecca

doi:10.1007/s11244-023-01840-5

Title: Carbon-Assisted, Continuous Syngas Production in a Chemical Looping Scheme

Journal Article · Wed Aug 16 00:00:00 EDT 2023 · Topics in Catalysis

DOI:https://doi.org/10.1007/s11244-023-01840-5· OSTI ID:2242412

Tian, Yuan ^[1]; Benedict, Zoe ^[2]; Li, Fanxing ^[3]; Yang, Yingchao ^[4]; Maiti, Debtanu ^[5]; Wang, Yixiao ^[5];

^[5]

Idaho National Laboratory (INL), Idaho Falls, ID (United States); North Carolina State University, Raleigh, NC (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States); University of Maine, Orono, ME (United States)
North Carolina State University, Raleigh, NC (United States)
University of Maine, Orono, ME (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States)

In the current energy and environment scenario, it is imperative to develop energy efficient routes for chemical manufacturing that also pave the way for mitigation of greenhouse gas emissions. This work presents an efficient pathway for continuous syngas production via a chemical looping conversion of the two most potent greenhouse gases—CH₄, and CO₂. The well-known dry-reforming process of converting CH₄, and CO₂ to syngas is energy-intensive and suffers from catalyst deactivation. The chemical looping approach, on the other hand, provides avenues for mitigating catalyst deactivation and enabling improved energy efficiency. The key to such process enhancements lies in the intricate structure–function relationships of the catalyst and its correlation to the process variables. We present the reduction and oxidation characteristics of 5 wt.% Ni/Ce_1-xZr_xO₂-based catalysts (x = 0, 0.4, and 0.625). We demonstrate low temperature CH4 activation over Ni-promoted samples as opposed to pure Ce_1-xZr_xO₂. Moreover, our results depict an optimum regeneration of these catalysts when oxidized by CO₂, and H₂O, which allows for chemical looping operation of steam reforming of methane as well. Process variables were tuned to optimize the CH₄ conversion (over 80%), and H₂/CO ratio at 650 °C. The critical surface reactions—carbon accumulation and gasification, and thermocatalytic CO₂ splitting were investigated to elucidate the dynamic nature of the catalyst surface. In conclusion, the impact of this work lies in showcasing the opportunities to design chemical looping reactors for energy efficient syngas production from waste greenhouse gases.

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Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC07-05ID14517; 21P1062-025FP

OSTI ID:: 2242412

Report Number(s):: INL/JOU-23-72417-Rev001

Journal Information:: Topics in Catalysis, Vol. 66, Issue 19-20; ISSN 1022-5528

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Carbon-Assisted, Continuous Syngas Production in a Chemical Looping Scheme

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