Kinetics of Pyrolysis and Thermal Evolution of Negev Desert Lithologies

Cockreham, Cody [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Washington State Univ., Pullman, WA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)] (ORCID:0000000287402197); Zhang, Xianghui [Washington State Univ., Pullman, WA (United States)]; Strzelecki, Andrew Charles [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Washington State Univ., Pullman, WA (United States)] (ORCID:0000000339289422); Benmore, Chris [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)]; Campe, Christopher Edward [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)]; Guo, Xiaofeng [Washington State Univ., Pullman, WA (United States)] (ORCID:000000033129493X); Rosenberg, Yoav O. [Geological Survey of Israel, Jerusalem (Israel)]; Reznik, Itay J. [Geological Survey of Israel, Jerusalem (Israel)] (ORCID:000000021932721X); Klein-BenDavid, Ofra [Nuclear Research Centre Negev, Beer Sheva (Israel); Ben Gurion Univ. of the Negev, Beer Sheva (Israel)]; Lucero, Dolan Diego [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)]; Stauffer, Philip H. [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:000000026976221X); Bussod, Gilles Yves A. [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000256101412); Xu, Hongwu [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Arizona State Univ., Tempe, AZ (United States)] (ORCID:0000000207936923); Wu, Di [Washington State Univ., Pullman, WA (United States)] (ORCID:000000016879321X); Boukhalfa, Hakim [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000163838503)

doi:10.1021/acsearthspacechem.4c00218

DOE OSTI · 2500877

Kinetics of Pyrolysis and Thermal Evolution of Negev Desert Lithologies

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Abstract

The Negev desert in Israel is home to large quantities of organic-rich, shallow marine sedimentary lithologies that could potentially accommodate the disposal of spent nuclear fuel. Previous thermal analyses of Negev carbonates have focused on industrially relevant considerations such as natural gas and oil extraction or pyrolysis for recovering hydrocarbon fuels. Here, this study addresses thermal evolution of the Negev organic-rich carbonate, siliceous, and phosphorite rocks and associated chemical, mineralogical, and microstructural changes that may occur under prolonged thermal loading in the vicinity of spent nuclear fuel disposal systems. Our employed methods include high-temperature X-ray diffraction, high-temperature infrared spectroscopy, and thermal analysis integrating thermogravimetry, differential scanning calorimetry, and mass spectrometry. Further, we apply iterative iso-conversional model-free methods to derive kinetic parameters for thermal decomposition of the Negev organic-rich carbonate rocks from 200 to 550 °C. Our results have provided mechanistic insights into the thermal evolution encompassing water desorption, decomposition of organic matter, and decarbonation of carbonate phases.

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58 GEOSCIENCES Negev Desert carbonate infrared spectroscopy kinetics organic matter pyrolysis thermal analysis x-ray diffraction

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Cockreham, Cody [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Washington State Univ., Pullman, WA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)] (ORCID:0000000287402197), Zhang, Xianghui [Washington State Univ., Pullman, WA (United States)], Strzelecki, Andrew Charles [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Washington State Univ., Pullman, WA (United States)] (ORCID:0000000339289422), Benmore, Chris [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)], Campe, Christopher Edward [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)], Guo, Xiaofeng [Washington State Univ., Pullman, WA (United States)] (ORCID:000000033129493X), Rosenberg, Yoav O. [Geological Survey of Israel, Jerusalem (Israel)], Reznik, Itay J. [Geological Survey of Israel, Jerusalem (Israel)] (ORCID:000000021932721X), Klein-BenDavid, Ofra [Nuclear Research Centre Negev, Beer Sheva (Israel); Ben Gurion Univ. of the Negev, Beer Sheva (Israel)], Lucero, Dolan Diego [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)], Stauffer, Philip H. [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:000000026976221X), Bussod, Gilles Yves A. [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000256101412), Xu, Hongwu [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Arizona State Univ., Tempe, AZ (United States)] (ORCID:0000000207936923), Wu, Di [Washington State Univ., Pullman, WA (United States)] (ORCID:000000016879321X), Boukhalfa, Hakim [Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000163838503). 2025-01-07. Kinetics of Pyrolysis and Thermal Evolution of Negev Desert Lithologies. https://doi.org/10.1021/acsearthspacechem.4c00218

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