Sequential Ammonia and Carbon Dioxide Adsorption on Pyrolyzed Biomass to Recover Waste Stream Nutrients

Krounbi, Leilah; Enders, Akio; Anderton, Christopher R.; Engelhard, Mark H.; Hestrin, Rachel; Torres-Rojas, Dorisel; Dynes, James J.; Lehmann, Johannes

doi:10.1021/acssuschemeng.0c01427

Sequential Ammonia and Carbon Dioxide Adsorption on Pyrolyzed Biomass to Recover Waste Stream Nutrients

Journal Article · Wed Apr 15 00:00:00 EDT 2020 · ACS Sustainable Chemistry & Engineering

DOI:https://doi.org/10.1021/acssuschemeng.0c01427· OSTI ID:1755114

Krounbi, Leilah ^[1]; Enders, Akio ^[1]; ^[2]; ^[2]; Hestrin, Rachel ^[1]; Torres-Rojas, Dorisel ^[1]; ^[3]; ^[1]

Cornell Univ., Ithaca, NY (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Canadian Light Sources, Inc., Saskatoon, SK (Canada)

Untreated fecal waste in unsewered communities and reactive nitrogen (N) loading from wastewater and urine disposal are important environmental challenges. Through pyrolysis, untreated fecal waste can be converted into amine-rich carbon dioxide (CO₂) sorbents, the chemisorption of which tunes the surface chemistry toward ammonia (NH₃) uptake. We compared the N-loading potential within amine-rich pyrolyzed human solid waste through exposure to CO₂ followed by NH₃ with the N-loading potential on carboxyl-rich, pyrolyzed oxidized wood using sequential adsorption of isotopically labeled CO₂ and NH₃. The total N content of pyrolyzed oxidized wood exposed once to NH3 was similar to native, pyrolyzed human solid waste (3.7% compared to 4.6%). However, sorption kinetics and spectroscopic evidence revealed distinct N forms between the two materials affecting subsequent CO₂ and NH₃ uptake. Tertiary amines comprised 70% of N in pyrolyzed waste, compared to only 53% in pyrolyzed oxidized wood. The high heat of adsorption of CO₂ on pyrolyzed human solid waste (50 kJ mol-1) at low concentrations (0.05 mmol CO₂ g^-1) was indicative of CO₂ reactivity with tertiary amines, consistent with the formation of carbamic acid (Figure S1). Conversely, after exposure to NH₃, pyrolyzed oxidized wood chemisorbed CO₂ at much higher concentrations (0.7 mmol CO₂ g-1), pointing to primary amines as the active functional moieties. Adsorption kinetics of pyrolyzed oxidized wood revealed continued, albeit diminishing NH₃ uptake with each consecutive CO₂ treatment, averaging 5.9 mmol NH₃ g^-1 for the first NH₃ exposure event, and still 3.5 and 2.9 mmol NH₃ g^-1 for the second and third. Penetration of ¹⁵NH₃ and ¹³CO₂ measured by NanoSIMS reached over 7 µm deep into both materials, explaining the large NH₃ capture. The significantly lower NH₃ adsorption compared to pyrolyzed oxidized wood may be a result of potassium (K) carbonate precipitation precluding a Lewis base interaction between NH₃ and chemisorbed CO₂, suggested by a 2-fold increase in surface K concentrations after exposure of pyrolyzed human solid waste to CO₂+NH₃ detected by XPS.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1755114

Report Number(s):: PNNL-SA-138582

Journal Information:: ACS Sustainable Chemistry & Engineering, Journal Name: ACS Sustainable Chemistry & Engineering Journal Issue: 18 Vol. 8; ISSN 2168-0485

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Sequential Ammonia and Carbon Dioxide Adsorption on Pyrolyzed Biomass to Recover Waste Stream Nutrients

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