“…These impacts in the HF-free process were found to be mostly due to the use of oxalic acid in the SX stage. Oxalic acid has been utilized in studies from different industries focused on applications that aim at improved sustainability. – However, currently, organic chemicals including oxalic acid are mainly produced from nonrenewable fossil resources . This highlights the importance of the chemical selection in the process and numerical observation of the environmental impacts of the use of those chemicals, which might under other circumstances be considered green but should be determined case by case.…”
Secondary hard metal contains valuable tantalum and niobium,
which
could be recovered after chemical recycling of the scrap; however,
the environmental impacts of their recycling have not been earlier
quantified. This study provides gate-to-gate life cycle inventory
data on tantalum and niobium recovery from the Ta–Nb-rich residue
after the leaching of cobalt in the chemical recycling of hard metal
and first assessment of the environmental impacts of tantalum and
niobium coproduction. The environmental impacts were quantified using
life cycle assessment (LCA) based on data acquired by process simulation.
Two processes were evaluated: one based on conventional HF leaching
used in the primary production of tantalum and niobium and one prospective
HF-free process using NaOH. The results show that environmental impacts
of Ta–Nb recycling can outperform primary production environmentally
if the Ta and Nb content in the raw material is high enough. At the
process level, a benefit is gained even with a lower content, but
at the product level, higher contents are required for tantalum recovery
to be worthwhile. In HF-based recycling, increasing the Ta and Nb
contents each from 2.5 to 5 wt % decreases the value of global warming
potential (GWP) of Ta recycling from 1.24 times the GWP of primary
tantalum production to 0.72 times the GWP of primary tantalum production.
The environmental impacts of the recycling processes mostly originate
from the background processes. The most burdening process hot spots
of recycling included the leaching and effluent treatment stages for
the HF-based process in which HF and lime were the largest contributors.
For the HF-free process, the largest contributions were due to NaOH
used in the caustic conversion as well as oxalic acid in the solvent
extraction.
“…These impacts in the HF-free process were found to be mostly due to the use of oxalic acid in the SX stage. Oxalic acid has been utilized in studies from different industries focused on applications that aim at improved sustainability. – However, currently, organic chemicals including oxalic acid are mainly produced from nonrenewable fossil resources . This highlights the importance of the chemical selection in the process and numerical observation of the environmental impacts of the use of those chemicals, which might under other circumstances be considered green but should be determined case by case.…”
Secondary hard metal contains valuable tantalum and niobium,
which
could be recovered after chemical recycling of the scrap; however,
the environmental impacts of their recycling have not been earlier
quantified. This study provides gate-to-gate life cycle inventory
data on tantalum and niobium recovery from the Ta–Nb-rich residue
after the leaching of cobalt in the chemical recycling of hard metal
and first assessment of the environmental impacts of tantalum and
niobium coproduction. The environmental impacts were quantified using
life cycle assessment (LCA) based on data acquired by process simulation.
Two processes were evaluated: one based on conventional HF leaching
used in the primary production of tantalum and niobium and one prospective
HF-free process using NaOH. The results show that environmental impacts
of Ta–Nb recycling can outperform primary production environmentally
if the Ta and Nb content in the raw material is high enough. At the
process level, a benefit is gained even with a lower content, but
at the product level, higher contents are required for tantalum recovery
to be worthwhile. In HF-based recycling, increasing the Ta and Nb
contents each from 2.5 to 5 wt % decreases the value of global warming
potential (GWP) of Ta recycling from 1.24 times the GWP of primary
tantalum production to 0.72 times the GWP of primary tantalum production.
The environmental impacts of the recycling processes mostly originate
from the background processes. The most burdening process hot spots
of recycling included the leaching and effluent treatment stages for
the HF-based process in which HF and lime were the largest contributors.
For the HF-free process, the largest contributions were due to NaOH
used in the caustic conversion as well as oxalic acid in the solvent
extraction.
“…The interface temperature and ion source temperature of the GC/MS were set to 280 °C and 230 °C, respectively, and the mass spectrum range was 35–500 m/z. The chromatographic peak was determined by comparison with spectra in the NIST11 spectral library, the F-Search PY-1110E-181 spectral library, and previous data [ 19 , 26 , 27 , 28 ]. The chromatographic peak area of each compound in the Py-GC/MS pyrolysis products was proportional to its concentration.…”
Section: Experimental Materials and Methodsmentioning
Fast pyrolysis of microcrystalline cellulose (MC) was carried out by pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS). The effects of temperature, time, and a catalyst on the distribution of the pyrolysis products were analyzed. The reaction temperature and time can significantly affect the types and yields of compounds produced by cellulose pyrolysis. A pyrolysis temperature of 500–600 °C and pyrolysis time of 20 s optimized the yield of volatile liquid in the pyrolysis products of cellulose. In all catalytic experiments, the relative contents of alcohols (1.97%), acids (2.32%), and esters (4.52%) were highest when K2SO4 was used as a catalyst. HZSM-5 promoted the production of carbohydrates (92.35%) and hydrocarbons (2.20%), while it inhibited the production of aldehydes (0.30%) and ketones (1.80%). MCM-41 had an obvious catalytic effect on cellulose, increasing the contents of aldehydes (41.58%), ketones (24.51%), phenols (1.82%), furans (8.90%), and N-compounds (12.40%) and decreasing those of carbohydrates (5.38%) and alcohols (0%).
“…The device contained a horizontal tubular heating furnace, a quartz tube reactor, and a condenser, as illustrated in our previous study. 11 Briefly, 1.0 g of cellulose was mechanically mixed with OA in different CL-to-OA ratios (1:1, 1:3, and 1:5). The sample was inserted into the pyrolysis center after the furnace was heated to the desired temperature (120−280 °C).…”
Section: Staged Pyrolysis Experimentsmentioning
confidence: 99%
“…Recently, we succeeded in producing DGP selectively by the copyrolysis of solid oxalic acid (OA) and cellulose. 11 OA completely decomposed during the copyrolysis process, not only avoiding the complex pretreatment processes but also circumventing challenges associated with catalyst recovery and regeneration. Notably, during the copyrolysis process of OA and cellulose for DGP production, a significant amount of FF and formic acid (FA) was also generated as byproducts.…”
Pyrolysis is a promising thermochemical conversion technology, which can convert biomass and cellulose into value-added products. Herein, a new approach of oxalic acid-assisted staged fast pyrolysis (OASFP) of cellulose was developed, achieving the coproduction of 1,4:3,6-dianhydro-α-D-glucopyranose (DGP), furfural (FF), and formic acid (FA) in separated pyrolysis stages. The lab-scale tests demonstrated that a selectivity of 71.6% and a yield of 31.5 wt % for FA in the aqueous phase, as well as a selectivity of 55.6% and a yield of 1.2 wt % for FF in the organic phase, were achieved in the primary pyrolysis stage under the optimized conditions (primary pyrolysis temperature of 220 °C and cellulose-to-oxalic acid (OA) ratio of 1:3). During the subsequent secondary pyrolysis process at 400 °C, the decomposition of the solid residue achieved a yield of 7.2 wt % and a selectivity of 32.7% for DGP. The interaction between OA and cellulose during the primary pyrolysis stage was essential for DGP generation. The formation mechanism of major products and the role of OA were revealed based on experiments and density functional theory calculations. In total, the OASFP of cellulose offers new possibilities and opportunities for biomass utilization.
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