Emily C. Hayward, Glen J. Smales, Brian R. Pauw, Masaki Takeguchi, Alexander Kulak, Robert D. Hunter and Zoe Schnepp
{"title":"The effect of catalyst precursors on the mechanism of iron-catalysed graphitization of cellulose†","authors":"Emily C. Hayward, Glen J. Smales, Brian R. Pauw, Masaki Takeguchi, Alexander Kulak, Robert D. Hunter and Zoe Schnepp","doi":"10.1039/D4SU00365A","DOIUrl":"https://doi.org/10.1039/D4SU00365A","url":null,"abstract":"<p >Iron-catalysed graphitization of biomass is a simple and sustainable route to carbons with high graphitic content. It uses abundant precursors and moderate processing temperatures and generates carbons with high porosity. Recently, it has been demonstrated that the choice of biomass precursor can have a significant impact on the textural and compositional properties of the resulting carbon. In this paper, we demonstrate that the choice of catalyst is also critical to the carbon structure. Aqueous iron(<small>III</small>) nitrate and iron(<small>III</small>) chloride convert cellulose to carbons with very different textural properties. This is due to the choice of iron catalyst changing the mechanism of cellulose decomposition and also the nature of the active graphitization catalyst.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3490-3499"},"PeriodicalIF":0.0,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00365a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Issaraporn Rakngam, Gustavo A. S. Alves, Nattawut Osakoo, Jatuporn Wittayakun, Thomas Konegger and Karin Föttinger
{"title":"Hydrothermal synthesis of ZnZrOx catalysts for CO2 hydrogenation to methanol: the effect of pH on structure and activity†","authors":"Issaraporn Rakngam, Gustavo A. S. Alves, Nattawut Osakoo, Jatuporn Wittayakun, Thomas Konegger and Karin Föttinger","doi":"10.1039/D4SU00522H","DOIUrl":"10.1039/D4SU00522H","url":null,"abstract":"<p >With the growing necessity of achieving carbon neutrality in the industrial sector, the catalytic hydrogenation of carbon dioxide into methanol has been widely considered one of the key strategies for the utilization of captured CO<small><sub>2</sub></small>. For this reason, the development of alternative catalysts such as ZnZrO<small><sub><em>x</em></sub></small> has attracted considerable interest, given its superior stability and versatility in comparison to the conventional Cu-based materials. In this work, ZnZrO<small><sub><em>x</em></sub></small> has been produced by a hydrothermal synthesis method at varied synthesis pH between 7 and 10 and a positive association between pH and catalytic CO<small><sub>2</sub></small> conversion is observed. At 2.0 MPa and 250 °C, ZnZrO<small><sub><em>x</em></sub></small> produced at pH 10 shows a methanol selectivity of 95% at a CO<small><sub>2</sub></small> conversion of 3.4%. According to characterization, basic pH conditions enable the formation of abundant t-ZrO<small><sub>2</sub></small> and the subsequent incorporation of Zn<small><sup>2+</sup></small> into this phase, although the content of surface Zn does not increase between pH 8 and 10. Nevertheless, synthesis pH values can be correlated with surface oxygen content and CO<small><sub>2</sub></small> adsorption capacity, which could be important contributors to the higher catalytic activity observed as a result of higher synthesis pH values. However, upon synthesis at pH 10, an inferior selectivity to methanol is observed above 250 °C, as a possible result of the excessive formation of ZnO. Interestingly, this secondary phase can be prevented and the selectivity can be slightly improved by utilizing NH<small><sub>4</sub></small>OH instead of NaOH in the hydrothermal method.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 12","pages":" 3798-3805"},"PeriodicalIF":0.0,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11484158/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142482701","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Gavan W. Lienhart, Thomas Palisin, William Gross, Amelia Moll and James M. Eagan
{"title":"Supramolecular purification of aromatic polyester monomers from chemical depolymerization†","authors":"Gavan W. Lienhart, Thomas Palisin, William Gross, Amelia Moll and James M. Eagan","doi":"10.1039/D4SU00330F","DOIUrl":"https://doi.org/10.1039/D4SU00330F","url":null,"abstract":"<p >The separation of poly(ethylene terephthalate) (PET) comonomers produced from the chemical recycling and depolymerization of PET is a critical step in realizing polyester material circularity. Various grades of PET (<em>e.g.</em>, fiber, bottle, tire-cord) each require precise degrees of crystallinity which is controlled by the introduction of isomeric phthalates, comonomers which then contaminate secondary monomer streams. The use of supramolecular interactions as a method of extracting and separating these comonomers is herein described. The binding constants (<em>K</em><small><sub>b</sub></small>) between various-sized cyclodextrins with dimethyl terephthalate/dimethyl isophthalate and bis-2-hydroxyethyl terephthalate/bis-2-hydroxyethyl isophthalate are measured by fluorescence quenching and titration measurements. It is shown that beta-cyclodextrins most favorably bind the monomers (<em>K</em><small><sub>b</sub></small> up to 830 M<small><sup>−1</sup></small>) and that methyl ester comonomers bind more strongly than the glycolysis products. Competitive binding measurements between isomeric aromatic esters indicate alpha cyclodextrin binds dimethyl terephthalate (<em>K</em><small><sub>b</sub></small> = 328 M<small><sup>−1</sup></small>) 6-times more strongly than the dimethyl isophthalate isomer (<em>K</em><small><sub>b</sub></small> = 55 M<small><sup>−1</sup></small>). Crosslinking of the cyclodextrins with diisocyanate or perfluorinated bis-cyanobenzene moieties resulted in particles that could effectively remove the monomers from depolymerization solutions (up to 0.6 mmol of monomer per gram of particle). The results suggest supramolecular extraction and separation may be a scalable means of improving the purity and atom recovery of secondary recycled polyester feedstocks.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 12","pages":" 3879-3887"},"PeriodicalIF":0.0,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00330f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142736727","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Britt Segers, Philippe Nimmegeers, Marc Spiller, Giorgio Tofani, Edita Jasiukaitytė-Grojzdek, Elina Dace, Timo Kikas, Jorge M. Marchetti, Milena Rajić, Güray Yildiz and Pieter Billen
{"title":"Lignocellulosic biomass valorisation: a review of feedstocks, processes and potential value chains and their implications for the decision-making process†","authors":"Britt Segers, Philippe Nimmegeers, Marc Spiller, Giorgio Tofani, Edita Jasiukaitytė-Grojzdek, Elina Dace, Timo Kikas, Jorge M. Marchetti, Milena Rajić, Güray Yildiz and Pieter Billen","doi":"10.1039/D4SU00342J","DOIUrl":"https://doi.org/10.1039/D4SU00342J","url":null,"abstract":"<p >Several studies have reported the importance of transforming the current fossil-based economy into a bio-economy. Lignocellulosic biomass, as the most abundant renewable feedstock, has high potential. However, in practice, its use is limited to energy generation. This study aims to provide an overview of the potential lignocellulosic valorisation pathways and identify the next steps that should be taken to move towards a bio-economy. The study reviews the lignocellulosic biomass feedstocks and their compositional differences, depending on the type, valorisation processes, and value chains that can be created by selecting the respective valorisation processes. The study shows the abundance of pathways that can be created when attempting to link lignocellulosic biomass with a high diversity of compositions to the many potential end-products that can be created. Due to this abundance, selecting the optimal biomass-end-product combinations for the development of a sustainable bio-economy is challenging. Current state-of-the-art process-based assessment methods (TEA/LCA) have limited genericity, as they are only valid for specific processes at a specific time and place. As a result, using these types of assessments to try to find optimal biomass-end-product combinations would require too much time, data, and expertise. This creates the need to shift away from process-based assessments to state-based assessments, where the path of least thermodynamic resistance is sought.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 12","pages":" 3730-3749"},"PeriodicalIF":0.0,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00342j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142736771","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anuradha Sureshrao Mohitkar, Nilanjan Dey and Subbalakshmi Jayanty
{"title":"Self-assembled tetracyanoquinodimethane derivatives: differential fluorescent responses on sensing copper and mercury ions in an aqueous medium†","authors":"Anuradha Sureshrao Mohitkar, Nilanjan Dey and Subbalakshmi Jayanty","doi":"10.1039/D4SU00445K","DOIUrl":"https://doi.org/10.1039/D4SU00445K","url":null,"abstract":"<p >Copper and mercury metal ions are known to cause serious harm to biological and environmental systems, and therefore the development of new efficient sensory systems for the detection of copper and mercury ions in aqueous media is always encouraged and in need. Herein, we present the employment of di-substituted tetracyanoquinodimethane (TCNQ) derivatives for metal ion recognition. Owing to their fluorescent properties, single-step synthesis and easy purification, small molecules, namely 7,7-bis(1-(2-aminoethyl)pyrrolidino)-8,8-dicyanoquinodimethane (AEPRDQ) <strong>[1]</strong>, 7,7-bis(1-(2-aminoethyl)piperidino)-8,8-dicyanoquinodimethane (AEPIDQ) <strong>[2]</strong> and 7,7-bis(<em>N</em>,<em>N</em>-diethylethylenediamino)-8,8-dicyanoquinodimethane (BDEDDQ) <strong>[3]</strong>, have been utilized for Cu<small><sup>2+</sup></small> and Hg<small><sup>2+</sup></small> sensing applications. <strong>[1]–[3]</strong> considered in this study showed the formation of self-assembled nanoaggregates in aqueous media. A thorough investigation on the effect of the microenvironment, such as temperature, pH, polarity, <em>etc.</em>, on the extent of self-agglomeration was done spectroscopically. Interestingly, in an acetonitrile–water (1 : 9) solvent mixture, the compounds showed diverse responses to Cu<small><sup>2+</sup></small> and Hg<small><sup>2+</sup></small> ions. <strong>[1]</strong> manifested fluorescence quenching with Cu<small><sup>2+</sup></small> ions, while enhanced emission was noted with Hg<small><sup>2+</sup></small>. Hg<small><sup>2+</sup></small> induced fluorescence quenching with <strong>[2]</strong> while no prominent quenching is seen on the addition of Cu<small><sup>2+</sup></small>. Adding Cu<small><sup>2+</sup></small> and Hg<small><sup>2+</sup></small> resulted in a turn-off fluorescence signal in <strong>[3]</strong>. Hence, alteration by simply varying the terminal functional groups among the said <strong>[1]–[3]</strong> resulted in varied metal ion sensing responses.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 12","pages":" 3946-3958"},"PeriodicalIF":0.0,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00445k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142736732","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Florian Schrenk, Lorenz Lindenthal, Hedda Drexler, Tobias Berger, Raffael Rameshan, Thomas Ruh, Karin Föttinger and Christoph Rameshan
{"title":"How reduction temperature influences the structure of perovskite-oxide catalysts during the dry reforming of methane†","authors":"Florian Schrenk, Lorenz Lindenthal, Hedda Drexler, Tobias Berger, Raffael Rameshan, Thomas Ruh, Karin Föttinger and Christoph Rameshan","doi":"10.1039/D4SU00483C","DOIUrl":"10.1039/D4SU00483C","url":null,"abstract":"<p >Dry reforming of methane is a promising reaction to convert CO<small><sub>2</sub></small> and combat climate change. However, the reaction is still not feasible in large-scale industrial applications. The thermodynamic need for high temperatures and the potential of carbon deposition leads to high requirements for potential catalyst materials. As shown in previous publications, the Ni-doped perovskite-oxide Nd<small><sub>0.6</sub></small>Ca<small><sub>0.4</sub></small>Fe<small><sub>0.97</sub></small>Ni<small><sub>0.03</sub></small>O<small><sub>3</sub></small> is a potential candidate as it can exsolve highly active Ni nanoparticles on its surface. This study focused on controlling the particle size by varying the reduction temperature. We found the optimal temperature that allows the Ni nanoparticles to exsolve while not yet enabling the formation of deactivating CaCO<small><sub>3</sub></small>. Furthermore, the exsolution process and the behaviour of the phases during the dry reforming of methane were investigated using <em>in situ</em> XRD measurements at the DESY beamline P02.1 at PETRA III in Hamburg. They revealed that the formed deactivated phases would, at high temperatures, form a brownmillerite phase, thus hinting at a potential self-healing mechanism of these materials.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3334-3344"},"PeriodicalIF":0.0,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11465801/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142482700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kaiying Wang, Baitang Jin, Xiaoqing He and Xinhua Liang
{"title":"Atomic layer deposition of Ru nanoclusters on Ba–LaCeOx: a highly efficient catalyst for ammonia synthesis under mild conditions†","authors":"Kaiying Wang, Baitang Jin, Xiaoqing He and Xinhua Liang","doi":"10.1039/D4SU00350K","DOIUrl":"https://doi.org/10.1039/D4SU00350K","url":null,"abstract":"<p >Ammonia synthesis has significant implications for global energy and environmental issues, driving the need for highly active catalysts that operate under mild conditions. This study reports the successful deposition of uniform ∼1.0 nm metallic ruthenium (Ru) nanoclusters onto Ba–LaCeO<small><sub><em>x</em></sub></small> particles <em>via</em> atomic layer deposition (ALD). The catalytic performance of the ALD-prepared Ru nanoclusters was assessed for ammonia synthesis and compared with two catalysts produced by conventional incipient wetness impregnation. For the ALD-prepared Ru nanoclusters, a pre-reaction H<small><sub>2</sub></small>-reduction step induced partial encapsulation of suboxide species on Ru sites due to strong metal–support interactions, limiting Ru nanocluster sintering and maintaining a reduced Ru size of 1.7 nm. The electron donation from the reduced support to Ru sites imparted an electron-rich character, which facilitated the weakening of the N<img>N bond and promoted the rate-determining step of ammonia synthesis. The ALD-Ru catalysts exhibited competitive ammonia synthesis activity under milder conditions, compared to the impregnated catalysts, with a lower requirement for initial reaction temperature. These results highlight the potential of ALD-synthesized Ru nanoclusters as highly efficient catalysts for low-temperature ammonia production, offering a promising avenue for advancing ammonia synthesis technologies.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3507-3519"},"PeriodicalIF":0.0,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00350k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565744","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Identifying the best ML model for predicting the bandgap in a perovskite solar cell†","authors":"Nita Samantaray, Arjun Singh and Anu Tonk","doi":"10.1039/D4SU00370E","DOIUrl":"https://doi.org/10.1039/D4SU00370E","url":null,"abstract":"<p >Perovskite solar cells (PSCs) have gained attention for their characteristics of high efficiency and commercial viability. However, the efficiency of a PSC depends on various factors. One such important parameter is the bandgap of the active layer as it plays an important role in PSCs with regards to the amount of light absorption. Thus, it influences the overall performance of the solar cell. It is important to predict the bandgap of the active layer in PSCs to achieve an effective fabrication process. In this study, we compared six machine learning (ML) models to predict the bandgap. The models were created using a dataset of 500 devices, such as MAPbI<small><sub>3</sub></small>, FAPbI<small><sub>3</sub></small>, CsSnI<small><sub>3</sub></small> and CsMAPbI<small><sub>3</sub></small>, obtained from The Perovskite Database Project. These models were further validated using a different dataset of 50 devices. The models were created using ML methods: random forest, gradient boosting regressor, k-nearest neighbours (KNN), AdaBoost, Gaussian process regressor, and bagging. The feature parameters considered for the models were the A coefficient, B coefficient, and C coefficient, out of various other parameters such as the perovskite dimension, perovskite thickness, perovskite deposition temperature, and perovskite deposition time. The random forest model showed better results compared to other models with a low mean absolute error (MAE) of 0.000775, low mean squared error (MSE) of 0.00000920, and high coefficient of determination (<em>r</em><small><sup>2</sup></small>) of 0.9994.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3520-3524"},"PeriodicalIF":0.0,"publicationDate":"2024-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00370e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Heba Alsharif, Matthew B. Conway, David J. Morgan, Thomas E. Davies, Stuart H. Taylor and Meenakshisundaram Sankar
{"title":"Controlling the nanoparticle size and shape of a Pt/TiO2 catalyst for enhanced hydrogenation of furfural to furfuryl alcohol†","authors":"Heba Alsharif, Matthew B. Conway, David J. Morgan, Thomas E. Davies, Stuart H. Taylor and Meenakshisundaram Sankar","doi":"10.1039/D4SU00388H","DOIUrl":"https://doi.org/10.1039/D4SU00388H","url":null,"abstract":"<p >We report the selective liquid phase hydrogenation of furfural to 2-furfuryl alcohol using a Pt/TiO<small><sub>2</sub></small> catalyst prepared by the wet-impregnation method under mild reaction conditions (30 °C and 3 bar H<small><sub>2</sub></small> pressure). The effect of heat treatment protocols on the catalyst structures and the resultant catalytic properties of 4.2%Pt/TiO<small><sub>2</sub></small> and 0.6%Pt/TiO<small><sub>2</sub></small> was investigated. For both Pt loadings, the calcined + reduced catalyst exhibited higher activity compared to the reduced only catalyst, with the difference in activity being more pronounced for 4.2%Pt/TiO<small><sub>2</sub></small> than for 0.6%Pt/TiO<small><sub>2</sub></small>. For the 4.2%Pt/TiO<small><sub>2</sub></small> catalyst, the reduced-only sample achieved 25% conversion with 90% selectivity for 2-furfuryl alcohol after 6 hours, while the calcined + reduced sample reached 99% conversion with 59% selectivity under identical reaction conditions. For the 0.6%Pt/TiO<small><sub>2</sub></small> catalyst, the reduced-only sample showed 70% conversion with 96% selectivity for 2-furfuryl alcohol, whereas the calcined + reduced sample achieved 97% conversion and 95% selectivity after a 2-h reaction. Characterisation of the samples using X-ray photoelectron spectroscopy, CO chemisorption and scanning transmission electron microscopy revealed that direct high temperature reduction resulted in a mixture of large Pt particles (>5 nm) with irregular shapes, small Pt nanoparticles (<em>ca.</em> 2 nm) and some sub-nm clusters. In contrast, calcination + reduction produced uniformly distributed Pt nanoparticles (<em>ca.</em> 2 nm) for both Pt loadings. Despite the presence of strong metal support interaction (SMSI) in Pt/TiO<small><sub>2</sub></small> catalysts, no spectroscopic evidence for such a strong interaction was found in this study. Therefore, the observed difference in catalytic activity is attributed to the variations in the shapes and sizes of the Pt nanoparticles. During the synthesis of Pt/TiO<small><sub>2</sub></small> catalysts, the calcination + reduction activation procedure is more beneficial for enhancing both activity and selectivity compared to a reduction only procedure.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 12","pages":" 3888-3896"},"PeriodicalIF":0.0,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00388h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142736728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Caleb M. Woodall, Katherine Vaz Gomes, Andreas Voigt, Kai Sundmacher and Jennifer Wilcox
{"title":"Tuning acid extraction of magnesium and calcium from platinum group metal tailings for CO2 conversion and storage†","authors":"Caleb M. Woodall, Katherine Vaz Gomes, Andreas Voigt, Kai Sundmacher and Jennifer Wilcox","doi":"10.1039/D4SU00443D","DOIUrl":"https://doi.org/10.1039/D4SU00443D","url":null,"abstract":"<p >Avoiding the worst impacts of climate change requires reducing greenhouse gas emissions and removing atmospheric CO<small><sub>2</sub></small> with permanent storage. The global shift to low- and zero-emission energy sources demands increased metal mining, resulting in substantial mine tailings. Mineral carbonation offers a method to store CO<small><sub>2</sub></small> in alkaline-rich mine tailings, addressing both waste and excess atmospheric CO<small><sub>2</sub></small>. This study explores the use of a pH-swing process to optimize the extraction of calcium and magnesium from plagioclase feldspar-rich platinum group metal (PGM) mine tailings from the Stillwater Mine in Nye, Montana. Various organic (citric, acetic, oxalic) and mineral (hydrochloric, sulfuric) acids were tested at different concentrations, solid/liquid ratios, and dissolution times. Organic acids, particularly citric and oxalic, were selective for magnesium and calcium, respectively, with citric acid extracting 44% of available magnesium in 72 hours. Sulfuric acid proved most effective in extracting both metals but may be impractical due to corrosion-resistant equipment costs. Carbonation of synthetic leachate indicated precipitation yields above 90% at pressures between 5 and 9 bar, producing carbonate products under 3 μm. Additionally, comparing <em>in situ</em> and <em>ex situ</em> base addition methods suggests that pH pre-swing, <em>i.e.</em>, before carbonation is comparable to adding base during the reaction. This study advances the understanding of divalent cation extraction from plagioclase feldspar-rich PGM mine tailings but highlights the need for further research to develop an economic process.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3320-3333"},"PeriodicalIF":0.0,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00443d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}