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The effect of catalyst precursors on the mechanism of iron-catalysed graphitization of cellulose† 催化剂前体对铁催化纤维素石墨化机理的影响†。
RSC sustainability Pub Date : 2024-10-14 DOI: 10.1039/D4SU00365A
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}
引用次数: 0
Hydrothermal synthesis of ZnZrOx catalysts for CO2 hydrogenation to methanol: the effect of pH on structure and activity† 水热合成 ZnZrO x 催化剂用于 CO2 加氢制甲醇:pH 值对结构和活性的影响。
RSC sustainability Pub Date : 2024-10-11 DOI: 10.1039/D4SU00522H
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}
引用次数: 0
Supramolecular purification of aromatic polyester monomers from chemical depolymerization† 从化学解聚中提纯芳香族聚酯单体的超分子技术†。
RSC sustainability Pub Date : 2024-10-11 DOI: 10.1039/D4SU00330F
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}
引用次数: 0
Lignocellulosic biomass valorisation: a review of feedstocks, processes and potential value chains and their implications for the decision-making process† 木质纤维素生物质增值:原料、工艺和潜在价值链及其对决策过程的影响综述†。
RSC sustainability Pub Date : 2024-10-10 DOI: 10.1039/D4SU00342J
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}
引用次数: 0
Self-assembled tetracyanoquinodimethane derivatives: differential fluorescent responses on sensing copper and mercury ions in an aqueous medium† 自组装的四氰醌二甲烷衍生物:在水介质中感应铜离子和汞离子时的不同荧光反应†。
RSC sustainability Pub Date : 2024-10-10 DOI: 10.1039/D4SU00445K
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}
引用次数: 0
How reduction temperature influences the structure of perovskite-oxide catalysts during the dry reforming of methane† 在甲烷干法转化过程中,还原温度如何影响过氧化物催化剂的结构。
RSC sustainability Pub Date : 2024-10-10 DOI: 10.1039/D4SU00483C
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}
引用次数: 0
Atomic layer deposition of Ru nanoclusters on Ba–LaCeOx: a highly efficient catalyst for ammonia synthesis under mild conditions† 在 Ba-LaCeOx 上原子层沉积 Ru 纳米团簇:温和条件下合成氨的高效催化剂†。
RSC sustainability Pub Date : 2024-10-07 DOI: 10.1039/D4SU00350K
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}
引用次数: 0
Identifying the best ML model for predicting the bandgap in a perovskite solar cell† 确定预测过氧化物太阳能电池带隙的最佳 ML 模型†。
RSC sustainability Pub Date : 2024-10-05 DOI: 10.1039/D4SU00370E
Nita Samantaray, Arjun Singh and Anu Tonk
{"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}
引用次数: 0
Controlling the nanoparticle size and shape of a Pt/TiO2 catalyst for enhanced hydrogenation of furfural to furfuryl alcohol† 控制 Pt/TiO2 催化剂的纳米颗粒尺寸和形状以增强糠醛加氢制糠醇的能力†。
RSC sustainability Pub Date : 2024-10-04 DOI: 10.1039/D4SU00388H
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 (&gt;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}
引用次数: 0
Tuning acid extraction of magnesium and calcium from platinum group metal tailings for CO2 conversion and storage† 从铂族金属尾矿中酸性提取镁和钙,用于二氧化碳转化和封存†。
RSC sustainability Pub Date : 2024-10-02 DOI: 10.1039/D4SU00443D
Caleb M. Woodall, Katherine Vaz Gomes, Andreas Voigt, Kai Sundmacher and Jennifer Wilcox
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