EES catalysis最新文献

筛选
英文 中文
Outstanding Reviewers for EES Catalysis in 2023 2023 年 EES Catalysis 杰出审稿人
EES catalysis Pub Date : 2024-07-03 DOI: 10.1039/D4EY90015D
{"title":"Outstanding Reviewers for EES Catalysis in 2023","authors":"","doi":"10.1039/D4EY90015D","DOIUrl":"10.1039/D4EY90015D","url":null,"abstract":"<p >We would like to take this opportunity to thank all of <em>EES Catalysis</em>'s reviewers for helping to preserve quality and integrity in chemical science literature. We would also like to highlight the Outstanding Reviewers for <em>EES Catalysis</em> in 2023.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1036-1036"},"PeriodicalIF":0.0,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey90015d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141512535","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
High photocatalytic yield in the non-oxidative coupling of methane using a Pd–TiO2 nanomembrane gas flow-through reactor† 利用 Pd-TiO2 纳米膜气体直流反应器实现甲烷非氧化偶联的高光催化产率
EES catalysis Pub Date : 2024-07-03 DOI: 10.1039/D4EY00112E
Victor Longo, Luana De Pasquale, Francesco Tavella, Mariam Barawi, Miguel Gomez-Mendoza, Víctor de la Peña O’Shea, Claudio Ampelli, Siglinda Perathoner, Gabriele Centi and Chiara Genovese
{"title":"High photocatalytic yield in the non-oxidative coupling of methane using a Pd–TiO2 nanomembrane gas flow-through reactor†","authors":"Victor Longo, Luana De Pasquale, Francesco Tavella, Mariam Barawi, Miguel Gomez-Mendoza, Víctor de la Peña O’Shea, Claudio Ampelli, Siglinda Perathoner, Gabriele Centi and Chiara Genovese","doi":"10.1039/D4EY00112E","DOIUrl":"10.1039/D4EY00112E","url":null,"abstract":"<p >The photocatalytic non-oxidative coupling of methane (NOCM) is a highly challenging and sustainable reaction to produce H<small><sub>2</sub></small> and C<small><sub>2+</sub></small> hydrocarbons under ambient conditions using sunlight. However, there is a lack of knowledge, particularly on how to achieve high photocatalytic yield in continuous-flow reactors. To address this, we have developed a novel flow-through photocatalytic reactor for NOCM as an alternative to the conventionally used batch reactors. Me/TiO<small><sub>2</sub></small> photocatalysts, where Me = Au, Ag and Pd, are developed, but only those based on Pd are active. Interestingly, the preparation method significantly impacts performance, going from inactive samples (prepared by wet impregnation) to highly active samples (prepared by strong electrostatic adsorption – SEA). These photocatalysts are deposited on a nanomembrane, and the loading effect, which determines productivity, selectivity, and stability, is also analysed. Transient absorption spectroscopy (TAS) analysis reveals the involvement of holes and photoelectrons after charge separation on Pd/TiO<small><sub>2</sub></small> (SEA) and their interaction with methane in ethane formation, reaching a production rate of about 1000 μmol g<small><sup>−1</sup></small> h<small><sup>−1</sup></small> and a selectivity of almost 95% after 5 hours of reaction. Stability tests involving 24 h of continuous irradiation are performed, showing changes in productivity and selectivity to ethane, ethylene and CO<small><sub>2</sub></small>. The effect of a mild oxidative treatment (80 °C) to extend the catalyst's lifetime is also reported.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1164-1175"},"PeriodicalIF":0.0,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00112e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141512536","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
Designing bifunctional perovskite catalysts for the oxygen reduction and evolution reactions† 设计用于氧还原和进化反应的双功能过氧化物催化剂
EES catalysis Pub Date : 2024-06-24 DOI: 10.1039/D4EY00084F
Casey E. Beall, Emiliana Fabbri, Adam H. Clark, Vivian Meier, Nur Sena Yüzbasi, Thomas Graule, Sayaka Takahashi, Yuto Shirase, Makoto Uchida and Thomas J. Schmidt
{"title":"Designing bifunctional perovskite catalysts for the oxygen reduction and evolution reactions†","authors":"Casey E. Beall, Emiliana Fabbri, Adam H. Clark, Vivian Meier, Nur Sena Yüzbasi, Thomas Graule, Sayaka Takahashi, Yuto Shirase, Makoto Uchida and Thomas J. Schmidt","doi":"10.1039/D4EY00084F","DOIUrl":"10.1039/D4EY00084F","url":null,"abstract":"<p >The development of unified regenerative fuel cells (URFCs) necessitates an active and stable bifunctional oxygen electrocatalyst. The unique challenge of possessing high activity for both the oxygen reduction (ORR) and oxygen evolution (OER) reactions, while maintaining stability over a wide potential window impedes the design of bifunctional oxygen electrocatalysts. Herein, two design strategies are explored to optimize their performance. The first incorporates active sites for the ORR and OER, Mn and Co, into a single perovskite structure, which is achieved with the perovskites Ba<small><sub>0.5</sub></small>Sr<small><sub>0.5</sub></small>Co<small><sub>0.8</sub></small>Mn<small><sub>0.2</sub></small>O<small><sub>3−<em>δ</em></sub></small> (BSCM) and La<small><sub>0.5</sub></small>Ba<small><sub>0.25</sub></small>Sr<small><sub>0.25</sub></small>Co<small><sub>0.5</sub></small>Mn<small><sub>0.5</sub></small>O<small><sub>3−<em>δ</em></sub></small> (LBSCM). The second combines an active ORR perovskite catalyst (La<small><sub>0.4</sub></small>Sr<small><sub>0.6</sub></small>MnO<small><sub>3−<em>δ</em></sub></small> (LSM)) with an OER active perovskite catalyst (Ba<small><sub>0.5</sub></small>Sr<small><sub>0.5</sub></small>Co<small><sub>0.8</sub></small>Fe<small><sub>0.2</sub></small>O<small><sub>3−<em>δ</em></sub></small> (BSCF)) in a physical mixed composite (BSCF/LSM). The success of the two strategies is investigated by measuring the catalysts’ catalytic performance and response to alternating reducing and oxidizing potentials to mimic the dynamic conditions experienced during the operation of URFCs. Additionally, the continuous, potentiodynamic change in Mn, Co, and Fe oxidation states during the ORR and OER is elucidated with <em>operando</em> X-ray absorption spectroscopy (XAS) measurements, revealing key insights into the nature of the active sites. The results reveal important catalyst physiochemical properties and provide a guide for future research and design principles for bifunctional oxygen electrocatalysts.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1152-1163"},"PeriodicalIF":0.0,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00084f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141507738","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
Active and highly durable supported catalysts for proton exchange membrane electrolysers† 用于质子交换膜电解器的活性和高耐久性支撑催化剂
EES catalysis Pub Date : 2024-06-21 DOI: 10.1039/D4EY00026A
Debora Belami, Matthew Lindley, Umesh S. Jonnalagadda, Annie Mae Goncalves Bullock, Qianwenhao Fan, Wen Liu, Sarah J. Haigh, James Kwan, Yagya N. Regmi and Laurie A. King
{"title":"Active and highly durable supported catalysts for proton exchange membrane electrolysers†","authors":"Debora Belami, Matthew Lindley, Umesh S. Jonnalagadda, Annie Mae Goncalves Bullock, Qianwenhao Fan, Wen Liu, Sarah J. Haigh, James Kwan, Yagya N. Regmi and Laurie A. King","doi":"10.1039/D4EY00026A","DOIUrl":"10.1039/D4EY00026A","url":null,"abstract":"<p >The design and development of supported catalysts for the oxygen evolution reaction (OER) is a promising pathway to reducing iridium loading in proton exchange membrane water electrolysers. However, supported catalysts often suffer from poor activity and durability, particularly when deployed in membrane electrode assemblies. In this work, we deploy iridium coated hollow titanium dioxide particles as OER catalysts to achieve higher Ir mass activities than the leading commercial catalysts. Critically, we demonstrate state-of-the-art durabilities for supported iridium catalysts when compared against the previously reported values for analogous device architectures, operating conditions and accelerated stress test profiles. Through extensive materials characterisations alongside rotating disk electrode measurements, we investigate the role of conductivity, morphology, oxidation state and crystallinity on the OER electrochemical performance. Our work highlights a new supported catalyst design that unlocks high-performance OER activity and durability in commercially relevant testing configurations.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1139-1151"},"PeriodicalIF":0.0,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00026a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141507739","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
Surface amorphization and functionalization of a NiFeOOH electrocatalyst for a robust seawater electrolyzer† 用于坚固海水电解槽的 NiFeOOH 电催化剂的表面非晶化和功能化
EES catalysis Pub Date : 2024-06-14 DOI: 10.1039/D4EY00106K
Hao Wang, Nannan Jiang, Bing Huang, Qiangmin Yu and Lunhui Guan
{"title":"Surface amorphization and functionalization of a NiFeOOH electrocatalyst for a robust seawater electrolyzer†","authors":"Hao Wang, Nannan Jiang, Bing Huang, Qiangmin Yu and Lunhui Guan","doi":"10.1039/D4EY00106K","DOIUrl":"10.1039/D4EY00106K","url":null,"abstract":"<p >Hydrogen production of seawater electrolysis has attracted considerable interest due to the abundant seawater resources. However, the chloride ions (Cl<small><sup>−</sup></small>) in seawater not only corrode the electrodes but also cause side reactions, severely impacting the electrode efficiency and stability of the oxygen evolution reaction (OER) in seawater electrolysis. These challenges are the key factors limiting the development of seawater electrolysis technology. Here, we developed a surface-functionalized high-performance catalyst, which not only resists Cl<small><sup>−</sup></small> corrosion using surface-functionalized ions, but also improves the OER activity by surface amorphization. The designed catalyst (Ru<small><sub>0.1</sub></small>-NiFeOOH/PO<small><sub>4</sub></small><small><sup>3−</sup></small>) is composed of Ru<small><sub>0.1</sub></small>-NiFeOOH and surface phosphate. On the one hand, a small amount of Ru doping can increase the surface amorphization of NiFeOOH and thus improve the catalytic activity. On the other hand, the phosphates on Ru<small><sub>0.1</sub></small>-NiFeOOH are resistant to Cl<small><sup>−</sup></small> corrosion, which in turn improves the electrode stability. This catalyst demonstrates robust performance operation over 1000 h in alkaline seawater solutions at an industrial current density of 0.5 A cm<small><sup>−2</sup></small>. The anion exchange membrane seawater electrolyzer assembled with Ru<small><sub>0.1</sub></small>-NiFeOOH/PO<small><sub>4</sub></small><small><sup>3−</sup></small> only needs 1.6 V to achieve 0.5 A cm<small><sup>−2</sup></small> when powered by sustainable solar energy. The electrolyzer efficiency is 75.1% at 0.5 A cm<small><sup>−2</sup></small>, which is superior to the 2030 technical target of 65% set by the U.S. DOE and most reported work. This work offers a new perspective for designing efficient and stable catalysts and is of great significance for advancing seawater electrolysis technology.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1092-1099"},"PeriodicalIF":0.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00106k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141507740","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
Bridging the structural gap of supported vanadium oxides for oxidative dehydrogenation of propane with carbon dioxide† 缩小支撑钒氧化物在丙烷与二氧化碳氧化脱氢过程中的结构差距
EES catalysis Pub Date : 2024-06-14 DOI: 10.1039/D4EY00094C
Li Wang, Heng-Bo Zhang, Rongrong Hu, Han-Qing Ge, Yong-Hong Song, Guo-Qing Yang, Yuefeng Li, Zhao-Tie Liu and Zhong-Wen Liu
{"title":"Bridging the structural gap of supported vanadium oxides for oxidative dehydrogenation of propane with carbon dioxide†","authors":"Li Wang, Heng-Bo Zhang, Rongrong Hu, Han-Qing Ge, Yong-Hong Song, Guo-Qing Yang, Yuefeng Li, Zhao-Tie Liu and Zhong-Wen Liu","doi":"10.1039/D4EY00094C","DOIUrl":"10.1039/D4EY00094C","url":null,"abstract":"<p >As an extensively used industrial catalyst for oxidation reactions, supported vanadium oxide (VO<small><sub><em>x</em></sub></small>) is a promising candidate for oxidative dehydrogenation of propane with carbon dioxide (CO<small><sub>2</sub></small>-ODP). Although the structure of VO<small><sub><em>x</em></sub></small> is found to be a key factor in determining the catalytic activity and stability of supported VO<small><sub><em>x</em></sub></small> for CO<small><sub>2</sub></small>-ODP, the essential reason still remains elusive at the molecular level. To shed some light on this fundamental issue, VO<small><sub><em>x</em></sub></small>/(−)SiO<small><sub>2</sub></small> catalysts with narrow distributions of V loading while well-defined structures of VO<small><sub><em>x</em></sub></small> species, <em>i.e.</em>, monomeric VO<small><sub><em>x</em></sub></small>, less polymeric VO<small><sub><em>x</em></sub></small>, highly polymeric VO<small><sub><em>x</em></sub></small> and V<small><sub>2</sub></small>O<small><sub>5</sub></small> crystallites, were purposely synthesized by appropriate methods, including one-pot hydrothermal synthesis, incipient wetness impregnation and physical grinding. We found that the catalytic activity and stability of VO<small><sub><em>x</em></sub></small> species decrease in the order of monomeric VO<small><sub><em>x</em></sub></small> &gt; less polymeric VO<small><sub><em>x</em></sub></small> &gt; highly polymeric VO<small><sub><em>x</em></sub></small> &gt; crystalline V<small><sub>2</sub></small>O<small><sub>5</sub></small>, which coincides with the ability for the re-oxidation of the correspondingly reduced VO<small><sub><em>x</em></sub></small> species by CO<small><sub>2</sub></small>. As a result of the most facile re-oxidation of the reduced monomeric VO<small><sub><em>x</em></sub></small> species by CO<small><sub>2</sub></small>, a well matched redox cycle of V<small><sup>5+</sup></small>/V<small><sup>4+</sup></small> oxides during CO<small><sub>2</sub></small>-ODP can be maintained with increasing the time on stream, leading to an improved stability of the catalyst with more monomeric VO<small><sub><em>x</em></sub></small>. These mechanistic findings on the redox properties of VO<small><sub><em>x</em></sub></small> with different structures can be guidelines for developing a high-performance VO<small><sub><em>x</em></sub></small>-based catalyst for CO<small><sub>2</sub></small>-ODP.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1126-1138"},"PeriodicalIF":0.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00094c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141507741","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
Catalytic upgrading of wet waste-derived carboxylic acids to sustainable aviation fuel and chemical feedstocks† 将湿废物衍生羧酸催化升级为可持续航空燃料和化学原料
EES catalysis Pub Date : 2024-06-12 DOI: 10.1039/D4EY00087K
Jacob H. Miller, Mayadhin Al Abri, Jim Stunkel, Andrew J. Koehler, Matthew R. Wiatrowski, Robert L. McCormick, Gina Fioroni, Jon Luecke, Cheyenne Paeper and Martha Arellano-Treviño
{"title":"Catalytic upgrading of wet waste-derived carboxylic acids to sustainable aviation fuel and chemical feedstocks†","authors":"Jacob H. Miller, Mayadhin Al Abri, Jim Stunkel, Andrew J. Koehler, Matthew R. Wiatrowski, Robert L. McCormick, Gina Fioroni, Jon Luecke, Cheyenne Paeper and Martha Arellano-Treviño","doi":"10.1039/D4EY00087K","DOIUrl":"10.1039/D4EY00087K","url":null,"abstract":"<p >We develop a catalytic process comprising exclusively of flow reactions for conversion of wet waste-derived volatile fatty acids to sustainable aviation fuel (SAF) and key aromatic building blocks (benzene, toluene, ethylbenzene, and xylene; BTEX). Acids are upgraded <em>via</em> sequential ketonization and either cyclization of light (C<small><sub>3–7</sub></small>) ketones to BTEX and an aromatic SAF blendstock or hydrodeoxygenation of C<small><sub>8+</sub></small> ketones to an alkane SAF blendstock. The enabling step investigated in this work is light ketone cyclization over H/ZSM-5, which was chosen through screening upgrading of 4-heptanone over solid acidic and basic catalysts. We then determined the reaction network of 4-heptanone upgrading by analyzing selectivity trends with conversion and concluded that the reaction should be run at full conversion. Finally, we demonstrated the entire acid upgrading process by converting commercial food waste-derived carboxylic acids to SAF blendstocks and BTEX. We blended the C<small><sub>9+</sub></small> aromatic and alkane products to create one SAF blendstock and show that this mixture can be blended 50/50 with Jet A and meet all critical property standards. Techno-economic analysis and life cycle assessment show that utilizing a food waste feedstock for the process can be economically feasible with current policy incentives and reduce greenhouse gas emissions by more than 250%.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1111-1125"},"PeriodicalIF":0.0,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00087k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141507742","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
Enhanced photocatalytic performance of tetraphenylethylene-based porous aromatic frameworks by bandgap adjustment for the synthesis of benzimidazoles† 通过带隙调整增强四苯乙烯基多孔芳香族框架的光催化性能以合成苯并咪唑
EES catalysis Pub Date : 2024-06-07 DOI: 10.1039/D4EY00071D
He Wang, Xinmeng Xu, Linzhu Cao, Zhenwei Zhang, Jiali Li, Xiaoming Liu, Xin Tao and Guangshan Zhu
{"title":"Enhanced photocatalytic performance of tetraphenylethylene-based porous aromatic frameworks by bandgap adjustment for the synthesis of benzimidazoles†","authors":"He Wang, Xinmeng Xu, Linzhu Cao, Zhenwei Zhang, Jiali Li, Xiaoming Liu, Xin Tao and Guangshan Zhu","doi":"10.1039/D4EY00071D","DOIUrl":"10.1039/D4EY00071D","url":null,"abstract":"<p >Porous aromatic frameworks (PAFs) as visible-light active and reusable photocatalysts provide a green and sustainable alternative to conventional metal-based photocatalysts. In this study, we design and synthesize three novel photoactive tetraphenylethylene (TPE) based PAF photocatalysts (TPE-PAFs) linked with thiophene units in an alternating donor (D)–acceptor (A) fashion. Photoelectrochemical measurements show that the introduction of different thiophene units can effectively regulate the optical band gap and energy level, which may further determine their photocatalytic performance. As a result, TPE-PAFs achieve excellent yields (up to 99%), broad substrate scope and high recyclability (up to 10 cycles) for the photosynthesis of benzimidazoles. The photocatalytic reaction is successfully monitored using <em>in situ</em> IR spectra. This work provides a feasible approach for designing PAFs with high photocatalytic activity and broadens the application of PAFs for photocatalytic organic transformations.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1100-1110"},"PeriodicalIF":0.0,"publicationDate":"2024-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00071d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141552177","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
Conversion of diverse post-consumer PVC waste materials to PE via dual catalytic tandem dehydrochlorination–hydrogenation† 通过双催化串联脱氢氯化-氢化将各种消费后聚氯乙烯废料转化为聚乙烯
EES catalysis Pub Date : 2024-06-05 DOI: 10.1039/D4EY00082J
Galahad O’Rourke, Alina Skorynina, Igor Beckers, Sam Van Minnebruggen, Christel Colemonts, Philippe Gabriels, Peter Van der Veken and Dirk De Vos
{"title":"Conversion of diverse post-consumer PVC waste materials to PE via dual catalytic tandem dehydrochlorination–hydrogenation†","authors":"Galahad O’Rourke, Alina Skorynina, Igor Beckers, Sam Van Minnebruggen, Christel Colemonts, Philippe Gabriels, Peter Van der Veken and Dirk De Vos","doi":"10.1039/D4EY00082J","DOIUrl":"10.1039/D4EY00082J","url":null,"abstract":"<p >Chemical recycling of polyvinyl chloride (PVC) waste poses challenges due to its high chloride content and varied additive formulations. We present a dual catalytic system enabling full conversion of post-consumer PVC waste <em>via</em> tandem dehydrochlorination–hydrogenation. Using a ZnCl<small><sub>2</sub></small> catalyst (0.1–0.2 eq.) for dehydrochlorination and a Ru catalyst (1.0 mol%) for hydrogenation, it directly converts PVC into a lower molecular weight polyethylene (PE)-like polymer. It prevents the problematic formation of polyenes and aromatic char during thermal processing. The system tolerates common additives (<em>e.g.</em> plasticisers and Pb-, Zn- and Ca/Zn-based stabilisers) and effectively dechlorinates materials with high inorganic filler content. The method can process PVC materials with a wide range of <em>M</em><small><sub>n</sub></small> values (29 000–120 000 g mol<small><sup>−1</sup></small>). Methyl cyclohexanecarboxylate emerges as a suitable solvent for the tandem reaction, thereby producing 100% dechlorinated products with low molar mass averages (<em>M</em><small><sub>n</sub></small> ∼ 2400 g mol<small><sup>−1</sup></small> and <em>M</em><small><sub>w</sub></small> ∼ 5000 g mol<small><sup>−1</sup></small>) and allows additive removal. X-ray absorption spectroscopy (XAS) and a study of the reactivity of a model compound elucidate the Ru-catalyst structure and the chain splitting mechanism. This tandem process yields soluble short-chained polymer fragments, facilitating industrial processing and additive removal from chlorinated plastic waste.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 1006-1018"},"PeriodicalIF":0.0,"publicationDate":"2024-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00082j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141252726","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
Understanding the charge transfer dynamics in 3D–1D nanocomposites over solar driven synergistic selective valorization of lignocellulosic biomass: a new sustainable approach† 在太阳能驱动的木质纤维素生物质协同选择性增值过程中,了解 3D-1D 纳米复合材料中的电荷转移动力学:一种新的可持续方法
EES catalysis Pub Date : 2024-05-25 DOI: 10.1039/D4EY00077C
Arpna Jaryal, Ajit Kumar Singh, Shivali Dhingra, Himanshu Bhatt, Manvi Sachdeva, Hirendra N. Ghosh, Arindam Indra and Kamalakannan Kailasam
{"title":"Understanding the charge transfer dynamics in 3D–1D nanocomposites over solar driven synergistic selective valorization of lignocellulosic biomass: a new sustainable approach†","authors":"Arpna Jaryal, Ajit Kumar Singh, Shivali Dhingra, Himanshu Bhatt, Manvi Sachdeva, Hirendra N. Ghosh, Arindam Indra and Kamalakannan Kailasam","doi":"10.1039/D4EY00077C","DOIUrl":"10.1039/D4EY00077C","url":null,"abstract":"<p >Photocatalytic redox valorization of lignocellulosic biomass to fine chemicals is in its infancy stages where it can be effectively utilized for sustainable energy conversion. In this direction, an effective 3D–1D (Aeroxide P25 TiO<small><sub>2</sub></small> and CdS) nanocomposite has been demonstrated to upgrade several biomass-derived platform chemicals (<em>e.g.</em> HMF, FFaL, vanillyl alcohol) in a selective and synergistic redox pathway under visible light irradiation for the first time. The successful utilization of the photocatalytic system resulted in the visible light-driven selective hydrogenation of HMF to BHMF along with the coproduction of H<small><sub>2</sub></small> without the addition of any reducing agent under natural sunlight. In addition, the simultaneous production of valuable commodity chemical, <em>i.e.</em> vanillin, through oxidation has also been earmarked. The intimate interfacial contact between CdS as a visible light active photocatalyst and P25 TiO<small><sub>2</sub></small> as an active hydrogenation site assists the facile migration of photogenerated electrons towards P25 TiO<small><sub>2</sub></small>. The coupling of electrons with <em>in situ</em> generated protons led to 95% yield of BHMF whereas oxidative photogenerated holes yielded 35% vanillin, thus abolishing the need for extra redox additives. The synergistic effect bestowed by the semiconductor heterojunction manifested excellent photoredox activity accompanying strong inter-particle interactions which were thoroughly investigated by employing electrochemical, PL, XPS and transient absorption spectroscopy (TAS). Thus, a new sustainable “biomass-based photo-refinery” and cost-effective low carbon-intensity approach has been elucidated for visible light-based hydrogenation activity of TiO<small><sub>2</sub></small> unveiling a fabrication strategy of photocatalysts with efficient solar spectrum harvesting.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 1019-1026"},"PeriodicalIF":0.0,"publicationDate":"2024-05-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00077c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141147635","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
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信