Reaction Chemistry & Engineering最新文献

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Immobilization of cationic dye on photoluminescent hydroxyapatite particles through a citric acid bonding layer† 通过柠檬酸键合层将阳离子染料固定在光致发光羟基磷灰石颗粒上†。
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-10-14 DOI: 10.1039/D4RE00277F
Daichi Noda, Wanyu Shi, Aiga Yamada, Zizhen Liu and Motohiro Tagaya
{"title":"Immobilization of cationic dye on photoluminescent hydroxyapatite particles through a citric acid bonding layer†","authors":"Daichi Noda, Wanyu Shi, Aiga Yamada, Zizhen Liu and Motohiro Tagaya","doi":"10.1039/D4RE00277F","DOIUrl":"https://doi.org/10.1039/D4RE00277F","url":null,"abstract":"<p >We demonstrated the surface functionalization using citric acid (Cit) as a bonding layer on hydroxyapatite (HAp) nanoparticles. The bonding layer on the Eu(<small>III</small>) ion-doped HAp nanoparticles could be immobilized with the larger amount of cationic porphyrin. The interactions between the immobilized molecules were enhanced at the monomer state with increasing the amount.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 11","pages":" 2863-2867"},"PeriodicalIF":3.4,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142518298","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Kinetics of the valorization of hexoses with Sn-USY catalysts in methanolic media: glycosidation vs. retroaldol cleavage† 在甲醇介质中使用 Sn-USY 催化剂进行己糖价值化的动力学:糖苷化与逆醛醇裂解†。
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-10-09 DOI: 10.1039/D4RE00307A
J. M. Jimenez-Martin, M. El Tawil-Lucas, C. García-Jerez, J. Moreno, A. García, B. Hernández and J. Iglesias
{"title":"Kinetics of the valorization of hexoses with Sn-USY catalysts in methanolic media: glycosidation vs. retroaldol cleavage†","authors":"J. M. Jimenez-Martin, M. El Tawil-Lucas, C. García-Jerez, J. Moreno, A. García, B. Hernández and J. Iglesias","doi":"10.1039/D4RE00307A","DOIUrl":"https://doi.org/10.1039/D4RE00307A","url":null,"abstract":"<p >Catalytic performance of potassium-exchanged Sn-containing USY zeolite ([K]Sn-USY) for the transformation of hexoses into methyl lactate in methanol has been studied. This work explores the effects of temperature and catalyst loading on this transformation process, shedding light on the kinetic aspects of this process in which the starting sugars undergo a complex network of different transformations to yield different biobased products with commercial interest. The proposed kinetic model integrates several key reactions: isomerization of the starting sugars, glycosidation with the alcohol solvent, retro-aldol cleavage of carbohydrates to minor sugars, and hydrolytic side transformations. By considering these steps, insights into the determining factors that influence overall transformation and high selectivity of the [K]Sn-USY zeolite for methyl lactate are clarified. Notably, this work highlights the formation of side products, including methoxy methyl 2-hydroxy-butanoate (MMHB) and glycolaldehyde dimethyl acetal (GADMA), which have been previously overlooked in other kinetic modelling and derived from the retroaldol cleavage of aldoses. The [K]Sn-USY catalysts exhibit promising activity and selectivity, making them attractive candidates for bio-based plastic production. A comprehensive understanding of the catalytic behavior and side product formation contributes to the optimization of these catalysts for sustainable carbohydrate valorization.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 1","pages":" 90-105"},"PeriodicalIF":3.4,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/re/d4re00307a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844670","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Technoeconomic analysis of fine chemical electrosynthesis: a case study using electrooxidation of 2-methylnaphthelene to vitamin K3†
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-10-08 DOI: 10.1039/D4RE00346B
Qifeng Yang, Liping Liang, Ning Xu, Yang Li, Zhihui Wang, Dadong Shen and Yiming Mo
{"title":"Technoeconomic analysis of fine chemical electrosynthesis: a case study using electrooxidation of 2-methylnaphthelene to vitamin K3†","authors":"Qifeng Yang, Liping Liang, Ning Xu, Yang Li, Zhihui Wang, Dadong Shen and Yiming Mo","doi":"10.1039/D4RE00346B","DOIUrl":"https://doi.org/10.1039/D4RE00346B","url":null,"abstract":"<p >Electroorganic synthesis has received significant attention due to its environmentally friendly nature, offering the potential to replace traditional hazardous chemical production routes. However, an in-depth technoeconomic analysis (TEA) of electrosynthesis technology is still necessary to objectively assess the economic viability of this technology as an alternative to the traditional chemical syntheses. In this study, we used the cerium-mediated electrosynthesis of 2-methyl-1,4-naphthoquinone (2-MNQ, also known as vitamin K<small><sub>3</sub></small>) as a case study. The process development was conducted in both small-scale and large-scale electrochemical flow cells with 6.25 cm<small><sup>2</sup></small> and 208 cm<small><sup>2</sup></small> electrode sizes, respectively, to investigate the process scalability. Under the optimal conditions, a 66% yield was achieved for 2-MNQ with 90% faradaic efficiency at 50 mA cm<small><sup>−2</sup></small> current density. We performed a comprehensive TEA on the key factors influencing electroorganic synthesis, including current density, electrode cost and lifespan, membranes, and electricity price. Furthermore, considering ongoing technological advancements in electrodes, membranes, and renewable electricity generation, we analyzed the trend of future projected cost reductions for electrosynthesis processes.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 1","pages":" 79-89"},"PeriodicalIF":3.4,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844669","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
C12 aromatic triol-furoin and diol-furil from bio-based 5-(hydroxymethyl)furfural: enhanced selective synthesis, scale-up and mechanistic insight into cyclic catalysis†
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-10-07 DOI: 10.1039/D4RE00212A
Thi Tuyet Thuy Vu, Shentan Liu, Mantas Jonušis, Simona Jonušienė, Jinsik Choi, Mohamed Ismail, Nicola Rehnberg, Rajni Hatti-Kaul and Sang-Hyun Pyo
{"title":"C12 aromatic triol-furoin and diol-furil from bio-based 5-(hydroxymethyl)furfural: enhanced selective synthesis, scale-up and mechanistic insight into cyclic catalysis†","authors":"Thi Tuyet Thuy Vu, Shentan Liu, Mantas Jonušis, Simona Jonušienė, Jinsik Choi, Mohamed Ismail, Nicola Rehnberg, Rajni Hatti-Kaul and Sang-Hyun Pyo","doi":"10.1039/D4RE00212A","DOIUrl":"https://doi.org/10.1039/D4RE00212A","url":null,"abstract":"<p >In this study, we investigate the valorization of 5-(hydroxymethyl)furfural (5-HMF), a versatile and pivotal renewable C6 platform chemical, into a C12 heteroaromatic triol, 5,5′-bis(hydroxymethyl)furoin (DHMF), and a C12 heteroaromatic diol, 5,5′-bis(hydroxymethyl)furil (BHMF). The carboligation of 5-HMF to DHMF is catalyzed by an N-heterocyclic carbene, 1,3,4-triphenyl-4,5-dihydro-1<em>H</em>-1,2,4-triazol-5-ylidene (TPT), generated <em>in situ</em> from its stable methoxy adduct, 5-methoxy-1,3,4-triphenyl-4,5-dihydro-1<em>H</em>-1,2,4-triazoline (TPA-OMe). This reaction achieves quantitative yield in dimethyl carbonate, a more environmentally friendly solvent. The resulting DHMF precipitate was readily purified <em>via</em> simple filtration and washing. Moreover, an enhanced selective oxidation was conducted at the secondary hydroxyl group of DHMF to generate the ketone group of BHMF in quantitative yield by using organo-catalysts, anionic exchanger, and NaOH. We proposed and subsequently validated a cyclic catalysis mechanism for the oxidation through the colorimetric detection of the by-product, H<small><sub>2</sub></small>O<small><sub>2</sub></small>, in the reaction. All synthetic processes to produce these C12 triol-furoin and diol-furil compounds were successfully demonstrated on a scale ranging from 20 to 400 grams. The feasibility of these processes was established with high yields achieved under moderate reaction conditions and ambient pressure, making them suitable for large-scale production. Consequently, these C12 multi-functional chemicals can find applications in the production of bio-based aromatic polymers such as polyesters, polyurethanes, and polycarbonates.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 1","pages":" 70-78"},"PeriodicalIF":3.4,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/re/d4re00212a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844668","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
ChemPren: a new and economical technology for conversion of waste plastics to light olefins ChemPren:将废塑料转化为轻质烯烃的新型经济技术
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-10-07 DOI: 10.1039/D4RE00354C
Anne Gaffney, Debtanu Maiti, Debasish Kuila and Gennaro Mafia
{"title":"ChemPren: a new and economical technology for conversion of waste plastics to light olefins","authors":"Anne Gaffney, Debtanu Maiti, Debasish Kuila and Gennaro Mafia","doi":"10.1039/D4RE00354C","DOIUrl":"https://doi.org/10.1039/D4RE00354C","url":null,"abstract":"<p >With the ever-increasing demand for plastics, sustainable recycling methods are key necessities. The current plastics industry can manage to recycle only 10% of the 400 million metric tons of plastic produced globally. Waste plastics, in the current infrastructure, land up mostly in landfills. Although a lot of research efforts have been spent on processing and recycling co-mingled mixed plastics, energy-efficient sustainable and scalable routes for plastic upcycling are still lacking. Catalytic valorization of waste plastic feedstock is one of the potential scalable routes for plastic upcycling. Silica-alumina based materials, and zeolites have shown a lot of promise. A major interest lies in restricting catalyst deactivation, and refining product selectivity and yield for such catalytic processes. This article highlights ChemPren technology as a clean energy solution to waste plastic recycling. Co-mingled, mixed plastic feedstock along with spray dried, attrition resistant, ZSM-5 containing catalysts is preprocessed with an extruder to form optimally sized particles and fed into a fluidized bed reactor for short contact times to produce selectively and in high yields ethylenes, propylenes and butylenes. This techno-economic perspective indicates that the ChemPren technology can produce propylene at $0.16 per lb, whereas the current selling price of virgin propylene is $0.54 per lb. This technology can serve as a platform for mixed plastic upcycling, with more advancements necessary in the form of robust and resilient catalysts and reactor operation strategies for tuning product selectivity.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 12","pages":" 3100-3104"},"PeriodicalIF":3.4,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672264","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
One-pot enzymatic synthesis of l-5-methyltetrahydrofolate from folic acid using enzyme cascades† 利用酶级联法以叶酸为原料一步酶法合成 l-5-甲基四氢叶酸†。
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-10-07 DOI: 10.1039/D4RE00237G
Linjiang Zhu, Yuxin Wang, Linyan Pan, Enyong Lin, Jiayan Wang and Xiaolong Chen
{"title":"One-pot enzymatic synthesis of l-5-methyltetrahydrofolate from folic acid using enzyme cascades†","authors":"Linjiang Zhu, Yuxin Wang, Linyan Pan, Enyong Lin, Jiayan Wang and Xiaolong Chen","doi":"10.1039/D4RE00237G","DOIUrl":"https://doi.org/10.1039/D4RE00237G","url":null,"abstract":"<p > <small>L</small>-5-Methyltetrahydrofolate (<small>L</small>-5-MTHF) is an active form of folate and widely used as a nutraceutical due to its high bioavailability. Herein, we report an efficient one-pot three-enzyme cascade reaction for the production of <small>L</small>-5-MTHF starting from synthetic folic acid (FA). The newly-designed synthesis route was validated by enzyme screening and process optimization. The highly-active dihydrofolate reductase from <em>Lactobacillus bulgaricus</em> (<em>Lbu</em>DHFR) was identified for asymmetric hydrogenation towards unnatural substrate FA, which could remarkably increase the synthetic efficiency. Dimethylsulfoniopropionate-dependent demethylase (DmdA) was successfully employed for directly converting tetrahydrofolate into <small>L</small>-5-MTHF using a cheap methyl donor. <em>Rco</em>DmdA from marine bacteria <em>Ruegeria conchae</em> was selected due to its high tolerance against the inhibition of the demethylated by-product. The optimal one-pot enzymatic synthesis could completely convert 34 mM of FA into 32.5 mM of <small>L</small>-5-MTHF with a molar conversion rate of 95.6%. No FA, dihydrofolate or tetrahydrofolate were detected in the final reaction mixture. Therefore, the new one-pot enzymatic method, circumventing the need for a transition metal catalyst, an unstable strong reductant and crystallization resolution, is proved to be simple, cost-effective, and easy to scale up for the green synthesis of <small>L</small>-5-MTHF.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 12","pages":" 3110-3115"},"PeriodicalIF":3.4,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Digital strategies to improve the product quality and production efficiency of fluorinated polymers: 2. Heat removal performance of reactor with internal and external cooling systems†
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-10-07 DOI: 10.1039/D4RE00203B
Xi-Bao Zhang, Yin-Ning Zhou, Hao Chen, Zheng-Hong Luo, Liyang Zhou, Guojun Yu, Wenwu Liu and Shiping Zhu
{"title":"Digital strategies to improve the product quality and production efficiency of fluorinated polymers: 2. Heat removal performance of reactor with internal and external cooling systems†","authors":"Xi-Bao Zhang, Yin-Ning Zhou, Hao Chen, Zheng-Hong Luo, Liyang Zhou, Guojun Yu, Wenwu Liu and Shiping Zhu","doi":"10.1039/D4RE00203B","DOIUrl":"https://doi.org/10.1039/D4RE00203B","url":null,"abstract":"<p >This work aims to study the heat transfer performance of a sophisticated industrial suspension polymerization reactor, which is distinguished by its complex blade structure and capability in efficient heat removal as well as its precise control over temperature distribution through adjusting the flow ratio of cooling water in the agitator and jacket. To achieve this goal, the impact of flow ratio and agitator speed on the heat removal rate and fluid temperature gradient is systematically investigated by CFD simulation. Several indicators are developed to quantitatively assess the reactor's heat transfer capability and fluid temperature uniformity. In addition, a thorough investigation is undertaken to analyze the possible mechanisms by which these factors exert their influence on the heat transfer performance of the reactor. Finally, some strategies for optimal performance through adjusting operational parameters of this type of reactors are proposed.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 1","pages":" 106-118"},"PeriodicalIF":3.4,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844634","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The kinetics of the polyurethane moisture curing reaction: a combined experimental and DFT mechanistic study†
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-09-30 DOI: 10.1039/D4RE00385C
Jie Zhou, Zhen Liu, Zhihua Zhu, Zuoxiang Zeng and Li Sun
{"title":"The kinetics of the polyurethane moisture curing reaction: a combined experimental and DFT mechanistic study†","authors":"Jie Zhou, Zhen Liu, Zhihua Zhu, Zuoxiang Zeng and Li Sun","doi":"10.1039/D4RE00385C","DOIUrl":"https://doi.org/10.1039/D4RE00385C","url":null,"abstract":"<p >An examination of the temporal dynamics of the moisture curing process of polyurethane (PUR) hot melt adhesives under varied humidity (65–85% RH) and temperature (20–40 °C) was performed <em>via in situ</em> Fourier transform infrared (FTIR) spectroscopy. The commencement of the moisture curing for PUR was substantiated by a reduction in peak intensity at 2271 cm<small><sup>−1</sup></small>. The data revealed that the nascent phase of the moisture curing reaction aligns with the first-order reaction kinetics. Further, there was a noticeable acceleration in the rate of the PUR's moisture curing reaction with an increment in environmental humidity and temperature. Density functional theory (DFT) was harnessed to delve into the effects of additional water clusters on the PUR's moisture curing progression. The theoretical model proposed that these additional water molecules catalyzed the hydrogen transfer, thus bolstering the moisture curing reaction, a finding that corroborated with our empirical observations.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 1","pages":" 38-47"},"PeriodicalIF":3.4,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844658","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mixed-conducting ceramic membrane reactors for hydrogen production 用于制氢的混合导电陶瓷膜反应器
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-09-26 DOI: 10.1039/D4RE00372A
Jingjing Tong, Peng Zhang, Fuwei Zhuang, Yanyan Zheng, Binyan Liu, Xiangping Qiao and Xuefeng Zhu
{"title":"Mixed-conducting ceramic membrane reactors for hydrogen production","authors":"Jingjing Tong, Peng Zhang, Fuwei Zhuang, Yanyan Zheng, Binyan Liu, Xiangping Qiao and Xuefeng Zhu","doi":"10.1039/D4RE00372A","DOIUrl":"https://doi.org/10.1039/D4RE00372A","url":null,"abstract":"<p >Hydrogen is widely used in industrial chemistry and acts as a promising clean energy carrier that can be produced from different hydrocarbons and water. Currently, the main sources of hydrogen are fossil fuels; however, they are associated with large CO<small><sub>2</sub></small> emissions. Alternatively, green hydrogen produced from water electrolysis using renewable energy is still far from large-scale industrial application owing to the poor reliability of renewable energy and water electrolysis. Therefore, the production of blue hydrogen, coupled with the CO<small><sub>2</sub></small> capture process, will play a dominant role in the near future in commercial hydrogen production. In this review, membrane reactor technologies based on ceramic-based dense membranes are comprehensively introduced. Membrane reactors are classified into three types according to the properties of the conductive carrier of membrane materials: (1) mixed protonic and electronic conductor (MPEC) membrane reactors, (2) mixed oxide-ionic and electronic conductor (MOEC) membrane reactors, and (3) mixed oxide-ionic and carbonate-ionic conductor (MOCC) membrane reactors. Their working principle, membrane materials, hydrogen sources, operating conditions, and performance are summarized. Finally, the challenges and prospectives of these membrane reactors are discussed for their future development.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 12","pages":" 3072-3099"},"PeriodicalIF":3.4,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/re/d4re00372a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672263","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Syngas production from phenolic pollutants via a series of hydroxylation, ring cleavage, and aqueous-phase reforming catalyzed by a hydrotalcite-supported Fe–Mn–Ni alloy† 在水滑石支撑的铁-锰-镍合金催化下,通过一系列羟化、裂环和水相重整过程从酚类污染物中生产合成气†。
IF 3.4 3区 化学
Reaction Chemistry & Engineering Pub Date : 2024-09-24 DOI: 10.1039/D4RE00348A
Hanifrahmawan Sudibyo, Daniela V. Cabrera, Rodrigo Labatut, Calvin J. Supriyanto, Budhijanto Budhijanto and Adhika Widyaparaga
{"title":"Syngas production from phenolic pollutants via a series of hydroxylation, ring cleavage, and aqueous-phase reforming catalyzed by a hydrotalcite-supported Fe–Mn–Ni alloy†","authors":"Hanifrahmawan Sudibyo, Daniela V. Cabrera, Rodrigo Labatut, Calvin J. Supriyanto, Budhijanto Budhijanto and Adhika Widyaparaga","doi":"10.1039/D4RE00348A","DOIUrl":"https://doi.org/10.1039/D4RE00348A","url":null,"abstract":"<p >A trifunctional catalyst facilitating a series of hydroxylation, oxidative ring opening, and aqueous-phase reforming reactions was developed to convert phenolic wastewater into syngas. The definitive screening design experiment at 250 °C for 5 h with 1.75% H<small><sub>2</sub></small>O<small><sub>2</sub></small> and 2 wt% catalyst loading demonstrated the importance of Fe, Mn, and Ni among the first-row transition metals to be impregnated into hydrotalcite to acquire the trifunctional feature. The surface chemistry characterization revealed that they improved the amount of strong and weak Brønsted (SBrA and WBrA) and Lewis (SLA and WLA) acidic active sites. The mechanistic roles of these sites <em>via</em> semi-continuous kinetic investigation at 200–300 °C for 1–5 h with 1.75% H<small><sub>2</sub></small>O<small><sub>2</sub></small> and 2 wt% catalyst loading were unraveled: (1) SBrA (surface metal oxyhydroxides) facilitated hydroxylation and homolytic cleavage producing hydroxyphenols; (2) WBrA (surface metal hydroxides) promoted ring opening of hydroxyphenols yielding oxo- and di-carboxylic acids; (3) WLA (mineral phase with a tetrahedral coordination) catalyzed reforming of acids into syngas; and (4) SLA (mineral phase with an octahedral coordination) improved the H<small><sub>2</sub></small> yield by promoting the water–gas shift reaction. The optimal content of Fe, Mn, and Ni was 49.4, 21.2, and 29.4 wt%, respectively, from 20 wt% of active metals on the support to achieve the maximal organic carbon removal (∼82%) and H<small><sub>2</sub></small> yield (∼80%) with a CO-to-H<small><sub>2</sub></small> ratio of 0.6, useful for chemical building block synthesis. The optimized catalyst demonstrated high activity and reusability, with a turnover number and frequency of ∼1 × 10<small><sup>6</sup></small> and ∼6 × 10<small><sup>4</sup></small> s<small><sup>−1</sup></small>, respectively, marking a breakthrough in sustainable syngas production.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 12","pages":" 3285-3298"},"PeriodicalIF":3.4,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142672284","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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