Reaction Chemistry & Engineering最新文献_第4页

Dynamic flow experiments for Bayesian optimization of a single process objective†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-11 DOI: 10.1039/D4RE00543K

Federico Florit, Kakasaheb Y. Nandiwale, Cameron T. Armstrong, Katharina Grohowalski, Angel R. Diaz, Jason Mustakis, Steven M. Guinness and Klavs F. Jensen

引用次数: 0

Highly efficient and selectivity controllable aerobic oxidation of ethyl lactate to ethyl pyruvate over VxOy/NC catalysts†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-11 DOI: 10.1039/D4RE00465E

Zonghui Liu, Jing Xu, Lei Cui, Na Liu, Bing Yan and Bing Xue

{"title":"Highly efficient and selectivity controllable aerobic oxidation of ethyl lactate to ethyl pyruvate over VxOy/NC catalysts†","authors":"Zonghui Liu, Jing Xu, Lei Cui, Na Liu, Bing Yan and Bing Xue","doi":"10.1039/D4RE00465E","DOIUrl":"https://doi.org/10.1039/D4RE00465E","url":null,"abstract":"Developing effective catalysts for the selective oxidative dehydrogenation of ethyl lactate (EL) to value-added ethyl pyruvate (EP) is of great significance in biomass utilization. Herein, a series of VxOy/NC_P (P denotes the NC precursor) catalysts were synthesized by a convenient impregnation–decomposition method, which can effectively catalyze EL to EP with high activity and stability. These catalysts were characterized by XRD, N2 physisorption, XRF, SEM, TEM, XPS, and H2-TPR in detail. When methenamine was used as the precursor, 98% EL conversion and 99% EP selectivity were achieved at 130 °C for only 0.5 h of the reaction, outperforming most catalysts in the literature. The high activity of VxOy/NC_methenamine is attributed to the presence of a large amount of pyridinic-N and low valence vanadium species. H2-TPR results show that VxOy/NC_methenamine presents the lowest reduction temperature and highest H2 consumption, which is also consistent with the experimental results. Moreover, this catalyst could be reused for at least five cycles without significant deactivation.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 676-685"},"PeriodicalIF":3.4,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489383","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

Thermo-regulating effect of Al–Si microencapsulated phase change material-based catalyst support on ammonia decomposition†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-10 DOI: 10.1039/D4RE00380B

Cholila Tamzysi, Yuto Shimizu, Tomokazu Nakamura, Melbert Jeem, Keita Tanahashi, Takahiro Kawaguchi, Kengo Mimura, Ade Kurniawan and Takahiro Nomura

{"title":"Thermo-regulating effect of Al–Si microencapsulated phase change material-based catalyst support on ammonia decomposition†","authors":"Cholila Tamzysi, Yuto Shimizu, Tomokazu Nakamura, Melbert Jeem, Keita Tanahashi, Takahiro Kawaguchi, Kengo Mimura, Ade Kurniawan and Takahiro Nomura","doi":"10.1039/D4RE00380B","DOIUrl":"https://doi.org/10.1039/D4RE00380B","url":null,"abstract":"Ammonia is important for energy diversification and security due to its ability to transport hydrogen in the form of relatively safe and high-energy-density compounds. Ammonia decomposes into hydrogen and nitrogen gases via a highly endothermic catalytic process. For an endothermic reversible reaction, an undesirable decrease in the reactor temperature shifts the operating line to a lower equilibrium conversion point, resulting in an economic loss for the plant. The objective of this study was to develop a strategy to provide alternative energy to the endothermic reaction during the decrease in temperature. Accordingly, an Al–Si-based microencapsulated phase change material (MEPCM) was used as a heat-regulating catalyst for the ammonia decomposition reaction. The MEPCM structure consists of a spherical oxide shell and metal core that can store thermal energy based on the principle of latent heat storage. Different transition metals, such as Ni, Co, and Fe, were impregnated into the as-prepared 45 μm Al–Si MEPCM catalyst support with a core melting point of 577 °C and heat storage capacity of 285 J g−1. The effects of these metals on the reaction performance were then evaluated. Furthermore, various parameters such as the phase composition, morphology, and thermal properties of the samples were characterized using X-ray diffraction, Brunauer–Emmett–Teller analysis, scanning electron microscopy-energy-dispersive X-ray spectroscopy, and differential scanning calorimetry. Under controlled cooling, the pre-melted core demonstrated heat regulation ability by maintaining a higher temperature and achieving 2–14% higher conversion than the solid core state. By implementing the concept proposed herein, chemical industries can improve their technology to stabilize the reaction temperature.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 593-604"},"PeriodicalIF":3.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489367","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

Competition between ammonia and nitrogen oxides during nitrogen fixation using N2 and H2O plasma without catalysis

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-09 DOI: 10.1039/D4RE00503A

Yuanyuan Wang, Bing Sun, Zhonglin Yu, Shaohua Sun, Jinglin Liu, Yanbin Xin and Xiaomei Zhu

{"title":"Competition between ammonia and nitrogen oxides during nitrogen fixation using N2 and H2O plasma without catalysis","authors":"Yuanyuan Wang, Bing Sun, Zhonglin Yu, Shaohua Sun, Jinglin Liu, Yanbin Xin and Xiaomei Zhu","doi":"10.1039/D4RE00503A","DOIUrl":"https://doi.org/10.1039/D4RE00503A","url":null,"abstract":"The global energy crisis highlights the need for sustainable energy solutions. Nitrogen fixation, converting N2 into valuable products, is gaining attention. In this study, we investigate the effect of water vapor in gas-phase nitrogen fixation via gas–liquid mixed-phase pulsed discharge. Results show that increasing water vapor enhances nitrogen fixation efficiency but introduces a competitive mechanism between NH4+ and NOx. This study examines the effect of water vapor on nitrogen fixation via pulsed discharge at 20 kV and 10 Hz. When water vapor content reached 100%, NH4+ concentration decreased by 49.2%, while NO3− concentration increased by 19%. Additionally, raising the liquid temperature from 6 °C to 80 °C reduced NH4+ by 57.6% and increased NO3− by 54.1%. Spectral diagnostics and radical scavenging experiments confirmed the key role of H and OH radicals in the fixation process. Reaction kinetics analysis further validated the competition between NH4+ and NOx synthesis. While water as a raw material is critical for green nitrogen fixation, its impact on product distribution must be considered in optimizing future applications.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 2","pages":" 466-476"},"PeriodicalIF":3.4,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107525","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

Paper strips loaded with ultrathin gold nanowires: catalytic activity and stability in the p-nitrophenol reduction†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-09 DOI: 10.1039/D4RE00443D

María S. Alvarez Cerimedo, Lucila I. Doumic, Cristina E. Hoppe and María A. Ayude

{"title":"Paper strips loaded with ultrathin gold nanowires: catalytic activity and stability in the p-nitrophenol reduction†","authors":"María S. Alvarez Cerimedo, Lucila I. Doumic, Cristina E. Hoppe and María A. Ayude","doi":"10.1039/D4RE00443D","DOIUrl":"https://doi.org/10.1039/D4RE00443D","url":null,"abstract":"Oleylamine-coated ultrathin gold nanowires (AuNWs) were utilized to create catalytic platforms by simply dropping the colloidal synthesis product onto filter paper strips without additional treatment. These platforms were tested for their ability to catalyze the reduction of p-nitrophenol (p-NP) to p-aminophenol (p-AP) using sodium borohydride as the reducing agent. Reactions were monitored in a stirred batch recycle reactor with in situ spectrophotometric measurements, and kinetic parameters were analyzed using the Langmuir–Hinshelwood model, taking into account the residence time distribution in the experimental setup. The catalytic activity halted when the catalyst was removed, indicating a heterogeneous process with no leaching. The AuNW platforms showed reusability, successfully operating in over 20 cycles with stable activity after the initial 12 cycles. Even after harsh pretreatments, catalytic performance remained acceptable, demonstrating system robustness. The study also examined how operational conditions like p-NP and NaBH4 concentrations, as well as the number of paper strips, affected performance. The increased exposed area from using multiple strips enhanced catalytic activity. These results highlight the potential for scalable and robust industrial use of paper-supported ultrathin AuNWs without extensive washing or pretreatment.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 614-624"},"PeriodicalIF":3.4,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489369","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

Advances in metal/zeolite catalysts for C1–C8 alkane dehydroaromatization 用于 C1-C8 烷烃脱氢芳构化的金属/沸石催化剂的研究进展

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-09 DOI: 10.1039/D4RE00538D

Yi Zhai, Wenqian Li, Qinming Wu, Na Sheng and Feng-Shou Xiao

引用次数: 0

Metallic nickel-anchored biochar with non-metallic heteroatom modification: remarkably effective catalyst for steam reforming of methane†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-09 DOI: 10.1039/D4RE00431K

Yu-e Zhao, Jinxiao Li, Ao Xu, Yulong Liu, Minghui Lian, Jing Zhang, Hexiang Zhong, Chunhua Yang, Rensheng Song and Liwei Pan

{"title":"Metallic nickel-anchored biochar with non-metallic heteroatom modification: remarkably effective catalyst for steam reforming of methane†","authors":"Yu-e Zhao, Jinxiao Li, Ao Xu, Yulong Liu, Minghui Lian, Jing Zhang, Hexiang Zhong, Chunhua Yang, Rensheng Song and Liwei Pan","doi":"10.1039/D4RE00431K","DOIUrl":"https://doi.org/10.1039/D4RE00431K","url":null,"abstract":"In this paper, the effect of H3PO4-activated biochar on nickel-based catalysts for steam methane reforming (SMR) was explored. FTIR, BET, XRD, Raman, TEM, HRTEM, H2-TPR and XPS analyses were used to characterize the supports and catalysts. The results showed that the activation of H3PO4 regulates the pore structure of the support and promotes the development of micropores into mesopores. Meanwhile, H3PO4 introduced more functional groups to promote the dispersion of Ni, which reduced the average particle size of the catalyst from 32 nm to 19 nm. In addition, it increased the number of defects of the catalyst and inhibited carbon deposition during the SMR process, which improved the activity and stability. The catalyst shows best performance at 650 °C, and the CH4 conversion reaches 80.89%. After 80 h, the conversion decreased by only 2%.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 2","pages":" 477-487"},"PeriodicalIF":3.4,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107526","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

Ultrasound-assisted condensation cyclization reaction: fast synthesis of quinazolinones from o-aminobenzamides and aldehydes under ambient conditions† 超声辅助缩合环化反应：在环境条件下从邻氨基苯甲酰胺和醛类快速合成喹唑啉酮类化合物†。

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-09 DOI: 10.1039/D4RE00479E

Xuerou Chen, Siqi Li, Shilong Sun and Wuji Sun

引用次数: 0

Continuous oxidation of toluene derivatives to aromatic aldehydes in an umbrella-shaped microchannel reactor

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-05 DOI: 10.1039/D4RE00484A

Shujin Shi, Yu Fan, Chunsheng Zhao, Yihan Shan, Jiaqi Yan, Anwei Wang, Junfeng Qian, Mingyang He and Weiyou Zhou

{"title":"Continuous oxidation of toluene derivatives to aromatic aldehydes in an umbrella-shaped microchannel reactor","authors":"Shujin Shi, Yu Fan, Chunsheng Zhao, Yihan Shan, Jiaqi Yan, Anwei Wang, Junfeng Qian, Mingyang He and Weiyou Zhou","doi":"10.1039/D4RE00484A","DOIUrl":"https://doi.org/10.1039/D4RE00484A","url":null,"abstract":"In an umbrella-shaped microchannel reactor, the continuous selective aerobic oxidation of toluene derivatives to aromatic aldehydes over a Co/Mn/Br catalytic system using acetic acid/water as the solvent was studied. Taking the oxidation of p-nitrotoluene (PNT) to p-nitrobenzaldehyde (PNBD) as a model, the effects of the Co2+(Mn2+) amount, ratio of Co2+, Mn2+ and Br−, reaction temperature, reaction pressure, oxygen flow rate, residence time and water content on the reaction were systematically investigated. Under the optimized reaction conditions, an 11.8% conversion could be achieved with a good selectivity of 67.1% to PNBD, significantly superior to the results obtained in a kettle reactor. In addition, various toluene derivatives could be tolerated by the present reaction process. This aerobic oxidation over the microchannel reaction technology has the features of an easy-to-operate process and easily controlled reaction parameters, providing an economical and environmentally friendly protocol for the synthesis of aromatic aldehydes.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 605-613"},"PeriodicalIF":3.4,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489368","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

Mechanistic insights into the formation and deconstruction of phenyl glycoside linkages in lignocellulosic biomass†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-04 DOI: 10.1039/D4RE00304G

Seth Beck and Samir H. Mushrif

{"title":"Mechanistic insights into the formation and deconstruction of phenyl glycoside linkages in lignocellulosic biomass†","authors":"Seth Beck and Samir H. Mushrif","doi":"10.1039/D4RE00304G","DOIUrl":"https://doi.org/10.1039/D4RE00304G","url":null,"abstract":"Covalent linkages between lignin and cellulose/hemicellulose, referred to as lignin carbohydrate complexes (LCCs), have been identified to significantly contribute to the refractory nature of lignocellulosic biomass. However, experimental resolution of LCCs is limited, leading to a very limited knowledge of the chemical and structural details of LCCs. As a result, the present work uses first-principles based computational methods to quantify the reaction mechanisms, kinetics and thermodynamics associated with the formation and deconstruction of the prominent phenyl glycoside (PG) LCC linkage in biomass. The two previously proposed formation mechanisms, hemi-acetal and transglycosylation, are associated with significant activation barriers, suggesting these pathways are kinetically limited. A new mechanism is proposed, the electrophilic addition of hemicellulose to a lignin quinone methide (QM) intermediate, that possesses facile kinetics and is exergonic, suggesting it could be the pathway responsible for the significant fraction of PG linkages observed in the native biomass. Moreover, PG formation showed a composition dependence, suggesting that xylans will have higher fractions of PG linkages compared to mannans, explaining why softwoods and hardwoods have different reported types of LCCs. Additionally, the reaction mechanisms, kinetics and thermodynamics associated with the deconstruction of the PG LCC linkages in biomass under acidic conditions are investigated. The chemical degradation of the hemicellulose moieties is the primary competing reaction; however, the deconstruction energetics demonstrate that breaking PG linkages is kinetically and thermodynamically favored in acid catalyzed deconstruction. This indicates that PG linkages may not significantly contribute to the biomass recalcitrance.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 2","pages":" 453-465"},"PeriodicalIF":3.4,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107524","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