Reaction Chemistry & Engineering最新文献_第3页

Boosting the electrocatalytic activity of LaCoO3 core–shell hollow spheres for oxygen evolution reaction through modulating inner oxygen vacancies†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-26 DOI: 10.1039/D4RE00539B

Long Li, Jinbo Guo, Jiang Shen and Qiang Hu

{"title":"Boosting the electrocatalytic activity of LaCoO3 core–shell hollow spheres for oxygen evolution reaction through modulating inner oxygen vacancies†","authors":"Long Li, Jinbo Guo, Jiang Shen and Qiang Hu","doi":"10.1039/D4RE00539B","DOIUrl":"https://doi.org/10.1039/D4RE00539B","url":null,"abstract":"Due to the limited active surface area of perovskite oxides, improving their electrocatalytic performance faces many challenges. To solve this problem, defect engineering and hollow nanostructures have become effective strategies. Therefore, there is an urgent need to develop an efficient synthesis method to prepare LaCoO3 catalysts containing both oxygen vacancies (Vo) and hollow nanostructures. In this study, we successfully synthesized LaCoO3−x core–shell hollow spheres with Vo modification by a solvothermal method which were subsequently heat treated in Ar/H2 atmosphere. It is worth mentioning that by adjusting the calcination time, we can effectively control the degree of Vo. In particular, the high concentration of Vo in LaCoO3 and its unique core–shell hollow structure not only promote the adsorption of water, but also accelerate the transfer of charge, thus giving it excellent electrocatalytic properties. This is demonstrated by the remarkable electrocatalytic activity of LaCoO3−x core–shell spheres for the oxygen evolution reaction (OER) in alkaline solutions with an overpotential of 394 mV and a Tafel slope of 89.1 mV at a current density of 10 mA cm−2 dec−1.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 4","pages":" 917-921"},"PeriodicalIF":3.4,"publicationDate":"2024-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143698411","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

A novel core–shell bimetallic ZrAl-MOF simultaneously boosting electrostatic attraction and ion exchange to eliminate excessive fluoride†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-23 DOI: 10.1039/D4RE00452C

Zhiwei Liu, Jingjing Wang, Qian Liu, Liying Wang, Zhenzhu Cao and Yongfeng Zhang

{"title":"A novel core–shell bimetallic ZrAl-MOF simultaneously boosting electrostatic attraction and ion exchange to eliminate excessive fluoride†","authors":"Zhiwei Liu, Jingjing Wang, Qian Liu, Liying Wang, Zhenzhu Cao and Yongfeng Zhang","doi":"10.1039/D4RE00452C","DOIUrl":"https://doi.org/10.1039/D4RE00452C","url":null,"abstract":"Excess fluoride in drinking water can cause poisoning. To solve this problem, a porous metal–organic framework (MOF) was fabricated via the solvothermal approach and employed for the removal of fluoride ions from water. ZrAl-MOF was fabricated by self-assembly of polyvalent Zr4+, Al3+metal ions and 4,4-biphenyldicarboxylic acid (BPDC). The developed metal-based ZrAl-MOF was used to remove fluoride ions from water and could remove fluoride ions to a maximum of 109.2 mg g−1 (308 K). ZrAl-MOF has a special core–shell structure with a layer of small balls stacked outside and cobweb-like structure inside. The properties of the bimetallic MOF can be adjusted by Zr4+, Al3+ metal ions and BPDC to meet the demand for maximum adsorption performance. Bimetallic MOFs commonly have a substantial specific surface area, capable of providing numerous active sites and being favorable for the adsorption reaction of substances. The electronic properties of different metals may lead to stronger electrostatic attraction and enhanced adsorption of fluoride ions. The factors affecting the adsorption effect, such as solution pH, ZrAl-MOF dosage, reaction time, initial fluoride concentration, temperature, and coexisting anions, were optimized. The fluorine adsorption capacity of ZrAl-MOF was less affected by the adsorbent under acidic conditions and by the presence of sulphate and nitrate ions in the water. In addition, the experimental data were fitted with various adsorption kinetic and isotherm models. It is shown that fluorine adsorption is feasible and spontaneous. The fluorine adsorption mechanism of ZrAl-MOF is mainly electrostatic attraction and ion exchange.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 694-705"},"PeriodicalIF":3.4,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489299","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

Structured internals for the intensified Fischer–Tropsch synthesis in fixed-bed reactors†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-23 DOI: 10.1039/D4RE00550C

Evert Boymans, Yadolah Ganjkhanlou, Marco Denneman, Ben Sutens, Jasper Lefevere and Sander Grootjes

{"title":"Structured internals for the intensified Fischer–Tropsch synthesis in fixed-bed reactors†","authors":"Evert Boymans, Yadolah Ganjkhanlou, Marco Denneman, Ben Sutens, Jasper Lefevere and Sander Grootjes","doi":"10.1039/D4RE00550C","DOIUrl":"https://doi.org/10.1039/D4RE00550C","url":null,"abstract":"To accelerate the energy transition, processes for the production of sustainable fuels are desired such as the conversion of syngas from biogenic residues into liquid fuel by using the Fischer–Tropsch synthesis (FTS). These novel conversion processes are often of smaller scale due to the feedstock for which intensified reactor concepts are required. Structured reactors present viable alternatives to conventional packed bed reactors. Structured reactors can be obtained by e.g. loading a conventional tubular reactor with structured internals. Here, two strategies were followed in an effort to obtain the highest productivity per reactor volume, namely application of 3D-printed catalysts and secondly, thermally conductive aluminium and copper contactors filled with catalyst particles. Superior productivities were obtained by applying Al foam and 3D-printed Cu contactors when packed with FTS catalyst particles, with heat duties of respectively 880 kW m−3 and 1238 kW m−3 compared with only 185 kW m−3 for the 3D-printed catalyst and 218 kW m−3 for a conventional packed bed. For the system using the ordered 3D-printed Cu contactors, it presented a productivity of at least 0.85 gC5+ gcat−1 h−1. The excellent productivities could be correlated to the high thermal conductivity of the metal contactors facilitating the heat transfer from the bed centreline to the reactor wall as revealed by laser flash analysis (LFA) thermal conductivity measurements.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 686-693"},"PeriodicalIF":3.4,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/re/d4re00550c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489384","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

The road to green efficiency: exploration of multicomponent reactions from transition metal catalysis to no catalyst conditions 绿色效率之路：从过渡金属催化到无催化剂条件下的多组分反应探索

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-20 DOI: 10.1039/D4RE00522H

Jie Li, Jiajun Cui, Hongying Guo, Jiyou Yang and Weiwei Huan

引用次数: 0

Correction: Combination of near-infrared spectroscopy and a transient flow method for efficient kinetic analysis of the Claisen rearrangement

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-19 DOI: 10.1039/D4RE90043J

Yoshihiro Takebayashi, Kiwamu Sue and Sho Kataoka

引用次数: 0

Nanostructural investigation of orthogonally stacked mesoporous silica films and their reactivity with phosphate buffer†

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-18 DOI: 10.1039/D4RE00453A

Reo Kimura, Yadong Chai, Rin Nakajima, Kenichiro Kosugi and Motohiro Tagaya

引用次数: 0

On the redox mechanism of methanol carbonylation on a dispersed ReOx/SiO2 catalyst† 关于分散 ReOx/SiO2 催化剂上甲醇羰基化的氧化还原机理†。

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-18 DOI: 10.1039/D4RE00496E

Neil D. Tran and Alexander V. Mironenko

{"title":"On the redox mechanism of methanol carbonylation on a dispersed ReOx/SiO2 catalyst†","authors":"Neil D. Tran and Alexander V. Mironenko","doi":"10.1039/D4RE00496E","DOIUrl":"https://doi.org/10.1039/D4RE00496E","url":null,"abstract":"Acetic acid is industrially produced by methanol carbonylation using Ir- or Rh-based homogeneous catalysts and a corrosive HI promoter. Recently, a heterogeneous catalyst with atomically dispersed ReO4 sites on an inert mesoporous SBA-15 support demonstrated high acetic acid yields and stability without the need for a promoter (J. Qi, J. Finzel, H. Robatjazi, M. Xu, A. S. Hoffman, S. R. Bare, X. Pan and P. Christopher, Selective methanol carbonylation to acetic acid on heterogeneous atomically dispersed ReO4/SiO2 catalysts, J. Am. Chem. Soc., 2020, 142(33), 14178–14189, https://doi.org/10.1021/jacs.0c05026). In this study, we investigate the reaction mechanisms of methanol carbonylation on monopodal –ORe(<img>O)3 sites using density functional theory calculations, natural bond orbital analysis, and the energetic span model. We find that the reduction of dispersed Re(VII) oxide by CO through an indirect mechanism is essential for catalyst activation. The C–C coupling of methyl and carbonyl ligands is favorable in both Re(V) and Re(III) complexes, with Re(III) being superior due to transition state stabilization by a metal-localized lone electron pair. The preceding C–O bond activation is favorable only on Re(V) and leads to a thermodynamic sink, posing challenges in interpreting the high carbonylation activity in terms of monopodal ReOx site catalysis. We hypothesize that multi-nuclear sites or more exotic ligand environments drive the cooperative reaction mechanism of selective carbonylation.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 534-549"},"PeriodicalIF":3.4,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489348","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

Surface-charged β-glucosidase synergizes cellulase for cellulose affinity in ionic liquid pretreated biomass in situ saccharification† 在离子液体预处理的生物质原位糖化过程中，表面带电的β-葡萄糖苷酶可协同纤维素酶提高纤维素亲和力†。

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-16 DOI: 10.1039/D4RE00466C

Yinghui Mu, Xin Ju, Cuiying Hu, Lishi Yan, Jiayi Tian, Su Ma and Liangzhi Li

{"title":"Surface-charged β-glucosidase synergizes cellulase for cellulose affinity in ionic liquid pretreated biomass in situ saccharification†","authors":"Yinghui Mu, Xin Ju, Cuiying Hu, Lishi Yan, Jiayi Tian, Su Ma and Liangzhi Li","doi":"10.1039/D4RE00466C","DOIUrl":"https://doi.org/10.1039/D4RE00466C","url":null,"abstract":"Protein surface charge engineering has promising applications for a deeper understanding of the adsorption and action mechanisms between enzymes and substrates. The engineering modification of β-glucosidase (BGL) is conducive to greatly reducing the negative feedback inhibition in biomass resource utilization and improving the utilization efficiency. Herein, the mutants BGL-14 and BGL-1, which had the largest difference in surface ζ-potential (−12.5 mV and −4.6 mV) obtained by rational design in previous studies, were selected to explore their adsorption behaviors on cellulose and lignin using an adsorption isotherm model. The results showed that more negative charges on the enzyme surface facilitated adsorptive contact with substrates while repelling lignin to reduce competitive adsorption, and that the monolayer coverage might be the main mechanism for cellulose/lignin adsorption of enzyme. Secondly, commercial cellulases were added to the modified BGLs to form a “cocktail” of enzymes (BGL-C) to synergistically participate in the in situ saccharification of biomass pretreated with ionic liquids (ILs). The BGL-14-C synergistic hydrolysis system presented a strong conversion ability in low concentrations of ILs, and its catalytic biomass production of reducing sugars at 5% (v/v) 1-ethyl-3-ethyl-imidazolium diethylphosphate ([EEIM]DEP) reached a yield of 1.24 g L−1, which was 130% and 136% of that of WT-C and BGL-1-C, respectively. BGL-1-C, on the other hand, exhibited higher thermal stability, with the catalytic rate remaining at 51% when the temperature was increased from 50 °C to 70 °C in 1-ethyl-3-methyl-imidazolium diethylphosphate ([EMIM]DEP). Our study delves into the role of enzyme surface charge in reducing unproductive adsorption and increasing the probability of contact with the substrate, providing a theoretical basis for understanding the role of surface charge in mixed systems.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 706-718"},"PeriodicalIF":3.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489300","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

Machine-learning-supported analysis of synergistic extraction systems towards enhanced selectivity of lithium extraction from brines

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-16 DOI: 10.1039/D4RE00439F

Natalia Kireeva, Vladimir E. Baulin and Aslan Yu. Tsivadze

{"title":"Machine-learning-supported analysis of synergistic extraction systems towards enhanced selectivity of lithium extraction from brines","authors":"Natalia Kireeva, Vladimir E. Baulin and Aslan Yu. Tsivadze","doi":"10.1039/D4RE00439F","DOIUrl":"https://doi.org/10.1039/D4RE00439F","url":null,"abstract":"The development of technologies concerned with extraction and separation processes aimed at the sustainable production of rare metals, as well as at metal recycling, is in high demand. This study presents machine-learning-supported analysis of the experimental data on synergistic binary extraction systems for selective extraction of lithium from brines. We consider the narrow class of extraction systems that combine β-diketonate ligands (4,4,4-trifluoro-1-phenyl-1,3-butanedione (HBTA), 2-thenoyl-trifluoroacetone (HTTA), 1-heptyl-3-phenyl-1,3-propanedione (LIX54), 2,2-dimethyl-6,6,7,7,8,8-heptafluoro-3,5-octanedione (HFDOD)) and neutral organophosphorus ligands, such as trioctylphosphine oxide (TOPO), tributyl phosphate (TBP), triphenylphosphine oxide (TPPO) and trialkylphosphine oxide (TRPO). In this study, an analysis of the literature on the synergistic systems published to date was provided. This analysis has allowed distillation of the common characteristics of the formed hydrogen-bond-supported associates for the binary systems investigated to date. These results readily fit into the theory of eutectics and the chemistry of solvation processes. Currently, an urgent goal of the experimental research in this field is the optimization of processes that allow the selective extraction of lithium from brines of various compositions, including brines containing both alkali and alkaline earth metals. The benefits of liquid–liquid extraction and separation methods, which are concerned with the capacity of the corresponding systems to extract target metals from diluted media, require a deep understanding of the processes occurring at the interface of the two immiscible liquid phases, as well as in both the aqueous and organic phases themselves. This allows the recommendation of appropriate compositions of binary systems, along with the corresponding technological parameters of extraction and separation for certain brine compositions, using machine learning.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 625-645"},"PeriodicalIF":3.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489370","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

Effects of Mn promotion on the structure and catalytic performance of Co2C-based catalysts for the Fischer–Tropsch to olefin reaction† 锰的促进对用于费托合成烯烃反应的 Co2C 基催化剂的结构和催化性能的影响†.

IF 3.4 3区化学

Reaction Chemistry & Engineering Pub Date : 2024-12-11 DOI: 10.1039/D4RE00515E

Xinxing Wang, Xuan Zhou, Huachen Shen, Wen Chen, Yunlei An, Yuanyuan Dai and Tiejun Lin

{"title":"Effects of Mn promotion on the structure and catalytic performance of Co2C-based catalysts for the Fischer–Tropsch to olefin reaction†","authors":"Xinxing Wang, Xuan Zhou, Huachen Shen, Wen Chen, Yunlei An, Yuanyuan Dai and Tiejun Lin","doi":"10.1039/D4RE00515E","DOIUrl":"https://doi.org/10.1039/D4RE00515E","url":null,"abstract":"An investigation into the effect of an Mn promoter on the structure and catalytic performance of Co3O4 catalysts for the Fischer–Tropsch to olefin (FTO) reaction was conducted. It was found that the introduction of the Mn promoter into Co3O4 precursors altered the morphology of the catalytic active phase from Co2C nanospheres to Co2C nanoprisms with specifically exposed facets of (101) and (020), which exhibited enhanced activity and C=2–4 selectivity compared to those of Mn-free Co2C nanospheres. Further studies suggested that the Mn promoter could interact with Co to form CoxMn1−xO intermediates, which were readily involved in the formation of Co2C nanoprisms rather than Co2C nanospheres. Additionally, Mn-doping improved CO adsorption capacity, creating a C-rich and H-poor micro-environment around Co2C active sites. As a result, the as-prepared 10Mn/Co3O4 catalyst exhibited the highest activity (25.8 C%) and C=2–4 selectivity (54.1 C%) together with a relatively lower CH4 selectivity (8.5 C%). Moreover, product distribution significantly deviated from classical Anderson–Schulz–Flory (ASF) distribution. However, excessive Mn addition would cover the Co2C active sites, leading to decreased catalytic activity and olefin selectivity.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 3","pages":" 550-560"},"PeriodicalIF":3.4,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489349","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