Yujue Du, Wende Hu, Yuanlin Cheng, Chuan-Ming Wang, Weimin Yang
Isolated single metal site within zeolite exhibits promising catalytic performances towards propane dehydrogenation (PDH), while the underlying relationship between the local structure of intrinsic site and the catalytic behavior remains elusive. Herein, the possible structures, relative stabilities and catalytic performances of three isolated single metal cations (M2+, M is Cu, Ni, or Co) within ZSM-5 zeolite were theoretically investigated by combining density functional theory calculations and microkinetic simulations. Both the extra-framework site and the framework-embedded site were taken into account for the sitting of single metal cation. The isolated divalent M2+ sites are more stable than the corresponding univalent MOH+ sites and both kinds of structures display distinct dependence of stability on temperature. The stepwise pathway rather than the concerted pathway is followed for the direct PDH under the reaction conditions of 853 K. Microkinetic simulations reveal that the PDH activity increases in the sequence of Co < Ni < Cu within the same local environment of active site. At the framework-embedded site, the divalent M2+ cations exhibit higher catalytic activity compared to the univalent MOH+ cations; on the contrary, the MOH+ motifs are more active than the divalent M2+ ones at the extra-framework site. It seems that the dissociative adsorption enthalpy of propane on isolated metal sites can be utilized to describe the PDH activity variation with different metal cations. The simulated results demonstrate that the framework-embedded single Cu site derived from silanol nest within ZSM-5 zeolite exhibits outstanding PDH activity, while may suffer from the weakness of stability. This work thus highlights the importance of local environment of single metal active site within zeolites and may open up novel avenue for the screening of high-performance catalysts towards the PDH reaction.
{"title":"Propane dehydrogenation on extra-framework and framework-embedded metal site within ZSM-5 zeolite from first-principles microkinetic simulations","authors":"Yujue Du, Wende Hu, Yuanlin Cheng, Chuan-Ming Wang, Weimin Yang","doi":"10.1039/d4re00269e","DOIUrl":"https://doi.org/10.1039/d4re00269e","url":null,"abstract":"Isolated single metal site within zeolite exhibits promising catalytic performances towards propane dehydrogenation (PDH), while the underlying relationship between the local structure of intrinsic site and the catalytic behavior remains elusive. Herein, the possible structures, relative stabilities and catalytic performances of three isolated single metal cations (M2+, M is Cu, Ni, or Co) within ZSM-5 zeolite were theoretically investigated by combining density functional theory calculations and microkinetic simulations. Both the extra-framework site and the framework-embedded site were taken into account for the sitting of single metal cation. The isolated divalent M2+ sites are more stable than the corresponding univalent MOH+ sites and both kinds of structures display distinct dependence of stability on temperature. The stepwise pathway rather than the concerted pathway is followed for the direct PDH under the reaction conditions of 853 K. Microkinetic simulations reveal that the PDH activity increases in the sequence of Co < Ni < Cu within the same local environment of active site. At the framework-embedded site, the divalent M2+ cations exhibit higher catalytic activity compared to the univalent MOH+ cations; on the contrary, the MOH+ motifs are more active than the divalent M2+ ones at the extra-framework site. It seems that the dissociative adsorption enthalpy of propane on isolated metal sites can be utilized to describe the PDH activity variation with different metal cations. The simulated results demonstrate that the framework-embedded single Cu site derived from silanol nest within ZSM-5 zeolite exhibits outstanding PDH activity, while may suffer from the weakness of stability. This work thus highlights the importance of local environment of single metal active site within zeolites and may open up novel avenue for the screening of high-performance catalysts towards the PDH reaction.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141885125","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}
Andrea du Preez, Andre Strydom, Derek Ndinteh, Elize Smit
Iron oxide nanoparticles (IONPs) are used in various applications, including magnetic solid phase extraction (MSPE), due to advantages such as excellent adsorption efficiency and easy separation from varied matrices using an external magnet. Here we introduce a low-cost 3D-printed modular flow system for the automated synthesis of phenyl-functionalized silica-coated iron oxide nanoparticles. This system consists of 3D-printed polypropylene (PP) reactors with varying geometries connected in series to synthesize bare IONPs, silica-coated IONPs, or phenyl-functionalized silica-coated IONPs using laminar flow regimes. The simplicity, affordability, robustness, and customizability of the system were illustrated. The synthesized IONPs were characterized using Fourier transform infrared (FTIR) spectroscopy, transmission electron microscopy (TEM), zeta potential, powder X-ray diffraction (XRD), thermogravimetric analysis (TGA) and vibrating sample magnetometry (VSM). The continuous flow system resulted in fast reactions under ambient conditions, with a production rate of approximately 5 mg/min. The produced IONPs were small (~10 nm), resulting in a larger surface-to-volume ratio. Furthermore, the synthesized IONPs retained large enough saturation magnetization values, which together with larger surface-to-volume ratios, is ideal for MSPE.
{"title":"Modular 3D printed flow system for efficient one-step synthesis of phenyl-functionalised silica-coated superparamagnetic iron oxide nanoparticles","authors":"Andrea du Preez, Andre Strydom, Derek Ndinteh, Elize Smit","doi":"10.1039/d4re00242c","DOIUrl":"https://doi.org/10.1039/d4re00242c","url":null,"abstract":"Iron oxide nanoparticles (IONPs) are used in various applications, including magnetic solid phase extraction (MSPE), due to advantages such as excellent adsorption efficiency and easy separation from varied matrices using an external magnet. Here we introduce a low-cost 3D-printed modular flow system for the automated synthesis of phenyl-functionalized silica-coated iron oxide nanoparticles. This system consists of 3D-printed polypropylene (PP) reactors with varying geometries connected in series to synthesize bare IONPs, silica-coated IONPs, or phenyl-functionalized silica-coated IONPs using laminar flow regimes. The simplicity, affordability, robustness, and customizability of the system were illustrated. The synthesized IONPs were characterized using Fourier transform infrared (FTIR) spectroscopy, transmission electron microscopy (TEM), zeta potential, powder X-ray diffraction (XRD), thermogravimetric analysis (TGA) and vibrating sample magnetometry (VSM). The continuous flow system resulted in fast reactions under ambient conditions, with a production rate of approximately 5 mg/min. The produced IONPs were small (~10 nm), resulting in a larger surface-to-volume ratio. Furthermore, the synthesized IONPs retained large enough saturation magnetization values, which together with larger surface-to-volume ratios, is ideal for MSPE.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141885123","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}
Correction for ‘Parameter investigation of an organic–inorganic hybrid resin for a 3D-printed microchannel heat exchanger’ by Sunjae Lee et al., React. Chem. Eng., 2024, 9, 2089–2097, https://doi.org/10.1039/D3RE00694H.
对 Sunjae Lee 等人在 React.Chem.Eng.，2024，9，2089-2097，https://doi.org/10.1039/D3RE00694H。
{"title":"Correction: Parameter investigation of an organic–inorganic hybrid resin for a 3D-printed microchannel heat exchanger","authors":"Sunjae Lee, Amirreza Mottafegh and Dong-Pyo Kim","doi":"10.1039/D4RE90029D","DOIUrl":"10.1039/D4RE90029D","url":null,"abstract":"<p >Correction for ‘Parameter investigation of an organic–inorganic hybrid resin for a 3D-printed microchannel heat exchanger’ by Sunjae Lee <em>et al.</em>, <em>React. Chem. Eng.</em>, 2024, <strong>9</strong>, 2089–2097, https://doi.org/10.1039/D3RE00694H.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.4,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/re/d4re90029d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141885122","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}
Denis O. Kuleshov, Ivan A. Gromov, Ilya I. Pikovskoi, Alexandra A. Onuchina, Ilya S. Voronov, Dmitrii M. Mazur, Albert T. Lebedev
The advent of ambient mass spectrometry has yielded novel approaches to chemical transformations for analytical and preparative applications. These methods utilize the microdroplets generated via spray ionization techniques. Numerous studies have demonstrated the superior efficiency of microdroplet-based chemical reactions. This efficiency is manifested in a substantial acceleration of reactions (up to a million-fold compared to bulk reactions) and a shift in reaction pathways, enabling the synthesis of compounds that are challenging to obtain using conventional methods. However, the widespread implementation of this approach has been hindered by its limited productivity. To address this challenge, this paper introduces a microdroplet chemical reactor prototype (MCR prototype) that employs multiplexed pneumatic/electrospray to enhance productivity. The performance of the MCR prototype was evaluated using the cyclohexanone phenylhydrazone synthesis reaction from phenylhydrazine and cyclohexanone in methanol as a model system. The prototype demonstrated a significant acceleration of the reaction relative to its occurrence in bulk, with the apparent acceleration factor (AAF) exceeding a value of 83 × 106. The MCR prototype can spray the reaction mixture at a rate of up to 17 mL min−1 while maintaining the acceleration effect, achieving a productivity of grams per hour. This prototype offers a promising solution for addressing practical and research challenges in microdroplet chemical synthesis.
{"title":"Microdroplet chemical reactor prototype based on multiplexed electrospray","authors":"Denis O. Kuleshov, Ivan A. Gromov, Ilya I. Pikovskoi, Alexandra A. Onuchina, Ilya S. Voronov, Dmitrii M. Mazur, Albert T. Lebedev","doi":"10.1039/d4re00264d","DOIUrl":"https://doi.org/10.1039/d4re00264d","url":null,"abstract":"The advent of ambient mass spectrometry has yielded novel approaches to chemical transformations for analytical and preparative applications. These methods utilize the microdroplets generated <em>via</em> spray ionization techniques. Numerous studies have demonstrated the superior efficiency of microdroplet-based chemical reactions. This efficiency is manifested in a substantial acceleration of reactions (up to a million-fold compared to bulk reactions) and a shift in reaction pathways, enabling the synthesis of compounds that are challenging to obtain using conventional methods. However, the widespread implementation of this approach has been hindered by its limited productivity. To address this challenge, this paper introduces a microdroplet chemical reactor prototype (MCR prototype) that employs multiplexed pneumatic/electrospray to enhance productivity. The performance of the MCR prototype was evaluated using the cyclohexanone phenylhydrazone synthesis reaction from phenylhydrazine and cyclohexanone in methanol as a model system. The prototype demonstrated a significant acceleration of the reaction relative to its occurrence in bulk, with the apparent acceleration factor (AAF) exceeding a value of 83 × 10<small><sup>6</sup></small>. The MCR prototype can spray the reaction mixture at a rate of up to 17 mL min<small><sup>−1</sup></small> while maintaining the acceleration effect, achieving a productivity of grams per hour. This prototype offers a promising solution for addressing practical and research challenges in microdroplet chemical synthesis.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141885124","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}
Iman Moshiritabrizi, Jonathan P. McMullen, Brian M. Wyvratt, Kimberley B. McAuley
A mechanistic model is developed to study the formation of 2,6-difluoropurine-9-THP from starting material 2,6-dichloropurine-9-THP. The 2,6-difluoropurine-9-THP product is an intermediate used in the synthesis of islatravir (MK-8591), a therapy for treatment of HIV. Kinetic parameters are estimated from 26 batch reactor experiments. An error-in-variables-model (EVM) approach is used for parameter estimation to address uncertainty in initial concentrations of trimethylamine (TMA), a gaseous reagent. A parameter subset selection method is used to determine that 33 out of 39 model parameters should be estimated along with 26 uncertain initial concentrations. The remaining six parameters are kept at their initial values to prevent overfitting of available data. EVM parameter estimates are compared with estimates obtained using a traditional weighted-least-squares approach that neglects input uncertainties. The EVM estimates provide a better fit to the data and, as shown using cross-validation, improved accuracy for model predictions. The resulting model and EVM parameter values are used to find reactor conditions that maximize product yield while obeying constraints on temperature, the initial ratio of TMA to starting material, batch time, and the volume of solvent. An optimal yield of 92.04% is predicted, which is higher than the yield of 90.26% at the best experimental conditions in the data set. Contour plots are used to highlight the insensitivity of the optimal yield to batch time and solvent volume, indicating that a yield of 91.83% could be obtained using a 50% lower batch time and 33% less solvent.
{"title":"Process knowledge for drug substance production via kinetic modeling, parameter estimability analysis and reaction optimization","authors":"Iman Moshiritabrizi, Jonathan P. McMullen, Brian M. Wyvratt, Kimberley B. McAuley","doi":"10.1039/d4re00210e","DOIUrl":"https://doi.org/10.1039/d4re00210e","url":null,"abstract":"A mechanistic model is developed to study the formation of 2,6-difluoropurine-9-THP from starting material 2,6-dichloropurine-9-THP. The 2,6-difluoropurine-9-THP product is an intermediate used in the synthesis of islatravir (MK-8591), a therapy for treatment of HIV. Kinetic parameters are estimated from 26 batch reactor experiments. An error-in-variables-model (EVM) approach is used for parameter estimation to address uncertainty in initial concentrations of trimethylamine (TMA), a gaseous reagent. A parameter subset selection method is used to determine that 33 out of 39 model parameters should be estimated along with 26 uncertain initial concentrations. The remaining six parameters are kept at their initial values to prevent overfitting of available data. EVM parameter estimates are compared with estimates obtained using a traditional weighted-least-squares approach that neglects input uncertainties. The EVM estimates provide a better fit to the data and, as shown using cross-validation, improved accuracy for model predictions. The resulting model and EVM parameter values are used to find reactor conditions that maximize product yield while obeying constraints on temperature, the initial ratio of TMA to starting material, batch time, and the volume of solvent. An optimal yield of 92.04% is predicted, which is higher than the yield of 90.26% at the best experimental conditions in the data set. Contour plots are used to highlight the insensitivity of the optimal yield to batch time and solvent volume, indicating that a yield of 91.83% could be obtained using a 50% lower batch time and 33% less solvent.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141885126","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}
The conversion of CO2 into high value-added chemicals is receiving increasing attention from the scientific community, commercial enterprises, and policymakers due to environmental problems like global warming. Herein, the metal-free quaternized boronate esters (QBE1-QBE8) were prepared and then used as potential efficient metal-free catalysts for the chemical valorization of CO2 to organic cyclic carbonates in solvent-free and under sustainable green atmospheric and high-pressure conditions (1 atm or 1.6 MPa, 100 oC, 2 h) as an alternative to toxic reagents such as phosgene. Analyzes performed with various spectroscopic tools (1H, 13C, and 11B NMR, FT-IR, UV-Vis, LC-MS/MS, elemental analysis, and melting point measurement together with thermal gravimetric analysis (TGA-DTA)) revealed that the targeted quaternized boronate esters were successfully synthesized. After that, the Lewis acidity of the synthesized quaternized boronate esters was investigated by the traditional Gutmann-Beckett method and found to range from 53.72 to 50.47 ppm, respectively. In the presence of 0.1 mol% metal-free quaternized boronate esters (QBE3) and 0.2 mol% co-catalyst DMAP, 4-chloromethyl-1,3-dioxalan-2-one was obtained as cyclic carbonate in 51.7% yield at 1 atm and 100 oC and then under 1.6 MPa and 100 °C in an excellent 94.9% yield with 97.9% selectivity in 2 h, allowing to facilitate the fixation of CO2 into cyclic carbonates rapidly. According to the catalytic findings, the optimum Cat./ECH ratio for CO2 cycloaddition reactions is 1/1000.
{"title":"Evaluating metal-free quaternized boronate esters as efficient catalysts for the fixation of CO2 with epoxide to form cyclic carbonates under suitable conditions","authors":"Ahmet Kilic, Eyyup Yasar, Emine Aytar","doi":"10.1039/d4re00282b","DOIUrl":"https://doi.org/10.1039/d4re00282b","url":null,"abstract":"The conversion of CO2 into high value-added chemicals is receiving increasing attention from the scientific community, commercial enterprises, and policymakers due to environmental problems like global warming. Herein, the metal-free quaternized boronate esters (QBE1-QBE8) were prepared and then used as potential efficient metal-free catalysts for the chemical valorization of CO2 to organic cyclic carbonates in solvent-free and under sustainable green atmospheric and high-pressure conditions (1 atm or 1.6 MPa, 100 oC, 2 h) as an alternative to toxic reagents such as phosgene. Analyzes performed with various spectroscopic tools (1H, 13C, and 11B NMR, FT-IR, UV-Vis, LC-MS/MS, elemental analysis, and melting point measurement together with thermal gravimetric analysis (TGA-DTA)) revealed that the targeted quaternized boronate esters were successfully synthesized. After that, the Lewis acidity of the synthesized quaternized boronate esters was investigated by the traditional Gutmann-Beckett method and found to range from 53.72 to 50.47 ppm, respectively. In the presence of 0.1 mol% metal-free quaternized boronate esters (QBE3) and 0.2 mol% co-catalyst DMAP, 4-chloromethyl-1,3-dioxalan-2-one was obtained as cyclic carbonate in 51.7% yield at 1 atm and 100 oC and then under 1.6 MPa and 100 °C in an excellent 94.9% yield with 97.9% selectivity in 2 h, allowing to facilitate the fixation of CO2 into cyclic carbonates rapidly. According to the catalytic findings, the optimum Cat./ECH ratio for CO2 cycloaddition reactions is 1/1000.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141862697","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}
The dissociation micro-states (DMSs) of an $N$-protic acid are described using set theory notation, which facilitates the mathematical description of the dissociation micro-equilibrium (DME). In particular, the DME constants are easily obtained in terms of the dissociation equilibrium constants and the molar fractions of the DMSs. Representing of the DMEs in terms of graph theory allows to identify permutations between DMSs that preserve the vertex-edge connectivity of the graph. These permutations, along with their compositions, led to the identification of the direct product $C_2times S_N$ of the cyclic group $C_2$, and the symmetric group $S_N$, as the graph automorphism group of the microdissociation of $N$-protic acids for $N=1,2,dots,6$. In this context the microdissociations are associated with the $C_2$ group while the tautomerizations are related to the $S_N$ group.
{"title":"The graph automorphism group of the dissociation microequilibrium of polyprotic acids","authors":"Nicolás Salas, Justin López, Carlos Arango","doi":"10.1039/d4re00271g","DOIUrl":"https://doi.org/10.1039/d4re00271g","url":null,"abstract":"The dissociation micro-states (DMSs) of an $N$-protic acid are described using set theory notation, which facilitates the mathematical description of the dissociation micro-equilibrium (DME). In particular, the DME constants are easily obtained in terms of the dissociation equilibrium constants and the molar fractions of the DMSs. Representing of the DMEs in terms of graph theory allows to identify permutations between DMSs that preserve the vertex-edge connectivity of the graph. These permutations, along with their compositions, led to the identification of the direct product $C_2times S_N$ of the cyclic group $C_2$, and the symmetric group $S_N$, as the graph automorphism group of the microdissociation of $N$-protic acids for $N=1,2,dots,6$. In this context the microdissociations are associated with the $C_2$ group while the tautomerizations are related to the $S_N$ group.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141862701","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}
Africa has a double burden of communicable and non-communicable diseases that account for 26 % of the global disease burden. Pharmaceutical medicines are a critical component in treating these diseases, however, only 3 % of the global drug production is carried out in Africa, which results in limited access to medicines. The local active pharmaceutical ingredient (API) manufacturing industry is not well-established, Africa hugely depends on imports. As such, the need for establishing local API manufacturing capability is obvious. In this review, we highlight the efforts and hurdles in the local manufacture of APIs and recommend sustainable ways to establishing local continuous flow API manufacturing capability. Continuous flow manufacture is an innovative and enabling technology platform which is increasingly impacting pharmaceutical industry. Africa can leverage continuous flow technology to establish a state-of-the-art, sustainable, competitive local API manufacturing industry. Although this approach is noble, it is not without its challenges. Some of the current challenges for the full-scale implementation of continuous flow manufacturing in Africa include the lack of pilot scale or demonstration facilities to bridge the chasm between research and commercialization, inadequate funding, prohibitive infrastructure costs and scarcity of skilled local talents with knowledge and expertise in modern manufacturing techniques. To put things into perspective, the review also showcases all examples where continuous flow technology has been successfully applied in API syntheses within the African continent exclusively. The grand vision is to contribute towards the transformation of Africa into an innovation-led, technology-based and knowledge-based continent through the adoption of cutting edge innovative and enabling technologies that can transform the local pharmaceutical industry into a responsive industry that meets the continental health security, social, economic and political needs pursuant to African Union’s Agenda 2063, Sustainable Development Goal 3 (SDG3) and the Universal Health Coverage (UHC) goals.
{"title":"Towards Continuous Flow Manufacturing of Active Pharmaceutical Ingredients in Africa: A Perspective","authors":"Sinazo Nqeketo, Cloudius Sagandira","doi":"10.1039/d4re00299g","DOIUrl":"https://doi.org/10.1039/d4re00299g","url":null,"abstract":"Africa has a double burden of communicable and non-communicable diseases that account for 26 % of the global disease burden. Pharmaceutical medicines are a critical component in treating these diseases, however, only 3 % of the global drug production is carried out in Africa, which results in limited access to medicines. The local active pharmaceutical ingredient (API) manufacturing industry is not well-established, Africa hugely depends on imports. As such, the need for establishing local API manufacturing capability is obvious. In this review, we highlight the efforts and hurdles in the local manufacture of APIs and recommend sustainable ways to establishing local continuous flow API manufacturing capability. Continuous flow manufacture is an innovative and enabling technology platform which is increasingly impacting pharmaceutical industry. Africa can leverage continuous flow technology to establish a state-of-the-art, sustainable, competitive local API manufacturing industry. Although this approach is noble, it is not without its challenges. Some of the current challenges for the full-scale implementation of continuous flow manufacturing in Africa include the lack of pilot scale or demonstration facilities to bridge the chasm between research and commercialization, inadequate funding, prohibitive infrastructure costs and scarcity of skilled local talents with knowledge and expertise in modern manufacturing techniques. To put things into perspective, the review also showcases all examples where continuous flow technology has been successfully applied in API syntheses within the African continent exclusively. The grand vision is to contribute towards the transformation of Africa into an innovation-led, technology-based and knowledge-based continent through the adoption of cutting edge innovative and enabling technologies that can transform the local pharmaceutical industry into a responsive industry that meets the continental health security, social, economic and political needs pursuant to African Union’s Agenda 2063, Sustainable Development Goal 3 (SDG3) and the Universal Health Coverage (UHC) goals.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141862698","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}
With the outburst in the proven exploitation of offshore oil as well as the prevenient decelerating of the consumption for auto fuels (gasoline and diesel), the technique of transforming oil into chemicals reveals enormous promise to boost the imminent industry transition. Herein, we proposed a novel route for maximizing chemicals from offshore crude oil by one-step leap (OCOCC). Within the innovative patented two-stage riser reactor, it is capable of executing diverse refining scenarios. A multi-objective optimization strategy was employed to conduct molecular-level modeling procedures. Furthermore, the case study of integrated offshore green wind power and seawater desalination in the OCOCC process is also executed. The results indicated that the integrated OCOCC process could expeditiously convert offshore paraffin-based crude oil into ethene and propene beyond 40 wt% and highlight outstanding finance, social, people's life, and ecological behavior. These discernments could energetically influence the technique enhancement, as well as optimization.
{"title":"Computer-aided multi-objective optimization integrated with multi-dimensional assessment for the offshore oil to chemical process","authors":"Xin Zhou, Zhibo Zhang, Huibing Shi, Deming Zhao, Yaowei Wang, Hao Yan, Hui Zhao, Yibin Liu, Haiyan Luo, Weitao Zhang, Xiaobo Chen, Lianying Wu, Chao He Yang","doi":"10.1039/d4re00219a","DOIUrl":"https://doi.org/10.1039/d4re00219a","url":null,"abstract":"With the outburst in the proven exploitation of offshore oil as well as the prevenient decelerating of the consumption for auto fuels (gasoline and diesel), the technique of transforming oil into chemicals reveals enormous promise to boost the imminent industry transition. Herein, we proposed a novel route for maximizing chemicals from offshore crude oil by one-step leap (OCOCC). Within the innovative patented two-stage riser reactor, it is capable of executing diverse refining scenarios. A multi-objective optimization strategy was employed to conduct molecular-level modeling procedures. Furthermore, the case study of integrated offshore green wind power and seawater desalination in the OCOCC process is also executed. The results indicated that the integrated OCOCC process could expeditiously convert offshore paraffin-based crude oil into ethene and propene beyond 40 wt% and highlight outstanding finance, social, people's life, and ecological behavior. These discernments could energetically influence the technique enhancement, as well as optimization.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141862702","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}
Tamara S. Kharlamova, Konstantin L. Timofeev, Denis P. Morilov, Mikhail A. Salaev, Andrey I. Stadnichenko, Olga A. Stonkus, Olga Vodyankina
Preparation of catalysts with predesigned composition, structure and distribution of active species is an important challenge as such characteristics determine the catalytic performance. This work introduces a strategy to rationally designing effective catalysts for the selective HMF oxidation to FDCA under mild conditions. We show the effect of the preparation technique (impregnation, deposition-precipitation, impregnation-reduction) on the active species formation in ZrO2-supported Au, Pd, and AuPd catalysts, discuss the effects of the metal dispersion and state on the catalyst performance and provide insight into reaction pathways of aerobic HMF oxidation over bimetallic AuPd/ZrO2 catalysts. The impregnation-reduction allows preparing the active mono- and bimetallic catalysts in contrast to other techniques used, with the bimetallic formulations featuring the enhanced catalyst performance caused by the synergistic effect. The alloyed Au0.56Pd0.44/ZrO2 catalyst shows a per-site TOF of 0.25 s-1 that is ~4 times higher than the one for the Au/ZrO2 catalysts.
{"title":"Design strategy for effective supported Au-Pd catalysts for selective oxidation of 5-hydroxymethylfurfural under mild conditions","authors":"Tamara S. Kharlamova, Konstantin L. Timofeev, Denis P. Morilov, Mikhail A. Salaev, Andrey I. Stadnichenko, Olga A. Stonkus, Olga Vodyankina","doi":"10.1039/d4re00355a","DOIUrl":"https://doi.org/10.1039/d4re00355a","url":null,"abstract":"Preparation of catalysts with predesigned composition, structure and distribution of active species is an important challenge as such characteristics determine the catalytic performance. This work introduces a strategy to rationally designing effective catalysts for the selective HMF oxidation to FDCA under mild conditions. We show the effect of the preparation technique (impregnation, deposition-precipitation, impregnation-reduction) on the active species formation in ZrO2-supported Au, Pd, and AuPd catalysts, discuss the effects of the metal dispersion and state on the catalyst performance and provide insight into reaction pathways of aerobic HMF oxidation over bimetallic AuPd/ZrO2 catalysts. The impregnation-reduction allows preparing the active mono- and bimetallic catalysts in contrast to other techniques used, with the bimetallic formulations featuring the enhanced catalyst performance caused by the synergistic effect. The alloyed Au0.56Pd0.44/ZrO2 catalyst shows a per-site TOF of 0.25 s-1 that is ~4 times higher than the one for the Au/ZrO2 catalysts.","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141862700","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}
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