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Programmable Cargo Release from Jet-Printed Microgel Particles via an In Situ Ionic Exchange Method 通过原位离子交换法从喷射打印的微凝胶颗粒中可编程释放货物
Chem & Bio Engineering Pub Date : 2025-04-24 DOI: 10.1021/cbe.5c0001710.1021/cbe.5c00017
Rong Ma, Jihpeng Sun, Sungwan Park, Fiona Nikolla and Albert Tianxiang Liu*, 
{"title":"Programmable Cargo Release from Jet-Printed Microgel Particles via an In Situ Ionic Exchange Method","authors":"Rong Ma,&nbsp;Jihpeng Sun,&nbsp;Sungwan Park,&nbsp;Fiona Nikolla and Albert Tianxiang Liu*,&nbsp;","doi":"10.1021/cbe.5c0001710.1021/cbe.5c00017","DOIUrl":"https://doi.org/10.1021/cbe.5c00017https://doi.org/10.1021/cbe.5c00017","url":null,"abstract":"<p >Hydrogel-based drug delivery systems hold significant clinical potential by enabling precise spatial and temporal control over therapeutic release, ranging from metabolites, macromolecules to other cellular and subcellular constructs. However, achieving programmable release of payloads with diverse molecular weights at distinct rates typically requires complex polymer designs that can compromise the accessibility and biocompatibility of the delivery system. We present a scalable method for producing injectable, micrometer-scale alginate hydrogel particles (microgels) with precisely tuned microstructures for multiplexed, programmable cargo release. Our approach integrates an established jetting technique with a simple postsynthesis ion-exchange process to fine-tune the cross-linked microstructure of alginate microgels. By varying cation type (Ca<sup>2+</sup>, Mg<sup>2+</sup>, Na<sup>+</sup>) and concentration, we systematically modulate the microgels’ chemical and physical properties to control release rates of model compounds, including rhodamine B, methylene blue, and dextrans of various molecular weights. Additionally, a PEG-alginate composite microgel system is used to demonstrate the pre-programmed stepwise release of rhodamine B. These findings offer a straightforward strategy for postsynthetic manipulation of ionic microgels with controllable release performances, paving the way for advanced biomedical applications.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 5","pages":"312–321 312–321"},"PeriodicalIF":0.0,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/cbe.5c00017","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104893","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Programmable Cargo Release from Jet-Printed Microgel Particles via an In Situ Ionic Exchange Method. 通过原位离子交换法从喷射打印的微凝胶颗粒中可编程释放货物。
Chem & Bio Engineering Pub Date : 2025-04-24 eCollection Date: 2025-05-22 DOI: 10.1021/cbe.5c00017
Rong Ma, Jihpeng Sun, Sungwan Park, Fiona Nikolla, Albert Tianxiang Liu
{"title":"Programmable Cargo Release from Jet-Printed Microgel Particles via an In Situ Ionic Exchange Method.","authors":"Rong Ma, Jihpeng Sun, Sungwan Park, Fiona Nikolla, Albert Tianxiang Liu","doi":"10.1021/cbe.5c00017","DOIUrl":"10.1021/cbe.5c00017","url":null,"abstract":"<p><p>Hydrogel-based drug delivery systems hold significant clinical potential by enabling precise spatial and temporal control over therapeutic release, ranging from metabolites, macromolecules to other cellular and subcellular constructs. However, achieving programmable release of payloads with diverse molecular weights at distinct rates typically requires complex polymer designs that can compromise the accessibility and biocompatibility of the delivery system. We present a scalable method for producing injectable, micrometer-scale alginate hydrogel particles (microgels) with precisely tuned microstructures for multiplexed, programmable cargo release. Our approach integrates an established jetting technique with a simple postsynthesis ion-exchange process to fine-tune the cross-linked microstructure of alginate microgels. By varying cation type (Ca<sup>2+</sup>, Mg<sup>2+</sup>, Na<sup>+</sup>) and concentration, we systematically modulate the microgels' chemical and physical properties to control release rates of model compounds, including rhodamine B, methylene blue, and dextrans of various molecular weights. Additionally, a PEG-alginate composite microgel system is used to demonstrate the pre-programmed stepwise release of rhodamine B. These findings offer a straightforward strategy for postsynthetic manipulation of ionic microgels with controllable release performances, paving the way for advanced biomedical applications.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 5","pages":"312-321"},"PeriodicalIF":0.0,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12104843/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144164135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rational Design of Superhydrophobic and Flexible Oriented MOF Nanosheet Membrane for Highly Efficient Ethanol–Water Separation 高效分离乙醇-水的超疏水柔性取向MOF纳米片膜的合理设计
Chem & Bio Engineering Pub Date : 2025-03-28 DOI: 10.1021/cbe.5c0000610.1021/cbe.5c00006
Wei Shao, Xiao-Feng Zhong, Yi-Le Chen, Zhen Chen, Miao-Miao Jia, Wen-Yong Yang, Jing-Ran Yu, Pan-Pan Zhang, Yi Li* and Ming Xue*, 
{"title":"Rational Design of Superhydrophobic and Flexible Oriented MOF Nanosheet Membrane for Highly Efficient Ethanol–Water Separation","authors":"Wei Shao,&nbsp;Xiao-Feng Zhong,&nbsp;Yi-Le Chen,&nbsp;Zhen Chen,&nbsp;Miao-Miao Jia,&nbsp;Wen-Yong Yang,&nbsp;Jing-Ran Yu,&nbsp;Pan-Pan Zhang,&nbsp;Yi Li* and Ming Xue*,&nbsp;","doi":"10.1021/cbe.5c0000610.1021/cbe.5c00006","DOIUrl":"https://doi.org/10.1021/cbe.5c00006https://doi.org/10.1021/cbe.5c00006","url":null,"abstract":"<p >Highly efficient and energy-conserving membrane separation technology holds vast potential for applications in the bioethanol production process. This work reports a strategy for the fast preparation of an oriented and flexible two-dimensional metal–organic framework (MOF) nanosheet membrane by an electrochemical deposition method. The oriented MOF nanosheet membrane growth, followed by spin-coating of polydimethylsiloxane, resulted in an efficiently formed superhydrophobic and ethanol affinity membrane for separating ethanol from aqueous solution. Vertically aligned MOF nanosheets with strong ethanol affinity and superhydrophobic membrane surfaces simultaneously promote the transport process, thus delivering a relatively high flux of 1.63 kg·m<sup>–2</sup>·h<sup>–1</sup> and good separation factor of 14.89 in the pervaporation of 5 wt % ethanol aqueous solution. The oriented arrangement of MOF nanosheets combined with polydimethylsiloxane can significantly enhance the pervaporation selectivity and flux, creating a preferential pathway for the production of biofuel.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 5","pages":"332–340 332–340"},"PeriodicalIF":0.0,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/cbe.5c00006","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104876","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rational Design of Superhydrophobic and Flexible Oriented MOF Nanosheet Membrane for Highly Efficient Ethanol-Water Separation. 高效分离乙醇-水的超疏水柔性取向MOF纳米片膜的合理设计。
Chem & Bio Engineering Pub Date : 2025-03-28 eCollection Date: 2025-05-22 DOI: 10.1021/cbe.5c00006
Wei Shao, Xiao-Feng Zhong, Yi-Le Chen, Zhen Chen, Miao-Miao Jia, Wen-Yong Yang, Jing-Ran Yu, Pan-Pan Zhang, Yi Li, Ming Xue
{"title":"Rational Design of Superhydrophobic and Flexible Oriented MOF Nanosheet Membrane for Highly Efficient Ethanol-Water Separation.","authors":"Wei Shao, Xiao-Feng Zhong, Yi-Le Chen, Zhen Chen, Miao-Miao Jia, Wen-Yong Yang, Jing-Ran Yu, Pan-Pan Zhang, Yi Li, Ming Xue","doi":"10.1021/cbe.5c00006","DOIUrl":"10.1021/cbe.5c00006","url":null,"abstract":"<p><p>Highly efficient and energy-conserving membrane separation technology holds vast potential for applications in the bioethanol production process. This work reports a strategy for the fast preparation of an oriented and flexible two-dimensional metal-organic framework (MOF) nanosheet membrane by an electrochemical deposition method. The oriented MOF nanosheet membrane growth, followed by spin-coating of polydimethylsiloxane, resulted in an efficiently formed superhydrophobic and ethanol affinity membrane for separating ethanol from aqueous solution. Vertically aligned MOF nanosheets with strong ethanol affinity and superhydrophobic membrane surfaces simultaneously promote the transport process, thus delivering a relatively high flux of 1.63 kg·m<sup>-2</sup>·h<sup>-1</sup> and good separation factor of 14.89 in the pervaporation of 5 wt % ethanol aqueous solution. The oriented arrangement of MOF nanosheets combined with polydimethylsiloxane can significantly enhance the pervaporation selectivity and flux, creating a preferential pathway for the production of biofuel.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 5","pages":"332-340"},"PeriodicalIF":0.0,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12104844/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144164164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Light-Controlled Adhesive Hydrogels for On-Demand Adhesion. 用于按需粘合的光控粘合剂水凝胶。
Chem & Bio Engineering Pub Date : 2025-03-26 eCollection Date: 2025-04-24 DOI: 10.1021/cbe.4c00177
Song Yang, Chenxi Qin, Zhizhi Zhang, Ming Zhang, Bin Li, Yanfei Ma, Feng Zhou, Weimin Liu
{"title":"Light-Controlled Adhesive Hydrogels for On-Demand Adhesion.","authors":"Song Yang, Chenxi Qin, Zhizhi Zhang, Ming Zhang, Bin Li, Yanfei Ma, Feng Zhou, Weimin Liu","doi":"10.1021/cbe.4c00177","DOIUrl":"https://doi.org/10.1021/cbe.4c00177","url":null,"abstract":"<p><p>The rapid and reversible adhesion between solids is of great significance, particularly in fields such as biomedicine, intelligent machines, and bioelectronic sensors. Hydrogels, as soft materials, play a vital role in reversible adhesion. To achieve a wider range of applications, it is essential to enhance the intelligence of hydrogels. However, the preparation of reversible adhesive hydrogels with remote control, reversible adhesion, rapid response, and no residue remains a challenge in the field. Herein, we developed a light-controlled reversible adhesive hydrogel by integrating temperature-controlled reversible adhesion with the photothermal response capabilities of Fe<sub>3</sub>O<sub>4</sub>. The hydrogel can adhere/desorb reversibly under temperature control and allows for remote adhesion control using infrared light. Under infrared light irradiation, surface water causes carboxylic acid groups to migrate to the surface, thereby shielding the catechol groups. This results in insufficient adhesive groups at the interface to form interactions with opposing surfaces. Without infrared light irradiation, the adhesive functional groups are exposed, allowing interaction forces to form between the surface with the adhesion groups and the opposing surfaces. This smart hydrogel holds significant potential for future applications in wound dressings, wearable devices, and soft robots.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 4","pages":"253-259"},"PeriodicalIF":0.0,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12035562/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144061263","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Light-Controlled Adhesive Hydrogels for On-Demand Adhesion 用于按需粘合的光控粘合剂水凝胶
Chem & Bio Engineering Pub Date : 2025-03-26 DOI: 10.1021/cbe.4c0017710.1021/cbe.4c00177
Song Yang, Chenxi Qin, Zhizhi Zhang, Ming Zhang, Bin Li*, Yanfei Ma*, Feng Zhou* and Weimin Liu, 
{"title":"Light-Controlled Adhesive Hydrogels for On-Demand Adhesion","authors":"Song Yang,&nbsp;Chenxi Qin,&nbsp;Zhizhi Zhang,&nbsp;Ming Zhang,&nbsp;Bin Li*,&nbsp;Yanfei Ma*,&nbsp;Feng Zhou* and Weimin Liu,&nbsp;","doi":"10.1021/cbe.4c0017710.1021/cbe.4c00177","DOIUrl":"https://doi.org/10.1021/cbe.4c00177https://doi.org/10.1021/cbe.4c00177","url":null,"abstract":"<p >The rapid and reversible adhesion between solids is of great significance, particularly in fields such as biomedicine, intelligent machines, and bioelectronic sensors. Hydrogels, as soft materials, play a vital role in reversible adhesion. To achieve a wider range of applications, it is essential to enhance the intelligence of hydrogels. However, the preparation of reversible adhesive hydrogels with remote control, reversible adhesion, rapid response, and no residue remains a challenge in the field. Herein, we developed a light-controlled reversible adhesive hydrogel by integrating temperature-controlled reversible adhesion with the photothermal response capabilities of Fe<sub>3</sub>O<sub>4</sub>. The hydrogel can adhere/desorb reversibly under temperature control and allows for remote adhesion control using infrared light. Under infrared light irradiation, surface water causes carboxylic acid groups to migrate to the surface, thereby shielding the catechol groups. This results in insufficient adhesive groups at the interface to form interactions with opposing surfaces. Without infrared light irradiation, the adhesive functional groups are exposed, allowing interaction forces to form between the surface with the adhesion groups and the opposing surfaces. This smart hydrogel holds significant potential for future applications in wound dressings, wearable devices, and soft robots.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 4","pages":"253–259 253–259"},"PeriodicalIF":0.0,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/cbe.4c00177","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143863102","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Crystallization-Assisted Asymmetric Synthesis of Enantiopure Amines Using Membrane-Immobilized Transaminase. 膜固定化转氨酶结晶辅助不对称合成对映纯胺。
Chem & Bio Engineering Pub Date : 2025-03-18 eCollection Date: 2025-04-24 DOI: 10.1021/cbe.4c00186
Hippolyte Meersseman Arango, Neal Bachus, Xuan Dieu Linh Nguyen, Basile Bredun, Patricia Luis, Tom Leyssens, David Roura Padrosa, Francesca Paradisi, Damien P Debecker
{"title":"Crystallization-Assisted Asymmetric Synthesis of Enantiopure Amines Using Membrane-Immobilized Transaminase.","authors":"Hippolyte Meersseman Arango, Neal Bachus, Xuan Dieu Linh Nguyen, Basile Bredun, Patricia Luis, Tom Leyssens, David Roura Padrosa, Francesca Paradisi, Damien P Debecker","doi":"10.1021/cbe.4c00186","DOIUrl":"https://doi.org/10.1021/cbe.4c00186","url":null,"abstract":"<p><p>The production of active pharmaceutical ingredients (APIs) requires enantiopure chiral amines, for which greener synthesis processes are needed. Transaminases (TAs) are enzymes that catalyze the enantioselective production of chiral amines from prochiral ketones through transamination under mild conditions. Yet, industrial applications of biocatalytic transamination remain currently hindered by the limited stability of soluble enzymes and by the unfavorable thermodynamic equilibrium of targeted asymmetric reactions. Enzyme immobilization can be applied to address stability, recoverability, and reusability issues. In the perspective of process intensification, we chose to immobilize TAs on polymeric (polypropylene) membranes. In the asymmetric synthesis of (R)-2-fluoro-α-methylbenzylamine ((R)-FMBA), such membrane-immobilized TAs exhibited superior specific activity and stability compared with soluble TAs; they also outperformed TAs immobilized on resins. The reaction yield remained, however, limited by thermodynamics. To further enhance the synthesis yield, the reaction was coupled with the <i>in situ</i> crystallization of (R)-FMBA with 3,3-diphenylpropionic acid (DPPA). By doing so, the theoretical equilibrium conversion was pushed from ∼44% to ∼83%. In fact, a 72% overall recovery yield of crystallized (R)-FMBA was demonstrated. The enantioselectivity of the reaction mixture was preserved. Importantly, purification was greatly facilitated since the target enantiopure amine was readily recovered as high-purity (R)-FMBA:DPPA crystals. The biocatalytic membranes were found to be fully reusable, performing successive high-yield asymmetric syntheses with only minor deactivation. Overall, the crystallization-assisted strategy proposed herein offers a greener path for the biocatalytic production of valuable chiral targets.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 4","pages":"272-282"},"PeriodicalIF":0.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12035565/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144016193","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Applying TiO2–x-Based Electrocatalysis and Photoelectrocatalysis Induced I–/IO3– Recycling for Green and Continuous Ozone Removal 基于tio2 - x的电催化和光电催化诱导I - /IO3 -回收在绿色连续臭氧去除中的应用
Chem & Bio Engineering Pub Date : 2025-03-17 DOI: 10.1021/cbe.4c0018710.1021/cbe.4c00187
Jiahong Liao, Wenyi Wang, Weicheng Tong, Lixia Qiu, Hao Cheng, Xinben Zhao, Yi He, Chunlin Yu* and Xingwang Zhang*, 
{"title":"Applying TiO2–x-Based Electrocatalysis and Photoelectrocatalysis Induced I–/IO3– Recycling for Green and Continuous Ozone Removal","authors":"Jiahong Liao,&nbsp;Wenyi Wang,&nbsp;Weicheng Tong,&nbsp;Lixia Qiu,&nbsp;Hao Cheng,&nbsp;Xinben Zhao,&nbsp;Yi He,&nbsp;Chunlin Yu* and Xingwang Zhang*,&nbsp;","doi":"10.1021/cbe.4c0018710.1021/cbe.4c00187","DOIUrl":"https://doi.org/10.1021/cbe.4c00187https://doi.org/10.1021/cbe.4c00187","url":null,"abstract":"<p >Solution absorption is a straightforward and efficient method for ozone treatment, but waste from inactive absorption solutions poses a risk of secondary pollution and raises the operating cost. Therefore, developing a sustainable recycling process for the absorption solution is essential for green ozone removal. In this study, we constructed a novel I<sup>–</sup>/IO<sub>3</sub><sup>–</sup> cycling system induced by electrocatalysis and photoelectrocatalysis to facilitate the reduction of KIO<sub>3</sub> in KI/KOH ozone absorption solution, thereby enabling absorption solution recycling. The stable operation of this system relies on high-performance cathode materials. By adjusting the concentration of oxygen vacancies on TiO<sub>2</sub>, we reduced the energy barrier for IO<sub>3</sub><sup>–</sup> reduction, optimized IO<sub>3</sub><sup>–</sup> adsorption on the electrode surface, and improved the band gap structure of the electrode material, resulting in a TiO<sub>2–<i>x</i></sub> cathode with good IO<sub>3</sub><sup>–</sup> reduction reaction (IO<sub>3</sub>RR) performance. Notably, this method achieves an ozone removal cost of $3.72 per kilogram, only one-third of the cost associated with conventional catalytic ozone decomposition. This approach provides a promising new direction for green and efficient ozone removal.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 5","pages":"322–331 322–331"},"PeriodicalIF":0.0,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/cbe.4c00187","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104875","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Crystallization-Assisted Asymmetric Synthesis of Enantiopure Amines Using Membrane-Immobilized Transaminase 膜固定化转氨酶结晶辅助不对称合成对映纯胺
Chem & Bio Engineering Pub Date : 2025-03-17 DOI: 10.1021/cbe.4c0018610.1021/cbe.4c00186
Hippolyte Meersseman Arango, Neal Bachus, Xuan Dieu Linh Nguyen, Basile Bredun, Patricia Luis, Tom Leyssens, David Roura Padrosa, Francesca Paradisi and Damien P. Debecker*, 
{"title":"Crystallization-Assisted Asymmetric Synthesis of Enantiopure Amines Using Membrane-Immobilized Transaminase","authors":"Hippolyte Meersseman Arango,&nbsp;Neal Bachus,&nbsp;Xuan Dieu Linh Nguyen,&nbsp;Basile Bredun,&nbsp;Patricia Luis,&nbsp;Tom Leyssens,&nbsp;David Roura Padrosa,&nbsp;Francesca Paradisi and Damien P. Debecker*,&nbsp;","doi":"10.1021/cbe.4c0018610.1021/cbe.4c00186","DOIUrl":"https://doi.org/10.1021/cbe.4c00186https://doi.org/10.1021/cbe.4c00186","url":null,"abstract":"<p >The production of active pharmaceutical ingredients (APIs) requires enantiopure chiral amines, for which greener synthesis processes are needed. Transaminases (TAs) are enzymes that catalyze the enantioselective production of chiral amines from prochiral ketones through transamination under mild conditions. Yet, industrial applications of biocatalytic transamination remain currently hindered by the limited stability of soluble enzymes and by the unfavorable thermodynamic equilibrium of targeted asymmetric reactions. Enzyme immobilization can be applied to address stability, recoverability, and reusability issues. In the perspective of process intensification, we chose to immobilize TAs on polymeric (polypropylene) membranes. In the asymmetric synthesis of (R)-2-fluoro-α-methylbenzylamine ((R)-FMBA), such membrane-immobilized TAs exhibited superior specific activity and stability compared with soluble TAs; they also outperformed TAs immobilized on resins. The reaction yield remained, however, limited by thermodynamics. To further enhance the synthesis yield, the reaction was coupled with the <i>in situ</i> crystallization of (R)-FMBA with 3,3-diphenylpropionic acid (DPPA). By doing so, the theoretical equilibrium conversion was pushed from ∼44% to ∼83%. In fact, a 72% overall recovery yield of crystallized (R)-FMBA was demonstrated. The enantioselectivity of the reaction mixture was preserved. Importantly, purification was greatly facilitated since the target enantiopure amine was readily recovered as high-purity (R)-FMBA:DPPA crystals. The biocatalytic membranes were found to be fully reusable, performing successive high-yield asymmetric syntheses with only minor deactivation. Overall, the crystallization-assisted strategy proposed herein offers a greener path for the biocatalytic production of valuable chiral targets.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 4","pages":"272–282 272–282"},"PeriodicalIF":0.0,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/cbe.4c00186","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143863097","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Applying TiO2-x -Based Electrocatalysis and Photoelectrocatalysis Induced I-/IO3 - Recycling for Green and Continuous Ozone Removal. 基于TiO2-x的电催化和光电催化诱导I-/IO3 -回收在绿色连续臭氧去除中的应用
Chem & Bio Engineering Pub Date : 2025-03-17 eCollection Date: 2025-05-22 DOI: 10.1021/cbe.4c00187
Jiahong Liao, Wenyi Wang, Weicheng Tong, Lixia Qiu, Hao Cheng, Xinben Zhao, Yi He, Chunlin Yu, Xingwang Zhang
{"title":"Applying TiO<sub>2-<i>x</i></sub> -Based Electrocatalysis and Photoelectrocatalysis Induced I<sup>-</sup>/IO<sub>3</sub> <sup>-</sup> Recycling for Green and Continuous Ozone Removal.","authors":"Jiahong Liao, Wenyi Wang, Weicheng Tong, Lixia Qiu, Hao Cheng, Xinben Zhao, Yi He, Chunlin Yu, Xingwang Zhang","doi":"10.1021/cbe.4c00187","DOIUrl":"10.1021/cbe.4c00187","url":null,"abstract":"<p><p>Solution absorption is a straightforward and efficient method for ozone treatment, but waste from inactive absorption solutions poses a risk of secondary pollution and raises the operating cost. Therefore, developing a sustainable recycling process for the absorption solution is essential for green ozone removal. In this study, we constructed a novel I<sup>-</sup>/IO<sub>3</sub> <sup>-</sup> cycling system induced by electrocatalysis and photoelectrocatalysis to facilitate the reduction of KIO<sub>3</sub> in KI/KOH ozone absorption solution, thereby enabling absorption solution recycling. The stable operation of this system relies on high-performance cathode materials. By adjusting the concentration of oxygen vacancies on TiO<sub>2</sub>, we reduced the energy barrier for IO<sub>3</sub> <sup>-</sup> reduction, optimized IO<sub>3</sub> <sup>-</sup> adsorption on the electrode surface, and improved the band gap structure of the electrode material, resulting in a TiO<sub>2-<i>x</i></sub> cathode with good IO<sub>3</sub> <sup>-</sup> reduction reaction (IO<sub>3</sub>RR) performance. Notably, this method achieves an ozone removal cost of $3.72 per kilogram, only one-third of the cost associated with conventional catalytic ozone decomposition. This approach provides a promising new direction for green and efficient ozone removal.</p>","PeriodicalId":100230,"journal":{"name":"Chem & Bio Engineering","volume":"2 5","pages":"322-331"},"PeriodicalIF":0.0,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12104842/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144163901","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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