ChemSusChem最新文献_第8页

Elucidating Carrier Dynamics and Interface Engineering in Sb2S3: Towards Efficient Photoanode for Water Oxidation. Sb2S3的载流子动力学和界面工程研究：迈向水氧化的高效光阳极。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-11 DOI: 10.1002/cssc.202402764

Sudhanshu Shukla, Irene Dei Tos, Angelica Simbula, Julian Guerrero, Thanh Dong, Sownder Subramaniam, Beatriz de la Fuente, Vishal K Jose, Tom Aernouts, Negar Naghavi, Bart Vermang, Yinghuan Kuang

{"title":"Elucidating Carrier Dynamics and Interface Engineering in Sb2S3: Towards Efficient Photoanode for Water Oxidation.","authors":"Sudhanshu Shukla, Irene Dei Tos, Angelica Simbula, Julian Guerrero, Thanh Dong, Sownder Subramaniam, Beatriz de la Fuente, Vishal K Jose, Tom Aernouts, Negar Naghavi, Bart Vermang, Yinghuan Kuang","doi":"10.1002/cssc.202402764","DOIUrl":"https://doi.org/10.1002/cssc.202402764","url":null,"abstract":"Conjugation of low-cost and high-performance semiconductors is essential in solar-driven photoelectrochemical (PEC) energy conversion. Sb2S3 is a wide-bandgap (≈1.7 eV) semiconductor with the potential to deliver a maximum photocurrent density of 24.5 mA cm-2, making it highly attractive for PEC water splitting applications. However, bulk Sb2S3 exhibits intrinsic recombination issues and low electron-hole separation, posing a limit to photocurrent generation. This study clarifies the carrier dynamics by ultrafast spectroscopy measurements and proposes the design of a heterojunction between Sb2S3 and SnO2, with suitable band-edge energy offset. The SnO2/Sb2S3 heterojunction enhances the charge separation efficiency, resulting in improvement of the photocurrent. The SnO2/Sb2S3 photoanode, fabricated entirely by vapor deposition processes, demonstrated photoelectrochemical water oxidation with a photocurrent density up to ca. 3 mA cm-2 at 1.38 V vs RHE.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402764"},"PeriodicalIF":7.5,"publicationDate":"2025-05-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143954891","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Closed-Loop Recyclable Polyhexahydrotriazine Aerogels Utilizing N,N-Dimethyl Lactamide as a Green Solvent. 以N，N-二甲基内酰胺为绿色溶剂的闭环可回收聚六氢三嗪气凝胶。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-10 DOI: 10.1002/cssc.202500125

Chang-Lin Wang, Ivona Glišić, Yi-Ru Chen, Željko Tomović

{"title":"Closed-Loop Recyclable Polyhexahydrotriazine Aerogels Utilizing N,N-Dimethyl Lactamide as a Green Solvent.","authors":"Chang-Lin Wang, Ivona Glišić, Yi-Ru Chen, Željko Tomović","doi":"10.1002/cssc.202500125","DOIUrl":"10.1002/cssc.202500125","url":null,"abstract":"Organic aerogels, known for their lightweight, highly porous structure, and ultralow thermal conductivity, have shown great potential in thermal insulation, chemical absorption, and energy storage. However, most aerogels to date pose environmental concerns, as their permanently cross-linked scaffold makes recycling back to the original monomers virtually impossible. Additionally, the use of toxic solvents in aerogel fabrication raises further environmental and health concerns, challenging their sustainable application. Moreover, the development of next-generation organic aerogels requires the design of recyclable materials with improved mechanical properties. In response to these challenges, this study demonstrates the synthesis of chemically recyclable polyhexahydrotriazine (PHT) aerogels based on an amide containing aromatic diamine, utilizing N,N-dimethyl lactamide, a nontoxic and label-free solvent, as gelation medium. Hansen solubility parameters provide key insights into how solvent choice influences the morphology and properties of PHT aerogels. The resulting PHT aerogels exhibit low bulk density (≈63 mg cm-3), high porosity (≈96%), excellent thermal insulation properties (≈17 mWm-1 K-1), and enhanced mechanical performance, all while being closed-loop recyclable. This work highlights the importance of solvent selection in tuning aerogel properties and demonstrates a green route for fabricating sustainable, high-performance thermal insulating materials.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500125"},"PeriodicalIF":7.5,"publicationDate":"2025-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143958741","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Carbon-Based Catalysts for Electrosynthesis of Hydrogen Peroxide. 电合成过氧化氢的碳基催化剂。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-10 DOI: 10.1002/cssc.202500675

Ting Lv, Huashuo Jin, Zhiyuan Sang, Zhenxin Li, Xia Li, Lin Wang, Shu Cai, Ji Liang, Qin Li, Xiao Yan

{"title":"Carbon-Based Catalysts for Electrosynthesis of Hydrogen Peroxide.","authors":"Ting Lv, Huashuo Jin, Zhiyuan Sang, Zhenxin Li, Xia Li, Lin Wang, Shu Cai, Ji Liang, Qin Li, Xiao Yan","doi":"10.1002/cssc.202500675","DOIUrl":"10.1002/cssc.202500675","url":null,"abstract":"Hydorgen peroxide (H2O2) is an eco-friendly and versatile chemical with extensive applications across various inductrial and househould scenario. Electrosynthesis of H2O2 via the two-electron oxygen reduction reaction (2e- ORR) offers an efficient and sustainable alterantives to conventional anthraquinone process. Carbon-based catalysts have garnered significant attention in this field due to their intrinsic advantages, including cost-effectiveness, structural tunability, high electrical conductivity, and abundant surface active sites. However, achieving industrially viable H2O2 productivity and selectivity demands a holistic optimization strategy encompassing catalyst design, electrode architectures, electrolyte modulation, and reactor configuration. This review systematically examines recent advances in carbon-based catalysts for electrochemical H2O2 generation, addressing fundamental mechanisms of 2e- ORR pathways; controlled synthesis strategies; and system-level optimizations of electrodes, electrolytes and reactors. State-of-the-art in situ/operando characterization techniques and machine learning-driven computational models are highlighted as indispensable tools for unraveling reaction mechanisms and accelerating catalyst discovery. Finally, Challenges and future research directions for advancing carbon-based electrocatalysts toward practical applications are critically discussed.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500675"},"PeriodicalIF":7.5,"publicationDate":"2025-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143959580","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Cobalt Coordinated Thiourea as Metal Organic Framework for Oxygen Evolution and Reduction Reactions and Its Al-Air Battery Applications. 钴配位硫脲作为析氧还原反应的金属有机骨架及其在铝-空气电池中的应用。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-09 DOI: 10.1002/cssc.202500739

Sivanesan Venkatesan, Pandian Ganesan

{"title":"Cobalt Coordinated Thiourea as Metal Organic Framework for Oxygen Evolution and Reduction Reactions and Its Al-Air Battery Applications.","authors":"Sivanesan Venkatesan, Pandian Ganesan","doi":"10.1002/cssc.202500739","DOIUrl":"10.1002/cssc.202500739","url":null,"abstract":"The critical process of fuel cells, metal-air batteries, and electrolyzers are the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR), which inherently have slow kinetics demand an electrocatalyst to enhance reaction rates, performance, and durability. Nonetheless, most nonprecious catalysts undergo heat treatment, involve multiple stages, and struggle with maintaining their active sites. Herein, the active sites is intended to maintain and the synthesis costs is lowered by eliminating the need for heat treatment, leading to the polymerization of cobalt thioamide linkages for a more efficient and durable cobalt thioamide polymer synthesized through a polycondensation. This coordination polymer catalyst is supported on Ketjen Black and exhibited superior OER (Ej10 = 1.57 V) and ORR (E1/2 = 0.71 V) performances. The potential efficiency during long-term durability of this polymer is examined by performing continuous OER operation for 260 h and exhibiting only 5.1% performance decay. For ORR durability, only 39 mV is required after 30 000 cycles in accelerated durability tests compared with the initial cycle. This study highlights the potential of cobalt-coordinated polymer on Ketjen Black as high-performing and durable alternatives to benchmark catalysts for OER and ORR.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500739"},"PeriodicalIF":7.5,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143957982","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Covalent Organic Frameworks-Based Dyads with Highly Exposed Active Sites and Promoted Mass Transfer for Photocatalytic Hydrogen Evolution. 具有高暴露活性位点和促进传质的共价有机骨架二元体光催化析氢。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-09 DOI: 10.1002/cssc.202500551

Ying Lu, Rongjian Sa, Fushuai Zhang, Xiaojuan Sun, Beibei Dong, Ruihu Wang

{"title":"Covalent Organic Frameworks-Based Dyads with Highly Exposed Active Sites and Promoted Mass Transfer for Photocatalytic Hydrogen Evolution.","authors":"Ying Lu, Rongjian Sa, Fushuai Zhang, Xiaojuan Sun, Beibei Dong, Ruihu Wang","doi":"10.1002/cssc.202500551","DOIUrl":"10.1002/cssc.202500551","url":null,"abstract":"Covalent organic frameworks (COFs)-based dyads are emerging photocatalysts in solar-driven hydrogen production, it is crucial to expose active sites and promote mass transfer for promoting photocatalytic efficiency. Herein, surfactant-induced dynamic pore-making strategy to construct noble-metal-free photocatalytic systems by combining the ketoenamine-linked COFs on the surface of spinel-structured CuCo2S4 (CuCo2S4/TpPa-Cl2) is developed. The open hierarchically porous dyads supply rich active sites and enough channels for mass transfer. Hydrogen evolution rate of CuCo2S4/TpPa-Cl2 is as high as 25.56 mmol g-1 h-1 under visible light irradiation, which significantly surpasses those in surfactant-free counterpart (1.63 mmol g-1 h-1) and Pt-loaded TpPa-Cl2 (12.38 mmol g-1 h-1). Apparent quantum efficiency at 420 nm reaches 2.24%. This study presents new protocols for constructing noble-metal-free COFs-based photocatalytic systems with efficient solar energy conversion.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500551"},"PeriodicalIF":7.5,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143951406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Asymmetric Benzene Sulfonamide Sodium Salt Enabling Stable Cycling in Solid-State Sodium Metal Batteries. 不对称苯磺酰胺钠盐在固态金属钠电池中实现稳定循环。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-08 DOI: 10.1002/cssc.202500245

Itziar Aldalur, Jorge Luis Olmedo-Martinez, Lorena Garcia, Asier Fernández De Añastro, Koray Cavusoglu, David Mecerreyes, Alejandro Jesus Müller, Michel Armand, María Martinez-Ibañez

{"title":"Asymmetric Benzene Sulfonamide Sodium Salt Enabling Stable Cycling in Solid-State Sodium Metal Batteries.","authors":"Itziar Aldalur, Jorge Luis Olmedo-Martinez, Lorena Garcia, Asier Fernández De Añastro, Koray Cavusoglu, David Mecerreyes, Alejandro Jesus Müller, Michel Armand, María Martinez-Ibañez","doi":"10.1002/cssc.202500245","DOIUrl":"10.1002/cssc.202500245","url":null,"abstract":"With renewable energy and electric vehicles driving demand, safer and cost-effective alternatives to lithium-ion batteries are being sought. This study explores the development of a novel sodium salt, sodium (benzenesulfonyl)(trifluoromethanesulfonyl) imide (NaBTFSI), for all-solid-state sodium metal batteries (ASSSMBs). NaBTFSI offers a promising electrolyte option by improving sodium-ion transference number ( <math> <semantics> <mrow><msubsup><mi>T</mi> <mrow><mtext>Na</mtext></mrow> <mo>+</mo></msubsup> </mrow> <annotation>$T_{text{Na}}^{&amp;amp;amp;amp;amp;amp;plus;}$</annotation></semantics> </math> ), conductivity, and stability of sodium metal (Na°) anode cycling. When combined with poly(ethylene oxide), NaBTFSI forms safe solid polymer electrolytes with high mechanical strength, effectively mitigating dendrite growth and polarization issues common in sodium anodes. Characterization shows NaBTFSI enhances the electrochemical performance through π-π stacking interactions, which stabilize the polymer matrix and increase ionic conductivity (≈4.0 × 10- 4 S cm-1) at elevated temperatures (70 °C). NaBTFSI-based electrolytes exhibit higher stability with sodium anodes than the conventional sodium bis(trifluoromethanesulfonyl)imide salt, supporting prolonged cycling in Nao||Nao symmetric cells and demonstrating potential for sustainable, high-performance ASSSMBs.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500245"},"PeriodicalIF":7.5,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144053385","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Photocatalytic Coproduction of Diesel Fuel Precursors and H₂ Promoted by [HSO₄ ^-] and Water. [HSO4-]和水催化柴油前驱体和H2的光催化联产。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-08 DOI: 10.1002/cssc.202500208

Shiyang Liu, Weifeng Liu, Nengchao Luo

{"title":"Photocatalytic Coproduction of Diesel Fuel Precursors and H2 Promoted by [HSO4 -] and Water.","authors":"Shiyang Liu, Weifeng Liu, Nengchao Luo","doi":"10.1002/cssc.202500208","DOIUrl":"10.1002/cssc.202500208","url":null,"abstract":"Photocatalytic CC coupling of 2,5-dimethylfuran (DMF) derived from processing lignocellulosic biomasses coproduces drop-in fuels and green hydrogen with a low-carbon footprint. However, the high reaction barrier for CH bond breaking and uphill overall reaction lead to the slow kinetics of DMF coupling. Here, we reveal that [HSO4 -] and water can collaboratively promote the rate-limiting step of the CH bond breaking on the Ru-ZnIn2S4 catalyst. An in-depth study suggests that water mediates hole transfer to the CH bond while [HSO4 -] facilitates electron extraction, thus promoting electron and proton transfer on the Ru-ZnIn2S4 surface. Consequently, photocatalytic DMF coupling over Ru-ZnIn2S4 produces diesel fuel precursors (DFPs) and H2 with benchmarking formation rates of 1.5 g gcatal. -1 h-1 and 9.7 mmol gcatal. -1 h-1, respectively. Moreover, the selectivity of branched-chain DFPs reaches 55%. This work puts forward new insight and strategy for photocatalytic CC coupling for the synthesis of biofuels.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500208"},"PeriodicalIF":7.5,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143958600","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Mechanochemical Activation of NaHCO₃: A Solid CO₂ Surrogate in Carboxylation Reactions. 机械化学活化NaHCO3：在羧化反应中的固体CO2替代物。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-08 DOI: 10.1002/cssc.202500461

Francesco Mele, Andrea Aquilini, Ana Maria Constantin, Francesco Pancrazzi, Lara Righi, Andrea Porcheddu, Raimondo Maggi, Daniele Alessandro Cauzzi, Giovanni Maestri, Elena Motti, Luca Capaldo, Nicola Della Ca'

{"title":"Mechanochemical Activation of NaHCO3: A Solid CO2 Surrogate in Carboxylation Reactions.","authors":"Francesco Mele, Andrea Aquilini, Ana Maria Constantin, Francesco Pancrazzi, Lara Righi, Andrea Porcheddu, Raimondo Maggi, Daniele Alessandro Cauzzi, Giovanni Maestri, Elena Motti, Luca Capaldo, Nicola Della Ca'","doi":"10.1002/cssc.202500461","DOIUrl":"10.1002/cssc.202500461","url":null,"abstract":"Carbon dioxide, a primary driver of global warming, offers a promising feedstock for valuable chemical synthesis. Nonetheless, the reliance on highly pressurized canisters and specialized equipment limits its practical application in fine chemical synthesis. This study explores the innovative use of sodium bicarbonate (NaHCO3) as a safe, solid, on-demand source of CO2 under mechanochemical conditions to perform carboxylation reactions. Two applications of the practical mechanochemical syntheses using sodium bicarbonate are developed: first, the synthesis of cyclic carbamates from propargylic amines is investigated, and second, cyclic organic carbonates are derived from epoxides. The potential of this approach in the pharmaceutical industry is further showcased by demonstrating the solvent-minimized synthesis of pharmaceutically relevant molecules and introducing a 13C-labeling strategy utilizing NaH13CO3.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500461"},"PeriodicalIF":7.5,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143954152","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Carboxyl-Functionalized Sulfonium Additive for Improved Crystallization and Defect Passivation in Ternary Cation Perovskite Solar Cells. 羧基功能化磺酸添加剂用于改善三元阳离子钙钛矿太阳能电池的结晶和缺陷钝化。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-08 DOI: 10.1002/cssc.202500421

Appiagyei Ewusi Mensah, Sanjay Sandhu, Md Mahbubur Rahman, Farihatun Jannat Lima, Francis Kwaku Asiam, Saif Ahmed, Ashok Kumar Kaliamurthy, Muhammad Zain Qamar, Jongdeok Park, Jae-Joon Lee

{"title":"Carboxyl-Functionalized Sulfonium Additive for Improved Crystallization and Defect Passivation in Ternary Cation Perovskite Solar Cells.","authors":"Appiagyei Ewusi Mensah, Sanjay Sandhu, Md Mahbubur Rahman, Farihatun Jannat Lima, Francis Kwaku Asiam, Saif Ahmed, Ashok Kumar Kaliamurthy, Muhammad Zain Qamar, Jongdeok Park, Jae-Joon Lee","doi":"10.1002/cssc.202500421","DOIUrl":"10.1002/cssc.202500421","url":null,"abstract":"This study explores the use of 2-(carboxyethyl) (dimethyl)sulfonium bromide (CDMSBr), a carboxyl-functionalized derivative of trimethylsulfonium (TMS+), as an additive in ternary cation, (Cs0.05FA0.90MA0.05Pb(I0.95Br0.05)3 [CsFAMA]), perovskite solar cells (PSCs) to enhance both stability and photovoltaic performance. In solution, it exhibits a zwitterionic form that controls nucleation and growth of perovskite crystals. It further protonates into CDMS+ during crystallization to facilitate the formation of larger and more uniform grains with better crystallinity. Optimized CsFAMA-based device achieves power conversion efficiency (PCE) of 21.02% (enhancement of 6.54%) at 1-sun condition and 38.79% (enhancement of 9.21%) under low-intensity indoor lighting (1000-lx, LED 5000 K). The dual role of the additive in defect passivation and grain size enhancement contributes to reduced trap density, promoting increased stability of the PSCs. Devices with CDMSBr maintain 88.53% of their initial PCE after 960 h in ambient conditions. These findings highlight the potential of carboxyl-functionalized sulfonium additives, like CDMSBr, to enhance perovskite morphology and stability, advancing the performance and operational durability of PSCs.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500421"},"PeriodicalIF":7.5,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143958032","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 Simple Strategy for Co-Immobilization of NADH-Dependent Enzymes and NADH for Efficient Biocatalysis in Continuous Flow Reactors. 连续流动反应器中NADH依赖酶和NADH高效生物催化的简单共固定策略。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-05-07 DOI: 10.1002/cssc.202500410

Reza Yekta, Xu Xiong, Marianne M Lee, Michael K Chan

{"title":"A Simple Strategy for Co-Immobilization of NADH-Dependent Enzymes and NADH for Efficient Biocatalysis in Continuous Flow Reactors.","authors":"Reza Yekta, Xu Xiong, Marianne M Lee, Michael K Chan","doi":"10.1002/cssc.202500410","DOIUrl":"10.1002/cssc.202500410","url":null,"abstract":"The application of nicotinamide adenine dinucleotide (NAD)(H)-dependent enzymes in continuous flow reactors poses significant challenges due to the high cost of NAD(H) and its inevitable loss during reactor operation. To overcome these limitations, a novel platform comprising Cry3Aa-enzyme fusion particles modified with polyethylenimine (PEI) is developed and its application for two catalytic processes is demonstrated. In the first system, two NAD(H)-dependent enzymes, formate dehydrogenase (FDH), and leucine dehydrogenase (LDH) are genetically co-immobilized within Cry3Aa particles and then modified with PEI to facilitate NADH co-immobilization. To adapt the system for continuous flow reactors, PEI-modified particles are entrapped within agarose beads, loaded with NADH, and then used to catalyze L-tert leucine production under continuous flow conditions for 30 days. This configuration achieved LDH and NADH turnover numbers of 22,196 and 7,202, respectively, and a space-time yield (STY) of 0.0262 g L-1 h-1. This platform is then validated for another NAD(H)-dependent multienzyme system comprised of FDH and alcohol dehydrogenase (ADH) and used for the continuous conversion of ethyl acetoacetate to ethyl-(R)-3-hydroxybutyrate. ADH and NADH turnover numbers of 15,074 and 3,256 are obtained after 30 days with a STY of 0.02 g L-1 h-1. These examples illustrate significant potential of this technology for facilitating NADH-dependent enzyme-mediated biocatalysis in continuous flow reactors.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500410"},"PeriodicalIF":7.5,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143958806","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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