RSC sustainability最新文献

{"title":"Ti3C2Tx MXene coupled Co(OH)2: a stable electrocatalyst for the hydrogen evolution reaction in alkaline media","authors":"Muhammad Yameen Solangi, Aashiq Ali Lakhair, Farkhanda Zaman Dayo, Rehan Ali Qureshi, Abdulaziz Alhazaa, Muhammad Ali Shar, Abdul Jalil Laghari, Imtiaz Ali Soomro, Muhammad Nazim Lakhan, Abdul Hanan and Umair Aftab","doi":"10.1039/D4SU00392F","DOIUrl":"https://doi.org/10.1039/D4SU00392F","url":null,"abstract":"<p >Green hydrogen (H<small>₂</small>) production <em>via</em> water electrolysis is a promising technique. Within this domain, two dimensional (2D) materials are gaining more attention throughout the world particularly in energy conversion/storage devices due to their unique features. Herein, this study focuses on the development of sustainable, durable, and economical electrocatalysts based on titanium carbide (Ti<small>₃</small>C<small>₂</small>T<small>_<em>x</em></small>) MXene and cobalt hydroxide (Co(OH)<small>₂</small>) as a composite. Ti<small>₃</small>C<small>₂</small>T<small>_<em>x</em></small> has been doped into Co(OH)<small>₂</small> (CT nanostructure) with varying concentrations by the aqueous chemical growth method. The as-prepared electrocatalysts (CT-15 and CT-30) have been investigated through different physicochemical characterization studies including X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), and electrochemical analysis in order to access their morphology, crystalline phase homogeneity, surface functionalization, and electrochemical behaviour for the HER. It is observed that the as-prepared material (CT-30) exhibits superior hydrogen evolution reaction (HER) activity in 1.0 M potassium hydroxide (KOH). The optimised electrocatalyst CT-30 demonstrates an overpotential of 380 mV at a current density of 10 mA cm<small>⁻²</small> with a 99 mV dec<small>⁻¹</small> Tafel slope value, showing fast reaction kinetics. Moreover, it offers a low charge transfer resistance (<em>R</em><small>_ct</small>) accompanied by good stability, high electrochemical active surface area (ECSA), and durability for 30 h, as evident for efficient HER activity. This novel electrocatalyst can contribute to the replacement of noble metal-based electrocatalysts for practical usage in energy conversion/storage systems.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3424-3435"},"PeriodicalIF":0.0,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00392f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565681","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}

{"title":"Fractional precipitation of Ni and Co double salts from lithium-ion battery leachates†","authors":"John R. Klaehn, Meng Shi, Luis A. Diaz, Daniel E. Molina, Reyixiati Repukaiti, Fazlollah Madani Sani, Margaret Lencka, Andre Anderko, Navamoney Arulsamy and Tedd E. Lister","doi":"10.1039/D4SU00303A","DOIUrl":"https://doi.org/10.1039/D4SU00303A","url":null,"abstract":"<p >Alternative sourcing of critical metals from lithium-ion batteries (LIBs) is necessary to secure the future supplies of Li, Ni, and Co. Most recovery processes of LIBs utilize pyrometallurgical and hydrometallurgical methodologies; however, these processes to recycle LIB cathode/anode materials can require several steps to isolate the desired metals. We have developed a facile isolation of the valued metals, where Ni and Co will co-crystallize as a sulfate double salt, called Tutton's salt [(NH<small>₄</small>)<small>₂</small>Ni/Co(SO<small>₄</small>)<small>₂</small>·6H<small>₂</small>O]. Thermodynamic modelling of these Ni(<small>II</small>)/Co(<small>II</small>) sulfate double salts shows that Ni is less soluble than Co which could enhance the separation of Ni and Co from electrochemical (EC) leachates. This calculated difference between Ni and Co can be controlled further by temperature and ammonium sulfate concentration. Here, Ni-rich sulfate double salts were achieved at 30–45 °C while Co-rich sulfate double salts were formed at 2–9 °C, where 99% Ni and 89% Co were recovered from the EC-leach solution. Further tests with the leachate solution show that crystallization occurs above pH 2 which allows for higher pulp density leachates. Chemical analyses and single crystal X-ray characterization confirm that the Ni-rich sulfate double salts contain Ni and Co. However, the Co-rich sulfate double salts have ∼30% Mn(<small>II</small>) in the crystal lattice with ∼37% of Ni. As a result, this process reduces the total number of steps to isolate the desired metals while also reducing chemical waste generation and without employing organic solvents.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3298-3310"},"PeriodicalIF":0.0,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00303a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565695","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}

{"title":"The FAIR principles as a key enabler to operationalize safe and sustainable by design approaches","authors":"Achilleas Karakoltzidis, Chiara Laura Battistelli, Cecilia Bossa, Evert A. Bouman, Irantzu Garmendia Aguirre, Ivo Iavicoli, Maryam Zare Jeddi, Spyros Karakitsios, Veruscka Leso, Magnus Løfstedt, Barbara Magagna, Denis Sarigiannis, Erik Schultes, Lya G. Soeteman-Hernández, Vrishali Subramanian and Penny Nymark","doi":"10.1039/D4SU00171K","DOIUrl":"https://doi.org/10.1039/D4SU00171K","url":null,"abstract":"<p >Safe and sustainable development of chemicals, (advanced) materials, and products is at the heart of achieving a healthy future environment in line with the European Green Deal and the Chemicals Strategy for Sustainability. Recently, the Joint Research Center (JRC) of the European Commission (EC) developed the safe and sustainable by design (SSbD) framework for definition of criteria and evaluation procedure proposed to be established in Research and Innovation (R&amp;I) activities. The framework aims to support the design of chemicals, materials and products that provide desirable functions (or services), while simultaneously minimizing the risk for harmful impacts to human health and the environment. While many industrial sectors already consider such aspects during R&amp;I, the framework aims to harmonize safety and sustainability assessment across diverse sectors and innovation strategies to meet the mentioned overarching policy goals. A cornerstone to successfully implement and operationalize the SSbD framework lies in the availability of high-quality data and tools, and their interoperability, aspects which also play a key role in ensuring transparency and thereby trust in the assessment outcomes. Availability of data and tools depend on their machine-actionability in terms of findability, accessibility, interoperability, and reusability, in line with the FAIR principles. The principles were developed in order to harmonize digitalization across all data domains, supporting unanticipated data-driven “seamless” integration of information and generation of new knowledge. Here we discuss the essentiality of FAIR data and tools to operationalize SSbD providing views and examples of activities within the European Partnership for the Assessment of Risks from Chemicals (PARC). The discussion covers five areas previously brought up in relation to the SSbD framework, and which are highly dependent on implementation of the FAIR principles; (i) digitalization to leverage innovation towards a green transition; (ii) existing data sources and their interoperability; (iii) navigating SSbD with data from new scientific developments (iv) transparency and trust through automated assessment of data quality and uncertainty; and (v) “seamless” integration of SSbD tools.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3464-3477"},"PeriodicalIF":0.0,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00171k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565740","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}

{"title":"Low-water-permeability foils based on bio-renewable cellulose derivatives†","authors":"Tanner J. Hickman, Li Tao, Natalie Stingelin and J. Carson Meredith","doi":"10.1039/D4SU00425F","DOIUrl":"https://doi.org/10.1039/D4SU00425F","url":null,"abstract":"<p >Packaging is one of the largest contributors to plastic waste. Hence, polymers produced from renewable sources have become attractive to substitute or fully replace petroleum-based plastics in packaging materials. However, the properties of some of the prime candidates—<em>e.g.</em>, cellulose and its derivatives—rapidly deteriorate already at a modest relative humidity rendering them impractical for use in packaging products. Here, we show by the example of carboxymethyl cellulose that chemical crosslinking with citric acid can be exploited to precisely control the moisture sensitivity of cellulose-based structures. Specifically, we demonstrate that the water vapor transmission rate (WVTR) of carboxymethyl cellulose can be manipulated in a controlled fashion over three orders of magnitude. Thereby, the lowest WVTR value, obtained for an optimal crosslinker content, is one order of magnitude lower than that measured for poly(ethylene terephthalate) even at a relatively humidity of up to 65%. Our work, thus, clearly illustrates that cellulose-based materials can be made insensitive to humidity, which is not only of great importance for providing a solution towards more sustainable plastic packaging but, generally, for expanding the scope of applications of cellulose and its derivatives, allowing us to leverage their natural abundance, chemical versatility, and biodegradability.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3451-3455"},"PeriodicalIF":0.0,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00425f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565738","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}

{"title":"Acyloxy, sulfate, and phosphate radicals as hydrogen atom transfer (HAT) agents for direct C(sp3)–H functionalization","authors":"Jia-Lin Tu and Binbin Huang","doi":"10.1039/D4SU00520A","DOIUrl":"https://doi.org/10.1039/D4SU00520A","url":null,"abstract":"<p >Selective activation of inert and ubiquitous C(sp<small>³</small>)–H bonds has long been a challenging task in organic synthesis, through which chemists can directly synthesize value-added compounds from inexpensive and readily available alkane feedstocks. By means of modern photochemistry, electrochemistry, as well as traditional thermochemistry, diverse hydrogen atom transfer (HAT) protocols have been established, employing various radicals, especially oxygen-centered ones, as the HAT agents. This review focuses on three unique classes of oxygen radicals, namely acyloxy, sulfate, and phosphate radicals, which have demonstrated significant potential for achieving direct intermolecular C(sp<small>³</small>)–H bond functionalization <em>via</em> HAT pathways. By focusing on the key developments from 2014 to 2024, this review discusses the generation mechanisms, reactivity characteristics and applications of these acid-related oxygen radicals, aiming to provide researchers with insights to further advance the techniques and innovations in the future C(sp<small>³</small>)–H functionalization strategy development.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3222-3234"},"PeriodicalIF":0.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00520a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565676","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}

{"title":"Incorporating biochar to make hydrogel composites with improved structural properties, valorized from waste-paper mill sludge and forestry residues using energy efficient protocols†","authors":"Keerthana Ketheeswaran, Shegufta Shetranjiwalla, Manokararajah Krishnapillai and Lakshman Galagedara","doi":"10.1039/D4SU00332B","DOIUrl":"https://doi.org/10.1039/D4SU00332B","url":null,"abstract":"<p >The transformation of waste-paper mill sludge into high-value materials with minimized chemical and energy consumption addresses the 12th United Nations Sustainable Development Goal, Responsible Consumption and Production. In this study, cellulose was recovered from dewatered sludge (DS), procured from a local paper mill, using energy-efficient microwave and ultrasonication techniques. Crosslinked hydrogel composites were synthesized from the recovered cellulose and citric acid, as agricultural amendments to optimize water consumption. Powdered biochar (BC) was incorporated into the crosslinked hydrogels, as a biocompatible filler to further enhance thermal stability and water retention. Four hydrogel composite samples were prepared containing BC compositions of 0 g (CH), 0.5 g (BH0.5), 1 g (BH1.0) and 1.5 g (BH1.5). The physicochemical composition, functional groups, thermal stability, water retention, gel fraction, and degradation rate of the extracted cellulose (EC) and prepared hydrogel composites were compared. The energy-efficient extraction process successfully yielded a high EC yield (81.5%) with a cellulose fraction of 93.8% compared to the raw DS at 66.6%, resulting in a conversion efficiency of 140.8%. Incorporating 1 g BC into the hydrogel matrix (BH1.0) improved water absorbency by 992% over CH. Water retention for the hydrogel composites enhanced in the order of BH1.0 &gt; CH &gt; BH0.5 &gt; BH1.5. BC addition also improved the gel fraction, and the thermal stability of the composites increased by up to 60%. Biodegradation studies using the soil burial method showed that cellulose-biochar composites degraded by 40% in 50 days, exhibiting promising potential as agricultural amendments for podzolic soils in the northern boreal ecosystem.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3478-3489"},"PeriodicalIF":0.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00332b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565741","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}

{"title":"A cobalt-based metal–organic framework as a sustainable catalyst for base-free transfer hydrogenation of biomass-derived carbonyl compounds†","authors":"Aashish, Ruchika Gupta and Rajeev Gupta","doi":"10.1039/D4SU00368C","DOIUrl":"https://doi.org/10.1039/D4SU00368C","url":null,"abstract":"<p >A bifunctional cobalt-based MOF <strong>1</strong>, offering both Lewis acidic–basic (Co and –OH<small>⁻</small>) and Brønsted acidic (–COOH) sites, has been synthesized and characterized. MOF <strong>1</strong> presents a double-chain structure and, therefore, remarkably exposed Lewis acidic–basic and Brønsted acidic sites. MOF <strong>1</strong> acts as a remarkable heterogeneous catalyst for the transfer hydrogenation (TH) of carbonyl compounds using isopropanol as a green hydrogen source without the requirement of any base. MOF <strong>1</strong> exhibits excellent catalytic performance for the TH of assorted aldehydes and ketones, resulting in high yield and excellent selectivity. Notably, several biomass-derived substrates such as furfural, 5-methylfurfural, 5-hydroxymethylfurfural, and levulinic acid were successively converted to their corresponding products in high yield. The substrate scope further encompassed biologically relevant ones such as vanillin, cinnamaldehyde, perillaldehyde, and estrone. Subsequently, both poisoning experiments and temperature-programmed desorption studies were employed to elucidate the role of Lewis acidic–basic and Brønsted acidic sites in this MOF. To further evaluate the role of Brønsted acidic sites in TH, an ester derivative of MOF, <strong>1-Et</strong>, was synthesized and utilized which exhibited a poor catalytic performance. Collectively, all experiments confirm a cooperative effect of Lewis acidic–basic (Co and –OH<small>⁻</small>) and Brønsted acidic (–COOH) sites in TH catalysis. The entire catalytic process encompassing reagents, solvents, and operating conditions, was assessed using the CHEM21 green metrics toolkit to highlight the environmental sustainability of the present catalytic method. The MOF <strong>1</strong> overcomes the limitations of conventional catalysts by excluding the need for a base, offering a broad substrate scope, and achieving high yield with excellent selectivity, thus acting as a more efficient and sustainable catalyst for TH reaction.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 11","pages":" 3409-3423"},"PeriodicalIF":0.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00368c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142565680","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}

{"title":"Clay mineral-based sustainable snow contaminant remediation technology†","authors":"Benilde Mizero, Saba Naderi, Sandeep Bose, Houjie Li and Parisa A. Ariya","doi":"10.1039/D4SU00155A","DOIUrl":"https://doi.org/10.1039/D4SU00155A","url":null,"abstract":"<p >Seasonal snow covers up to 33% of the Earth's surface. Fresh falling snow serves as a snapshot of atmospheric processes and can take up pollutants. Once deposited, snow can affect the Earth's radiation and climate change, and its melting and accumulation processes can affect human health. Little has been done for snow pollution remediation, especially regarding emerging materials and nano/microplastics in urban regions. We present a sustainable, cost-effective snow remediation filtering system made of multilayer clay-based minerals, specifically kaolin and montmorillonite, capable of removing nano/micro-contaminants from snow. In addition, a recycled metallic mesh with various pore sizes, including nano/micro size, can remove substantial snow contaminants. Using a suite of technologies including high-resolution S/TEM, Pelletier ice nucleation counter, NALDI mass spectrometry, Photoacoustic Extinctiometer (PAX), triple quad ICP-MS/MS, and TOC counter, we found that the clay-mineral setup is highly efficient. For instance, it removes metallic species (&gt;95%), plastic micro/nanoparticles like polyethylene glycol and polyethylene (&gt;99%), black carbon (&gt;93%), and total organic carbon (&gt;50%) from dirty snow sampled in the primary snow depository in downtown Montreal. This sustainable and inexpensive method is promising for significantly reducing the environmental impact of snow pollutants, improving current snow remediation practices in urban areas, decreasing the re-emission of contaminants in air, soil, and water leaching, and improving the ecosystem and human health.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 10","pages":" 3123-3138"},"PeriodicalIF":0.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00155a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142368718","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}

{"title":"Towards green visible range active photocatalytic Au/TiO2 nanocomposites through rutin-based synthesis and their application in the degradation of ciprofloxacin†","authors":"Inês Catarina Gomes Espada, Noelia González-Ballesteros, Carlos J. Tavares, Senentxu Lanceros-Méndez and Pedro M. Martins","doi":"10.1039/D4SU00186A","DOIUrl":"https://doi.org/10.1039/D4SU00186A","url":null,"abstract":"<p >Photocatalysis is a low-cost solution to efficiently remove resilient emergent pollutants from wastewater with complex chemical structures, such as pharmaceuticals. Titanium dioxide (TiO<small>₂</small>) is the most studied photocatalyst and is usually functionalised with gold (Au) nanoparticles to prevent electron–hole pair recombination and extend visible radiation absorption. However, conventional synthesis techniques use toxic chemicals and present high energy consumption. The focus of this work is to present and optimize a green synthesis method using the flavonoid rutin – a natural compound found in various plants – as the reducing agent at room temperature to decrease the environmental impact and optimise the chemical, physical, and photocatalytic properties of Au/TiO<small>₂</small> nanoparticles with concentrations of Au of 0.025, 0.1, and 1 wt%. Through ciprofloxacin (CIP) degradation under UV and simulated solar radiation, enhanced photocatalytic efficiency is observed due to adding Au nanoparticles, proving that rutin is a suitable reducing agent for green nanoparticle synthesis.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 10","pages":" 3090-3099"},"PeriodicalIF":0.0,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00186a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142368716","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}

{"title":"Membrane-immobilized transaminases for the synthesis of enantiopure amines†","authors":"Hippolyte Meersseman Arango, Xuan Dieu Linh Nguyen, Patricia Luis, Tom Leyssens, David Roura Padrosa, Francesca Paradisi and Damien P. Debecker","doi":"10.1039/D4SU00293H","DOIUrl":"10.1039/D4SU00293H","url":null,"abstract":"<p >For the manufacture of enantiopure amines, greener synthesis processes are needed. Transaminases (TAs) are able to produce chiral amines with excellent enantioselectivity and in mild conditions, and can be immobilized to target stability, recoverability, and reusability. In the perspective of process intensification, we propose to study TA immobilization onto polymeric membranes. Two main immobilization strategies were investigated, requiring prior membrane surface functionalization. On the one hand, a polyacrylonitrile (PAN) membrane surface was partially hydrolyzed and coated with polyethyleneimine (PEI) to electrostatically trap TAs. On the second hand, a polypropylene (PP) membrane was coated with polydopamine (PDA), which was subsequently modified with glycerol diglycidyl ether (GDE) in order to covalently graft TAs. The successful membrane functionalization was confirmed by surface characterization techniques (infrared spectroscopy, X-ray photoelectron spectroscopy, contact angle measurements, and scanning electron microscopy). Enzyme leaching was observed from the functionalized PAN membrane, highlighting the need to post-treat the reversibly immobilized TAs to improve their anchoring. The covalent coupling of TAs with PEI using glutaraldehyde (GA) was found highly effective to avoid leaching and to increase the enzyme loading, without affecting the specific activity of the biocatalyst. Similarly, the covalent grafting of TA onto functionalized PP membranes yielded very efficient biocatalysts (retaining 85% specific activity with respect to soluble TA) displaying perfect recyclability throughout successive cycles. Immobilizing either the S-selective HeWT or the R-selective TsRTA resulted in robust heterogeneous biocatalysts with antagonist enantioselectivities. Thus, chiral amine synthesis can be performed effectively with biocatalytic membranes, which paves the way to intensified continuous flow synthesis processes.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":" 10","pages":" 3139-3152"},"PeriodicalIF":0.0,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00293h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142262094","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}