ACS Sustainable Chemistry & Engineering最新文献

{"title":"Sustainable and General Production of Carboxylated Cellulose Nanocrystals via Synergistic Lewis-Acid/Organic-Acid Hydrolysis under Ambient Conditions","authors":"Junjie Zhou,&nbsp;, ,&nbsp;Somia Yassin Hussain Abdalkarim,&nbsp;, ,&nbsp;Xuefei Chen,&nbsp;, and ,&nbsp;Hou-Yong Yu*,&nbsp;","doi":"10.1021/acssuschemeng.5c08214","DOIUrl":"10.1021/acssuschemeng.5c08214","url":null,"abstract":"<p >Cellulose nanocrystals (CNCs) stand out as promising biobased nanomaterials owing to their nanoscale dimensions, abundant surface groups, and excellent reinforcement capabilities in polymer composites. However, traditional preparation methods rely on harsh mineral acids, raising environmental and thermal stability concerns. In this work, a chloride/citric acid system of ZnCl₂ or FeCl₃ with citric acid (CA) was employed as a comparative platform to investigate the distinct roles of acid-catalyzed and oxidative hydrolysis in the preparation of carboxylated CNCs under mild conditions. The contrasting Lewis acidity and oxidative behavior of ZnCl₂ and FeCl₃ enabled mechanistic insights into their hydrolytic pathways, while alkaline pretreatment of cellulose further amplified these differences. Carboxylated CNCs produced with ZnCl₂ exhibited markedly better thermal stability. Mild alkaline pretreatment was further introduced to improve molecular accessibility, significantly enhancing surface carboxylation. Carboxylated CNCs prepared via the ZnCl₂/CA system with alkaline pretreatment demonstrated excellent thermal stability (<i>T</i>_max = 375.0 °C), substantial carboxyl content (1.3 mmol/g), and exceptional yield (89.2%). The generality of this method was validated across multiple cellulose sources, highlighting its potential as a sustainable and efficient alternative to conventional acid hydrolysis for CNCs preparation.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 38","pages":"16192–16203"},"PeriodicalIF":7.3,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145073030","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Engineering the Distal Loci of SAM Synthase for High-Yield Synthesis of SAM Using Whole-Cell Catalysis","authors":"Haowei Huang,&nbsp;, ,&nbsp;Qiulin Liu,&nbsp;, ,&nbsp;Wenhan Xiao,&nbsp;, ,&nbsp;Qiqi Kang,&nbsp;, ,&nbsp;Dejing Yin,&nbsp;, ,&nbsp;Jianguo Xu,&nbsp;, ,&nbsp;Xiaomei Zhang,&nbsp;, ,&nbsp;Jinsong Gong,&nbsp;, ,&nbsp;Guoqiang Xu*,&nbsp;, ,&nbsp;Zhenming Lu,&nbsp;, ,&nbsp;Jinsong Shi,&nbsp;, and ,&nbsp;Zhenghong Xu,&nbsp;","doi":"10.1021/acssuschemeng.5c04717","DOIUrl":"10.1021/acssuschemeng.5c04717","url":null,"abstract":"<p ><i>S</i>-adenosyl methionine (SAM) is a vital metabolic intermediate with wide applications ranging from medicine to agriculture. The high-yield synthesis of SAM in <i>Escherichia coli</i> using whole-cell catalysis offers many advantages, including environmental friendliness. However, the heterologous expression of SAM synthase (SAM2) from <i>Saccharomyces cerevisiae</i> in <i>E. coli</i> mainly suffers from low enzymatic activity. In this study, we propose a novel molecular design strategy targeting distal sites to address these limitations. When combined with expression optimization, this strategy enabled the development of a highly efficient <i>E. coli</i> whole-cell catalytic system. Through distal site engineering, an I189 V/V266H double mutant was designed and obtained, which resulted in a 1353.08% increase in enzymatic activity, a substantial improvement in thermal stability, and a 524.62% enhancement in whole-cell catalytic yield. Molecular dynamics simulations and structural analysis revealed that the distal site mutations synergistically enhanced the enzyme structural stability and optimized substrate binding. Using a green feeding strategy (45 mM ATP), the system achieved a conversion rate of 91.3% within 12 h at an <i>E. coli</i> OD₆₀₀ of 60, yielding 16.39 g/L of SAM─the highest production reported to date. Ion-exchange resin-based separation and purification yielded a SAM recovery rate of up to 82.5% and a product purity exceeding 95%. This work not only pioneers a distal site-based molecular design for SAM synthetase modification and establishes an integrated whole-cell catalytic synthesis system, but also provides a promising green and sustainable strategy for the high-yield synthesis of SAM and SAM-dependent chemicals.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 38","pages":"15859–15874"},"PeriodicalIF":7.3,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145073020","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Effect of the Ferrite Phase on Phase Evolution and Hydration Properties in Quaternary Phase–Ferrite Phase (QF) Low-Carbon Clinkers","authors":"Minwang Lv,&nbsp;, ,&nbsp;Lu Yang*,&nbsp;, ,&nbsp;Fazhou Wang,&nbsp;, and ,&nbsp;Shuguang Hu,&nbsp;","doi":"10.1021/acssuschemeng.5c04757","DOIUrl":"10.1021/acssuschemeng.5c04757","url":null,"abstract":"<p >To promote the sustainable development and efficient utilization of high-alumina cement clinkers, this study designed a binary composite clinker consisting of the quaternary (Q) phase (Ca₂₀Al₂₆Mg₃Si₃O₆₈) and the ferrite phase. The effects of ferrite content (10–30 wt %) on clinker synthesis, hydration kinetics, and mechanical properties were systematically investigated using multiple characterization techniques. The results indicate that the incorporation of ferrite facilitates the formation of the Q phase at lower temperatures, reducing energy consumption during sintering; however, it induces partial decomposition to C₁₂A₇ above 1300 °C, necessitating precise temperature control for phase stability. Hydration tests reveal that an appropriate ferrite content (10–20%) effectively optimizes the hydration process: it not only mitigates early stage rapid hydration, reducing the risk of heat accumulation, but also significantly enhances mid-to-late-stage hydration activity, contributing to sustained strength development. The low-calcium composition reduces limestone consumption, enabling over 30% theoretical carbon reduction compared to that of ordinary Portland cement. This discovery advances the sustainability-driven design of high-performance, low-carbon cementitious materials via ecofriendly phase engineering.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 38","pages":"15897–15911"},"PeriodicalIF":7.3,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145073027","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Thermally-Induced in Situ Synthesis of Ethylene-Linked Viologen Ionic Radical Polymers for Photocatalytic CO2 Cycloaddition","authors":"Shuo Wang,&nbsp;, ,&nbsp;Qing Shi,&nbsp;, ,&nbsp;Yulong Lin,&nbsp;, ,&nbsp;Juan Chen,&nbsp;, ,&nbsp;Yunjie Mao,&nbsp;, ,&nbsp;Xiaomeng Bai,&nbsp;, ,&nbsp;Jinfeng Yu,&nbsp;, ,&nbsp;Yanli Gai,&nbsp;, ,&nbsp;Zhouyang Long,&nbsp;, and ,&nbsp;Guojian Chen*,&nbsp;","doi":"10.1021/acssuschemeng.5c02952","DOIUrl":"10.1021/acssuschemeng.5c02952","url":null,"abstract":"<p >This study presents a facile one-pot quaternization strategy for constructing conjugated ethylene-linked viologen ionic radical polymers (designated as EVIRPs) to enable visible-light-enhanced photocatalytic CO₂ cycloaddition under ambient conditions. The optimized polymer EVIRP-180 was synthesized by thermally induced <i>in situ</i> quaternization between commercially available monomers 1,2-bis(4-pyridyl)ethylene (BPE) and 1,2,4,5-tetrakis(bromomethyl)benzene (TBMB) in the high-boiling-point solvent <i>N</i>-methylpyrrolidone (NMP) at 180 °C for 24 h without requiring external catalysts and reducing agents. Remarkably, electron paramagnetic resonance (EPR) spectroscopy and X-ray photoelectron spectroscopy (XPS) analyses revealed a temperature-dependent enhancement of radical intensity, with EVIRP-180 exhibiting stronger radical signals compared to the control polymers EVIRP-100 and EVIRP-140 prepared at lower temperatures (100 and 140 °C, respectively). This phenomenon arises from two synergistic effects: (1) a higher temperature promotes the formation of more ethylene-linked viologen ionic radicals via a thermally induced process; (2) the solvent NMP can be partially converted into activated NMP (denoted as NMP*) at elevated temperatures, which serves as an effective reducing agent for facilitating one-electron reduction of viologen dications to cationic radicals. The optimized polymer EVIRP-180 demonstrated an enhanced visible-light-harvesting ability and superior photoinduced charge transfer capability. As a metal-free heterogeneous photocatalyst, EVIRP-180 achieved exceptional photocatalytic efficiency in the photocatalytic cycloaddition of CO₂ and epoxides to cyclic carbonates under ambient conditions (room temperature, atmospheric pressure) without using cocatalysts or solvents. This work establishes a sustainable pathway for developing multifunctional ionic radical polymers as efficient photocatalysts for CO₂ conversion under ambient conditions.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 38","pages":"15805–15816"},"PeriodicalIF":7.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145073047","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Corecycling of Granular Steel Slag and Phosphogypsum for Preparing Sustainable Cement Clinker via Fusion Adhering Calcined Technique","authors":"Deqiang Zhao,&nbsp;, ,&nbsp;Weiguo Shen*,&nbsp;, ,&nbsp;Angeles G. De la Torre,&nbsp;, ,&nbsp;Piqi Zhao*,&nbsp;, ,&nbsp;Dongbing Jiang,&nbsp;, and ,&nbsp;Xin Cheng,&nbsp;","doi":"10.1021/acssuschemeng.5c06060","DOIUrl":"10.1021/acssuschemeng.5c06060","url":null,"abstract":"<p >The large-scale stockpiling of steel slag and phosphogypsum (PG) is a global challenge in industrial solid waste management. Direct utilization of granular steel slag for preparing steel slag fusion adhering calcined (SFAC) cement clinker is effective for carbon emission reduction and conserving resources. Nevertheless, SFAC cement clinker synthesized by high-proportion moderate-alkalinity steel slag inherently suffers from poor mechanical properties. In this study, PG was innovatively employed as a mineralizer within the SFAC clinker system to systematically evaluate its influences on the chemical composition, mineralogical evolution, microstructural characteristics, and mechanical properties of the SFAC clinker. The results demonstrate that PG significantly promoted the decomposition of carbonate and improved the burnability of the cement raw meal. Petrographically, small-sized irregular C₂S crystals with high hydration activity formed in the high-ferrite (HF) zone due to the decomposition of C₃S. Therefore, the PG mineralized SFAC clinker exhibited a relatively low content of C₃S while presenting a high content of C₃A and amorphous phase. Residual SO₃ persisted predominantly as CaSO₄ and (Ca₂K₂)(SO₄)₃, which scarcely evaporated into the air during the sintering process and promoted the early-stage hydration of C₃S and C₃A. Benefiting from synergistically elevated crystalline imperfections in C₃S and β-C₂S, enhanced hydration degree, and refinement of the hardened paste microstructure, the 3d and 28d compressive strengths of PG mineralized SFAC clinker increased by 16.93 and 18.72%, respectively, compared with the control sample without PG. This study proposes a sustainable low-carbon production way of mechanical enhanced SFAC clinker for the corecycling of original granular steel slag and PG in cement industry.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 38","pages":"16016–16035"},"PeriodicalIF":7.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145073045","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The ACS Sustainable Family─Complementary yet Distinct: Some Evolving Thoughts from the Editors’ Desks","authors":"Thalappil Pradeep,&nbsp;Michael K. C. Tam,&nbsp;Danielle Julie Carrier,&nbsp;Jingwen Chen,&nbsp;Bing Joe Hwang,&nbsp;Michael Meier,&nbsp;Bala Subramaniam,&nbsp;Rowan S. Brower and Peter Licence*,&nbsp;","doi":"10.1021/acssuschemeng.5c08629","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c08629","url":null,"abstract":"","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 36","pages":"14675–14676"},"PeriodicalIF":7.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145056990","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Techno-Economic Assessment of Renewably Powered Electrocatalytic Nitrate Reduction for a Sustainable Nitrogen Cycle","authors":"Biyu Kang,&nbsp;, ,&nbsp;Mingshuo Jiao,&nbsp;, ,&nbsp;Fengting Li,&nbsp;, ,&nbsp;Zhenhai Wen,&nbsp;, ,&nbsp;Chao Zhang,&nbsp;, and ,&nbsp;Ying Wang*,&nbsp;","doi":"10.1021/acssuschemeng.5c06239","DOIUrl":"10.1021/acssuschemeng.5c06239","url":null,"abstract":"<p >Electrocatalytic nitrate reduction (eNO₃RR) exhibits substantial potential in eliminating waste NO₃^– by selectively converting it into N₂ or valuable resources NH₃. Since eNO₃RR has made rapid progress recently, it is vital to conduct a systematic evaluation of its feasibility. Herein, we provide a comprehensive techno-economic assessment (TEA) and life cycle assessment (LCA) of eNO₃RR and propose economically and environmentally favorable thresholds to systematically guide its industrial-scale implementation. Sensitivity analysis suggests that current density is the most crucial factor for N₂, showing an even greater impact than electricity price, while voltage ranks second only to electricity price for NH₃, highlighting optimization priorities. The profitability of eNO₃RR-to-NH₃ at $0.03/kWh depends on the progression of performance: the full-cell energy efficiency exceeds 50% at a current density &gt;500 mA/cm². Through continuous technological optimization, the levelized cost of ammonia (LCOA) is projected to decrease from $0.92/kg to $0.14/kg, substantially below current NH₃ market prices. LCA reveals that renewable-electricity-powered eNO₃RR achieves near-zero global warming potential (GWP, &lt;0.4 kg CO₂e/kg NO₃^–-N), offering superior decarbonization compared to conventional wastewater treatment (WWTP) and Haber-Bosch (H–B) processes.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 38","pages":"16046–16057"},"PeriodicalIF":7.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145073031","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Pulsed Oxidation-Driven Catalyst Regeneration Enabling Durable CO-Tolerant Low-Temperature Electrochemical Hydrogen Pumps","authors":"Kritika Sharma,&nbsp;, ,&nbsp;Suchithra Ashoka Sahadevan,&nbsp;, and ,&nbsp;Vijay Ramani*,&nbsp;","doi":"10.1021/acssuschemeng.5c04730","DOIUrl":"10.1021/acssuschemeng.5c04730","url":null,"abstract":"<p >Efficient hydrogen recovery from impure gas streams remains a key challenge for a scalable hydrogen infrastructure. While low-temperature electrochemical hydrogen pumps (LT-EHPs) offer simultaneous hydrogen purification and compression, their performance is severely compromised in the presence of carbon monoxide (CO) due to strong CO adsorption on Pt active sites, leading to pronounced catalyst poisoning and reduced hydrogen throughput. Existing approaches, such as high-temperature operation and air bleeding, are either energy- or resource-intensive or suffer from side reactions and undesirable byproducts. Thus, developing efficient, durable, and practical strategies for CO mitigation remains a major barrier to the wide deployment of LT-EHPs for hydrogen purification. This work investigates an LT-EHP fed with 1% CO in H₂/N₂, evaluating separation and energy efficiencies (SE/EE). To sustain performance under prolonged CO exposure, we systematically investigated advanced pulse oxidation protocols for CO mitigation, focusing on dynamic voltage-triggered pulsing as a promising solution. A cutoff voltage was used to trigger dynamic pulse oxidation, applying pulses only when cell voltage exceeded a set cutoff (e.g., 0.45 V), unlike fixed-interval pulsing, which delivers pulses at regular intervals regardless of cell voltage and can result in excessive overpotentials and increased catalyst corrosion. Dynamic pulsing ensures targeted catalyst regeneration while minimizing unnecessary stress. This approach delivered more than 10% higher SE and over 15% higher EE compared to the no-pulse scenario. Additionally, it surpassed fixed-interval pulsing by over 8% in SE and 10% in EE under identical impurity conditions. Five days of stable operation confirmed the promise of dynamic pulse oxidation as the most effective strategy for impurity-resilient hydrogen pumping in clean energy systems. A stable five-day operation demonstrated the viability of pulse oxidation for impurity-resilient hydrogen pumping in clean energy systems.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 38","pages":"15875–15886"},"PeriodicalIF":7.3,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145073048","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Intensified Continuous Flow Synthesis of Oxazolidones","authors":"Lionel Crane,&nbsp;, ,&nbsp;Thomas Habets,&nbsp;, ,&nbsp;Bruno Grignard,&nbsp;, ,&nbsp;Jean-Christophe M. Monbaliu*,&nbsp;, ,&nbsp;Pierre Stiernet*,&nbsp;, and ,&nbsp;Christophe Detrembleur*,&nbsp;","doi":"10.1021/acssuschemeng.5c06628","DOIUrl":"10.1021/acssuschemeng.5c06628","url":null,"abstract":"<p >Cyclic urethane compounds, known as oxazolidones (Oxas), have historically been synthesized using toxic, phosgene-based isocyanates, prompting the pursuit for greener alternatives. However, those alternatives face obstacles like the use of hazardous reagents and reliance on metal catalysts, leading to scalability limitations. Flow chemistry provides an effective solution, enabling safer, more efficient, and continuous production of Oxas, with enhanced catalyst recovery, reduced reaction times, and greater control over reaction conditions. Leveraging these advancements, a novel flow-based method using the aminolysis of CO₂-derived α-alkylidene cyclic carbonates (αCCs) was developed, achieving yields of about 99% for aliphatic amines in just 1–5 min, with a very high selectivity for Oxas over hydrolysis and uncyclized byproducts. This process was further optimized to synthesize oxazolidones in under 1 min, without solvents and with minimal side reactions. Furthermore, a process utilizing supported catalysts was developed, further improving catalyst recovery and overall reaction efficiency.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 38","pages":"16107–16116"},"PeriodicalIF":7.3,"publicationDate":"2025-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145073032","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Green Design of Renewable Dual-Curing Polymers with Self-Healing and Recyclable Networks for 3D Printing","authors":"Rafael T. Alarcon*,&nbsp;, ,&nbsp;Alberto Cellai,&nbsp;, ,&nbsp;Matilde Porcarello,&nbsp;, ,&nbsp;Bernhard Sölle,&nbsp;, ,&nbsp;Elisabeth Rossegger,&nbsp;, ,&nbsp;Carla C. Schmitt,&nbsp;, and ,&nbsp;Marco Sangermano*,&nbsp;","doi":"10.1021/acssuschemeng.5c07154","DOIUrl":"10.1021/acssuschemeng.5c07154","url":null,"abstract":"<p >This work presents a green design approach for a novel class of dual-curing, self-healing polymers derived from vegetable oils for additive manufacturing. The polymer network is constructed from methacrylated and epoxidized monomers derived through environmentally friendly transformations, allowing for UV-curing radical polymerization followed by thermal curing via acid–epoxy reactions. The resulting materials exhibit self-healing behavior, supporting thermal reprocessing and chemical recycling via transesterification. Designed for circularity, polymers containing the vegetable oil derivatives─methacrylated and epoxidized─reached a biobased content of up to 98% and a biobased carbon content above 77%, far exceeding industry standards. The materials also display alkaline hydrolytic degradation, aligning with end-of-life strategies under a circular economy model. Dual-curing systems achieved an epoxy conversion of over 90% and gel contents above 97%, resulting in stable polymer networks suitable for reprocessing. The formulations were successfully processed using 3D printing platforms, producing well-defined structures despite viscosities exceeding the ideal printability window. The system containing the maleinized/methacrylated grapeseed oil and epoxidized castor oil showed the most favorable behavior, with lower overcuring and the lowest critical energy (37 mJ cm^– 2). Successful printing confirms the applicability of these systems.</p><p >Renewable dual-curing polymers from vegetable oils enable 3D printing, self-healing, and recyclability, offering a sustainable, circular alternative to photopolymer resins.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 38","pages":"16136–16153"},"PeriodicalIF":7.3,"publicationDate":"2025-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acssuschemeng.5c07154","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145073033","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}