ACS Sustainable Chemistry & Engineering最新文献

{"title":"Multidimensional Utilization of Kraft Lignin: Upgrading Glycerol to Sustainable Fuel Additives Using Lignin-Derived Benzaldehyde over Lignin-Based Acid Catalyst","authors":"Chi Zhang, Xueru Sheng, Haiyuan Jia, Na Li, Jian Zhang, Bing Wang, Haiqiang Shi, Qingwei Ping, Ning Li","doi":"10.1021/acssuschemeng.5c02247","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c02247","url":null,"abstract":"This study aims to explore a lignin-based catalyst for the green synthesis of sustainable fuel additive using lignin-derived benzaldehyde and glycerol, byproducts from the paper industry and biodiesel preparation, respectively. This sustainable fuel additive can be refilled into biodiesel to improve the carbon atom economy, promoting resource efficiency and environmental sustainability. Kraft lignin was modified with phosphoric acid and sulfuric acid to prepare solid acid catalysts KL-HP-SO₃H. A series of characterization techniques showed that phosphorylation can markedly enhance the specific surface area, while sulfonation can notably increase the acid sites and acid strength. The synergistic physical–chemical effect of phosphorylation and sulfonation collectively enhances the activity of the KL-HP-SO₃H catalyst. In addition, ball milling and thermal catalysis were compared and analyzed in this study. The results show that the ball milling technology offers an advantage: it achieves a high product yield within only 15 min. The ball milling process consumes less energy than the hydrothermal reactor (21.3 vs 493.8 kWh·mol^–1). From a long-term investment perspective, the ball milling process is economically superior. This study contributes an efficient catalyst strategy to green chemical synthesis while providing multifunctional utilization of lignin.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"78 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875839","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":"Supramolecular Deep Eutectic Solvents and Their Aqueous Solutions: Green Carriers for Essential Oils","authors":"Chengmin Gui, Qinghua Liu, Zhigang Lei, Yanyan Guo, Miriana Kfoury, Dong Xiang, Sophie Fourmentin","doi":"10.1021/acssuschemeng.5c00881","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00881","url":null,"abstract":"In the search for alternatives to synthetic chemicals and drugs, there is growing interest in the aromatic and biological properties of essential oils. However, essential oils and their constituents are poorly soluble in aqueous systems and are highly sensitive to degradation and evaporation. Here, we evaluated the applicability of supramolecular deep eutectic solvents (SUPRADES) based on naturally occurring <span>l</span>-lactic acid (LA) and four cyclodextrins (CDs) as carriers for two essential oil components, 3-carene and limonene. The obtained partition coefficient in water was 1200 times higher than that in SUPRADES, which indicated that SUPRADES has a remarkable enhancing effect on the dissolution of the two essential oils. Adding water could significantly reduce the viscosity of SUPRADES and effectively control the release of essential oils. Evidence for a randomly methylated β-CD–3-carene inclusion complex was provided by molecular dynamics simulation. In addition, the formation of the inclusion complex is enhanced by increasing the water content within a specific range. Furthermore, the formation of SUPRADES is attributed to hydrogen bonds between the hydroxyl groups on CDs and LA. In particular, the van der Waals interaction plays a major role in the dissolution of 3-carene. Overall, SUPRADES and their aqueous solutions are promising carriers for essential oils due to their strong inclusion ability and controlled release.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"16 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875840","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":"Review and Perspectives on the Sustainability of Organic Aerogels","authors":"Carlos A. García-González, María Blanco-Vales, Joana Barros, Antonella Caterina Boccia, Tatiana Budtova, Luisa Durães, Can Erkey, Marta Gallo, Petra Herman, József Kalmár, Ana Iglesias-Mejuto, Wim J. Malfait, Shanyu Zhao, Lara Manzocco, Stella Plazzotta, Stoja Milovanovic, Monica Neagu, Loredana E. Nita, Patrina Paraskevopoulou, Anna Roig, Rosana Simón-Vázquez, Irina Smirnova, Željko Tomović, Clara López-Iglesias","doi":"10.1021/acssuschemeng.4c09747","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09747","url":null,"abstract":"Aerogels are exceptionally lightweight materials characterized by their high open porosity and remarkable specific surface area, currently used across a wide array of industrial sectors from construction to energy storage and have great potential for expanding their applicability and unlocking new market opportunities. Driven by global economic growth and an intensifying environmental crisis, there is a growing demand for engineering innovations that prioritize sustainability. Aerogels are well-positioned to support these sustainability efforts. Their unique properties make them ideal for energy-saving solutions, environmental remediation, and more efficient use of resources. As the demand for eco-conscious technologies rises, aerogels are poised to contribute significantly to the development of greener, more efficient products and processes across multiple industries. The sustainability of aerogel technology is crucial for the mid-to-long-term future, yet its current status has been scarcely reviewed in the literature. This Perspective explores and critically reviews significant advances on organic and hybrid aerogels in the current socioeconomic scenario, with selected case studies endorsing their contribution to the UN Sustainable Development Goals. It also identifies research gaps while proposing innovative strategies to enhance the sustainability of aerogel production through the application of circular economy principles. Key strategies discussed involve the fabrication of aerogels using eco-friendly sources, such as biopolymers derived from biorefinery processes or from waste materials. Additionally, this Perspective examines the development of methods for the reuse, recycling, and end-of-life management of aerogels, along with the implementation of more efficient processing routes. Ultimately, this work highlights the need for comprehensive assessments of aerogel sustainability through life cycle assessment (LCA) and evaluations of safety and toxicity. By addressing these critical aspects, the potential of aerogels to contribute to a more sustainable future appears highly favorable from both commercial and research perspectives, paving the way for a circular aerogel economy and providing a lasting impact to the society in which we live.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"136 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875841","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":"Reuse of Wind Turbine Blades for High-Performance Flame-Retardant Epoxy Composites via Surface Modification","authors":"Dawei Luo, Shuangqiao Yang, Qi Wang","doi":"10.1021/acssuschemeng.5c00726","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00726","url":null,"abstract":"With the rapid development of clean and renewable energy sources, particularly wind energy, the recycling of wind turbine (WT) blades has emerged as a significant challenge in addressing environmental impacts. In this study, a novel flame retardant, designated as Fr@WGE@PDA, was synthesized by using recycled fine powder from WT blades. The synthesis was accomplished using polydopamine (PDA) as the interlayer and hexachlorocyclotriphosphazene (HCCP) as the primary raw material via a two-step process. The successful fabrication of Fr@WGE@PDA was confirmed via multiple characterizations. The incorporation of Fr@WGE@PDA significantly enhanced the flame retardancy of the epoxy (EP) composites. Notably, the enhancement was achieved without significantly compromising the mechanical properties of the composites. The EP composite incorporated with Fr@WGE@PDA at a loading level of 20 wt % exhibited a tensile strength of ∼69.4 MPa and an elongation at break of ∼6.6%. Additionally, the EP composite achieved a limiting oxygen index (LOI) of 31.9% and a UL-94 V-0 rating. Based on analyses of both the gas phase and condensed phase, a degradation mechanism for the EP composite was proposed. This study presents a sustainable strategy to recycle WT blades into an efficient flame retardant, offering promising prospects for both fundamental research and practical applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"72 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875894","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":"Chemically Recyclable and Enzymatically Degradable Thermostable Polyesters with Inherent Strain from α-Pinene-Derived Chiral Diols","authors":"Ganapathy Ranjani, Sathiyaraj Subramaniyan, Ximena Lopez-Lorenzo, Minna Hakkarainen, Per-Olof Syrén","doi":"10.1021/acssuschemeng.5c01374","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c01374","url":null,"abstract":"Accelerated production of recyclable and biodegradable polymers is crucial in combating the socioeconomic and environmental issues connected to traditional plastics. While renewable diacids have been in the spotlight for the generation of biobased polyesters with tailored properties by varying the alkyl chain length, capitalizing on diols from biomass for this purpose is underexplored and has mainly focused on linear and branched shorter chain alcohols. Here, we explored the potential of two (−)-α-pinene-derived diols (PDOs) as building blocks to generate biobased polyesters harboring bicyclic ring structures in their backbones that can mimic aromatic fossil-based plastics’ properties. We demonstrate a concise synthesis of two novel unsymmetrical chiral PDOs on the 20–40 g scale, together with eight structurally differing heat-resistant polyesters, as reflected by high glass transition (<i>T</i>_g<i>)</i> temperatures (90 and 121 °C) for two of the polymers. The stereochemistry of PDO-derived polyesters is guided by intramolecular hydrogen bonding made possible by the protruding rings and the polyester backbone. Most of the synthesized polyesters (five) in this study showed potential as adhesives based on the analysis of tensile strength and adhesive properties on paper boards. The steric hindrance of the intact bicyclic α-pinene ring structure protruding from the backbone of the polymers can also aid in the degradation process, manifested by facile chemical recycling of these polyesters under mild conditions to recover both monomers. Finally, our results show how the generated rigid polymers are susceptible to enzymatic degradation by PETase and cutinase without any chemical pretreatment. Our results illuminate the potential of expanding the current scope of biobased monomers to bicyclic diols to generate biomaterials with tailor-made properties.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"57 1 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875893","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":"Agricultural Waste–Biochar (Reclaiming Phosphate from Wastewater)–Soil (Slow-Release Phosphate Fertilizer)–Plant (Peanut Growth) System: Economical and Environmentally Sustainable Strategy","authors":"Xue Shao, Xudong Sun, Junjie Yuan, Yao Zhu, Jizhang Wang, Yuting Dai, Tao Zhang, Fengxian Qiu","doi":"10.1021/acssuschemeng.5c02580","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c02580","url":null,"abstract":"Excessive use of traditional phosphate fertilizers has led to excess phosphorus entering the environment through leaching, volatilization, and agricultural runoff, causing a series of problems such as eutrophication, soil degradation, and phosphorus resource exhaustion. Therefore, the reclamation of phosphorus from wastewater is essential for ecological protection and sustainable agricultural development. Herein, an effective strategy for the synthesis of calcium-modified porous biochar (CEBC) was provided and designed for the recovery of phosphorus from phosphorus-containing wastewater, followed by its application as a slow-release phosphorus fertilizer. CEBC exhibited an excellent phosphate recovery performance with a maximum adsorption capacity of 193.93 mg P/g. Furthermore, slow-release experiments demonstrated that the nutrient release rate of phosphorus-loaded biochar-based slow-release fertilizer (CEBC-P) was 8.95% within 24 h. After application of CEBC-P, the total biomass accumulation and net photosynthetic rate of peanuts increased by 2.54-fold and 4.91-fold, respectively. Mechanistic studies revealed that phosphate was retained within the biochar through precipitation, coordination, hydrogen bonding, and electrostatic attraction. Moreover, release kinetics optimally fitted the Peppas–Sahlin model (<i>R</i>² = 0.996), suggesting that the nutrient release from CEBC-P was synergized by diffusion and dissolution. Overall, this study provides an economical and environmentally sustainable strategy for the recovery and recycling of phosphorus resources.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"51 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866453","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":"Toward Low-Temperature Regeneration of CO2 Capture Adsorbents: Functionalization of Polyethylenimine","authors":"Abdullah J. Al Abdulghani, Florian Weisshar, Jannis Hack, Adroit T. N. Fajar, Guillaume Lambard, Nobutaka Maeda","doi":"10.1021/acssuschemeng.5c01250","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c01250","url":null,"abstract":"This study aimed to design materials for CO₂ capture with low regeneration temperatures without compromising the adsorption capacity (AC). Branched polyethylenimine (BPEI) functionalized with acrylonitrile (AN), 2-ethylhexyl acrylate (EHA), and butyl acrylate (BA) was impregnated onto fumed silica and tested for its adsorption and desorption properties. Higher functionalization degrees led to decreased desorption temperatures (DTs) from 73 to 97 °C to as low as 25 °C, which was attributed to the higher percentages of secondary amines upon functionalization and changes in the CO₂ adsorption mechanism. However, the adsorption capacities also decreased with functionalization. Bayesian optimization using machine learning models predicted optimal compositions of adsorbents for high adsorption capacities at low regeneration temperatures. The isothermal operation of CO₂ capture and release was also demonstrated to lower the energy requirement for CO₂ capturing systems. The functionalized BPEI materials steadily adsorb and release CO₂ for 20 cycles under isothermal conditions without any deterioration of the performance. BPEI 10,000 functionalized with AN, EHA, and BA offers a promising balance between AC and DT, making it suitable for industrial applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866452","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":"Native Lignin Isolation Facilitated by Cellulase Desorption","authors":"Jiaming Cao, Xuke Chen, Kexin Yan, Huifang Liu, Junyou Shi, Ning Li","doi":"10.1021/acssuschemeng.5c00942","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00942","url":null,"abstract":"Isolating lignin in its native form is essential to understand the lignin chemistry involved in the processing pathway. However, native lignin, due to its heterogeneous aromatic structures and spatial entanglement with carbohydrates, is challenging to separate quantitatively. Cellulase hydrolysis, a mild and effective treatment, allows lignin to be separated in its solid form. However, nonspecific adsorption of cellulases onto lignin during the enzymatic hydrolysis leads to protein contamination, thus interferencing with characterization and quantification of lignin. Addressing is crucial for obtaining high-quality lignin. In this study, this issue is addressed by adopting an alkaline-buffered solution to effectively remove cellulase residues from enzymatic lignin. The efficiency and extent of cellulase desorption were qualitatively and quantitatively analyzed, while the impact of buffer treatment on lignin composition and structure was evaluated in detail. The isolated lignin exhibited over 97% yield, with a carbohydrate content of approximately 5%. The lignin-derived monophenol yield from alkaline nitrobenzene oxidation exceeded 40 wt %, approaching the theoretical maximum yield from native lignin. Furthermore, a simplified purification process achieved nearly 99% purity, resulting in the production of a high-molecular-weight native lignin. The alkaline buffer treatment provides a straightforward and effective method to improve the native lignin isolation with high yield and purity.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"109 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866456","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":"Optimizing Wood’s Thermal Performance: Lignin Modification for Energy-Efficient Buildings","authors":"Yanan She, Haocheng Xu, Feiyu Tian, Qinglin Wu, Xinwu Xu","doi":"10.1021/acssuschemeng.5c00529","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00529","url":null,"abstract":"Delignification and chemical modification of lignin in wood through alkaline and oxidation treatments were investigated with its enhanced thermal performance for energy-saving potential in wood buildings. EnergyPlus simulations are then adopted for applying delignified wood to radiative cooling systems, serving as rooftop radiators to reflect heat to the sky for heat dissipation purposes, to partially replace active energy requirements of wood buildings. Results show that alkaline treatment enhances photon absorption by stabilizing β-O-4′ bonds, leading to more heat absorption, and alkali-treated wood provides an annual building energy saving of up to 4.67 MJ/m² through saving heating systems’ energy. On the other hand, oxidation degrades the aromatic structure of lignin and conjugated double bonds, leading to a reduction in heat absorbance and enhanced radiative cooling properties, which results in a maximum building energy saving of 12.77 MJ/m² through saving cooling systems’ energy. These results highlight the potential for tailoring wood lignin modifications to improve the energy efficiency of wood-based buildings.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"5 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866455","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":"Electrolyte Flow-Driven Coupling of Oxygen Evolution Reaction and CO2 Electroreduction for Promoting Selective HCOOH Production under Acidic Conditions","authors":"Shanshan Wu, Xiangyang Yin, Zhihao Liu, Weifeng Zhang, Yongkui Huang, Fan Dong, Daijun Zhang","doi":"10.1021/acssuschemeng.5c00707","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00707","url":null,"abstract":"The electrocatalytic CO₂ reduction reaction (ECO₂RR) toward liquid fuels is one of the most promising routes to sustainable carbon neutrality. However, reducing energy consumption and improving product selectivity of the ECO₂RR in acidic environments remain challenging. To address these issues, we propose a novel process by coupling the oxygen evolution reaction (OER) and ECO₂RR using an anode-to-cathode electrolyte flow to enhance formic acid (HCOOH) production under acidic conditions. The coupling process achieves an outstanding Faradaic efficiency (FE) of 95.9% for HCOOH production, reduces cathodic energy consumption by 19.5% compared with the traditional ECO₂RR, and exhibits superior stability with FE_HCOOH &gt; 80% for over 80 h at 200 mA cm^–2. Dissolved oxygen is activated on the Bi-Bi₂O₂CO₃@CNTs cathode to produce *OOH, lowering the activation energy barrier of CO₂ and facilitating the formation of key intermediates (*OCHO) for HCOOH production. Furthermore, the coupling process can modulate the local interfacial electric field to promote the activation of CO₂ in the acidic electrolyte. Dissolved oxygen facilitates the Bi/Bi^δ+ redox cycle to provide active sites for the conversion of CO₂ to HCOOH during long-term electrolysis. This study provides a proof-of-concept demonstration of the ECO₂RR/OER coupling process, making CO₂ electroreduction more energy-efficient and economical.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"70 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866665","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}