{"title":"Enhanced Leaching of Lithium-Ion Battery Cathode Scraps with In Situ Electrogenerated Persulfates","authors":"Mark M. Pradja, Christian Modrzynski","doi":"10.1021/acssuschemeng.5c04940","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c04940","url":null,"abstract":"A sustainable and efficient leaching procedure using electrochemistry for recycling cathode scraps from lithium-ion batteries (LIBs) is demonstrated. The additional use of chemicals, except the leaching medium itself, is avoided by in situ electrogeneration of peroxydisulfate from sulfuric acid on a boron-doped diamond (BDD) electrode. The leaching of LCO, NCM, and black mass with and without the addition of persulfates (peroxymono- and disulfate) was investigated in detail. Using persulfates as salts at 65 °C, the conversion rate of cobalt almost doubled to 83%. When leaching NCM, the cobalt, nickel, and manganese conversion rates increase significantly to achieve almost quantitative conversion. When persulfates were in situ electrogenerated, even lower concentrations were efficient for leaching LCO and NCM. The use of persulfates also substantially accelerates the leaching of all valuable metals of industrial black mass, which is completed in under 5 min.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"57 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204031","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}
Jiayuan Tian, Jingjing Wu, Feng Lin, Yu-long Ma, Yong-gang Sun
{"title":"Defect Engineering-Regulated Electron Transfer of NiAl-MMO for Catalyzing Directed Conversion of Lignin into Cyclohexanol-Based Chemicals","authors":"Jiayuan Tian, Jingjing Wu, Feng Lin, Yu-long Ma, Yong-gang Sun","doi":"10.1021/acssuschemeng.5c06157","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c06157","url":null,"abstract":"Regulating electron transfer through defect engineering to selectively catalyze the cleavage of lignin C–O bonds is of significant scientific importance for the directed conversion of biomass into high-value chemicals. However, the precise dissociation of chemical bonds remains challenging. In this study, a 2D nanoflower-like NiAl-MMO catalyst was successfully constructed via a hydrothermal <i>in situ</i> pyrolysis synergistic strategy. An Al doping strategy was employed to fabricate Ni and Al<sup>3+</sup>-O<sub>v</sub> (O<sub>v</sub> denotes oxygen vacancy) synergistic dual active centers in NiAl-MMO. The research results indicate that the introduction of Al significantly enhances the catalytic performance. When an appropriate amount of Al is doped, it not only effectively increases the specific surface area of the catalyst and optimizes its pore structure but also enables the formation of moderate-strength interactions between metallic Ni and Al. Meanwhile, the presence of Al induces an increase in the concentration of O<sub>v</sub> in the catalyst. O<sub>v</sub> can regulate the electronic state of Ni active sites by modulating electron density while also enhancing the Lewis acidity of the catalyst, thereby improving its adsorption capacity for reactants. This electronic regulation optimized the electronic coupling environment of bimetallic sites and significantly strengthened the synergistic effect between Al<sup>3+</sup>-O<sub>v</sub> and Ni sites, improving the hydrogen activation capability and directed C–O bond cleavage performance of the catalytic system. The catalyst exhibited excellent C–O bond dissociation selectivity in the lignin hydrodeoxygenation (HDO) process with a total liquid yield of 45.7 wt % (68.4% selectivity for C<sub>6+</sub> cyclohexanol), providing a new approach for the synthesis of aviation fuel precursors. This work offers a novel strategy for the directed conversion of lignin through the synergistic regulation of interfacial defects and electronic structures.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"114 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204036","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":"Magnetically Responsive PLA-MXene Composite Membrane for Oil Removal at Oil–Water Interfaces","authors":"Hui He, Lujia Xuan, Qin Zhou, Yihe Lin, Kami Hu, Yongshun Song, Min Zhang, Rui Ding, Yifan Huang, Ruojia Wang, Changying Wang, Ruoyang Chen","doi":"10.1021/acssuschemeng.5c07125","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c07125","url":null,"abstract":"Oil pollution at water interfaces, caused by spills and industrial discharge, severely threatens ecosystems and public health. Cleaning such oil remains challenging due to its rapid spreading, high flammability risk, and susceptibility to environmental disturbances. A promising solution involves magnetically responsive, self-floating oil absorbers that enable safe and remote removal of oil pollutants. Here, we develop a multifunctional membrane via electrospinning a polylactic acid composite with MXene-supported iron oxide nanoparticles, rendering it with hydrophobicity, lipophilicity, and strong superparamagnetism. We demonstrate that the membrane enables magnetically targeted delivery to oil–water interfaces, self-floats on the water surface, and exhibits high adsorption capacities for various oils, including chili oil (∼30 g/g), motor oil (∼24 g/g), diesel oil (∼20 g/g), and sunflower oil (∼14 g/g). We also show that the membrane has robust oil adsorption ability, retaining ∼90% of its capacity after 10 adsorption–desorption cycles, along with stable magnetic responsiveness under harsh conditions, including saline water and UV exposure. Our findings offer a green and sustainable strategy for interfacial oil removal and recovery.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"10 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204033","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}
Emma Harrison, Austin Zheng, Joshua Wicks, Ke Xie, Edward H. Sargent, Radhakrishnan Mahadevan
{"title":"Cascading the Electrochemical Reduction of CO2 with Bioprocesses for the Production of Reduced-Carbon-Intensity Chemicals","authors":"Emma Harrison, Austin Zheng, Joshua Wicks, Ke Xie, Edward H. Sargent, Radhakrishnan Mahadevan","doi":"10.1021/acssuschemeng.5c04176","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c04176","url":null,"abstract":"Electrochemical reduction of CO<sub>2</sub> (eCO<sub>2</sub>R) offers a route to one- and two-carbon (C1/C2) intermediates, and these can serve as lower-carbon-intensity feedstocks for the biobased synthesis of C3+ products. We evaluate the energy inputs for ∼1000 cases of the integrated system, considering 9 intermediates and 50+ bioproducts. The most energetically compelling options include aerobic bioconversion of C2 intermediates or methanol to more oxidized products. As an intermediate, ethanol provides the highest overall bioproduction mass yield among candidate substrates, with over 25% of the products having a mass yield greater than one. For fuels, the anaerobic bioconversion of methanol and CO each appear promising, with energy inputs in the range of 40–60 GJ/ton. We find that the recycling of CO<sub>2</sub> generated during bioproduction is optimal when CO<sub>2</sub> capture costs for eCO<sub>2</sub>R exceed the separation costs of the bioreactor gas stream. Overall, this analysis points to privileged {intermediate, product} pairings in such integrated systems.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"126 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204030","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}
Joseph Dumpler, Amy McMackin, Magdalena Herren, Sina Hashemi Zadeh, Alexander Mathys
{"title":"Rapeseed Refined: Extraction of Polyphenols, Glucosinolates, Phytate, and Protein from Whole Dehulled Rapeseed Using Natural Deep Eutectic Solvents","authors":"Joseph Dumpler, Amy McMackin, Magdalena Herren, Sina Hashemi Zadeh, Alexander Mathys","doi":"10.1021/acssuschemeng.5c06105","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c06105","url":null,"abstract":"Natural deep eutectic solvents (NADES) have been shown to provide excellent extraction capabilities for phenolic compounds from plant materials. In this study, we investigated the kinetics and efficiency of choline chloride- and betaine-1,2-propanediol-based NADES to extract phenolic compounds, glucosinolates, phytate, and proteins from whole dehulled rapeseed kernels. These NADES were compared to 1,2-propanediol, water, and 60% aqueous ethanol. Solvent temperature (55 °C) and solid-to-liquid ratio (1:10 w/w) were kept constant. The extraction rate constant for phenolic compounds and glucosinolates increased more than ten times with increasing water content in the range of 10–40% w/w in NADES or 1,2-propanediol. Choline chloride-based NADES extracted the highest amounts of total phenolic compounds, up to 6.79 g kg<sup>–1</sup>, while betaine-based NADES extracted the highest amounts of glucosinolates, up to 3.48 g kg<sup>–1</sup>. Phytate solubility increased with increasing water content in NADES and 1,2-propanediol. Protein extraction also increased with an increasing water content but followed slower kinetics than the extraction of phenolic compounds. Limiting solvent water content and extraction duration will help exploit differences between the analytes’ extraction kinetics, ensuring low protein coextraction. The extracted rapeseed could be further processed to recover purified, white, and plain-tasting oleosomes, rapeseed protein, and fiber.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"100 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204041","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}
Paola Alzate, Nora Valderruten, Silvia Flores, Giovanni Rojas
{"title":"Facile and Green Synthesis of Chitosan-Based Microcapsules: Bridging Organic and Polymer Chemistry for Sustainable Biocidal Applications","authors":"Paola Alzate, Nora Valderruten, Silvia Flores, Giovanni Rojas","doi":"10.1021/acssuschemeng.5c05807","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c05807","url":null,"abstract":"A facile and eco-friendly synthesis approach was developed to fabricate chitosan-based microcapsules for the encapsulation and controlled release of commercial eucalyptus essential oil. The process relies on a mild emulsification and ionic gelation method, ensuring high efficiency, minimal energy consumption, and possible scalable production. Comprehensive structural and physicochemical characterization confirmed strong polymer-oil interactions, facilitating enhanced stability, controlled diffusion, and biocidal activity. The microcapsules exhibited potent antifungal properties, highlighting their potential for sustainable pathogen control in agricultural and environmental applications. This strategy bridges organic and polymer chemistry, leveraging green chemistry principles to develop biopolymeric carriers with optimized encapsulation efficiency and release kinetics. By integrating an exceptionally simple yet effective fabrication process with demonstrated functional performance, this work contributes to next-generation eco-friendly biocidal formulations and expands the application of biopolymers in green synthesis.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"76 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204037","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}
Tiina Belt, Muhammad Awais, Paula Nousiainen, Lauri Rautkari, Mikko Mäkelä
{"title":"Cell Wall Polymer Degradation during Rhodonia placenta Brown Rot Decay of Thermally Modified and Unmodified Wood","authors":"Tiina Belt, Muhammad Awais, Paula Nousiainen, Lauri Rautkari, Mikko Mäkelä","doi":"10.1021/acssuschemeng.5c08352","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c08352","url":null,"abstract":"Thermal modification produces decay-resistant wood suitable for sustainable applications. Although thermally modified wood remains degradable by fungi, its degradation mechanisms are poorly understood, impacting long-term eco-friendly use. This study investigated thermally modified wood degradation by elucidating chemical changes to wood cell wall polymers during <i>Rhodonia placenta</i> brown rot decay. Modified and unmodified Scots pine samples were exposed to <i>R</i>. <i>placenta</i> in stacked-sample decay tests, generating decay stage progressions. Decayed samples were analyzed by near-infrared spectroscopy with multivariate analysis to identify key chemical changes. Milled wood lignin was isolated and analyzed by two-dimensional nuclear magnetic resonance spectroscopy for further lignin chemistry insight. Results showed that <i>R</i>. <i>placenta</i> degraded thermally modified wood to high mass losses. Chemical changes were characterized by carbohydrate degradation and oxidative lignin modification, typical for brown rot. While most degradative changes were similar between modified and unmodified wood, differences in lignin modification patterns were observed. Interestingly, spectroscopic data revealed different chemical changes in the early and late decay stages in modified and unmodified wood. These findings highlight the time-dependent nature of <i>R</i>. <i>placenta</i> degradation and show that thermally modified and unmodified woods are degraded by similar yet different mechanisms, providing new insight into brown rot wood degradation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"18 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204040","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}
Sergio Serrano-Blanco, Priscila Melo, Adam P. Harvey, Sharon B. Velasquez-Orta
{"title":"Mechanical Reinforcement of Paper Biocomposites Using Filamentous Cyanobacteria","authors":"Sergio Serrano-Blanco, Priscila Melo, Adam P. Harvey, Sharon B. Velasquez-Orta","doi":"10.1021/acssuschemeng.5c02889","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c02889","url":null,"abstract":"Rising concerns over plastic packaging and the growing demand for e-commerce have increased paper-based materials production, thereby intensifying environmental impacts of the paper industry, one of the most polluting industries worldwide. The need to source nonwood fibers to alleviate environmental pressure has brought microalgae into the spotlight as a sustainable and renewable resource. For the first time, this study proposes and evaluates replacing cellulose fibers in paper-like biocomposites with the cyanobacterium <i>Leptolyngbya</i> sp. SB090721. The effect of using cyanobacteria as a cellulose replacement (0%, 3%, 30% w/w) was evaluated. Addition of cyanobacterial biomass (3–30%) maintained or enhanced tensile properties. The standard biocomposite showed the highest tensile strength (4.8 kN·m<sup>–1</sup>) and tensile energy absorption (195.63 J·m<sup>–2</sup>). Both the standard and high biomass composites showed enhanced elasticity moduli of 997.1 and 903.4 MPa. Significant structural differences were observed on the SEM micrographs, with the high biomass specimen displaying a distinct structure, attributed to its elevated cyanobacterial content. In conclusion, the study confirmed the feasibility of using unprocessed cyanobacterial biomass as a nonwood fiber source for paper and paperboard materials. This reduces the amount of cellulose used in the paper industry, offering new properties and production routes that could potentially be more sustainable.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"37 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204034","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}
Khim Hoong Chu, Mohd Ali Hashim, Mohd Hafiz Zawawi
{"title":"Comment on “Green Synthesis of Waste-Derived Metal–Organic Frameworks for Organic Substance Extraction from Piggery Wastewater as Biofertilizers”","authors":"Khim Hoong Chu, Mohd Ali Hashim, Mohd Hafiz Zawawi","doi":"10.1021/acssuschemeng.5c00805","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00805","url":null,"abstract":"No data were used for the research described in the article. K.H.C. and M.H.Z. acknowledge the support from Tenaga Nasional Berhad (TNB) and UNITEN through the BOLD Refresh Postdoctoral Fellowships under the project code of J510050002-IC-6 BOLDREFRESH2025-Centre of Excellence. This article references 8 other publications. This article is cited by 1 publications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"98 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204042","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":"Ultrafast Material Separation by Electrochemical Delamination for Spent Lithium-Ion Batteries Recycling","authors":"Erkang Feng, Peng Li, Ziyu Huang, Wenyan Zan, Teng Wang, Zhenyu Ren, Mingyue Xu, Hao Bi, Yanze Liu, Guoyong Huang, Wenjing Lu, Sidian Li, Dongbei Yue, Bing Deng","doi":"10.1021/acssuschemeng.5c06070","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c06070","url":null,"abstract":"The rapid growth of lithium-ion batteries in personal electronics and electric vehicles is leading to a substantial increase in end-of-life battery waste. Recycling these batteries is essential to closing the materials loop for sustainable energy systems. A crucial step in battery recycling is the separation of active materials from current collectors. However, current processes often require extensive use of acids, bases, or solvents, which intensifies environmental impacts. Here, we report an electrochemical delamination process for efficient and ultrafast separation of battery materials. By applying a mild voltage, gas bubbles form between the current collectors and active materials, facilitating their rapid separation with a separation efficiency of ∼100% and a metal recovery yield of >97%. Notably, no aluminum impurities are introduced into the recovered cathode materials. Mechanistic studies reveal that the superior hydrogen evolution capability of the current collectors, compared to the cathode and anode materials, drives the mechanical separation. This electrochemical delamination technique is versatile for various battery chemistries, as demonstrated by the successful separation of LiMn<sub>2</sub>O<sub>4</sub>, LiFePO<sub>4</sub>, and LiNiCoMnO<sub>2</sub> cathodes from aluminum, as well as separating graphite anode from copper. Life-cycle assessment and techno-economic analysis indicate that this process can reduce carbon emissions by 23–98% and operating costs by 28–98% compared to current methods, underscoring its potential for real-world implementation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"6 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145204044","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}