{"title":"High-Barrier, Photothermal Conversion, and Antibacterial Composite Enabled by Kraft Lignin-Coated Cellulose Paper for Plastic Replacement","authors":"Xiaoqian Gai, Chao Liu, Liucheng Meng, Zhaochuan Yu, Shan Jiang, Xinman Liu, Yuqian Liu, Chao Deng, Huining Xiao","doi":"10.1021/acssuschemeng.4c06798","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06798","url":null,"abstract":"Paper-based materials demonstrate considerable potential as a substitute for plastic packaging. However, their limited barrier properties, singular functionality, and intricate preparation methods pose challenges to further advancement. Specifically, the inadequate barrier adversely impacts the preservation of paper-based packaging materials under conditions characterized by high humidity and prolonged exposure to sunlight. Herein, a refined preparation strategy is proposed for the direct and enhanced production of a biodegradable multifunctional barrier packaging paper. Lignin is deposited onto the surface of cellulose paper (CP) via vacuum filtration followed by conversion into lignin/cellulose paper (LCP) through a simple hot-pressing process. The resulting LCP exhibits outstanding barrier properties (Kit grade of 12, water vapor permeability of 197 g/(m<sup>2</sup>·24 h) at 37 °C and 90% RH) and wet strength (50.79 MPa). Moreover, the prepared LCP also exhibits rapid and stable photothermal conversion capability, along with remarkable photothermal antibacterial activity (photothermal antibacterial rate >99.9%). The overall prepared LCP exhibits numerous advantages, encompassing an intact biobased composition, degradability, environmental protection, and exceptional barrier properties. Therefore, it presents an optimal alternative to conventional plastic packaging materials, offering an efficient solution for product storage across diverse environments while also providing a sustainable and cost-effective approach to the production of barrier packaging materials.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"1 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809291","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}
Tianyu Zheng, Lianjing Mao, Xiao Li, Chunsen Ye, Pengrui Zhang, Wei Sun, Jinhe Sun
{"title":"Elucidating the Mechanism of Lithium Ion Extraction in a Tributyl Phosphate-Ionic Liquid Mixed System from the Perspective of Water Coordination","authors":"Tianyu Zheng, Lianjing Mao, Xiao Li, Chunsen Ye, Pengrui Zhang, Wei Sun, Jinhe Sun","doi":"10.1021/acssuschemeng.4c07349","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c07349","url":null,"abstract":"With the rapid development of the lithium-ion battery industry, the demand for lithium resources is becoming more and more urgent. Lithium extraction is a widely used process; especially, tributyl phosphate (TBP) systems have attracted much attention. During the extraction and purification process of lithium ions, the extractant TBP may encounter issues including aging, emulsification, precipitation, and low utilization rates. These problems arise due to an inadequate understanding of the extraction mechanism. In this work, the TBP-ionic liquid system was utilized to extract Li<sup>+</sup>, the variations of trace water in the organic phase were systematically and quantitatively investigated, and the extraction mechanism was further investigated. Experiments have confirmed that TBP forms a 1:1 complex with water. Various complex ratios of TBP, Li<sup>+</sup>, and water were determined, and the structures were verified by simulations. The complexes have three different ratios of TBP, Li<sup>+</sup>, and water: 2:1:2, 3:1:1, and 4:1:0. Water molecules are substituted during the complexation of Li<sup>+</sup> with TBP, and meanwhile, the NTf<sub>2</sub><sup>–</sup> anion equilibrates the charge of the Li<sup>+</sup>-TBP complex. This work provides experimental data and a theoretical basis for understanding Li<sup>+</sup> extraction in the TBP-ionic liquid system, which is conducive to the sustainable development of the lithium industry.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"21 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142804703","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}
Zongxi Zhang, Mei Hong, Hui Cao, Yingxiong Wang, Shuai Chen, Yan Qiao
{"title":"Dual Modulation Strategy of NiMoOx Active Site by Ionic Liquid for Boosting Electrocatalytic HMF Oxidation Reaction","authors":"Zongxi Zhang, Mei Hong, Hui Cao, Yingxiong Wang, Shuai Chen, Yan Qiao","doi":"10.1021/acssuschemeng.4c07570","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c07570","url":null,"abstract":"The electrooxidation of 5-hydroxymethylfurfural (HMF) to produce value-added chemicals provides an efficient and economical way for the sustainable development of society. However, the development of novel, cost-effective, and environmentally friendly techniques for the synthesis of electrocatalysts to improve HMF oxidation is still a challenge. Herein, we adopted a novel dual modulation strategy based on ionic liquid (IL) regulation to obtain F-doped amorphous nickel molybdenum oxides (NiMoO<sub><i>x</i></sub>/NF-IL). The acquired NiMoO<sub><i>x</i></sub>/NF-IL showed excellent catalytic activity (141.3 mA/cm<sup>2</sup>@1.40 V vs RHE), stability (20 successive cycles), and high yield and FE<sub>FDCA</sub> (all over 95%@1.40 V vs RHE) in electrocatalytic HMF oxidation reaction. Specifically, the introduction of an amorphous structure endowed numerous unsaturated sites for the generation of catalytic active sites. Several characterization techniques and theoretical calculation results demonstrated that F doping effectively modulates the coordination environment of the NiOOH active species through its electronegativity, further improving the adsorption behavior of the substrate. The combination of these innate advantages makes NiMoO<sub><i>x</i></sub>/NF-IL exhibit excellent performance in the electrocatalytic oxidation reaction of HMF to 2,5-furandicarboxylic acid.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"47 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809292","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}
Thamsanqa Ncube, Hans C. Oskierski, Gamini Senanayake, Martin Bertau, Jakub Skut, Juan Canales, Bogdan Z. Dlugogorski
{"title":"Refining α-Spodumene with Potassium Sulfate Compared to the Conventional Sulfuric Acid Process","authors":"Thamsanqa Ncube, Hans C. Oskierski, Gamini Senanayake, Martin Bertau, Jakub Skut, Juan Canales, Bogdan Z. Dlugogorski","doi":"10.1021/acssuschemeng.4c06207","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06207","url":null,"abstract":"The conventional process of extracting lithium by decrepitating the concentrates of α-spodumene and then baking β-spodumene with concentrated sulfuric acid is the most economic to operate but nonsustainable because of its feedstock, energy, and waste byproduct intensity. Directly extracting lithium from α-spodumene by roasting it with potassium sulfate (K<sub>2</sub>SO<sub>4</sub>) followed by leaching it with water offers a more sustainable alternative. We optimized the potassium sulfate process (PSP) at a ratio of K<sub>2</sub>SO<sub>4</sub> to spodumene concentrate of 0.6:1 (w/w), 1050 °C, and 30 min roasting time, achieving a lithium extraction efficiency of 96.3 ± 1.4% (w/w), in comparison to 96.66 ± 0.37% (w/w) for the conventional process, for the same feedstock of spodumene concentrate. While the purification of the leach liquor from PSP is more complex, requiring the addition of aluminum sulfate to recover potassium as potash alum, its byproducts have high economic value. Both processes display a similar energy demand, based on 200 kt y<sup>–1</sup> of the spodumene concentrate feed. The use of aluminum sulfate increases the overall cost of PSP by $12.8 million, but sales of potassium alum elevate the revenue by $45.8 million. We reveal that the key advantage of PSP lies in its capability of leveraging the byproducts (leucite and potash alum), while the sulfuric acid process (SAP) may incur disposal cost for its hydrogen aluminosilicate (HAS) byproduct. For PSP to breakeven with SAP, leucite must be converted to a fertilizer and sold at a price of $102.6 t<sup>–1</sup> if HAS requires no disposal cost. With the process development focused on the byproduct value, the proposed PSP provides an efficient, more sustainable, and potential near zero-waste alternative to the conventional refining of the lithium chemicals from spodumene.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"43 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797722","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}
Eleanora Charnetskaya, Manjunath Chatti, Brittany V. Kerr, Thanh Tran-Phu, Tam D. Nguyen, Pavel V. Cherepanov, Dijon A. Hoogeveen, Bernt Johannessen, Antonio Tricoli, Douglas R. MacFarlane, Rosalie K. Hocking, Alexandr N. Simonov
{"title":"Correction to “Intrinsic Catalytic Activity for the Alkaline Hydrogen Evolution of Layer-Expanded MoS2 Functionalized with Nanoscale Ni and Co Sulfides”","authors":"Eleanora Charnetskaya, Manjunath Chatti, Brittany V. Kerr, Thanh Tran-Phu, Tam D. Nguyen, Pavel V. Cherepanov, Dijon A. Hoogeveen, Bernt Johannessen, Antonio Tricoli, Douglas R. MacFarlane, Rosalie K. Hocking, Alexandr N. Simonov","doi":"10.1021/acssuschemeng.4c09479","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09479","url":null,"abstract":"The authors regret that the affiliation recorded for Bernt Johannessen is incomplete. The full affiliation should be ‘Australian Synchrotron, ANSTO, Clayton VIC 3168, Australia’. This change is reflected in the authorship of this Correction. The authors would like to apologize for any inconvenience caused. The correction does not in any way affect results or conclusions of the article. This article has not yet been cited by other publications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"20 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797723","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":"Copper/Iron Cocatalyzed Depolymerization of Postconsumer Polycarbonate: A One-Pot Strategy to Synthesize Aryl Ethers","authors":"Nageswararao Moyilla, Ganeshdev Padhi, Deepti Kalsi, Nagaraju Barsu","doi":"10.1021/acssuschemeng.4c06990","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06990","url":null,"abstract":"The synthesis of value-added chemicals from plastic waste, which poses a significant environmental threat, is both intriguing and challenging. Consequently, developing new methods for the depolymerization of plastic has become essential due to its increasing demand and usage. In this context, we have developed a base-driven, Cu/Fe-cocatalyzed depolymerization method for polycarbonates (PC), transforming them into diaryl ether and diaryl diethers in a one-pot process. This methodology exclusively utilized postconsumed real-life PCs. By varying reaction parameters, we successfully utilized PC as a nucleophile source to produce a range of products including diaryl ethers and diaryl diethers. A wide array of aryl halides and PCs with molecular weights ranging from 86,000 to 20,000 were screened using this approach. Gram-scale reactions underscored the potential and scalability of ether synthesis. The synthetic utility of the obtained ethers was further explored, leading to the synthesis of diverse value-added products. NMR experiments revealed that the depolymerization of PCs is driven by the base, which subsequently generates potassium diphenolate for cross-coupling with aryl halides in the presence of the Cu/Fe cocatalytic system.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"2 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142788802","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":"Comparative Industrial-Scale Life Cycle Assessment of Base Case and Heat Recovery Scenarios for Carbon Capture from Natural Gas Combined Cycle Power Plants Using Aqueous Ammonia","authors":"Pancy Ang, Wayne Goh, Jie Bu, Shuying Cheng","doi":"10.1021/acssuschemeng.4c06660","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06660","url":null,"abstract":"As social and economic activities return to pre-COVID-19 levels, greenhouse gas emissions continue to rise, exacerbating climate change. This study explores carbon capture and sequestration (CCS) technologies to mitigate carbon dioxide (CO<sub>2</sub>) emissions from natural gas combined cycle (NGCC) power plants, proposing aqueous ammonia as a solvent due to its high reactivity and lower energy regeneration requirements. A life cycle assessment (LCA) was conducted to compare a base case with a heat recovery scenario for capturing 300 kilotonnes of CO<sub>2</sub> annually from NGCC flue gas. The cradle-to-gate LCA, using a functional unit of 1 tonne of CO<sub>2</sub> input, encompasses the process from flue gas extraction to the production of purified CO<sub>2</sub>. The heat recovery scenario outperformed the base case in all environmental impact categories. The LCA results indicated a net carbon abatement of 94.49 kg CO<sub>2</sub> eq for the base case and 508.69 kg CO<sub>2</sub> eq for the heat recovery scenario. Key contributors to global warming potential (GWP) included electricity consumption and heat production, while the human toxicity potential (HTP) and marine aquatic ecotoxicity potential (MAETP) were significant environmental impact categories. Sensitivity analysis and Monte Carlo simulation highlighted critical parameters and uncertainties, and scenario analysis examined additional variables for a comprehensive assessment. Aqueous ammonia not only lowers emissions but also provides cost-effectiveness and high absorption efficiency, positioning it as a viable option for large-scale CO<sub>2</sub> capture. Additionally, it has potential for future integration with the carbonation of municipal and industrial solid waste, contributing to sustainable waste management and carbon sequestration.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"82 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142789851","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}
Shuntaro Uenuma, Di Liu, Cong Liu, Shota Ando, Hideaki Yokoyama, Kohzo Ito
{"title":"Environmentally Friendly Supramolecular Nanosheet Particles for Surface Coating","authors":"Shuntaro Uenuma, Di Liu, Cong Liu, Shota Ando, Hideaki Yokoyama, Kohzo Ito","doi":"10.1021/acssuschemeng.4c06972","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06972","url":null,"abstract":"Global environmental problems have become increasingly severe in the recent years. Although inorganic nanoparticles and nanosheets (NSs) have been developed for their high functionality and stability, their toxicity and nonbiodegradability significantly impact the environment owing to their accumulation within ecosystems. This paper reports the fabrication of environmentally friendly supramolecular NS particles composed of cyclodextrin (CyD), a natural oligosaccharide, and highly biocompatible polyethers, and their stabilization, antifouling, and biodegradation properties. Supramolecules are typically unstable due to their noncovalent bonds; however, end-capped-pseudopolyrotaxane nanosheets (PPRNSs), featuring a bulky group at the axis end, is water-insoluble, maintaining stability even under extreme dilution. The capped-NSs possess polymer brushes, which, when coated on substrates, do not dissolve in water and exhibit repeatable antifouling properties. The crystalline CyDs in the capped-NSs are not water-soluble; however, biochemical oxygen demand (BOD) tests in seawater demonstrate their biodegradability. Thus, PPRNSs have the potential to be novel NS materials that can address environmental challenges. This study is expected to pave the way for advancements in nanosheet materials science and supramolecular chemistry.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"27 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142788803","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":"Enhanced Rapid and Efficient Recycling of Lithium-Ion Battery Cathode by Synergistic Effects of Ternary Deep Eutectic Solvents ChCl/MClx/Levulinic Acid","authors":"Fengyi Zhou, Yurun Tian, Hongyuan Zhang, Yijun Yin, Zeyu Wang, Rui Qin, Yu Chen, Zhiyong Li, Tiancheng Mu","doi":"10.1021/acssuschemeng.4c06556","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06556","url":null,"abstract":"The rapid growth of spent lithium-ion batteries (LIBs) raises concerns over the supply chain of critical metals and environmental impacts, emphasizing the urgent need for efficient recycling technologies. Due to their potential to reduce the consumption of energy and avoid the use of corrosive acid, deep eutectic solvents (DESs) have been widely studied to selectively leach and recover valuable metals from spent LIBs. There is general agreement that DESs with high acidity, coordination, reducibility, and low viscosity could efficiently dissolve cathode materials. However, it is hard to design binary DES compositions to fulfill all of these requirements simultaneously. Herein, this study focuses on the design of ternary DESs, leveraging the synergistic effects of their components to achieve strong coordination and low viscosity, enhanced acidity, and reducibility to efficiently extract valuable metals. Specifically, ChCl/CuCl:4Levulinic acid demonstrated exceptional leaching capabilities, recovering over 90% of LiCoO<sub>2</sub> within 10 min. Furthermore, to ensure the purity of recovered metal products, ChCl/LiCl:8Levulinic acid was investigated to realize the efficient leaching, recovery, and DES regeneration process. It was verified that ChCl/LiCl/8Levulinic acid has high leaching efficiency and good cycling stability and facilitates a convenient recycling process. Overall, this work demonstrates the potential of tailored ternary DESs for the efficient leaching of cathode materials and proposes a sustainable process to realize metal recovery from spent LIB cathode and DES regeneration.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"9 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142763407","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":"Carbon Dioxide-Induced Separations of Terephthalic Acid from Aqueous Disodium Terephthalate Solutions for Polyester Upcycling","authors":"Diego T. Melfi, Aaron M. Scurto","doi":"10.1021/acssuschemeng.4c05645","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c05645","url":null,"abstract":"Depolymerization of polyethylene terephthalate (PET) with sodium hydroxide has been shown to be highly productive and selective toward disodium terephthalate (Na<sub>2</sub>TPA). However, the traditional method to recover terephthalic acid (TPA) from aqueous solution uses strong inorganic acids. As a potential sustainable alternative, gaseous carbon dioxide (CO<sub>2</sub>) may be used as an acid switch for the recovery of pure TPA and the capture of CO<sub>2</sub>. TPA yields up to 94% were verified experimentally. Low temperatures and higher pressures, i.e., high CO<sub>2</sub> solubility, favor the recovery of terephthalic acid. A preliminary sustainability assessment indicates that the choice of CO<sub>2</sub> over HCl may lead to fewer environmental impacts.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"7 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758230","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}