ACS Sustainable Chemistry & Engineering最新文献

{"title":"Highly Selective Separation of Thorium Using an Extraction Resin by Encapsulating an Amine-Based Ionic Liquid In Situ within a Porous Silica–Polymer Matrix Instead of Conventional Impregnation Method","authors":"Zhuang Wang, Dongping Su, Ting Luo, Qiao Yu, Yiting Wang, Xingyue Liu, Xuanhao Huang, Songdong Ding","doi":"10.1021/acssuschemeng.5c00056","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00056","url":null,"abstract":"The separation of thorium from uranium and rare earths is of great significance for a thorium molten salt reactor nuclear energy system. Herein, a novel Aliquat 336@SiO₂–P extraction resin, prepared by the in situ encapsulation of an amine-based ionic liquid (Aliquat 336) into a porous silica–polymer matrix at the same time as the polymerization, was developed for the highly selective separation of Th(IV) over U(VI) and rare earth ions. Batch adsorption studies showed that the prepared Aliquat 336@SiO₂–P extraction resin has excellent selectivity, strong adsorption affinity, and high adsorption capacity for Th(IV). The adsorption process of Th(IV) follows pseudo-second-order kinetics and the Langmuir model, and the adsorption of Th(IV) is a monolayer-type, chemical, exothermic, and spontaneous process with increased entropy, achieving a maximum Th(IV) adsorption capacity (<i>q</i>_max) of 52.4 mg/g. Thorium is adsorbed as a complex anion in an HNO₃ solution, and its adsorption conforms to the anion exchange mechanism. Furthermore, column experiments indicated that Th(IV) can be selectively separated from simulated monazite HNO₃ leach liquor with a recovery rate as high as 97.7%, and the prepared extraction resin has good reusability. Compared to the conventional impregnation method, the Aliquat 336 extractant encapsulated in a porous silica–polymer matrix has significantly lower loss during the adsorption process. Overall, this new extraction resin demonstrates great application potential for the highly efficient separation and recovery of Th(IV) from monazite HNO₃ leach liquor.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"107 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766481","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":"Novel, Clean, and Controlled Method for Surface Oxidation of Photovoltaic Silicon Cutting Waste for High-Performance Si–C Anode Materials","authors":"Liang Wang, Fengshuo Xi, Jie Yu, Shaoyuan Li, Jijun Lu, Zhongqiu Tong, Xiuhua Chen, Kuixian Wei, Wenhui Ma","doi":"10.1021/acssuschemeng.5c00541","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00541","url":null,"abstract":"The trend of large-scale wafer thinning has led to increased surface activity, oxidation, and uneven oxidation interfaces in photovoltaic silicon cutting waste (SCW) produced by diamond wire cutting, posing significant challenges for its use as a silicon–carbon anode material. To address these issues, we propose a green recycling method that utilizes alkaline solutions to recover silicates from etched SCWs, avoiding the highly corrosive HF acid. By combining inexpensive chitosan (CTS) as a soft template, we achieve controllable reshaping of silicates into amorphous oxide layers (1 to 16 nm) on submicron SCW surfaces. This process involves a one-step method in a vacuum autoclave, which simultaneously eliminates the chitosan template and forms both the oxide layer and the phenolic resin. Unlike self-crystallizing oxide layers, the amorphous layers ensure uniform expansion and contraction, facilitate Li⁺ transfer, and introduce structural defects, enhancing lithium storage performance. The resulting Si@SiOx@C composite with a 5 nm thick oxide interface significantly improves the cycling performance, coulombic efficiency, and rate capability of the silicon–carbon material, achieving a reversible capacity of over 1000 mAh g^–1 after 200 cycles at 1 A g^–1. This work demonstrates the value-added utilization of submicron SCWs in the commercial production of high-performance silicon-based lithium-ion battery anodes.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"20 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766480","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":"Porous Sand Disc: A Sustainable Approach for High-Efficiency Solar-Driven Evaporation","authors":"Changzheng Li, Jiaqiang Liao, Jingying Dai, Tao Rui, Hengyi Guo, Xiantao Zhang, Yanjun Chen, Zhi Qun Tian","doi":"10.1021/acssuschemeng.5c01740","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c01740","url":null,"abstract":"The scarcity of freshwater resources represents a significant challenge to the advancement of humanity and society. While solar-driven interfacial evaporation technology offers distinctive advantages, the acquisition and preparation of photothermal materials have significantly hindered its further development. Herein, we introduce a novel approach employing porous sand disc (PSD) as a photothermal material, showcasing exceptional evaporation performance. The natural sand is transformed into a micron-sized superhydrophilic PSD, which is then used to design a one-dimensional and self-water-supplied T-shaped evaporator (T-PSD), that is similar in function to plant transpiration. The T-PSD demonstrates a remarkable evaporation rate of 1.428 kg/(m²·h) with low surface temperature (36.5 °C) under 1 sun, resulting in an impressive evaporation efficiency of 86.1%. The T-PSD maintains a high evaporation performance even when evaporating salt water, attributed to the PSD crystallizing preferentially at the edge. The edge-preferential crystallization significantly enhances the evaporator’s continuous operational capability. Leveraging abundant and cost-effective natural sand as a photothermal material offers a sustainable development approach for advancing interfacial evaporation technology.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"58 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766482","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":"Pathway-Dependent Ion Effects for Electrocatalytic Olefin Epoxidation","authors":"Shuangshuang Cha, Yizhou Yang, Yujia Liu, Chenyang Zhao, Yupeng Tian, Wei Xu, Wei Du, Mengxin Qu, Hanlin Jin, Xuejing Yang, Bing Sun, Ming Gong","doi":"10.1021/acssuschemeng.5c01296","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c01296","url":null,"abstract":"Electrocatalytic oxidation is an emerging substitute for industrially relevant oxidation processes due to its mild conditions and high safety, and the catalytic performance is not only associated with the catalyst structure but also closely related to the interfacial ionic microenvironment. In this work, by using electrocatalytic olefin epoxidation as a representative example, we elucidated the different influencing mechanisms of the interfacial ionic environment toward two distinct mechanisms of indirect oxidation and direct oxidation through a combinatory study via kinetics, capacitance analysis, in situ spectroscopy, and theoretical calculation. In the indirect epoxidation system, the reaction pathway involves the hydrophilic activation of the mediator and its further reaction with olefin near the hydrophobic environment. The hydrophilicity/hydrophobicity characteristics of the anions tailor the interface for dispersing the solvent domains and active species, and the amphipathic sulfonimide anions create optimal performance. In the direct epoxidation system, the large olefin substrate must penetrate into the densely packed anion double layer to contact the surface oxygen species generated in situ on the electrode to be epoxidized, and the limiting factor turns into the crowdedness of the double layer or the anion size. The smaller tetrafluoroborate anions outperformed other larger anions by minimally impacting mass transfer. This work not only highlights the key role of the interfacial ionic environment in modulating organic electrosynthesis but also emphasizes the distinct influences of the microenvironment under different reaction pathways.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"38 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766485","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":"Technoeconomic Assessment of Offshore Carbon Storage Multiphase Source-Sink Matching Based on Multiwell Optimization in Eastern Coastal China","authors":"Xiaoqing Lin, Xingyu Zan, Yuxuan Ying, Panjie Ji, Angjian Wu, Qi Lu, Qunxing Huang, Xiaodong Li, Jianhua Yan","doi":"10.1021/acssuschemeng.4c10624","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10624","url":null,"abstract":"Offshore carbon capture utilization and storage (CCUS) is essential for addressing greenhouse gas emissions in China’s emission-intensive, land-constrained coastal regions. This study combines a dynamic reservoir estimation model with a drilling economic model to develop a multiwell optimization scheme that efficiently balances cost efficiency and storage capacity. The cost of saline aquifer storage varies from $3.69 to $12.51/t_CO2. A multiphase offshore storage source-sink matching model underpinned by a multiwell optimization framework is proposed to minimize full-process costs by integrating emission sources, coastal hubs, transport pipelines, and storage sinks. The network is economically optimized over a 25 year planning horizon to identify the optimal matching schemes, pipeline development, and phased economic evaluations. The results suggest that a 4.59 Gt emission reduction from 154 stationary sources in Zhejiang Province is economically feasible at an expenditure of $236.03 billion. The optimal CCUS network incurs a unit cost of $51.22/t_CO2, dominated by capture cost at 84.23%. The Qiantang, Minjiang, and Fuzhou basins are progressively developed and utilized. Notably, as the learning rate of technological advancements increases from 0.02 to 0.08, the unit capture cost decreases by 50.12%. This study provides guidance for the green low-carbon transition of offshore storage in the coastal regions of China.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"38 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766538","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":"Adjusting the Coordination and Deposition Environment of Zinc Ions to Stabilize the Zn Anode","authors":"Qu Yue, Yu Wan, Lu Qiu, Junhui He, Yuhang Chen, Taotao Gao, Qian Zhao, Xiaoqin Li, Dan Xiao","doi":"10.1021/acssuschemeng.4c10583","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10583","url":null,"abstract":"An economical and eco-friendly food sweetener erythritol with abundant hydroxyl groups and suitable site resistance has been added to ZnSO₄ electrolytes in aqueous Zn ion batteries (AZIBs). Density functional theory (DFT) calculations demonstrate that the O atoms in erythritol molecules can supply electrons to Zn²⁺, thus mitigating an electron transfer from H₂O to Zn²⁺, resulting in erythritol entering the solvation structure of Zn[(H₂O)₆]²⁺ and replacing some water molecules. Spectroscopic analysis confirms the altered solvation structure of Zn²⁺ and the reconstructed hydrogen-bonding network of the ZnSO₄ and erythritol electrolytes. With an equilibrium between “network water” and “free water” induced by erythritol additives, the possibility of active water decomposition is degraded, which further inhibits water-splitting and corrosion side reactions. In addition, theoretical studies and experimental characterizations verify that erythritol additives preferentially adsorb on the surface of Zn anodes, thus effectively protecting Zn anodes and inhibiting the mad growth of dendrites. As a result, the cells with ZnSO₄ + erythritol electrolytes demonstrated significantly higher Coulombic efficiency values and longer lifetimes than those of pure ZnSO₄ electrolytes. This study could advance the research process of small-molecule polyol additives for AZIBs.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"23 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766483","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":"Uranium Extraction from Radioactive Wastewater by NH2-MIL-125 Immobilized in a Double-Network Aerogel Microsphere","authors":"Lu Zhang, Ming-Yi Sun, Xiang-Yu Li, Meng-Yuan Liu, Hong-Yu Chu, Chong-Chen Wang, Peng Wang, Xiao-Hong Yi, Yi Wang, Jiguang Deng","doi":"10.1021/acssuschemeng.5c00543","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00543","url":null,"abstract":"An environmentally friendly adsorbent for recovering nuclear energy source U(VI) from wastewater plays a crucial role in resource recovery and environmental preservation. In this work, a double-network aerogel adsorbent composite constructed from sodium alginate, poly(acrylic acid), and NH₂-MIL-125 (NM@SA) was fabricated by a mild method, which was adopted to remove and concentrate U(VI) in the corresponding simulated wastewater samples. According to the results of adsorption kinetic and isotherm models, the adsorption of U(VI) on NM@SA was a monolayer chemisorption process. The maximum adsorption capacity of NM@SA for U(VI) calculated from the Langmuir model was 703.6 mg·g^–1. In addition, the adsorbent maintained excellent adsorption capacity, recoverability, and reuse in large-scale operation. The same abilities can be demonstrated in real seawater environments. Finally, the potential adsorption mechanisms of U(VI) on NM@SA were discussed in conjunction with the experimental determination and characterization results. Overall, this study introduces an advantageous research approach for treating U(VI)-containing radioactive wastewater.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"40 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737034","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":"One-Pot Biomass Pretreatment for Ethanol Production by Engineered Saccharomyces cerevisiae","authors":"Mairui Zhang, Linjing Jia, Mi Li, Haixin Peng, Ying Tan, Shubhangi Arvelli, Ye Huang, Adriana C. Neves, Eun Joong Oh, Jikai Zhao","doi":"10.1021/acssuschemeng.4c10101","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10101","url":null,"abstract":"This study presents a novel and cost-effective approach to biomass pretreatment that addresses the limitations of conventional methods, which often result in high water and chemical usage as well as the production of chemical-laden wastewater. We investigated the integration of metal oxides (specifically CaO and MgO) for biomass pretreatment and mineral acids (H₂SO₄ or H₃PO₄) for pH adjustment at a high solid loading of 20 wt %. This innovative method allows for direct enzymatic hydrolysis and fermentation of the resulting slurry, effectively eliminating the need for solid–liquid separation and extensive washing. Our findings reveal that hydrolysates from MgO combined with H₃PO₄ or H₂SO₄ were inhibitory to <i>Saccharomyces cerevisiae</i>, resulting in no ethanol production. In contrast, corn stover that was pretreated with CaO and subsequently adjusted to pH with H₃PO₄ demonstrated a higher enzymatic hydrolysis efficiency than the case of adjusting pH with H₂SO₄, achieving over 65% glucan conversion and 80% xylan conversion, along with an ethanol concentration of approximately 33 g/L following separate hydrolysis and fermentation. This enhanced performance can be attributed to reduced osmotic stress, decreased salt toxicity, and minimal formation of inhibitors, as CaO neutralized with H₃PO₄ generated the minimally soluble precipitate Ca₃(PO₄)₂. Furthermore, employing a semisimultaneous saccharification and fermentation process improved sugar utilization efficiency, resulting in an increased ethanol concentration of 46 g/L. The corn stover fermentation residue (CSFR) contained 93% lignin, predominantly of syringyl and guaiacyl types. This study offers a sustainable and scalable method for producing cellulosic ethanol, significantly lowering chemical and water consumption while achieving a high conversion efficiency.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"72 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143734100","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":"Enhancing the Substrate Specificity of Nitrilase toward Aliphatic Nitriles Based on Substrate Channel Design","authors":"Shi-Qian Bian, Zikai Wang, Jin-Song Gong, Chang Su, Heng Li, Zheng-Hong Xu, Jin-Song Shi","doi":"10.1021/acssuschemeng.5c00435","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00435","url":null,"abstract":"Nitrilase has attracted widespread attention due to its efficiency, specificity, and ecofriendliness in the hydrolysis reactions of nitrile compounds. These enzymes can catalyze various substrates, including aliphatic nitriles and aromatic nitriles. However, high substrate specificity is key to efficient catalysis and high-purity product synthesis. This study aims to enhance the preference of nitrilase for aliphatic nitriles through substrate channel engineering to expand its industrial applications. We developed a semirational design workflow that integrates extensive search and deep optimization strategies, relying on computational tools such as substrate channel modeling and molecular docking to systematically identify and optimize key amino acid residues related to substrate binding. Taking 3-chloropropionitrile as an example, the specific activity of the optimal mutant G191A/L194W increased from 2.47 to 58.35 U·mg^–1, with the substrate conversion rate approaching 100%, while the catalytic activity toward aromatic nitriles significantly decreased. Molecular dynamics simulations revealed the correlation between substrate specificity and channel morphology regulated by W194 and promoted the formation of a specificity-enhanced mutant network. This study provides a structural and mechanistic basis for substrate channel design and enzyme function modification and validates its potential for industrial applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"2 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736376","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":"Cold-Pressing Strategy for Constructing Simple and High-Performance Dendrite-Free Zinc Anodes for Aqueous Zinc-Ion Batteries","authors":"Yu Zhang, Zhenyu Hu, Yiyang Bi, Songlin Tian, Haoran Sun, Kai Li, Wanqiang Liu, Lianshan Sun, Wei Liu, Dong Wang","doi":"10.1021/acssuschemeng.5c00832","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00832","url":null,"abstract":"Dendrite growth, corrosion, and side reactions on zinc anodes significantly hinder the commercialization of aqueous zinc-ion batteries (AZIBs). To address these challenges, we propose a simple and cost-effective room-temperature cold-pressing process to build dendrite-free zinc anodes by means of a special collector-composite structure. Specifically, the symmetric cell assembled with copper mesh (CM) based Zn anodes exhibited remarkable cycling stability over 4000 h at 1 mA cm^–2 current density and also exhibited an exceptionally long life of over 2800 h at 5 mA cm^–2 current density, reflecting the Stability of Zn zinc plating/stripping cycles. In situ optical microscopy was employed to investigate the deposition behavior of the CM electrode during repeated plating and stripping processes. Density functional theory (DFT) calculates that Zn²⁺ ions are preferentially adsorbed on the copper surface, while COMSOL simulation elucidates the homogeneous electric field and current density distribution due to the unique three-dimensional structure of the CM electrode. These synergistic effects effectively inhibited the growth of dendrites, ensuring a stable zinc deposition process. This work provides a scalable approach for designing dendrite-free zinc anodes for practical AZIB applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"31 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723601","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}