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Lithium Recovery and Conversion from Wastewater Produced by Recycling of Li-Ion Batteries via Two-Stage Electrodialysis 通过两级电渗析从回收锂离子电池产生的废水中回收和转化锂
IF 8.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.4c07708
A.H.M. Golam Hyder, Bintang Nuraeni, Sabine M. Gallagher, Mason Wasilk, Jessica D. Macholz, Albert L. Lipson, Jeffrey Spangenberger
Electrodialysis (ED) is a membrane separation technique that has been well-established in various applications such as desalination, drinking water production, wastewater treatment, and lithium salt production. A limited number of studies have explored its application in lithium salt production, especially from secondary resources like wastewater. This study investigated a route to recover lithium from wastewater generated from the recycling of end-of-life Li-ion batteries. Two electrodialysis methods, namely standard electrodialysis (ED) and bipolar-membrane electrodialysis (BPED), were combined to concentrate lithium ions and convert them to lithium hydroxide (LiOH), a valuable product that can be fed back into the supply chain for manufacturing Li-ion batteries. Lithium (Li+) concentration in recycling wastewater was successfully increased by 58% using ED and converted to LiOH (>96% purity) with a further increase in Li+ concentration by 67% using BPED. The Coulombic efficiency of the experiments was 91.0 and 92.2%, with specific energy consumption of 1 and 2.5 kWh/kg, and a production rate of 1.01 and 0.14 kg/h/m2 for the ED and BPED processes, respectively. In addition, preliminary techno-economic and environmental impact analyses show a significant improvement (GHG emission reduction by 77% and total energy reduction by 53%) by producing LiOH via electrodialysis compared to conventional lithium production via brine extraction. The process was assessed to be beneficial for lithium extraction from secondary resources and to enhance overall battery recycling efforts.
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引用次数: 0
Enhancing Biological CO to Formate Conversion: Application of Aerophobic Coatings to Mitigate Bubble Coalescence
IF 7.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.5c0019810.1021/acssuschemeng.5c00198
Tae-Hwan Kim, Jiung Yun, Jang-Seob Lee, Myeong-Jun Lee, Jung Kyu Kim, Jinwon Lee, Yong Hwan Kim, Jeong-Geol Na* and Byung-Keun Oh*, 

Biological carbon monoxide (CO) conversion to formate is hindered by gas–liquid mass transfer limitations due to bubble coalescence, which reduces the interfacial area for gas exchange. In this study, we introduce a novel approach by applying an aerophobic coating to a perforated baffle in an airlift bioreactor. This aerophobic coating prevents bubble coalescence, thereby enhancing mass transfer efficiency and increasing the conversion rate of CO to formate. First, we confirmed that in enzymatic reactions, the mass transfer rate of CO gas determines the maximum productivity under optimal conditions. We optimized the aerophobic coating conditions for the perforated baffle to achieve effective bubble breakage. By installing the aerophobic-coated perforated baffle with optimized coating conditions into the reactor, we promoted efficient bubble breakage, reduced bubble size, and increased gas–liquid mass transfer coefficients. This resulted in the maximum volumetric productivity of 60.4 mM/h in CO-to-formate conversion, a 72% increase over the bioreactor without a coated baffle. This significant improvement demonstrates the effectiveness of aerophobic coatings in enhancing gas–liquid mass transfer, providing a new strategy to increase efficiency and scalability in the biological gas conversion industry.

{"title":"Enhancing Biological CO to Formate Conversion: Application of Aerophobic Coatings to Mitigate Bubble Coalescence","authors":"Tae-Hwan Kim,&nbsp;Jiung Yun,&nbsp;Jang-Seob Lee,&nbsp;Myeong-Jun Lee,&nbsp;Jung Kyu Kim,&nbsp;Jinwon Lee,&nbsp;Yong Hwan Kim,&nbsp;Jeong-Geol Na* and Byung-Keun Oh*,&nbsp;","doi":"10.1021/acssuschemeng.5c0019810.1021/acssuschemeng.5c00198","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00198https://doi.org/10.1021/acssuschemeng.5c00198","url":null,"abstract":"<p >Biological carbon monoxide (CO) conversion to formate is hindered by gas–liquid mass transfer limitations due to bubble coalescence, which reduces the interfacial area for gas exchange. In this study, we introduce a novel approach by applying an aerophobic coating to a perforated baffle in an airlift bioreactor. This aerophobic coating prevents bubble coalescence, thereby enhancing mass transfer efficiency and increasing the conversion rate of CO to formate. First, we confirmed that in enzymatic reactions, the mass transfer rate of CO gas determines the maximum productivity under optimal conditions. We optimized the aerophobic coating conditions for the perforated baffle to achieve effective bubble breakage. By installing the aerophobic-coated perforated baffle with optimized coating conditions into the reactor, we promoted efficient bubble breakage, reduced bubble size, and increased gas–liquid mass transfer coefficients. This resulted in the maximum volumetric productivity of 60.4 mM/h in CO-to-formate conversion, a 72% increase over the bioreactor without a coated baffle. This significant improvement demonstrates the effectiveness of aerophobic coatings in enhancing gas–liquid mass transfer, providing a new strategy to increase efficiency and scalability in the biological gas conversion industry.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 12","pages":"4897–4907 4897–4907"},"PeriodicalIF":7.1,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737433","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}
引用次数: 0
Simulated Environmental Nanoplastics Induce Zebrafish Developmental Toxicity and Stress Response
IF 7.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.4c1084710.1021/acssuschemeng.4c10847
Astrid Saraceni, Andrey Ethan Rubin, Yair Wexler, Yoav Gothilf, Patrizia Bovolin and Ines Zucker*, 

Nanoplastics (NPs) pose emerging risks to both the environment and human health. In this study, we use a zebrafish in vivo model to study─and compare─the physicochemical and toxicological effects of two distinct polystyrene NPs: widely used commercial polymeric nanobeads and nanoscale simulated environmental plastics (SEPs) engineered using a top-down accelerated weathering protocol. Zebrafish embryos and larvae exposed to NPs were assessed for changes in development, growth, locomotor activity, and stress and hypoxic responses. SEP─besides being more environmentally relevant than the commercial nanobeads─significantly delayed hatching and reduced body length (up to 150 μm shorter) compared to the minor effects of the nanobeads at the same concentrations. Moreover, SEPs impaired locomotor activity (40% reduction in distance traveled) and triggered a dose-dependent stress response, increasing cortisol levels (2–3 fold) and upregulating stress and hypoxia-related genes. The stress-related condition induced by SEP exposure, observed throughout the study, involved alterations in the hypothalamic-pituitary-adrenal-interrenal (HPA/HPI) axis, particularly in glucocorticoid signaling (i.e., cortisol), which plays a crucial role in regulating stress responses and developmental processes. These alterations could potentially influence the development and adult life of living organisms, including the onset of associated pathologies. Furthermore, these findings underscore significant ecological and health risks, as even low concentrations of NPs in aquatic ecosystems may impair fish populations and biodiversity while also presenting potential human health hazards through the contamination of water sources and seafood. Notably, all reported effects occurred at a relatively low concentration (0.1 μg/L), emphasizing the need for rigorous NP risk assessment and the importance of selecting an appropriate and environmentally relevant experimental model.

This study compares the toxicity of two polystyrene nanoplastics in zebrafish larvae and examines the impact on the stress axis.

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引用次数: 0
New Insights for Biomass Utilization by Brown-Rot and White-Rot Fungi: the Differing Role of Hemicellulose Degradation in the Incipient Decay Process
IF 7.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.5c0088210.1021/acssuschemeng.5c00882
Yan Li, Chenpu Huang, Yaru Mao, Wei Zeng, Xu Zhao, Yuan Zhu* and Xianjun Li*, 

Both brown-rot fungi and white-rot fungi are known to degrade hemicellulose in incipient decay, but the role of hemicellulose degradation in the wood decay process remains unclear. Here, Trametes versicolor and Gloeophyllum trabeum were used to colonize poplar wood for 3, 6, 9, 12, and 15 days to analyze the changes in chemistry, crystalline structure, and microstructure. Poplar wood incubated with G. trabeum (a brown-rot fungus) for 15 days released 13.5 mg/g of total soluble sugars, nearly three times the 4.5 mg/g observed in wood with T. versicolor (a white-rot fungus) incubation. All data indicate that G. trabeum has a limited capacity to utilize hemicellulose, resulting in diffusion that opens the cell walls and exposes cellulose for degradation. T. versicolor efficiently depolymerizes and utilizes hemicellulose, promoting mycelial growth and resulting in erosion-type decay. These findings contribute to a deeper understanding of fungal degradation mechanisms, offering valuable insights for modifying wood microstructures to develop novel wood-based functional materials and for improving biomass resource refining and wood protection.

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引用次数: 0
Tannic Acid-Fe3+ Network-Coated Defective Bimetallic ZnM-ZIF (M = Cu and Ni) for Enhanced Pesticide-Loading Capacity and Pest Control
IF 8.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.5c00662
Jie Zhou, Guangyang Liu, Ying Zhang, Zhihao Lin, Miao Wang, Bining Jiao, Yiming Zhao, Ge Chen, Xin Yang, Jun Lv, Donghui Xu
Zeolite imidazolate frameworks (ZIFs) are ideal candidates for pesticide carriers due to their simple preparation and biocompatibility. However, the reported ZIF carriers generally have low loading capacity with an unclear structure–property relationship. Herein, two novel defective bimetallic ZnM-ZIFs (M = Cu and Ni) based on leafy ZIF-L were prepared as carriers, and the correlation between structural property and loading capacity was studied using gray correlation analysis. The results showed that the second metal created defects in leafy ZnM-ZIFs that increased its mesoporosity and oxygen vacancy, thus improving the pesticide loading rate. Among them, Zn0.6Cu0.4-ZIF (30.96%) and Zn0.4Ni0.6-ZIF (19.03%) showed the highest loading rate for imidacloprid (IMI), which was 2.31 and 1.42 times higher than that of ZIF-L, respectively. After coating the metal-phenolic network (MPN) as a blocker, the final ZnM-ZIF@IMI@MPN showed higher insecticidal activity against Bemisia tabaci (1.47–1.98 times) and longer efficacy duration (1.51–1.65 times) than IMI technical (TC). Besides, the ZnM-ZIF@IMI@MPN exhibited higher photostability (2.33–2.97 times that of the TC), good pH-responsive release, stronger foliar adhesion, and favorable safety. This work gives deep insight into the effect of the second metal on the loading performance of ZnM-ZIF and provides a strategy for developing a defective bimetallic ZIF pesticide system.
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引用次数: 0
Simulated Environmental Nanoplastics Induce Zebrafish Developmental Toxicity and Stress Response 模拟环境纳米塑料诱导斑马鱼发育毒性和应激反应
IF 8.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.4c10847
Astrid Saraceni, Andrey Ethan Rubin, Yair Wexler, Yoav Gothilf, Patrizia Bovolin, Ines Zucker
Nanoplastics (NPs) pose emerging risks to both the environment and human health. In this study, we use a zebrafish in vivo model to study─and compare─the physicochemical and toxicological effects of two distinct polystyrene NPs: widely used commercial polymeric nanobeads and nanoscale simulated environmental plastics (SEPs) engineered using a top-down accelerated weathering protocol. Zebrafish embryos and larvae exposed to NPs were assessed for changes in development, growth, locomotor activity, and stress and hypoxic responses. SEP─besides being more environmentally relevant than the commercial nanobeads─significantly delayed hatching and reduced body length (up to 150 μm shorter) compared to the minor effects of the nanobeads at the same concentrations. Moreover, SEPs impaired locomotor activity (40% reduction in distance traveled) and triggered a dose-dependent stress response, increasing cortisol levels (2–3 fold) and upregulating stress and hypoxia-related genes. The stress-related condition induced by SEP exposure, observed throughout the study, involved alterations in the hypothalamic-pituitary-adrenal-interrenal (HPA/HPI) axis, particularly in glucocorticoid signaling (i.e., cortisol), which plays a crucial role in regulating stress responses and developmental processes. These alterations could potentially influence the development and adult life of living organisms, including the onset of associated pathologies. Furthermore, these findings underscore significant ecological and health risks, as even low concentrations of NPs in aquatic ecosystems may impair fish populations and biodiversity while also presenting potential human health hazards through the contamination of water sources and seafood. Notably, all reported effects occurred at a relatively low concentration (0.1 μg/L), emphasizing the need for rigorous NP risk assessment and the importance of selecting an appropriate and environmentally relevant experimental model.
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引用次数: 0
New Insights for Biomass Utilization by Brown-Rot and White-Rot Fungi: the Differing Role of Hemicellulose Degradation in the Incipient Decay Process 褐根真菌和白根真菌利用生物质的新见解:半纤维素降解在萌芽腐烂过程中的不同作用
IF 8.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.5c00882
Yan Li, Chenpu Huang, Yaru Mao, Wei Zeng, Xu Zhao, Yuan Zhu, Xianjun Li
Both brown-rot fungi and white-rot fungi are known to degrade hemicellulose in incipient decay, but the role of hemicellulose degradation in the wood decay process remains unclear. Here, Trametes versicolor and Gloeophyllum trabeum were used to colonize poplar wood for 3, 6, 9, 12, and 15 days to analyze the changes in chemistry, crystalline structure, and microstructure. Poplar wood incubated with G. trabeum (a brown-rot fungus) for 15 days released 13.5 mg/g of total soluble sugars, nearly three times the 4.5 mg/g observed in wood with T. versicolor (a white-rot fungus) incubation. All data indicate that G. trabeum has a limited capacity to utilize hemicellulose, resulting in diffusion that opens the cell walls and exposes cellulose for degradation. T. versicolor efficiently depolymerizes and utilizes hemicellulose, promoting mycelial growth and resulting in erosion-type decay. These findings contribute to a deeper understanding of fungal degradation mechanisms, offering valuable insights for modifying wood microstructures to develop novel wood-based functional materials and for improving biomass resource refining and wood protection.
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引用次数: 0
Lithium Recovery and Conversion from Wastewater Produced by Recycling of Li-Ion Batteries via Two-Stage Electrodialysis
IF 7.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.4c0770810.1021/acssuschemeng.4c07708
A.H.M. Golam Hyder, Bintang Nuraeni, Sabine M. Gallagher, Mason Wasilk, Jessica D. Macholz*, Albert L. Lipson and Jeffrey Spangenberger, 

Electrodialysis (ED) is a membrane separation technique that has been well-established in various applications such as desalination, drinking water production, wastewater treatment, and lithium salt production. A limited number of studies have explored its application in lithium salt production, especially from secondary resources like wastewater. This study investigated a route to recover lithium from wastewater generated from the recycling of end-of-life Li-ion batteries. Two electrodialysis methods, namely standard electrodialysis (ED) and bipolar-membrane electrodialysis (BPED), were combined to concentrate lithium ions and convert them to lithium hydroxide (LiOH), a valuable product that can be fed back into the supply chain for manufacturing Li-ion batteries. Lithium (Li+) concentration in recycling wastewater was successfully increased by 58% using ED and converted to LiOH (>96% purity) with a further increase in Li+ concentration by 67% using BPED. The Coulombic efficiency of the experiments was 91.0 and 92.2%, with specific energy consumption of 1 and 2.5 kWh/kg, and a production rate of 1.01 and 0.14 kg/h/m2 for the ED and BPED processes, respectively. In addition, preliminary techno-economic and environmental impact analyses show a significant improvement (GHG emission reduction by 77% and total energy reduction by 53%) by producing LiOH via electrodialysis compared to conventional lithium production via brine extraction. The process was assessed to be beneficial for lithium extraction from secondary resources and to enhance overall battery recycling efforts.

{"title":"Lithium Recovery and Conversion from Wastewater Produced by Recycling of Li-Ion Batteries via Two-Stage Electrodialysis","authors":"A.H.M. Golam Hyder,&nbsp;Bintang Nuraeni,&nbsp;Sabine M. Gallagher,&nbsp;Mason Wasilk,&nbsp;Jessica D. Macholz*,&nbsp;Albert L. Lipson and Jeffrey Spangenberger,&nbsp;","doi":"10.1021/acssuschemeng.4c0770810.1021/acssuschemeng.4c07708","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c07708https://doi.org/10.1021/acssuschemeng.4c07708","url":null,"abstract":"<p >Electrodialysis (ED) is a membrane separation technique that has been well-established in various applications such as desalination, drinking water production, wastewater treatment, and lithium salt production. A limited number of studies have explored its application in lithium salt production, especially from secondary resources like wastewater. This study investigated a route to recover lithium from wastewater generated from the recycling of end-of-life Li-ion batteries. Two electrodialysis methods, namely standard electrodialysis (ED) and bipolar-membrane electrodialysis (BPED), were combined to concentrate lithium ions and convert them to lithium hydroxide (LiOH), a valuable product that can be fed back into the supply chain for manufacturing Li-ion batteries. Lithium (Li<sup>+</sup>) concentration in recycling wastewater was successfully increased by 58% using ED and converted to LiOH (&gt;96% purity) with a further increase in Li<sup>+</sup> concentration by 67% using BPED. The Coulombic efficiency of the experiments was 91.0 and 92.2%, with specific energy consumption of 1 and 2.5 kWh/kg, and a production rate of 1.01 and 0.14 kg/h/m<sup>2</sup> for the ED and BPED processes, respectively. In addition, preliminary techno-economic and environmental impact analyses show a significant improvement (GHG emission reduction by 77% and total energy reduction by 53%) by producing LiOH via electrodialysis compared to conventional lithium production via brine extraction. The process was assessed to be beneficial for lithium extraction from secondary resources and to enhance overall battery recycling efforts.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 12","pages":"4651–4660 4651–4660"},"PeriodicalIF":7.1,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737435","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}
引用次数: 0
Reactive Capture and Conversion of Carbon Dioxide to Methanol with ZnZrO2 and Alkali-Promoted Mg3AlOx Mixed Oxide Catalytic Sorbents
IF 7.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.4c1056210.1021/acssuschemeng.4c10562
Laura Proaño, Katlo Galefete, Guanhe Rim, Gabriel Gusmão and Christopher W. Jones*, 

Reactive capture and conversion (RCC) explores the use of a single-unit process to capture CO2 and produce a product, in this case, methanol (MeOH). In this study, different configurations of a catalytic sorbent (CS) composed of ZnZrO2 catalyst and Mg3AlOx sorbent with and without alkali modification are evaluated for CO2 adsorption, steady-state catalysis with cofed CO2 and H2, and transient RCC performance. A catalyst composed of a physical mixture of Mg3AlOx with ZnZrO2 resulted in a slight increase in CO2 uptake, with a low impact on the catalytic activity and RCC of the materials compared to ZnZrO2 alone. In contrast, Na impregnation significantly increased the level of CO2 uptake from 0.28 mmol/g (ZnZrO2 alone) to 0.6 and 1.1 mmol/g for the CS with Na on the catalyst or Mg3AlOx, respectively. However, Na impregnation reduced the CO2 conversion rate and MeOH selectivity during steady-state cofeed experiments at 300 °C and 6 bar. In contrast to steady-state catalysis conditions, RCC, which is a cyclic capture and conversion process, creates dynamic CO2 and H2 surface coverages, favoring CH4 in the early stages of the conversion step and then CO and MeOH as the catalyst CO2 coverage reduces. The highest MeOH productivity during RCC was achieved with CS that balanced the CO2 uptake with only moderate catalyst rate reductions caused by Na addition. The optimal material, ZnZrO2+10%Na/Mg3AlOx, achieved a CO2 uptake of 0.8 mmol/g and a MeOH productivity of 0.5 mmol/g with 100% selectivity at 260 °C and 6 bar during RCC. This marks the highest RCC MeOH productivity reported to date, although the process needs further optimization and even with optimization, may remain impractical. The results further demonstrate that optimization of catalytic sorbents under steady-state flow conditions does not easily correlate to transient capture and conversion cycles for methanol synthesis from CO2.

Catalytic sorbent configurations were evaluated for reactive capture and conversion of CO2 to CH3OH.

{"title":"Reactive Capture and Conversion of Carbon Dioxide to Methanol with ZnZrO2 and Alkali-Promoted Mg3AlOx Mixed Oxide Catalytic Sorbents","authors":"Laura Proaño,&nbsp;Katlo Galefete,&nbsp;Guanhe Rim,&nbsp;Gabriel Gusmão and Christopher W. Jones*,&nbsp;","doi":"10.1021/acssuschemeng.4c1056210.1021/acssuschemeng.4c10562","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10562https://doi.org/10.1021/acssuschemeng.4c10562","url":null,"abstract":"<p >Reactive capture and conversion (RCC) explores the use of a single-unit process to capture CO<sub>2</sub> and produce a product, in this case, methanol (MeOH). In this study, different configurations of a catalytic sorbent (CS) composed of ZnZrO<sub>2</sub> catalyst and Mg<sub>3</sub>AlO<sub><i>x</i></sub> sorbent with and without alkali modification are evaluated for CO<sub>2</sub> adsorption, steady-state catalysis with cofed CO<sub>2</sub> and H<sub>2</sub>, and transient RCC performance. A catalyst composed of a physical mixture of Mg<sub>3</sub>AlO<sub><i>x</i></sub> with ZnZrO<sub>2</sub> resulted in a slight increase in CO<sub>2</sub> uptake, with a low impact on the catalytic activity and RCC of the materials compared to ZnZrO<sub>2</sub> alone. In contrast, Na impregnation significantly increased the level of CO<sub>2</sub> uptake from 0.28 mmol/g (ZnZrO<sub>2</sub> alone) to 0.6 and 1.1 mmol/g for the CS with Na on the catalyst or Mg<sub>3</sub>AlO<sub><i>x</i></sub>, respectively. However, Na impregnation reduced the CO<sub>2</sub> conversion rate and MeOH selectivity during steady-state cofeed experiments at 300 °C and 6 bar. In contrast to steady-state catalysis conditions, RCC, which is a cyclic capture and conversion process, creates dynamic CO<sub>2</sub> and H<sub>2</sub> surface coverages, favoring CH<sub>4</sub> in the early stages of the conversion step and then CO and MeOH as the catalyst CO<sub>2</sub> coverage reduces. The highest MeOH productivity during RCC was achieved with CS that balanced the CO<sub>2</sub> uptake with only moderate catalyst rate reductions caused by Na addition. The optimal material, ZnZrO<sub>2</sub>+10%Na/Mg<sub>3</sub>AlOx, achieved a CO<sub>2</sub> uptake of 0.8 mmol/g and a MeOH productivity of 0.5 mmol/g with 100% selectivity at 260 °C and 6 bar during RCC. This marks the highest RCC MeOH productivity reported to date, although the process needs further optimization and even with optimization, may remain impractical. The results further demonstrate that optimization of catalytic sorbents under steady-state flow conditions does not easily correlate to transient capture and conversion cycles for methanol synthesis from CO<sub>2</sub>.</p><p >Catalytic sorbent configurations were evaluated for reactive capture and conversion of CO<sub>2</sub> to CH<sub>3</sub>OH.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 12","pages":"4811–4822 4811–4822"},"PeriodicalIF":7.1,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acssuschemeng.4c10562","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737386","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tannic Acid-Fe3+ Network-Coated Defective Bimetallic ZnM-ZIF (M = Cu and Ni) for Enhanced Pesticide-Loading Capacity and Pest Control
IF 7.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-21 DOI: 10.1021/acssuschemeng.5c0066210.1021/acssuschemeng.5c00662
Jie Zhou, Guangyang Liu*, Ying Zhang, Zhihao Lin, Miao Wang, Bining Jiao, Yiming Zhao, Ge Chen, Xin Yang, Jun Lv and Donghui Xu*, 

Zeolite imidazolate frameworks (ZIFs) are ideal candidates for pesticide carriers due to their simple preparation and biocompatibility. However, the reported ZIF carriers generally have low loading capacity with an unclear structure–property relationship. Herein, two novel defective bimetallic ZnM-ZIFs (M = Cu and Ni) based on leafy ZIF-L were prepared as carriers, and the correlation between structural property and loading capacity was studied using gray correlation analysis. The results showed that the second metal created defects in leafy ZnM-ZIFs that increased its mesoporosity and oxygen vacancy, thus improving the pesticide loading rate. Among them, Zn0.6Cu0.4-ZIF (30.96%) and Zn0.4Ni0.6-ZIF (19.03%) showed the highest loading rate for imidacloprid (IMI), which was 2.31 and 1.42 times higher than that of ZIF-L, respectively. After coating the metal-phenolic network (MPN) as a blocker, the final ZnM-ZIF@IMI@MPN showed higher insecticidal activity against Bemisia tabaci (1.47–1.98 times) and longer efficacy duration (1.51–1.65 times) than IMI technical (TC). Besides, the ZnM-ZIF@IMI@MPN exhibited higher photostability (2.33–2.97 times that of the TC), good pH-responsive release, stronger foliar adhesion, and favorable safety. This work gives deep insight into the effect of the second metal on the loading performance of ZnM-ZIF and provides a strategy for developing a defective bimetallic ZIF pesticide system.

{"title":"Tannic Acid-Fe3+ Network-Coated Defective Bimetallic ZnM-ZIF (M = Cu and Ni) for Enhanced Pesticide-Loading Capacity and Pest Control","authors":"Jie Zhou,&nbsp;Guangyang Liu*,&nbsp;Ying Zhang,&nbsp;Zhihao Lin,&nbsp;Miao Wang,&nbsp;Bining Jiao,&nbsp;Yiming Zhao,&nbsp;Ge Chen,&nbsp;Xin Yang,&nbsp;Jun Lv and Donghui Xu*,&nbsp;","doi":"10.1021/acssuschemeng.5c0066210.1021/acssuschemeng.5c00662","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00662https://doi.org/10.1021/acssuschemeng.5c00662","url":null,"abstract":"<p >Zeolite imidazolate frameworks (ZIFs) are ideal candidates for pesticide carriers due to their simple preparation and biocompatibility. However, the reported ZIF carriers generally have low loading capacity with an unclear structure–property relationship. Herein, two novel defective bimetallic ZnM-ZIFs (M = Cu and Ni) based on leafy ZIF-L were prepared as carriers, and the correlation between structural property and loading capacity was studied using gray correlation analysis. The results showed that the second metal created defects in leafy ZnM-ZIFs that increased its mesoporosity and oxygen vacancy, thus improving the pesticide loading rate. Among them, Zn<sub>0.6</sub>Cu<sub>0.4</sub>-ZIF (30.96%) and Zn<sub>0.4</sub>Ni<sub>0.6</sub>-ZIF (19.03%) showed the highest loading rate for imidacloprid (IMI), which was 2.31 and 1.42 times higher than that of ZIF-L, respectively. After coating the metal-phenolic network (MPN) as a blocker, the final ZnM-ZIF@IMI@MPN showed higher insecticidal activity against <i>Bemisia tabaci</i> (1.47–1.98 times) and longer efficacy duration (1.51–1.65 times) than IMI technical (TC). Besides, the ZnM-ZIF@IMI@MPN exhibited higher photostability (2.33–2.97 times that of the TC), good pH-responsive release, stronger foliar adhesion, and favorable safety. This work gives deep insight into the effect of the second metal on the loading performance of ZnM-ZIF and provides a strategy for developing a defective bimetallic ZIF pesticide system.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 13","pages":"5131–5144 5131–5144"},"PeriodicalIF":7.1,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143785022","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}
引用次数: 0
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