Anion exchange membrane water electrolyzer (AEMWE) represents a promising sustainable method for large-scale industrial-grade hydrogen manufacturing. However, the sluggish kinetics of the bifunctional oxygen/hydrogen evolution reaction (OER/HER) electrocatalysts makes it imperative to develop high-performance anode and cathode materials. Herein, P-doped β-phase NiMoO4 (p-β-NiMoO4) nanorods were first constructed as the cathode material for HER, and then α-phase NiMoO4 (p-β-NiMoO4-A) derived by an electrochemical phase transformation mechanism was further applied for OER. A series of characterizations supported that applying sufficient anode potential to β-NiMoO4 can drive the phase transformation from beta to alpha. Compared with the directly prepared counterpart, this dynamic phase transformation results in the catalyst tuning the atomic configuration environment, modifying the electronic state, and optimizing the *OH adsorption ability. Consequently, the assembled two-electrode electrolytic cell system contributes remarkable overall water/seawater splitting capacity and outstanding long-term durability even under industrial-grade operating conditions. The AEMWE device with an ultralow cell voltage of 2.15 V at 2.0 A·cm–2 current density confirms the applicability of anode and cathode electrocatalysts. This study could provide a promising path to realize the efficient phase transition of nickel–molybdenum-based materials for industrial clean energy conversion.
{"title":"In Situ Phase Transformation-Induced High-Activity Nickel–Molybdenum Catalyst for Enhancing High-Current-Density Water/Seawater Splitting","authors":"Xinyu Wang, Xu Yu, Pinyi He, Guohui Yang, Fu Qin, Yongkang Yao, Jianliang Bai, Guojun Yuan, Lili Ren","doi":"10.1021/acssuschemeng.4c09957","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09957","url":null,"abstract":"Anion exchange membrane water electrolyzer (AEMWE) represents a promising sustainable method for large-scale industrial-grade hydrogen manufacturing. However, the sluggish kinetics of the bifunctional oxygen/hydrogen evolution reaction (OER/HER) electrocatalysts makes it imperative to develop high-performance anode and cathode materials. Herein, P-doped β-phase NiMoO<sub>4</sub> (<i>p</i>-β-NiMoO<sub>4</sub>) nanorods were first constructed as the cathode material for HER, and then α-phase NiMoO<sub>4</sub> (<i>p</i>-β-NiMoO<sub>4</sub>-A) derived by an electrochemical phase transformation mechanism was further applied for OER. A series of characterizations supported that applying sufficient anode potential to β-NiMoO<sub>4</sub> can drive the phase transformation from beta to alpha. Compared with the directly prepared counterpart, this dynamic phase transformation results in the catalyst tuning the atomic configuration environment, modifying the electronic state, and optimizing the *OH adsorption ability. Consequently, the assembled two-electrode electrolytic cell system contributes remarkable overall water/seawater splitting capacity and outstanding long-term durability even under industrial-grade operating conditions. The AEMWE device with an ultralow cell voltage of 2.15 V at 2.0 A·cm<sup>–2</sup> current density confirms the applicability of anode and cathode electrocatalysts. This study could provide a promising path to realize the efficient phase transition of nickel–molybdenum-based materials for industrial clean energy conversion.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"19 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462457","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}
Pub Date : 2025-02-20DOI: 10.1021/acssuschemeng.4c07565
Mengdi Li, Anyan He, Liheng Deng, Qingmao Yang, Haodong Chu, Chun Shen, Tianwei Tan
Catalytic conversion of cellulose in biomass into 2,5-hexanedione is a significant step for the production of biobased p-xylene (PX), and a precise understanding about the effect of the coexisting hemicellulose and lignin components is extremely essential and desirable, but still severely deficient. Herein, we investigate the above issue by catalytic tests, structural characterizations, and composition analysis. Catalytic tests confirm that the coexisting hemicellulose does not affect cellulose conversion and could be converted into 5-chloro-2-pentanone, while the lignin component plays a detrimental role. Lignin and the oligomers from lignin hydrogenolysis can block the catalytic active sites via deposition due to the strong interaction between lignin and Pd/C catalyst. Meanwhile, there is noncovalent interaction between lignin and cellulose, reducing the accessibility of cellulose to the catalytic active sites including the Pd/C and acidic sites. Basic treatment by NaOH aqueous solution could result in simultaneous removal of lignin and fracture of the biomass structure and hence higher accessibility for the Pd/C catalyst. When the biomass is treated by NaOH with the concentration of 1.0 wt %, the amount of lignin (8.3 wt %) is low enough and the structure is fractured enough to achieve the yield of HDO and DMF comparable to that using sole cellulose as the reactant.
{"title":"Investigation on the Impact of Coexisting Component for the Catalytic Hydrogenolysis of Cellulose in Bagasse to 2,5-Hexanedione","authors":"Mengdi Li, Anyan He, Liheng Deng, Qingmao Yang, Haodong Chu, Chun Shen, Tianwei Tan","doi":"10.1021/acssuschemeng.4c07565","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c07565","url":null,"abstract":"Catalytic conversion of cellulose in biomass into 2,5-hexanedione is a significant step for the production of biobased <i>p</i>-xylene (PX), and a precise understanding about the effect of the coexisting hemicellulose and lignin components is extremely essential and desirable, but still severely deficient. Herein, we investigate the above issue by catalytic tests, structural characterizations, and composition analysis. Catalytic tests confirm that the coexisting hemicellulose does not affect cellulose conversion and could be converted into 5-chloro-2-pentanone, while the lignin component plays a detrimental role. Lignin and the oligomers from lignin hydrogenolysis can block the catalytic active sites via deposition due to the strong interaction between lignin and Pd/C catalyst. Meanwhile, there is noncovalent interaction between lignin and cellulose, reducing the accessibility of cellulose to the catalytic active sites including the Pd/C and acidic sites. Basic treatment by NaOH aqueous solution could result in simultaneous removal of lignin and fracture of the biomass structure and hence higher accessibility for the Pd/C catalyst. When the biomass is treated by NaOH with the concentration of 1.0 wt %, the amount of lignin (8.3 wt %) is low enough and the structure is fractured enough to achieve the yield of HDO and DMF comparable to that using sole cellulose as the reactant.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"2 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452300","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}
Pub Date : 2025-02-20DOI: 10.1021/acssuschemeng.4c03754
Gaia Salvatori, Angela Marchetti, Anna Maria Russo, Jesus Rodriguez, Vadim Scerbacov, Francesco Fianelli, Sara Alfano, Simona Crognale, Alessio Massimi, Simona Rossetti, Giacomo Canali, Tiziana De Micheli, David Bolzonella, Marianna Villano
The production of polyhydroxyalkanoates (PHAs) has been herein investigated by using an organic acid mixture originated from a pilot-scale acidogenic fermentation (AF) of reground pasta (RP) byproduct. The pilot-scale AF process was conducted either under no pH control or with the pH maintained at a value of 5.90, with the two obtained fermented mixtures termed RP-fermented 1 and RP-fermented 2, respectively. The fermented mixtures were fed to a lab-scale sequencing batch reactor (SBR), operated at short hydraulic retention time (HRT, 0.5 days) and sludge retention time (SRT, 1 day) and at two values of the applied organic loading rate (OLR) of 2.12 gCODACIDS/Ld and 4.25 gCODACIDS/Ld. During all of the SBR operating conditions, a high selective microbial pressure was established, as confirmed by both the microbiology analysis and the detected values of the storage yield (which reached a maximum value of 0.68 ± 0.04 CODPHA/CODACIDS). A poly(hydroxybutyrate/hydroxyvalerate) copolymer and a poly(hydroxybutyrate/hydroxyvalerate/hydroxyhexanoate) terpolymer were produced with the RP-fermented 1 and RP-fermented 2 streams, respectively. When the OLR of 2.12 gCODACIDS/Ld was applied to the SBR, the stored copolymer and terpolymer presented very similar molecular weights of 339 and 389 kDa, respectively.
{"title":"Pilot-Scale Acidogenic Fermentation of Reground Pasta Byproduct for Polyhydroxyalkanoate Production with Mixed Microbial Cultures","authors":"Gaia Salvatori, Angela Marchetti, Anna Maria Russo, Jesus Rodriguez, Vadim Scerbacov, Francesco Fianelli, Sara Alfano, Simona Crognale, Alessio Massimi, Simona Rossetti, Giacomo Canali, Tiziana De Micheli, David Bolzonella, Marianna Villano","doi":"10.1021/acssuschemeng.4c03754","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c03754","url":null,"abstract":"The production of polyhydroxyalkanoates (PHAs) has been herein investigated by using an organic acid mixture originated from a pilot-scale acidogenic fermentation (AF) of reground pasta (RP) byproduct. The pilot-scale AF process was conducted either under no pH control or with the pH maintained at a value of 5.90, with the two obtained fermented mixtures termed RP-fermented 1 and RP-fermented 2, respectively. The fermented mixtures were fed to a lab-scale sequencing batch reactor (SBR), operated at short hydraulic retention time (HRT, 0.5 days) and sludge retention time (SRT, 1 day) and at two values of the applied organic loading rate (OLR) of 2.12 gCOD<sub>ACIDS</sub>/Ld and 4.25 gCOD<sub>ACIDS</sub>/Ld. During all of the SBR operating conditions, a high selective microbial pressure was established, as confirmed by both the microbiology analysis and the detected values of the storage yield (which reached a maximum value of 0.68 ± 0.04 COD<sub>PHA</sub>/COD<sub>ACIDS</sub>). A poly(hydroxybutyrate/hydroxyvalerate) copolymer and a poly(hydroxybutyrate/hydroxyvalerate/hydroxyhexanoate) terpolymer were produced with the RP-fermented 1 and RP-fermented 2 streams, respectively. When the OLR of 2.12 gCOD<sub>ACIDS</sub>/Ld was applied to the SBR, the stored copolymer and terpolymer presented very similar molecular weights of 339 and 389 kDa, respectively.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"2 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462279","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}
Pub Date : 2025-02-20DOI: 10.1021/acssuschemeng.4c09449
Zhe Zhang, Chuangang Yao, Haixia Zhang, Yuxi Sun, Baixi Xia, Wanning Liu, Jingyi Ding, Li Zhang, Xiaoshi Lang, Kedi Cai
LiCoO2 is widely used in lithium-ion batteries. Innovatively, this study reveals that by employing a synergistic strategy of Li volatilization and anion doping, LiCoO2-based materials demonstrate exceptional performance as solid oxide fuel cell (SOFC) cathodes. At high temperatures, Li volatilization forms a Co3O4 phase. Concurrently, anionic doping is achieved by substituting F ions for O ions. The synergy of these two strategies increases the concentration of oxygen vacancies and the formation of heterogeneous interfaces, effectively enhancing the adsorption, dissociation, and diffusion rates of oxygen, thereby significantly improving the oxygen reduction reaction (ORR) of LiCoO2 (LCO). LCOF1 (LiCoO1.9F0.1+Co3O4) exhibits an oxygen diffusion coefficient (Dchem) and surface exchange coefficient (Kchem) of 8.85 × 10–5 cm2 s–1 and 7.61 × 10–3 cm s–1, respectively, which are 45% and 26% higher than those of undoped LCO. Furthermore, at 800 °C, LCOF1 achieves a PPD of 0.86 W cm–2 and an Rp as low as 0.012 Ω cm2, representing improvements of 110% in PPD and a reduction of 78.6% in Rp compared to LCO. These findings indicate that the synergistic effect of Li volatilization and F doping is an effective strategy for enhancing the performance of Li-containing cathodes, offering valuable perspectives for the development of high-performance SOFC cathodes.
{"title":"Enhanced Oxygen Reduction Reaction Kinetics of Li-Containing Oxide as a High-Performance Cathode for Solid Oxide Fuel Cells Through Synergistic Li Volatilization and Anion Doping","authors":"Zhe Zhang, Chuangang Yao, Haixia Zhang, Yuxi Sun, Baixi Xia, Wanning Liu, Jingyi Ding, Li Zhang, Xiaoshi Lang, Kedi Cai","doi":"10.1021/acssuschemeng.4c09449","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09449","url":null,"abstract":"LiCoO<sub>2</sub> is widely used in lithium-ion batteries. Innovatively, this study reveals that by employing a synergistic strategy of Li volatilization and anion doping, LiCoO<sub>2</sub>-based materials demonstrate exceptional performance as solid oxide fuel cell (SOFC) cathodes. At high temperatures, Li volatilization forms a Co<sub>3</sub>O<sub>4</sub> phase. Concurrently, anionic doping is achieved by substituting F ions for O ions. The synergy of these two strategies increases the concentration of oxygen vacancies and the formation of heterogeneous interfaces, effectively enhancing the adsorption, dissociation, and diffusion rates of oxygen, thereby significantly improving the oxygen reduction reaction (ORR) of LiCoO<sub>2</sub> (LCO). LCOF1 (LiCoO<sub>1.9</sub>F<sub>0.1</sub>+Co<sub>3</sub>O<sub>4</sub>) exhibits an oxygen diffusion coefficient (<i>D</i><sub>chem</sub>) and surface exchange coefficient (<i>K</i><sub>chem</sub>) of 8.85 × 10<sup>–5</sup> cm<sup>2</sup> s<sup>–1</sup> and 7.61 × 10<sup>–3</sup> cm s<sup>–1</sup>, respectively, which are 45% and 26% higher than those of undoped LCO. Furthermore, at 800 °C, LCOF1 achieves a PPD of 0.86 W cm<sup>–2</sup> and an Rp as low as 0.012 Ω cm<sup>2</sup>, representing improvements of 110% in PPD and a reduction of 78.6% in Rp compared to LCO. These findings indicate that the synergistic effect of Li volatilization and F doping is an effective strategy for enhancing the performance of Li-containing cathodes, offering valuable perspectives for the development of high-performance SOFC cathodes.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"37 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452301","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}
Pub Date : 2025-02-20DOI: 10.1021/acssuschemeng.4c08826
Taynara Oliveira Silva, Rafael Granados-Fernández, Justo Lobato, Marcos R. V. Lanza, Manuel Andrés Rodrigo
This work presents a novel electrochemical cell design, developed using 3D printing technology, which enhances turbulence within the cell to promote increased hydrogen peroxide production. This new design is compared to a conventional flow cell that utilizes the same electrodes, membrane, and interelectrode distance, which has demonstrated strong performance in previous studies. Fluid dynamics and H2O2 production are analyzed in both reactors to assess their performance. Additionally, a scale factor of 12.5 is applied to the new concept to evaluate its effectiveness on a larger scale and increase the technology readiness level (TRL). The results demonstrate Faradaic efficiencies of 90% and energy consumption as low as 13 kW h kg–1, placing them among the highest reported in the literature. The use of identical materials and operating conditions underscores the critical role of mechanical design in electrochemical cells, suggesting that future research in environmental electrochemical technology should prioritize cell designs tailored to specific target processes.
{"title":"Boosting New Electrochemical Reactor Designs to Improve the Performance in H2O2 Production Using Gas Diffusion Electrodes","authors":"Taynara Oliveira Silva, Rafael Granados-Fernández, Justo Lobato, Marcos R. V. Lanza, Manuel Andrés Rodrigo","doi":"10.1021/acssuschemeng.4c08826","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c08826","url":null,"abstract":"This work presents a novel electrochemical cell design, developed using 3D printing technology, which enhances turbulence within the cell to promote increased hydrogen peroxide production. This new design is compared to a conventional flow cell that utilizes the same electrodes, membrane, and interelectrode distance, which has demonstrated strong performance in previous studies. Fluid dynamics and H<sub>2</sub>O<sub>2</sub> production are analyzed in both reactors to assess their performance. Additionally, a scale factor of 12.5 is applied to the new concept to evaluate its effectiveness on a larger scale and increase the technology readiness level (TRL). The results demonstrate Faradaic efficiencies of 90% and energy consumption as low as 13 kW h kg<sup>–1</sup>, placing them among the highest reported in the literature. The use of identical materials and operating conditions underscores the critical role of mechanical design in electrochemical cells, suggesting that future research in environmental electrochemical technology should prioritize cell designs tailored to specific target processes.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"50 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462280","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}
Pub Date : 2025-02-20DOI: 10.1021/acssuschemeng.4c09852
Gaofeng Chen, Zhiwei Wang, Na Guo, Lei Liu, Huina Zhu, Qun Wang, Tingzhou Lei
Alcohols, being a substantial category of hydrogen storage liquid fuels, exhibit promising development potential. Alcohol-based hydrogen storage liquid fuels can be efficiently produced from biomass-derived syngas (CO and H2). Considerable efforts have been made in the conversion of syngas to alcohols through a higher alcohol synthesis (HAS) reaction. However, inevitably, there will be significant generation of H2O and C1 byproducts (CO2 and CH4). In this study, a hydrophobic CoCuSNT@C60 catalyst modified with fullerene (C60, an all-carbon cage molecule) was designed to hinder the formation of H2O and C1 byproducts. The hydrophobic C60 shortened the retention of H2O on the active site interface, restraining the water–gas shift reaction. This leads to a significant decrease in CO2 generation, accompanied by an increase in the CO conversion and selectivity toward alcohols. The hydrophobic CoCuSNT@C60 catalyst was characterized by X-ray diffraction, Fourier transform infrared spectra, N2 adsorption–desorption isotherms, X-ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy. Compared to the unmodified CoCuSNT, the C60-modified hydrophobic CoCuSNT@C60 catalyst possesses higher CO hydrogenation activity and high alcohol selectivity, along with an impressive stability of up to 350 h to meet industrial applications.
{"title":"Preparation of Hydrogen Storage Liquid Fuel by Biomass-Based Syngas from Corn Straw over a C60 Modified Hydrophobic Catalyst","authors":"Gaofeng Chen, Zhiwei Wang, Na Guo, Lei Liu, Huina Zhu, Qun Wang, Tingzhou Lei","doi":"10.1021/acssuschemeng.4c09852","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09852","url":null,"abstract":"Alcohols, being a substantial category of hydrogen storage liquid fuels, exhibit promising development potential. Alcohol-based hydrogen storage liquid fuels can be efficiently produced from biomass-derived syngas (CO and H<sub>2</sub>). Considerable efforts have been made in the conversion of syngas to alcohols through a higher alcohol synthesis (HAS) reaction. However, inevitably, there will be significant generation of H<sub>2</sub>O and C1 byproducts (CO<sub>2</sub> and CH<sub>4</sub>). In this study, a hydrophobic CoCuSNT@C<sub>60</sub> catalyst modified with fullerene (C<sub>60</sub>, an all-carbon cage molecule) was designed to hinder the formation of H<sub>2</sub>O and C1 byproducts. The hydrophobic C<sub>60</sub> shortened the retention of H<sub>2</sub>O on the active site interface, restraining the water–gas shift reaction. This leads to a significant decrease in CO<sub>2</sub> generation, accompanied by an increase in the CO conversion and selectivity toward alcohols. The hydrophobic CoCuSNT@C<sub>60</sub> catalyst was characterized by X-ray diffraction, Fourier transform infrared spectra, N<sub>2</sub> adsorption–desorption isotherms, X-ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy. Compared to the unmodified CoCuSNT, the C<sub>60</sub>-modified hydrophobic CoCuSNT@C<sub>60</sub> catalyst possesses higher CO hydrogenation activity and high alcohol selectivity, along with an impressive stability of up to 350 h to meet industrial applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"28 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452303","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}
CO2 mineralization-coupled amine-looping has great potential for large-scale CO2 emissions reduction. However, it remains uncertain if amine-looping successfully improves CO2 sequestration of typical industrial solid wastes of steel slag and iron tailings and whether this enhancing occurs through an increase in CO2 concentration in solution or by promoting the leaching of calcium ions. Herein, we systematically evaluate the CO2 mineralization of steel slag and iron tailings in the presence of three typical amines: monoethanolamine (MEA), 2-amino-2-methyl-1-propanol (AMP), and piperazine (PZ). Results show that all three amines could significantly enhance the CO2 mineralization performance of steel slag and iron tailings, especially in PZ solution, where the CO2 sequestration capacity of steel slag and iron tailings is promoted from 114.4 and 12.6 g/kg to 202.4 and 50.6 g/kg, respectively. Furthermore, Ca2+/Mg2+ leaching experiments indicate that the enhanced CO2 mineralization by amine may be a result of more CO32– provided by amine-generated carbamate, which facilitates the formation of precipitates by combining with Ca2+/Mg2+. Additionally, the carbonation efficiency of steel slag is stabilized at approximately 51 and 71% by recycling MEA and PZ in four successive reactions, showing a good potential in sequestrating CO2 with an affordable additive cost.
{"title":"Exploring the Enhancement on CO2 Mineralization of Solid Wastes via Amine-Looping","authors":"Yiming Cheng, Zijian Li, Jianan Li, Chang Gao, Changlei Qin","doi":"10.1021/acssuschemeng.4c10088","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10088","url":null,"abstract":"CO<sub>2</sub> mineralization-coupled amine-looping has great potential for large-scale CO<sub>2</sub> emissions reduction. However, it remains uncertain if amine-looping successfully improves CO<sub>2</sub> sequestration of typical industrial solid wastes of steel slag and iron tailings and whether this enhancing occurs through an increase in CO<sub>2</sub> concentration in solution or by promoting the leaching of calcium ions. Herein, we systematically evaluate the CO<sub>2</sub> mineralization of steel slag and iron tailings in the presence of three typical amines: monoethanolamine (MEA), 2-amino-2-methyl-1-propanol (AMP), and piperazine (PZ). Results show that all three amines could significantly enhance the CO<sub>2</sub> mineralization performance of steel slag and iron tailings, especially in PZ solution, where the CO<sub>2</sub> sequestration capacity of steel slag and iron tailings is promoted from 114.4 and 12.6 g/kg to 202.4 and 50.6 g/kg, respectively. Furthermore, Ca<sup>2+</sup>/Mg<sup>2+</sup> leaching experiments indicate that the enhanced CO<sub>2</sub> mineralization by amine may be a result of more CO<sub>3</sub><sup>2–</sup> provided by amine-generated carbamate, which facilitates the formation of precipitates by combining with Ca<sup>2+</sup>/Mg<sup>2+</sup>. Additionally, the carbonation efficiency of steel slag is stabilized at approximately 51 and 71% by recycling MEA and PZ in four successive reactions, showing a good potential in sequestrating CO<sub>2</sub> with an affordable additive cost.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"22 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452302","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}
Pub Date : 2025-02-20DOI: 10.1021/acssuschemeng.4c10420
Wenjin Zhou, Kashif Iqbal, Fuyu Liu, Chun Deng
With the evolution of hydraulic fracturing technology, shale gas development in China’s Sichuan region has become commercialized and highly active. This process consumes a substantial amount of water, currently primarily sourced from rivers and the direct reuse of flowback water. However, there is a lack of systematic water resource management, leading to high water usage per well and potentially significant adverse impacts on the regional ecosystem. This paper proposes an optimization-based water management model for shale gas development, focusing on total dissolved solids (TDS) as the key pollutant. The model considers three wastewater treatment methods: onsite treatment, commercial treatment centers, and reinjection wells, along with wastewater reuse among well pads. The model accounts for geographic factors, treatment capacities, and wastewater composition, ensuring a comprehensive approach to wastewater management in shale gas development. A case study was conducted on three well pads in the Weiyuan shale gas block in Sichuan. The results show that onsite desalination and wastewater reuse between well pads can significantly reduce water management costs and freshwater consumption. Due to geographic factors, such as the mountainous terrain and distance from existing treatment facilities, commercial treatment centers and reinjection wells are not suggested. The average optimized single-well freshwater consumption in Weiyuan is 15,078 m3, which is comparable to the Eagle Ford site’s average of 16,100 m3 in Texas, USA, but significantly lower than the average of 24,415 m3 in Sichuan.
{"title":"Optimization and Analysis of Holistic Wastewater Reusing and Treatment Strategies in Shale Gas Hydraulic Fracturing: A Case Study in Sichuan, China","authors":"Wenjin Zhou, Kashif Iqbal, Fuyu Liu, Chun Deng","doi":"10.1021/acssuschemeng.4c10420","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10420","url":null,"abstract":"With the evolution of hydraulic fracturing technology, shale gas development in China’s Sichuan region has become commercialized and highly active. This process consumes a substantial amount of water, currently primarily sourced from rivers and the direct reuse of flowback water. However, there is a lack of systematic water resource management, leading to high water usage per well and potentially significant adverse impacts on the regional ecosystem. This paper proposes an optimization-based water management model for shale gas development, focusing on total dissolved solids (TDS) as the key pollutant. The model considers three wastewater treatment methods: onsite treatment, commercial treatment centers, and reinjection wells, along with wastewater reuse among well pads. The model accounts for geographic factors, treatment capacities, and wastewater composition, ensuring a comprehensive approach to wastewater management in shale gas development. A case study was conducted on three well pads in the Weiyuan shale gas block in Sichuan. The results show that onsite desalination and wastewater reuse between well pads can significantly reduce water management costs and freshwater consumption. Due to geographic factors, such as the mountainous terrain and distance from existing treatment facilities, commercial treatment centers and reinjection wells are not suggested. The average optimized single-well freshwater consumption in Weiyuan is 15,078 m<sup>3</sup>, which is comparable to the Eagle Ford site’s average of 16,100 m<sup>3</sup> in Texas, USA, but significantly lower than the average of 24,415 m<sup>3</sup> in Sichuan.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"15 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452304","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}
Pub Date : 2025-02-19DOI: 10.1021/acssuschemeng.4c07279
Shuang Liang, Xuechuan Wang, Chao Wei, Long Xie, Xugang Dang
Here, a series of novel multifunctional active smart packaging films (CPTAn) with ammonia sensing and extended food freshness were prepared by using chitosan (CS) and poly(vinyl alcohol) (PVA). Titanium dioxide nanoparticles (TiO2 NPs) and purple cabbage anthocyanins (PKA) were used as functional additives. The CPTA(n) has excellent physical and mechanical properties, antimicrobial properties, UV-blocking properties, and antioxidant activity. Especially, when in a subambient atmosphere, the surface temperature of the CPTA-3 film is reduced by ∼9.6 °C, offering significant advantages for food storage and low-temperature transport over traditional packaging materials. The application of CPTA(n) film in banana preservation showed that the shelf life of bananas packaged with CPTA(n) film could reach at least 10 days. Similarly, the colorimetric dipsticks prepared from CPTA-0 and CPTA-3 were successfully applied to the freshness monitoring of shrimp. This investigation provides a novel perspective on the development of intelligent active packaging with broad applications in seafood and fruit preservation.
{"title":"Engineering a Natural Multifunctional Biomass-Based Composite Nanosystem for Active Smart Packaging and Colorimetric Labels","authors":"Shuang Liang, Xuechuan Wang, Chao Wei, Long Xie, Xugang Dang","doi":"10.1021/acssuschemeng.4c07279","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c07279","url":null,"abstract":"Here, a series of novel multifunctional active smart packaging films (CPTA<i>n</i>) with ammonia sensing and extended food freshness were prepared by using chitosan (CS) and poly(vinyl alcohol) (PVA). Titanium dioxide nanoparticles (TiO<sub>2</sub> NPs) and purple cabbage anthocyanins (PKA) were used as functional additives. The CPTA(<i>n</i>) has excellent physical and mechanical properties, antimicrobial properties, UV-blocking properties, and antioxidant activity. Especially, when in a subambient atmosphere, the surface temperature of the CPTA-3 film is reduced by ∼9.6 °C, offering significant advantages for food storage and low-temperature transport over traditional packaging materials. The application of CPTA(<i>n</i>) film in banana preservation showed that the shelf life of bananas packaged with CPTA(<i>n</i>) film could reach at least 10 days. Similarly, the colorimetric dipsticks prepared from CPTA-0 and CPTA-3 were successfully applied to the freshness monitoring of shrimp. This investigation provides a novel perspective on the development of intelligent active packaging with broad applications in seafood and fruit preservation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"89 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452306","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}
Pub Date : 2025-02-19DOI: 10.1021/acssuschemeng.4c09826
Dingyi Fu, Xin Zhang, Yue Zhou, Kun Yang, Jianming Fan, Liping Li, Chaochao Fu
Inorganic components of the cathode electrolyte interphase (CEI) are key to enhance the electrochemical performance of Li-rich cathode materials. However, optimizing inorganic components to stabilize CEI is still a great challenge due to the complex interfacial side reactions in the cycling process. Herein, the inorganic components of the CEI are modulated by constructing a heteroepitaxial spinel@layered interface on the surface of Li-rich materials via H3BO3-assisted solvothermal post-treatment. The spinel@layered interface regulates the evolution pathway of CEI and the decomposition pathway of the LiPF6-based electrolyte by altering the inherent surface catalytic properties of Li-rich materials, thereby in situ-forming the Li3PO4-dominated CEI. The robust Li3PO4-rich CEI inhibits electrolyte decomposition, shields the cathode from various side reactions, and prevents the layered-to-spinel phase transition, thus significantly improving the electrochemical performance of Li-rich cathode materials. The treated Li-rich oxide exhibits 83.9% and 84.9% capacity and voltage retention after 150 cycles at 200 mA/g, much better than the pristine Li-rich cathode. The findings provide new insights into the regulation of CEI components in improving the electrochemical performance of Li-rich oxide materials.
{"title":"Regulating the Evolution Pathway of the Cathode Electrolyte Interphase to Stabilize Li-Rich Cathode Materials","authors":"Dingyi Fu, Xin Zhang, Yue Zhou, Kun Yang, Jianming Fan, Liping Li, Chaochao Fu","doi":"10.1021/acssuschemeng.4c09826","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09826","url":null,"abstract":"Inorganic components of the cathode electrolyte interphase (CEI) are key to enhance the electrochemical performance of Li-rich cathode materials. However, optimizing inorganic components to stabilize CEI is still a great challenge due to the complex interfacial side reactions in the cycling process. Herein, the inorganic components of the CEI are modulated by constructing a heteroepitaxial spinel@layered interface on the surface of Li-rich materials via H<sub>3</sub>BO<sub>3</sub>-assisted solvothermal post-treatment. The spinel@layered interface regulates the evolution pathway of CEI and the decomposition pathway of the LiPF<sub>6</sub>-based electrolyte by altering the inherent surface catalytic properties of Li-rich materials, thereby in situ-forming the Li<sub>3</sub>PO<sub>4</sub>-dominated CEI. The robust Li<sub>3</sub>PO<sub>4</sub>-rich CEI inhibits electrolyte decomposition, shields the cathode from various side reactions, and prevents the layered-to-spinel phase transition, thus significantly improving the electrochemical performance of Li-rich cathode materials. The treated Li-rich oxide exhibits 83.9% and 84.9% capacity and voltage retention after 150 cycles at 200 mA/g, much better than the pristine Li-rich cathode. The findings provide new insights into the regulation of CEI components in improving the electrochemical performance of Li-rich oxide materials.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"42 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443936","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}
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