ACS Sustainable Chemistry & Engineering最新文献

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Selective Construction of Linear Carbon Chains Using Synthesis Gas (CO/H2) for C1-Elongation via a Three-Step Reaction Cycle
IF 7.1 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-24 DOI: 10.1021/acssuschemeng.4c1067710.1021/acssuschemeng.4c10677
Jeroen T. Vossen, Walter Leitner and Andreas J. Vorholt*, 
{"title":"Selective Construction of Linear Carbon Chains Using Synthesis Gas (CO/H2) for C1-Elongation via a Three-Step Reaction Cycle","authors":"Jeroen T. Vossen,&nbsp;Walter Leitner and Andreas J. Vorholt*,&nbsp;","doi":"10.1021/acssuschemeng.4c1067710.1021/acssuschemeng.4c10677","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10677https://doi.org/10.1021/acssuschemeng.4c10677","url":null,"abstract":"<p >Linear carbon chains in the medium and long-range are ubiquitous structural motifs in alcohols and olefins, constituting major intermediates and products of the chemical industry. In this work, we present a reaction concept to produce and elongate linear carbon chains of defined carbon numbers selectively using synthesis gas as a renewable C1 source. This is achieved via a three-step reaction cycle consisting of alcohol dehydration, C═C bond hydroformylation, and C═O hydrogenation of the intermediate aldehydes, thus restoring the alcohol function after each C1-elongation. In a proof-of-principle study, the dehydration was catalyzed by phosphoric acid, Rh/Biphephos was used for the hydroformylation, and Ru/C was used for the hydrogenation step. Each of the catalyst systems applied in the process was recycled effectively, allowing stepwise C1-elongation. An extension of a C<sub>6</sub> chain up to C<sub>10</sub> was achieved over four cycles involving 12 individual catalytic reactions, and the effects of repeating such a cycle multiple times on the reactions and product mixtures were investigated. The successfully demonstrated concept provides selective access to individual long chain olefins and alcohols of medium and long chain lengths with even or odd carbon numbers starting from renewable feedstocks in a highly flexible and controlled reaction sequence.</p><p >Biobased alcohols can be converted in a three-step reaction cycle with synthesis gas to longer chain products such as olefins, aldehydes, and alcohols selectively with recycling of all the catalysts involved.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 9","pages":"3797–3805 3797–3805"},"PeriodicalIF":7.1,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acssuschemeng.4c10677","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576522","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
Anaerobic Storage of Erythromycin Fermentation Residue for Sustainable Management and Antibiotic Resistance Mitigation
IF 7.1 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-24 DOI: 10.1021/acssuschemeng.5c0010210.1021/acssuschemeng.5c00102
Jianjun Ren, Chuanyang Xu, Jian Zhang, Xuanhe Chen, Dongmin Yin, Chunyu Li, Taoli Huhe and Dongze Niu*, 
{"title":"Anaerobic Storage of Erythromycin Fermentation Residue for Sustainable Management and Antibiotic Resistance Mitigation","authors":"Jianjun Ren,&nbsp;Chuanyang Xu,&nbsp;Jian Zhang,&nbsp;Xuanhe Chen,&nbsp;Dongmin Yin,&nbsp;Chunyu Li,&nbsp;Taoli Huhe and Dongze Niu*,&nbsp;","doi":"10.1021/acssuschemeng.5c0010210.1021/acssuschemeng.5c00102","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c00102https://doi.org/10.1021/acssuschemeng.5c00102","url":null,"abstract":"<p >Ensiling is an effective method for preserving solid organic wastes prior to anaerobic digestion; however, its potential in treating antibiotic fermentation residues remains unclear. This study evaluated the effectiveness of ensiling erythromycin fermentation residue (EFR) with rice straw and a silage additive for erythromycin degradation and reduction of antibiotic resistance genes (ARGs). After 56 days of ensiling, the treated samples showed high fermentation quality; in addition, the erythromycin concentration and ARG abundance decreased by 67 and 78.4%, respectively. Microbial community analysis revealed that the addition of silage additives resulted in a more complex and stable microbial network, suppressing the growth of undesirable microorganisms such as <i>Ruminococcaceae</i> and <i>Clostridiaceae</i>. Compared to traditional methods such as hydrothermal treatment and spray-drying, ensiling achieved cost reductions of 33–61% and significantly reduced CO<sub>2</sub>, SO<sub>2</sub>, and NO<i><sub>x</sub></i> emissions. These findings underscore the potential of optimized silage fermentation to enhance the management of antibiotic fermentation wastes, reduce antibiotic resistance risks, and promote environmental sustainability. Future research should aim to refine fermentation processes further and explore the potential use of ensiled EFR for biogas production, providing a comprehensive solution for waste management and renewable energy generation.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 9","pages":"3806–3816 3806–3816"},"PeriodicalIF":7.1,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576732","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
Encapsulated Platinum–Tin Nanoparticles in Silicalite-1 Zeolite for Methylcyclohexane Dehydrogenation
IF 7.1 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-23 DOI: 10.1021/acssuschemeng.4c0976210.1021/acssuschemeng.4c09762
Wei Shi, Akira Oda*, Yuta Yamamoto, Seio Harada, Takeshi Ohtsu, Kyoichi Sawabe and Atsushi Satsuma, 
{"title":"Encapsulated Platinum–Tin Nanoparticles in Silicalite-1 Zeolite for Methylcyclohexane Dehydrogenation","authors":"Wei Shi,&nbsp;Akira Oda*,&nbsp;Yuta Yamamoto,&nbsp;Seio Harada,&nbsp;Takeshi Ohtsu,&nbsp;Kyoichi Sawabe and Atsushi Satsuma,&nbsp;","doi":"10.1021/acssuschemeng.4c0976210.1021/acssuschemeng.4c09762","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09762https://doi.org/10.1021/acssuschemeng.4c09762","url":null,"abstract":"<p >Catalytic dehydrogenation of methylcyclohexane (MCH) is of great importance for hydrogen storage and transportation, but currently used Pt-based nanoparticle catalysts still suffer from insufficient activity, low selectivity, and short-term stability. In this study, we encapsulated Pt–Sn nanoparticles into the silicalite-1 (S-1) matrix and incorporated Sn into the zeolite framework through one-pot hydrothermal synthesis to overcome the above problems. These Pt–Sn bimetallic catalysts were designed for the first time with a high Sn content (2.8–3.9 wt %, Sn/Pt ratio = 6–8) in zeolite mother gel for MCH dehydrogenation. The introduction of Sn significantly improved the activity and durability of Pt@S-1. Especially, the PtSn@S-1 (Sn/Pt ratio = 6) catalyst showed high MCH conversion (&gt;80% for 2 h) and toluene (TOL) selectivity (∼100%) without cofeeding H<sub>2</sub>. Even after a long-term stability test for 33 h under a weight hourly space velocity (WHSV) of 120,000 mL/g/h, no obvious deactivation was observed, and this catalyst retained a superior H<sub>2</sub> evolution rate normalized with a surface Pt content of 1343 mmol<sub>H<sub>2</sub></sub>/g<sub>Pt</sub>/min. The structure–catalytic property relationship of PtSn@S-1 catalysts was systematically studied. Upon Sn introduction, PtO<sub><i>x</i></sub> species on Pt@S-1 were transformed into the PtSn alloy. With the further increase of the Sn/Pt ratio from 1 to 6, Sn was gradually incorporated into the zeolite framework, and this PtSn alloy evolved into a core–shell structure with a Pt core and a Sn shell. Despite the reduced proportion of surface Pt, these unique structures enabled the modification of the Pt local structure, promoted TOL desorption, and enhanced the stability of Pt–Sn nanoparticles, therefore achieving high activity, selectivity, and durability for MCH dehydrogenation.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 9","pages":"3608–3621 3608–3621"},"PeriodicalIF":7.1,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576676","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
Preparation of High Antibacterial, Easy Coating, and Easy Cleaning Pea Protein Isolate/Zein-Carboxymethyl Cellulose Composite Coating Material and Its Preservation Application
IF 7.1 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-23 DOI: 10.1021/acssuschemeng.4c1029810.1021/acssuschemeng.4c10298
Runyi Qu, Bihua Xia*, Mingxuan Hou, Jin Xu, Yijie Wang, Ting Li, Mingqing Chen, Shibo Wang and Weifu Dong*, 
{"title":"Preparation of High Antibacterial, Easy Coating, and Easy Cleaning Pea Protein Isolate/Zein-Carboxymethyl Cellulose Composite Coating Material and Its Preservation Application","authors":"Runyi Qu,&nbsp;Bihua Xia*,&nbsp;Mingxuan Hou,&nbsp;Jin Xu,&nbsp;Yijie Wang,&nbsp;Ting Li,&nbsp;Mingqing Chen,&nbsp;Shibo Wang and Weifu Dong*,&nbsp;","doi":"10.1021/acssuschemeng.4c1029810.1021/acssuschemeng.4c10298","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10298https://doi.org/10.1021/acssuschemeng.4c10298","url":null,"abstract":"<p >This paper fabricated a new kind of pea protein isolate/Zein-carboxymethyl cellulose composite coating material with Pickering emulsion morphology through the solution blending method. The pea protein isolate/Zein-carboxymethyl cellulose composite coating material exhibited high antibacterial properties, delayed spoilage, and easy-to-coat and easy-to-clean properties. In addition, the ultraviolet shielding properties, hydrophilicity and hydrophobicity, antibacterial properties, antioxidant properties, and preservation properties of fruits were studied. This pea protein isolate/Zein-carboxymethyl cellulose composite coating material avoided the volatilization of clove essential oil and achieved long-term antibacterial properties, and it is fit for the preservation material field.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 9","pages":"3728–3740 3728–3740"},"PeriodicalIF":7.1,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576679","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
Encapsulated Platinum–Tin Nanoparticles in Silicalite-1 Zeolite for Methylcyclohexane Dehydrogenation
IF 8.4 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-23 DOI: 10.1021/acssuschemeng.4c09762
Wei Shi, Akira Oda, Yuta Yamamoto, Seio Harada, Takeshi Ohtsu, Kyoichi Sawabe, Atsushi Satsuma
{"title":"Encapsulated Platinum–Tin Nanoparticles in Silicalite-1 Zeolite for Methylcyclohexane Dehydrogenation","authors":"Wei Shi, Akira Oda, Yuta Yamamoto, Seio Harada, Takeshi Ohtsu, Kyoichi Sawabe, Atsushi Satsuma","doi":"10.1021/acssuschemeng.4c09762","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09762","url":null,"abstract":"Catalytic dehydrogenation of methylcyclohexane (MCH) is of great importance for hydrogen storage and transportation, but currently used Pt-based nanoparticle catalysts still suffer from insufficient activity, low selectivity, and short-term stability. In this study, we encapsulated Pt–Sn nanoparticles into the silicalite-1 (S-1) matrix and incorporated Sn into the zeolite framework through one-pot hydrothermal synthesis to overcome the above problems. These Pt–Sn bimetallic catalysts were designed for the first time with a high Sn content (2.8–3.9 wt %, Sn/Pt ratio = 6–8) in zeolite mother gel for MCH dehydrogenation. The introduction of Sn significantly improved the activity and durability of Pt@S-1. Especially, the PtSn@S-1 (Sn/Pt ratio = 6) catalyst showed high MCH conversion (&gt;80% for 2 h) and toluene (TOL) selectivity (∼100%) without cofeeding H<sub>2</sub>. Even after a long-term stability test for 33 h under a weight hourly space velocity (WHSV) of 120,000 mL/g/h, no obvious deactivation was observed, and this catalyst retained a superior H<sub>2</sub> evolution rate normalized with a surface Pt content of 1343 mmol<sub>H<sub>2</sub></sub>/g<sub>Pt</sub>/min. The structure–catalytic property relationship of PtSn@S-1 catalysts was systematically studied. Upon Sn introduction, PtO<sub><i>x</i></sub> species on Pt@S-1 were transformed into the PtSn alloy. With the further increase of the Sn/Pt ratio from 1 to 6, Sn was gradually incorporated into the zeolite framework, and this PtSn alloy evolved into a core–shell structure with a Pt core and a Sn shell. Despite the reduced proportion of surface Pt, these unique structures enabled the modification of the Pt local structure, promoted TOL desorption, and enhanced the stability of Pt–Sn nanoparticles, therefore achieving high activity, selectivity, and durability for MCH dehydrogenation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"25 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477442","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
Preparation of High Antibacterial, Easy Coating, and Easy Cleaning Pea Protein Isolate/Zein-Carboxymethyl Cellulose Composite Coating Material and Its Preservation Application
IF 8.4 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-23 DOI: 10.1021/acssuschemeng.4c10298
Runyi Qu, Bihua Xia, Mingxuan Hou, Jin Xu, Yijie Wang, Ting Li, Mingqing Chen, Shibo Wang, Weifu Dong
{"title":"Preparation of High Antibacterial, Easy Coating, and Easy Cleaning Pea Protein Isolate/Zein-Carboxymethyl Cellulose Composite Coating Material and Its Preservation Application","authors":"Runyi Qu, Bihua Xia, Mingxuan Hou, Jin Xu, Yijie Wang, Ting Li, Mingqing Chen, Shibo Wang, Weifu Dong","doi":"10.1021/acssuschemeng.4c10298","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10298","url":null,"abstract":"This paper fabricated a new kind of pea protein isolate/Zein-carboxymethyl cellulose composite coating material with Pickering emulsion morphology through the solution blending method. The pea protein isolate/Zein-carboxymethyl cellulose composite coating material exhibited high antibacterial properties, delayed spoilage, and easy-to-coat and easy-to-clean properties. In addition, the ultraviolet shielding properties, hydrophilicity and hydrophobicity, antibacterial properties, antioxidant properties, and preservation properties of fruits were studied. This pea protein isolate/Zein-carboxymethyl cellulose composite coating material avoided the volatilization of clove essential oil and achieved long-term antibacterial properties, and it is fit for the preservation material field.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"27 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477346","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
Temperature Gradient Design for Elevated Performance in Proton Exchange Membrane Fuel Cells (PEMFCs) under High Current Density
IF 7.1 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-22 DOI: 10.1021/acssuschemeng.4c1034010.1021/acssuschemeng.4c10340
Fengyang Cai, Zhengkai Tu* and Siew Hwa Chan, 
{"title":"Temperature Gradient Design for Elevated Performance in Proton Exchange Membrane Fuel Cells (PEMFCs) under High Current Density","authors":"Fengyang Cai,&nbsp;Zhengkai Tu* and Siew Hwa Chan,&nbsp;","doi":"10.1021/acssuschemeng.4c1034010.1021/acssuschemeng.4c10340","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10340https://doi.org/10.1021/acssuschemeng.4c10340","url":null,"abstract":"<p >High current density (HCD) operation in proton exchange membrane fuel cells (PEMFCs) presents significant water and thermal management challenges, mainly due to excessive production and uneven distribution of water and heat. Constructing an in-plane temperature difference (TD) in the cathode to match the water–gas state variations is a promising approach. This study innovatively reconstructs the cathode liquid cooling channels of a hydrogen-air PEMFC to create an in-plane TD, experimentally investigating various designs across different inlet relative humidities (RH), with deeper mechanism analysis, including electrochemical impedance spectroscopy (EIS) and local current density distribution. Results show that a positive temperature difference (PTD) enhances HCD performance, improving voltage and current uniformity by 10% and 2% at 2100 mA/cm<sup>2</sup>, while the enhancement weakens with increasing inlet humidity. Reverse temperature differences (RTDs) persistently have an adverse effect, which worsens with higher difference amplitude and RH. Mechanism exploration for TDs reveals that PTD improves membrane hydration upstream and reduces flooding downstream under low humidity conditions while tending to cause flooding upstream under high humidity conditions. RTD causes drying upstream and exacerbates downstream flooding, which is more pronounced at higher humidity. This research provides novel insights into optimizing thermal management at HCDs in low-humidity environments like automotive applications and high-humidity environments.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 9","pages":"3752–3765 3752–3765"},"PeriodicalIF":7.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576659","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
Interface-Engineered Co4N–CeF3 Heterostructure Induces Electronic Redistribution and Significantly Enhances Oxygen Evolution at Large Current Density
IF 7.1 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-22 DOI: 10.1021/acssuschemeng.4c0844310.1021/acssuschemeng.4c08443
Vikas Pundir, Ashish Gaur, Rajdeep Kaur,  Aashi and Vivek Bagchi*, 
{"title":"Interface-Engineered Co4N–CeF3 Heterostructure Induces Electronic Redistribution and Significantly Enhances Oxygen Evolution at Large Current Density","authors":"Vikas Pundir,&nbsp;Ashish Gaur,&nbsp;Rajdeep Kaur,&nbsp; Aashi and Vivek Bagchi*,&nbsp;","doi":"10.1021/acssuschemeng.4c0844310.1021/acssuschemeng.4c08443","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c08443https://doi.org/10.1021/acssuschemeng.4c08443","url":null,"abstract":"<p >The process of water electrolysis is an effective approach to generate extremely pure hydrogen. Nevertheless, the anodic oxygen evolution reaction (OER) is often slow and requires a high overpotential, resulting in excessive electricity consumption during water electrolysis. Hence, the utilization of exceptionally effective OER electrocatalysts with minimal overpotential, particularly under high current density, will undeniably accelerate the development of water electrolysis in industrial situations. Herein, we fabricated a heterostructure using CeF<sub>3</sub> and Co<sub>4</sub>N phases, where electrocatalytically, nonactive CeF<sub>3</sub> is used to alter the electronic structure of Co<sub>4</sub>N through the interface. This electronic modulation resulted in the generation of high-valent Co atoms on the catalyst surface, which are effective for the adsorption of the intermediates that are responsible for carrying out the OER. At a very low overpotential of 400 mV, the Co<sub>4</sub>N–CeF<sub>3</sub> heterostructure yields a large current density of 1000 mA cm<sup>–2</sup>. We also measured the ultralong durability of the catalyst for 500 h at a very large current density of 500 mA cm<sup>–2</sup>. Remarkably, the water electrolyzer consisting of Pt/C||Co<sub>4</sub>N–CeF<sub>3</sub> needs only a cell voltage of 1.61 and 1.68 V, respectively, to achieve a current density of 100 and 500 mA cm<sup>–2</sup>. The electronic reallocation was well investigated by using X-ray photoelectron spectroscopy (XPS) and X-ray absorption near-edge spectra (XANES) analysis.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 9","pages":"3491–3499 3491–3499"},"PeriodicalIF":7.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576658","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
Closing the Loop: Greener and Efficient Hydrolytic Depolymerization for the Recycling of Polyesters Using Biobased Eutectic Solvents
IF 7.1 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-21 DOI: 10.1021/acssuschemeng.4c0954510.1021/acssuschemeng.4c09545
Vinícius de Paula, Simão V. Pandeirada, Paulo J. A. Ribeiro-Claro, Armando J. D. Silvestre and Andreia F. Sousa*, 
{"title":"Closing the Loop: Greener and Efficient Hydrolytic Depolymerization for the Recycling of Polyesters Using Biobased Eutectic Solvents","authors":"Vinícius de Paula,&nbsp;Simão V. Pandeirada,&nbsp;Paulo J. A. Ribeiro-Claro,&nbsp;Armando J. D. Silvestre and Andreia F. Sousa*,&nbsp;","doi":"10.1021/acssuschemeng.4c0954510.1021/acssuschemeng.4c09545","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09545https://doi.org/10.1021/acssuschemeng.4c09545","url":null,"abstract":"<p >The imperative for achieving circularity in the realm of postconsumer polymers predominantly hinges upon the adoption of efficient recycling methodologies with a greener footprint. As such, this study introduces an innovative and eco-friendly depolymerization process for recycling highly consumed poly(ethylene terephthalate) (PET) and innovative bioderived poly(ethylene 2,5-furandicarboxylate) (PEF) which is easily extrapolated to other polyesters. This study demonstrates the pivotal role of eutectic solvents based on biobased phenols with safe design to efficiently mediate the hydrolytic depolymerization, under alkaline conditions, of these recalcitrant polymers into terephthalic acid (TPA) or 2,5-furandicarboxylic acid (FDCA). Additionally, optimization through a design of experiments approach yields TPA and FDCA with over 90% and 80% recovery, respectively, under mild conditions of temperature, below 150 °C, and not exceeding 5 h of reaction time. Structural characterization analyses confirm the chemical nature and the high purity of the recovered products, while eutectic solvent reuse assessments underscore its potential for multiple cycles with minimal loss of catalytic activity, reducing process waste. A proof-of-concept for monomer repolymerization demonstrates feasibility. Green metrics align with the fine chemicals industry, indicating promising market potential for this low-energy eutectic solvent-based approach to enhance circularity in polyester waste management.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 9","pages":"3577–3587 3577–3587"},"PeriodicalIF":7.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576549","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
In Situ Phase Transformation-Induced High-Activity Nickel–Molybdenum Catalyst for Enhancing High-Current-Density Water/Seawater Splitting
IF 8.4 1区 化学
ACS Sustainable Chemistry & Engineering Pub Date : 2025-02-21 DOI: 10.1021/acssuschemeng.4c09957
Xinyu Wang, Xu Yu, Pinyi He, Guohui Yang, Fu Qin, Yongkang Yao, Jianliang Bai, Guojun Yuan, Lili Ren
{"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}
引用次数: 0
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