Pub Date : 2025-04-22DOI: 10.1021/acssuschemeng.4c09995
Jiayi Wang, Yichen Hao, Jinping Li, Jiangfeng Yang
The shortage of lithium resources and the accumulation of retired batteries are strategic issues that need to be addressed urgently. Here, we propose an innovative and efficient strategy for the preferential extraction of Li+, followed by the sequential recovery of Mn2+ and Co2+, utilizing GIS zeolite from battery leachate. Li+ ions were preferentially exchanged, achieving a 95% recovery rate at 0 °C; subsequently, 94% of Mn2+ and 97% of Co2+ were recovered by increasing the temperature to 40 and 60 °C; meanwhile, 90% of Ni2+ remains in solution. The fastest kinetic rate of Li+ in GIS zeolite and its efficient extraction at low temperatures were verified through ion exchange processes; at higher temperatures, the adsorption capacity and selectivity of GIS zeolite for Co2+ and Mn2+ increased. We found the diffusion rate of Li+ in GIS zeolite to be over 2.5 times faster than that of Mn2+, Co2+, and Ni2+, which all have the same rate by molecular dynamics simulations. The ion exchange of Mn2+, Co2+, and Ni2+ was an endothermic reaction, with the ΔH0 and ΔG0 following the order Mn2+ < Co2+ < Ni2+ by thermodynamic calculations. The regeneration ability of GIS zeolite indicated its promising industrial application prospects.
{"title":"Priority Extraction of Li+ and Sequential Recovery of Divalent Metals from Retired LiNixCoyMn1–x–yO2 Batteries Using GIS Zeolite","authors":"Jiayi Wang, Yichen Hao, Jinping Li, Jiangfeng Yang","doi":"10.1021/acssuschemeng.4c09995","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09995","url":null,"abstract":"The shortage of lithium resources and the accumulation of retired batteries are strategic issues that need to be addressed urgently. Here, we propose an innovative and efficient strategy for the preferential extraction of Li<sup>+</sup>, followed by the sequential recovery of Mn<sup>2+</sup> and Co<sup>2+</sup>, utilizing GIS zeolite from battery leachate. Li<sup>+</sup> ions were preferentially exchanged, achieving a 95% recovery rate at 0 °C; subsequently, 94% of Mn<sup>2+</sup> and 97% of Co<sup>2+</sup> were recovered by increasing the temperature to 40 and 60 °C; meanwhile, 90% of Ni<sup>2+</sup> remains in solution. The fastest kinetic rate of Li<sup>+</sup> in GIS zeolite and its efficient extraction at low temperatures were verified through ion exchange processes; at higher temperatures, the adsorption capacity and selectivity of GIS zeolite for Co<sup>2+</sup> and Mn<sup>2+</sup> increased. We found the diffusion rate of Li<sup>+</sup> in GIS zeolite to be over 2.5 times faster than that of Mn<sup>2+</sup>, Co<sup>2+</sup>, and Ni<sup>2+</sup>, which all have the same rate by molecular dynamics simulations. The ion exchange of Mn<sup>2+</sup>, Co<sup>2+</sup>, and Ni<sup>2+</sup> was an endothermic reaction, with the Δ<i>H</i><sup>0</sup> and Δ<i>G</i><sup>0</sup> following the order Mn<sup>2+</sup> < Co<sup>2+</sup> < Ni<sup>2+</sup> by thermodynamic calculations. The regeneration ability of GIS zeolite indicated its promising industrial application prospects.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"15 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857559","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 : 2025-04-22DOI: 10.1021/acssuschemeng.5c02289
Sri Hari Anandhi Rajendran, Sabrina Kogler, Philipp Kögl, Wilfried M. Braje, Sándor B. Ötvös, C. Oliver Kappe
The widespread use of peptide-based drugs and the prevalence of amide-containing pharmaceuticals underscore the critical need for efficient, sustainable, and environmentally friendly amidation methods in the pharmaceutical industry. However, traditional approaches rely on harmful solvents, highlighting the urgent need for a paradigm shift toward greener alternatives. We leveraged continuous slurry flow technology to facilitate solid handling and develop scalable and sustainable protocols for amide bond formation in water as the reaction medium. To ensure optimal mass transfer through efficient active mixing, we utilized a spinning disc reactor and an agitated continuous stirred-tank reactor series, both of which are commercially available, including industrial-scale versions. As model reactions, we selected the synthesis of a key efaproxiral intermediate and a technically challenging amidation involving a protected tryptophan derivative. The best results were achieved using hydroxypropyl methylcellulose, a cost-effective, nontoxic, cellulose-derived surface-active agent in water. The optimized lab-scale protocols enabled rapid amidations with productivities of up to 2 kg per day. Notably, neither the synthesis nor the isolation processes required any organic solvents, resulting in minimal waste generation.
{"title":"Sustainable and Scalable Amidations in Water Using Continuous Slurry-Flow Technology","authors":"Sri Hari Anandhi Rajendran, Sabrina Kogler, Philipp Kögl, Wilfried M. Braje, Sándor B. Ötvös, C. Oliver Kappe","doi":"10.1021/acssuschemeng.5c02289","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c02289","url":null,"abstract":"The widespread use of peptide-based drugs and the prevalence of amide-containing pharmaceuticals underscore the critical need for efficient, sustainable, and environmentally friendly amidation methods in the pharmaceutical industry. However, traditional approaches rely on harmful solvents, highlighting the urgent need for a paradigm shift toward greener alternatives. We leveraged continuous slurry flow technology to facilitate solid handling and develop scalable and sustainable protocols for amide bond formation in water as the reaction medium. To ensure optimal mass transfer through efficient active mixing, we utilized a spinning disc reactor and an agitated continuous stirred-tank reactor series, both of which are commercially available, including industrial-scale versions. As model reactions, we selected the synthesis of a key efaproxiral intermediate and a technically challenging amidation involving a protected tryptophan derivative. The best results were achieved using hydroxypropyl methylcellulose, a cost-effective, nontoxic, cellulose-derived surface-active agent in water. The optimized lab-scale protocols enabled rapid amidations with productivities of up to 2 kg per day. Notably, neither the synthesis nor the isolation processes required any organic solvents, resulting in minimal waste generation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"68 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857565","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 : 2025-04-21DOI: 10.1021/acssuschemeng.4c10451
Claire Morand, Daniele Mantione, Andrew P. Dove, Haritz Sardón, Coralie Jehanno
Replacing fossil-derived polymers with biobased alternatives is essential to reduce the environmental impact of plastics production, as it helps to decrease reliance on finite fossil resources and promotes sustainability by using renewable raw materials. However, biobased options remain scarce in the industry, as it is difficult to produce fully biobased polymers at a reasonable cost with the same functional properties. In this study, 100% biobased unsaturated polyesters are synthesized from maleic acid and 1,3-propanediol through bulk polycondensation mediated by biosourced catalysts. The resulting materials present different degrees of double bond isomerization depending on the catalyst employed, with higher trans content obtained using catalysts that exhibit greater nucleophilicity. With the objective of using these polyester resins for additive manufacturing, the reactivity of the double bonds was analyzed through FTIR and photo-DSC, while the cross-linking process was studied by photorheology, which highlighted the superior reactivity of the trans double bonds. This study opens avenues for the synthesis of 100% biosourced polyester resins with tunable cis/trans content.
{"title":"Controlling the cis/trans Content of Biobased Unsaturated Polyesters by Judicious Choice of a Biosourced Catalyst","authors":"Claire Morand, Daniele Mantione, Andrew P. Dove, Haritz Sardón, Coralie Jehanno","doi":"10.1021/acssuschemeng.4c10451","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10451","url":null,"abstract":"Replacing fossil-derived polymers with biobased alternatives is essential to reduce the environmental impact of plastics production, as it helps to decrease reliance on finite fossil resources and promotes sustainability by using renewable raw materials. However, biobased options remain scarce in the industry, as it is difficult to produce fully biobased polymers at a reasonable cost with the same functional properties. In this study, 100% biobased unsaturated polyesters are synthesized from maleic acid and 1,3-propanediol through bulk polycondensation mediated by biosourced catalysts. The resulting materials present different degrees of double bond isomerization depending on the catalyst employed, with higher <i>trans</i> content obtained using catalysts that exhibit greater nucleophilicity. With the objective of using these polyester resins for additive manufacturing, the reactivity of the double bonds was analyzed through FTIR and photo-DSC, while the cross-linking process was studied by photorheology, which highlighted the superior reactivity of the <i>trans</i> double bonds. This study opens avenues for the synthesis of 100% biosourced polyester resins with tunable <i>cis/trans</i> content.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"66 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853691","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 : 2025-04-21DOI: 10.1021/acssuschemeng.4c07823
Lilian C. Alarcón-Segovia, Kenneth E. Madsen, Claire Liu, Sun Hong Kim, Tae Wan Park, Yayun Du, Joanna L. Ciatti, Kathrin H. Salame, Jae-Young Yoo, John A. Rogers
Global access to quality healthcare remains one of the most pressing issues for modern society. Despite advances in wearable and point-of-care biomedical devices, the dissemination of these technologies to resource-limited populations remains challenging, partially due to limitations imposed by cost. One of the largest cost drivers in the adoption of wearable devices for electrophysiological (ExG) monitoring, for instance, is the consumable overhead (electrolytes, adhesives, and electrodes) necessary to support patient use. Herein, we report the development and optimization of ultralow-cost (<0.03 USD per electrode), stable, and resource-available ExG electrolytes fabricated from agricultural byproducts widely available in local settings, thereby negating the dependency on importation. We show that composite hydrogels can be prepared from a variety of starch precursors via a facile one-pot sol–gel method to yield ionically conductive, mechanically compliant gel electrolytes. We further demonstrate that food starch materials for these purposes are resistant to dehydration and, when coupled with a wireless recording platform, can facilitate long-term (8 h) signal recording without significant loss in signal quality. Together, these characteristics mark starch-based electrolytes as possible alternatives to commercial formulations for skin-interfaced measurement electrodes, compatible with mobile sensing apparatus in resource-limited settings with cost, sustainability, and supply chain advantages without sacrificing clinical performance.
{"title":"Ultralow-Cost Hydrogel Electrolytes Based on Agricultural Byproducts for Distributed Electrophysiological Recording in Resource-Limited Settings","authors":"Lilian C. Alarcón-Segovia, Kenneth E. Madsen, Claire Liu, Sun Hong Kim, Tae Wan Park, Yayun Du, Joanna L. Ciatti, Kathrin H. Salame, Jae-Young Yoo, John A. Rogers","doi":"10.1021/acssuschemeng.4c07823","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c07823","url":null,"abstract":"Global access to quality healthcare remains one of the most pressing issues for modern society. Despite advances in wearable and point-of-care biomedical devices, the dissemination of these technologies to resource-limited populations remains challenging, partially due to limitations imposed by cost. One of the largest cost drivers in the adoption of wearable devices for electrophysiological (ExG) monitoring, for instance, is the consumable overhead (electrolytes, adhesives, and electrodes) necessary to support patient use. Herein, we report the development and optimization of ultralow-cost (<0.03 USD per electrode), stable, and resource-available ExG electrolytes fabricated from agricultural byproducts widely available in local settings, thereby negating the dependency on importation. We show that composite hydrogels can be prepared from a variety of starch precursors via a facile one-pot sol–gel method to yield ionically conductive, mechanically compliant gel electrolytes. We further demonstrate that food starch materials for these purposes are resistant to dehydration and, when coupled with a wireless recording platform, can facilitate long-term (8 h) signal recording without significant loss in signal quality. Together, these characteristics mark starch-based electrolytes as possible alternatives to commercial formulations for skin-interfaced measurement electrodes, compatible with mobile sensing apparatus in resource-limited settings with cost, sustainability, and supply chain advantages without sacrificing clinical performance.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"68 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853692","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}
Agricultural biomass such as rice straws represents a significant volume of waste generated worldwide; disposal of which through landfilling and burning is a major global challenge. In the present study, strategic functionalization of rice straws through delignification-cum-phosphorylation using low-cost agrochemicals followed by scalable processing into films and beverage cups is developed. The phosphorylated films with high charge content (1488–2199 mmol kg–1) show improved mechanical strength under both dry and wet conditions with high thermal stability and flame retardancy. A detailed mechanistic study using FTIR and XPS spectroscopy confirmed the covalently bonded phosphate groups on the cellulose backbone along with the formation of silicon phosphate cross-linkages upon heating. Interestingly, the all-cellulose films could be heat-sealed, improving the shelf life of highly perishable stored fruits and vegetables. Molded cups demonstrate high solvothermal stability with antifizzing and improved washability (for 3 times) post consumption. The proposed valorization of rice straws into packaging films and beverage cups with lower ecological impacts and commercial feasibility provides a sustainable alternative for a plastic-free world.
{"title":"All-Biomass-Derived Cellulose Phosphate-Based Heat-Sealable Films and Thermally Stable Antifizzing Cups with Improved Recyclability","authors":"Rahul Ranjan, Vedang P. Mone, Rohit Rai, Chandra Kant, Prodyut Dhar","doi":"10.1021/acssuschemeng.4c09105","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09105","url":null,"abstract":"Agricultural biomass such as rice straws represents a significant volume of waste generated worldwide; disposal of which through landfilling and burning is a major global challenge. In the present study, strategic functionalization of rice straws through delignification-<i>cum</i>-phosphorylation using low-cost agrochemicals followed by scalable processing into films and beverage cups is developed. The phosphorylated films with high charge content (1488–2199 mmol kg<sup>–1</sup>) show improved mechanical strength under both dry and wet conditions with high thermal stability and flame retardancy. A detailed mechanistic study using FTIR and XPS spectroscopy confirmed the covalently bonded phosphate groups on the cellulose backbone along with the formation of silicon phosphate cross-linkages upon heating. Interestingly, the all-cellulose films could be heat-sealed, improving the shelf life of highly perishable stored fruits and vegetables. Molded cups demonstrate high solvothermal stability with antifizzing and improved washability (for 3 times) post consumption. The proposed valorization of rice straws into packaging films and beverage cups with lower ecological impacts and commercial feasibility provides a sustainable alternative for a plastic-free world.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"58 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857460","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 : 2025-04-21DOI: 10.1021/acssuschemeng.4c08815
Rarosue J. Amaraibi, Babu Joseph, John N. Kuhn
This paper conducts a comprehensive life cycle assessment (LCA) of the intensified biogas to liquids (IBGTL) process, focusing on its global warming potential (GWP) and comparing it to alternative biogas utilization pathways. Landfill gas (LFG), derived from municipal solid waste (MSW) decomposition, contributes significantly to methane emissions and poses environmental risks. Regulatory initiatives promote LFG capture and utilization for renewable energy production. The IBGTL process, integrating bi-reforming and Fischer–Tropsch synthesis into a compact reactor design, offers advantages in reduced capital and operating costs. This study quantifies the life cycle impacts of IBGTL diesel production and benchmarks it against other LFG utilization routes, including TriFTS diesel, LFG to electricity, and LFG to compressed renewable natural gas. Using a “well-to-wheel” boundary, the study evaluates emissions from production to usage. Findings indicate substantial reductions in greenhouse gas (GHG) emissions across all LFG-to-energy pathways compared to fossil alternatives, with the most significant savings achieved by IBGTL diesel with electricity cogeneration (Scenario 4, 221 gCO2eq/MJ reduction), followed by LFG to electricity (159 gCO2eq/MJ reduction), TriFTS diesel (107 gCO2eq/MJ reduction), and IBGTL diesel with material recycling (Scenario 2, 91.6 gCO2eq/MJ reduction). Sensitivity analyses reveal nuances in emissions impacts. The results highlight the importance of process optimization and grid characteristics in shaping the environmental performance. This research contributes insights for decision-makers, informing sustainable waste management strategies and guiding future LFG-to-energy technologies.
{"title":"Life Cycle Assessment of Liquid Transportation Fuel Produced by the Intensified Biogas to Liquid (IBGTL) Process","authors":"Rarosue J. Amaraibi, Babu Joseph, John N. Kuhn","doi":"10.1021/acssuschemeng.4c08815","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c08815","url":null,"abstract":"This paper conducts a comprehensive life cycle assessment (LCA) of the intensified biogas to liquids (IBGTL) process, focusing on its global warming potential (GWP) and comparing it to alternative biogas utilization pathways. Landfill gas (LFG), derived from municipal solid waste (MSW) decomposition, contributes significantly to methane emissions and poses environmental risks. Regulatory initiatives promote LFG capture and utilization for renewable energy production. The IBGTL process, integrating bi-reforming and Fischer–Tropsch synthesis into a compact reactor design, offers advantages in reduced capital and operating costs. This study quantifies the life cycle impacts of IBGTL diesel production and benchmarks it against other LFG utilization routes, including TriFTS diesel, LFG to electricity, and LFG to compressed renewable natural gas. Using a “well-to-wheel” boundary, the study evaluates emissions from production to usage. Findings indicate substantial reductions in greenhouse gas (GHG) emissions across all LFG-to-energy pathways compared to fossil alternatives, with the most significant savings achieved by IBGTL diesel with electricity cogeneration (Scenario 4, 221 gCO<sub>2</sub>eq/MJ reduction), followed by LFG to electricity (159 gCO<sub>2</sub>eq/MJ reduction), TriFTS diesel (107 gCO<sub>2</sub>eq/MJ reduction), and IBGTL diesel with material recycling (Scenario 2, 91.6 gCO<sub>2</sub>eq/MJ reduction). Sensitivity analyses reveal nuances in emissions impacts. The results highlight the importance of process optimization and grid characteristics in shaping the environmental performance. This research contributes insights for decision-makers, informing sustainable waste management strategies and guiding future LFG-to-energy technologies.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"23 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857566","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 : 2025-04-21DOI: 10.1021/acssuschemeng.5c01403
Chun-Shuai Cao, Wenjie Liu, Aijing Ma, Xuan Jiao, Yuanyuan Yang, Jiahao Li, Feiyan Fu
The organophosphorus compounds, as nerve agents and more broadly used as chemical warfare agents (CWAs), are difficult to remove through traditional water treatment due to their low concentrations. Single-atom (SA) catalysts, owing to their spatial atomic isolation, unsaturated coordination centers, and distinct electronic structures, can realize a maximum atom-utilization efficiency of up to 100%, thus offering outstanding catalytic performance. A highly efficient photocatalyst was synthesized by assembling single-atom Pt on TiO2 nanotubes as support, and its physicochemical properties were confirmed through X-ray diffraction, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, high-angle annular dark-field scanning transmission electron microscopy, and high-resolution transmission electron microscopy. This unique structure of SA-Pt/TiO2 exhibited significantly high performance in photocatalytic degradation of dimethyl methylphosphonate (DMMP) in water, achieving a removal efficiency of 95% at an initial concentration of 80 ppm under xenon lamp irradiation. Introducing single-atom Pt led to a photocatalytic degradation rate that was 6.3 times that of the blank TiO2 sample, which can be explained by the fact that single-atom Pt effectively promoted the transfer of photogenerated electrons from TiO2 sites to Pt, thereby facilitating the separation of charge carriers. Additionally, density functional theory (DFT) calculations indicated that Pt doping on the TiO2(101) surface enhanced the adsorption capacity for DMMP and improved the redox capability, leading to a high photocatalytic activity. The study provides a strategy for developing highly efficient single-metal-atom-based photocatalysts, which is of great significance for efficiently removing trace amounts of chemical warfare agents from water.
{"title":"Single-Atom Pt-Decorated TiO2 Nanotubes for Boosted Photocatalytic Degradation of Chemical Warfare Agents","authors":"Chun-Shuai Cao, Wenjie Liu, Aijing Ma, Xuan Jiao, Yuanyuan Yang, Jiahao Li, Feiyan Fu","doi":"10.1021/acssuschemeng.5c01403","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c01403","url":null,"abstract":"The organophosphorus compounds, as nerve agents and more broadly used as chemical warfare agents (CWAs), are difficult to remove through traditional water treatment due to their low concentrations. Single-atom (SA) catalysts, owing to their spatial atomic isolation, unsaturated coordination centers, and distinct electronic structures, can realize a maximum atom-utilization efficiency of up to 100%, thus offering outstanding catalytic performance. A highly efficient photocatalyst was synthesized by assembling single-atom Pt on TiO<sub>2</sub> nanotubes as support, and its physicochemical properties were confirmed through X-ray diffraction, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, high-angle annular dark-field scanning transmission electron microscopy, and high-resolution transmission electron microscopy. This unique structure of SA-Pt/TiO<sub>2</sub> exhibited significantly high performance in photocatalytic degradation of dimethyl methylphosphonate (DMMP) in water, achieving a removal efficiency of 95% at an initial concentration of 80 ppm under xenon lamp irradiation. Introducing single-atom Pt led to a photocatalytic degradation rate that was 6.3 times that of the blank TiO<sub>2</sub> sample, which can be explained by the fact that single-atom Pt effectively promoted the transfer of photogenerated electrons from TiO<sub>2</sub> sites to Pt, thereby facilitating the separation of charge carriers. Additionally, density functional theory (DFT) calculations indicated that Pt doping on the TiO<sub>2</sub>(101) surface enhanced the adsorption capacity for DMMP and improved the redox capability, leading to a high photocatalytic activity. The study provides a strategy for developing highly efficient single-metal-atom-based photocatalysts, which is of great significance for efficiently removing trace amounts of chemical warfare agents from water.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"1 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857567","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 : 2025-04-21DOI: 10.1021/acssuschemeng.5c03526
Peter Licence
I am sure that many of us, when we look back, will remember 2025 as a period of tremendous change be that on a geo-political level or indeed within institutions and organizations that are very much closer to home. As the world around us changes and adjusts to the “new normal” of today, we can rest assured that commitment, vibrancy, and above all else a thirst for new insight lives long within the global scientific community. It is with this reassuring familiarity that I have the great pleasure in sharing with you all the winners of this year’s ACS Sustainable Chemistry & Engineering Lectureship Awards. These lectureship awards recognize leading contributions of scientists and engineers active in the general fields of green chemistry, green engineering, and sustainability in the broadest sense of the chemical enterprise and are awarded each year in collaboration with the ACS Green Chemistry Institute. The <i>ACS Sustainable Chemistry & Engineering</i> Lectureship awards were created to celebrate early-to-mid-career investigators who completed academic training no more than 10 years prior to nomination. In support of our commitment to nurture and stimulate a global community of outstanding practice, we award three Lectureship Awards to recognize outstanding levels of contribution from The Americas, Europe/Middle East/Africa, and Asia/Pacific. The winners of the 2025 <i>ACS Sustainable Chemistry & Engineering</i> Lectureship Awards are as follows: <b>Professor Milad Abolhasani</b> of North Carolina State University (Raleigh, NC), honored for his pioneering work on “Self-Driving Laboratories”─integrating flow reactors, online reaction monitoring, and autonomous experimentation (1−3) <b>Professor Athina Anastasaki</b> of ETH Zürich (Zürich, Switzerland), honored for her pioneering contributions demonstrating low-temperature radical depolymerization of vinyl polymers (4−6) <b>Professor Hong Chen</b> of Southern University of Science and Technology (Shenzhen, China), honored for his innovative application of clean technologies, notably electrochemical- and photochemical-driven processes to address pollution control and circular processing of technical materials (7−9) Our awardees will be honored at the 29th Annual Green Chemistry & Engineering Conference in Pittsburgh (June 23–26, 2025). We warmly invite the readership of <i>ACS Sustainable Chemistry & Engineering</i> to join us and celebrate these achievements in Pittsburgh this June. In closing, we thank the global community of scientists and engineers devoted to sustainable chemistry and engineering for their active response to this year’s call for nominations. We are thrilled to report that the nominations received, spanning all regions, continue to grow and are truly reflective of a multidisciplinary community that continues to strive to deliver the objectives of the UN Sustainable Development Goals. Details of the next award cycle will be available in Fall 2025 or by sending in
{"title":"Abolhasani, Anastasaki, and Chen: 2025 Winners of the ACS Sustainable Chemistry & Engineering Lectureship Award","authors":"Peter Licence","doi":"10.1021/acssuschemeng.5c03526","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c03526","url":null,"abstract":"I am sure that many of us, when we look back, will remember 2025 as a period of tremendous change be that on a geo-political level or indeed within institutions and organizations that are very much closer to home. As the world around us changes and adjusts to the “new normal” of today, we can rest assured that commitment, vibrancy, and above all else a thirst for new insight lives long within the global scientific community. It is with this reassuring familiarity that I have the great pleasure in sharing with you all the winners of this year’s ACS Sustainable Chemistry & Engineering Lectureship Awards. These lectureship awards recognize leading contributions of scientists and engineers active in the general fields of green chemistry, green engineering, and sustainability in the broadest sense of the chemical enterprise and are awarded each year in collaboration with the ACS Green Chemistry Institute. The <i>ACS Sustainable Chemistry & Engineering</i> Lectureship awards were created to celebrate early-to-mid-career investigators who completed academic training no more than 10 years prior to nomination. In support of our commitment to nurture and stimulate a global community of outstanding practice, we award three Lectureship Awards to recognize outstanding levels of contribution from The Americas, Europe/Middle East/Africa, and Asia/Pacific. The winners of the 2025 <i>ACS Sustainable Chemistry & Engineering</i> Lectureship Awards are as follows: <b>Professor Milad Abolhasani</b> of North Carolina State University (Raleigh, NC), honored for his pioneering work on “Self-Driving Laboratories”─integrating flow reactors, online reaction monitoring, and autonomous experimentation (1−3) <b>Professor Athina Anastasaki</b> of ETH Zürich (Zürich, Switzerland), honored for her pioneering contributions demonstrating low-temperature radical depolymerization of vinyl polymers (4−6) <b>Professor Hong Chen</b> of Southern University of Science and Technology (Shenzhen, China), honored for his innovative application of clean technologies, notably electrochemical- and photochemical-driven processes to address pollution control and circular processing of technical materials (7−9) Our awardees will be honored at the 29th Annual Green Chemistry & Engineering Conference in Pittsburgh (June 23–26, 2025). We warmly invite the readership of <i>ACS Sustainable Chemistry & Engineering</i> to join us and celebrate these achievements in Pittsburgh this June. In closing, we thank the global community of scientists and engineers devoted to sustainable chemistry and engineering for their active response to this year’s call for nominations. We are thrilled to report that the nominations received, spanning all regions, continue to grow and are truly reflective of a multidisciplinary community that continues to strive to deliver the objectives of the UN Sustainable Development Goals. Details of the next award cycle will be available in Fall 2025 or by sending in","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"26 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853704","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 : 2025-04-20DOI: 10.1021/acssuschemeng.5c01108
Robin Lemmens, Neal Strijckmans, Robin Coeck, Wouter Stuyck, Dirk De Vos
The incorporation of heteroatoms in the polyethylene backbone enables chemical recycling through chemolysis. In this work, ketone-functionalized polyethylenes (kf-PEs) are converted into amide-functionalized PEs (af-PEs) through ammoximation and Beckmann rearrangement. The ammoximation involves the in situ production of NH2OH from base chemicals NH3 and H2O2, using a heterogeneous TS-1 catalyst, and allows us to convert up to 91% of the ketones to oximes. The subsequent Beckmann rearrangement was investigated using heterogeneous Brønsted acidic zeolite catalysts. H-ITQ-2, a delaminated zeolite with MWW topology, was found to be the most effective catalyst, converting up to 80% of oximes into in-chain amides. Both the external surface area and the amount of Brønsted acid sites are found to be key factors in the reaction. Finally, it is shown that the obtained af-PE can be depolymerized through ammonolysis coupled with hydrogenation in a one-pot system, highlighting its applicability for chemical recycling.
{"title":"Upcycling of Polyethylene through Sustainable Introduction of In-Chain Amides Using Zeolite Catalysis","authors":"Robin Lemmens, Neal Strijckmans, Robin Coeck, Wouter Stuyck, Dirk De Vos","doi":"10.1021/acssuschemeng.5c01108","DOIUrl":"https://doi.org/10.1021/acssuschemeng.5c01108","url":null,"abstract":"The incorporation of heteroatoms in the polyethylene backbone enables chemical recycling through chemolysis. In this work, ketone-functionalized polyethylenes (kf-PEs) are converted into amide-functionalized PEs (af-PEs) through ammoximation and Beckmann rearrangement. The ammoximation involves the <i>in situ</i> production of NH<sub>2</sub>OH from base chemicals NH<sub>3</sub> and H<sub>2</sub>O<sub>2</sub>, using a heterogeneous TS-1 catalyst, and allows us to convert up to 91% of the ketones to oximes. The subsequent Beckmann rearrangement was investigated using heterogeneous Brønsted acidic zeolite catalysts. H-ITQ-2, a delaminated zeolite with MWW topology, was found to be the most effective catalyst, converting up to 80% of oximes into in-chain amides. Both the external surface area and the amount of Brønsted acid sites are found to be key factors in the reaction. Finally, it is shown that the obtained af-PE can be depolymerized through ammonolysis coupled with hydrogenation in a one-pot system, highlighting its applicability for chemical recycling.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"10 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143850998","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 : 2025-04-19DOI: 10.1021/acssuschemeng.4c10527
Ya Wang, Bin Zhang, Jie Bao
Utilizing lignocellulosic biomass to produce high-purity l-lactic acid as the monomer of poly(lactic acid) (PLA) is an important pathway for reducing greenhouse gas (GHG) emissions. This study developed an Aspen Plus simulation model and a life-cycle assessment model for producing high-purity l-lactic acid using corn stover feedstock based on thermodynamic principles and experimental data. An advanced dry biorefinery technology is selected as the process platform because of its high conversion performance, close to the dry milling of corn, as well as the significantly reduced energy consumption and wastewater generation. The GHG emissions of corn stover during the growth period are not considered due to its agricultural waste property and to prevent double counting from corn. Full evaporation of wastewater is used to provide process water and steam supplies, considering the weak infrastructure for wastewater treatment and the freshwater supply in agricultural regions. The rigorous calculations show that producing one metric ton of purified l-lactic acid consumes 2.87 ton of corn stover as carbohydrate feedstock, 219.3 kWh of electricity, and 2.98 ton of fresh water for process use with the generation of 1.24 ton of wastewater. No external heat energy input is needed, because the lignin residue combustion provides sufficient heat energy for process use. Based on the detailed data, the calculated GHG emissions for producing one kg l-lactic acid by dry biorefining of corn stover is 0.618 kg CO2 equiv which is only 18% of that produced by dry milling of corn. This study provides an important sustainability basis and decision-making support for biobased plastic implementation.
{"title":"Rigorous Calculation of Greenhouse Gases (GHG) in Sustainable l-lactic Acid Production from Lignocellulosic Biomass based on Advanced Biorefinery Processing Technology","authors":"Ya Wang, Bin Zhang, Jie Bao","doi":"10.1021/acssuschemeng.4c10527","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10527","url":null,"abstract":"Utilizing lignocellulosic biomass to produce high-purity <span>l</span>-lactic acid as the monomer of poly(lactic acid) (PLA) is an important pathway for reducing greenhouse gas (GHG) emissions. This study developed an Aspen Plus simulation model and a life-cycle assessment model for producing high-purity <span>l</span>-lactic acid using corn stover feedstock based on thermodynamic principles and experimental data. An advanced dry biorefinery technology is selected as the process platform because of its high conversion performance, close to the dry milling of corn, as well as the significantly reduced energy consumption and wastewater generation. The GHG emissions of corn stover during the growth period are not considered due to its agricultural waste property and to prevent double counting from corn. Full evaporation of wastewater is used to provide process water and steam supplies, considering the weak infrastructure for wastewater treatment and the freshwater supply in agricultural regions. The rigorous calculations show that producing one metric ton of purified <span>l</span>-lactic acid consumes 2.87 ton of corn stover as carbohydrate feedstock, 219.3 kWh of electricity, and 2.98 ton of fresh water for process use with the generation of 1.24 ton of wastewater. No external heat energy input is needed, because the lignin residue combustion provides sufficient heat energy for process use. Based on the detailed data, the calculated GHG emissions for producing one kg <span>l</span>-lactic acid by dry biorefining of corn stover is 0.618 kg CO<sub>2</sub> equiv which is only 18% of that produced by dry milling of corn. This study provides an important sustainability basis and decision-making support for biobased plastic implementation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"10 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143849804","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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