Jinglun Du, Huiling You, Changyan Zhu, Changhua Wang, Xintong Zhang, Yichun Liu
{"title":"Energy-Efficient, Sustainable Nitrogen Fixation in Water via In Situ Electrode-Activated Pulsed Plasma","authors":"Jinglun Du, Huiling You, Changyan Zhu, Changhua Wang, Xintong Zhang, Yichun Liu","doi":"10.1021/acssuschemeng.4c10131","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10131","url":null,"abstract":"Sustainable nitrogen fixation is essential for advancing agriculture and chemical production. However, existing methods face trade-offs between energy intensity and efficiency. Low-activation-energy approaches fail to dissociate nitrogen effectively due to the strong N<sub>2</sub> bond, while energy-intensive methods face energy loss from product decomposition. Here, we present an in-water plasma-based nitrogen fixation system that integrates metal electrodes (W, Al, and Fe) to achieve in situ activation of pulsed discharging plasma. This design enables efficient nitrogen dissociation and selective product formation of soluble nitrogen species (nitrate, nitrite, and ammonia), while minimizing decomposition through optimized product diffusion. This system achieves an energy consumption of 1.14 MJ mol<sup>–1</sup> and a production rate of 12.9 mmol h<sup>–1</sup> cm<sup>–2</sup> for total soluble nitrogen species, surpassing other water-assisted methods and rivaling the Haber–Bosch process. Operating under ambient conditions, this electricity-driven, carbon-neutral approach offers a sustainable and efficient solution for decentralized application in agriculture and chemical production.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"27 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077089","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Confined Complexation Induced Size Control of Fe/Fe2O3/Fe5C2 Multicomponent Nanoparticles Embedded in Fe, N-Doped Mesoporous Carbon toward Efficient Oxygen Electrocatalysis","authors":"Siying Fan, Ming Li, Yuqi Chen, Qianqian Fan, Junhao Zhang, Xiangjun Zheng, Yuanjun Liu, Zhongyao Duan, Xingmei Guo","doi":"10.1021/acssuschemeng.4c07837","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c07837","url":null,"abstract":"Controlling particle size and phase hybridization in metal-compound-based catalysts is crucial for optimizing oxygen catalytic activity in zinc-air batteries (ZABs), yet precise regulation remains a substantial challenge. In this work, a novel confined complexation-calcination method is explored to synthesize a series of size-controllable Fe/Fe<sub>2</sub>O<sub>3</sub>/Fe<sub>5</sub>C<sub>2</sub> multicomponent nanoparticles embedded in Fe, N-doped mesoporous carbon (Fe–N–C). By modulation of the size of nitrogen-source ligands during confined complexation, the particle size and dispersion of Fe/Fe<sub>2</sub>O<sub>3</sub>/Fe<sub>5</sub>C<sub>2</sub> are precisely regulated, resulting in varied oxygen electrocatalytic performances. Notably, the electrocatalyst synthesized using a medium-sized nitrogen-source ligand 1,10-phenanthroline (Fe/Fe<sub>2</sub>O<sub>3</sub>/Fe<sub>5</sub>C<sub>2</sub>/Fe–N–C (PEN)) demonstrates the smallest particle size (∼19 nm) and superior dispersion of Fe/Fe<sub>2</sub>O<sub>3</sub>/Fe<sub>5</sub>C<sub>2</sub>, which not only increases the exposure of active sites but also enhances charge/mass transfer efficiency. The optimized Fe/Fe<sub>2</sub>O<sub>3</sub>/Fe<sub>5</sub>C<sub>2</sub>/Fe–N–C (PEN) shows excellent catalytic activity for oxygen reduction reaction with a half-wave potential of 0.835 V vs RHE. In addition, high stability and good activity for oxygen evolution reaction are also demonstrated, establishing it as an ideal bifunctional catalyst for secondary ZABs. The assembled ZAB achieves a peak power density of 148.9 mW cm<sup>–2</sup>, surpassing that of its Pt/C-based counterpart. This work provides new insights into precise particle size control of advanced electrocatalysts for sustainable energy applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"11 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077088","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}
Jie Sun, Haoyan Zhang, Jifan Chen, Xinjian Yu, Bingxue Rong, Wenli Zhong, Weixing Wang
{"title":"Synergistic Effect of Boric Acid and Sodium Dodecyl Sulfate in Promoting CO2 Hydrate Formation under Static Conditions","authors":"Jie Sun, Haoyan Zhang, Jifan Chen, Xinjian Yu, Bingxue Rong, Wenli Zhong, Weixing Wang","doi":"10.1021/acssuschemeng.4c10477","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10477","url":null,"abstract":"Hydrate-based CO<sub>2</sub> capture and storage (HCCS) is a promising approach to mitigate the greenhouse effect. However, the formation rate of the CO<sub>2</sub> hydrate is extremely slow, making it difficult to industrialize the HCCS technology. Here, we first report that the synergistic combination of boric acid (BA) and sodium dodecyl sulfate (SDS) significantly promotes CO<sub>2</sub> hydrate formation under static conditions. At the optimum concentration ratio (0.3 wt % BA + 0.2 wt % SDS), the capacity of the composite system reached 323.5 mg g<sup>–1</sup>, which is much higher than that of 0.5 wt % BA (47.7 mg g<sup>–1</sup>) or 0.5 wt % SDS (49.9 mg g<sup>–1</sup>). In addition, visual observations of the morphologies of the produced CO<sub>2</sub> hydrates indicated that the promotion mechanism was based on the capillary-driven theory. This work may open the door to the design of highly effective CO<sub>2</sub> hydrate promoters for HCCS technology.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"23 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143057349","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}
Krista Carlson, Brian J. Riley, Joshua Turner, David C. Cantu, Dev Chidambaram, Charmayne Lonergan, Jeffrey D. Rimer
{"title":"Dual-Bed Radioiodine Capture from Complex Gas Streams with Zeolites: Regeneration and Reuse of Primary Sorbent Beds for Sustainable Waste Management","authors":"Krista Carlson, Brian J. Riley, Joshua Turner, David C. Cantu, Dev Chidambaram, Charmayne Lonergan, Jeffrey D. Rimer","doi":"10.1021/acssuschemeng.4c09546","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09546","url":null,"abstract":"This article has not yet been cited by other publications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"74 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056795","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Leveraging a Dynamic Physical Cross-Linking Architecture to Enable Recycled PET with Exceptional Thermoplasticity and Toughness","authors":"Jinrui Hu, Xiao Xu, XinYi Cao, Lulu Dong, Lixia Bao, Weibo Kong, Jiliang Wang","doi":"10.1021/acssuschemeng.4c09372","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09372","url":null,"abstract":"The recycling of poly(ethylene terephthalate) (PET) is vital for environmental sustainability, yet achieving recycled PET (rPET) and its composites with optimal processability and flexibility remains a challenge. This study presents a solvent-free reactive extrusion method to extend the chains of rPET using a macromolecular chain extender (i.e., methyl methacrylate-glycidyl methacrylate copolymer, marked as PMG) rich in epoxy groups and to produce rPET/recycled polyethylene (rPET/rPE) composites. The resulting composites exhibit excellent thermoplasticity and controllable mechanical properties, such as the rPET/rPE composite (70:30 by mass), with a tensile strength of 39.2 MPa and an elongation at a break of 81.4%. After five extrusion cycles, their mechanical properties just encounter a subtle decline, indicating robust sustainability and cycle performance. The formation of a dynamic physical cross-linking network arises from the distinct polarity, hydrophobicity, and melt viscosity of rPET and rPE, where the hard spherical rPET phase is evenly dispersed in the soft rPE matrix with PMG acting as an interfacial compatibilizer. This innovative approach not only enhances the properties of the recycled composites but also promotes their cost-effectiveness and environmental benefits, thus broadening the potential applications of rPET and rPE as partial substitutes for virgin PET and PE.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"10 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056382","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}
Bin Sun, BingBing Li, Kai Li, Shennan Wang, Juan Xu, Yuxin Liu, Qi Zhou
{"title":"Correction to “Cellulose Microgel Toughening of Starch Nanocomposites: Exploiting the Advantages of Micro-Nanoscale Networks”","authors":"Bin Sun, BingBing Li, Kai Li, Shennan Wang, Juan Xu, Yuxin Liu, Qi Zhou","doi":"10.1021/acssuschemeng.4c10821","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c10821","url":null,"abstract":"In our original paper, in Figure 4, panels C and D are identical because we accidentally used the same image. Figure 4. (A) Tensile stress–strain curves of neat PLS, CM/PLS nanocomposites, and CNF/PLS nanocomposites. (B) Photographs of neat PLS, CM/PLS-4, and CNF/PLS-4 specimens stretched at 30% strain. (C) Toughness comparison of samples with different filler contents. (D) Break elongation comparison of samples with different filler contents. (E) Tensile stress–strain curves of PLS and CM/PLS nanocomposites during five cycles of loading and unloading to 30% strain. (F) Dissipation of energy difference between the first cycle and fifth cycle of the samples. The correct Figure 4 is below. No other content or conclusion of the published paper is affected. This article has not yet been cited by other publications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"122 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056716","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}
Olawumi Sadare, Garyfalia A. Zoumpouli, Y. M. John Chew, Jannis Wenk, Bernardo Castro-Dominguez, Davide Mattia
{"title":"Lignin- and Cellulose-Derived Sustainable Nanofiltration Polyelectrolyte Membranes","authors":"Olawumi Sadare, Garyfalia A. Zoumpouli, Y. M. John Chew, Jannis Wenk, Bernardo Castro-Dominguez, Davide Mattia","doi":"10.1021/acssuschemeng.4c08611","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c08611","url":null,"abstract":"Nanofiltration (NF) polymeric membranes are typically made from fossil fuel-derived feedstocks and toxic solvents, requiring a shift to more sustainable materials. This study pioneers the use of two biopolymers–cationic lignin and sodium carboxymethyl cellulose–as polycation and polyanion, respectively, to fabricate a polyelectrolyte membrane (PEM) via the layer-by-layer method with water as the sole solvent and on a poly(ether sulfone) (PES) support. At a transmembrane pressure of 2 bar, the pure water permeance was 6 LMHB (L/m<sup>2</sup> h bar) for 5 bilayers with a 96% rejection for positively charged methylene blue and 93% for negatively charged reactive orange-16, with a mass balance above 90%, indicating minimal adsorption on the membrane surface. The molecular weight cutoff (MWCO) of the PEM ranged from 300 and 620 Da, corresponding to a loose NF membrane. Additionally, the PEM demonstrated excellent stability after 30 days in deionized water, attributed to strong electrostatic interactions between the polyelectrolyte layers. This study demonstrates that effective NF membranes can be produced using sustainable biopolymeric materials and benign solvents. The efficient rejection of small, charged molecules makes the PEM membrane promising for protein removal, wastewater treatment, biotechnology, and pharmaceutical applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"261 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056717","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}
Xin Sun, Jin-Biao Wang, Ming-Qing Liao, Qian You, Ya Zheng, Yuan Liu, Xiao-Hang Han, Nan Qu, Zheng-Bai Zhao
{"title":"A Cooling Strategy for Photovoltaic Modules in Rear Encapsulation Film","authors":"Xin Sun, Jin-Biao Wang, Ming-Qing Liao, Qian You, Ya Zheng, Yuan Liu, Xiao-Hang Han, Nan Qu, Zheng-Bai Zhao","doi":"10.1021/acssuschemeng.4c09706","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c09706","url":null,"abstract":"Heat accumulation poses a significant issue for photovoltaic (PV) modules, leading to reduced electricity generation in cells and accelerated material aging. Improving heat dissipation performance without altering the existing mature structure and functionality of the PV modules presents a formidable, yet highly pragmatic and valuable challenge. This work reports a strategy to construct a boron nitride (BN) filler network in the rear encapsulation film to boost the heat dissipation of PV modules. The thermal conductivity of the fabricated film can be enhanced by 192% with approximately 2 wt % filler content in comparison to the commercial film, while preserving a light reflectivity of 68.4%. The enhanced thermal conductivity of the rear encapsulation film contributes to improved moisture and heat aging resistance, superior high-temperature resistance, and increased electricity generation efficiency for the module. The benefits of improving the thermal conductivity of encapsulation materials for PV modules warrant attention in this field.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"12 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056383","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}
Lara Wehbe, Rémi Bascou, Alla Nesterenko, Erwann Guénin
{"title":"Green Strategy for Sustainable Silk Lipopeptide Production using Mechanochemistry","authors":"Lara Wehbe, Rémi Bascou, Alla Nesterenko, Erwann Guénin","doi":"10.1021/acssuschemeng.4c05049","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c05049","url":null,"abstract":"A mechanochemical approach to peptide <i>N</i>-acylation was used for silk sericin lipopeptide production. A one-pot, two-step method with 1,1′-carbonyldiimidazole (CDI) fatty acid activation, followed by acylation, was implemented. First, the procedure was optimized on model amino acids such as leucine, glycine, serine, and aspartic acid using two different types of ball mill equipment: a vibrational ball mill and a planetary ball mill. High conversion rates of 99% were observed for amino acid acylation under optimal conditions with both types. Then, grafting hydrophobic chains on to two different silk sericin hydrolysates was studied. The peptide acylation rate of 48–51% was obtained with three fatty acids with chain lengths of 10, 12, and 14. Lipopeptides obtained using the mechanochemical methodology showed good surface activity and reduced surface tension of up to 26 mN/m. The advantage of the proposed approach compared to conventional Schotten–Baumann <i>N</i>-acylation was confirmed with green metrics calculation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"25 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056384","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Photocatalyzed Direct Decarboxylation for Biobased Cadaverine Production under Mild Conditions","authors":"Zhanling Ma, Zongwu Xin, Yuan Yao, Shaojie Qin, Yuhong Huang","doi":"10.1021/acssuschemeng.4c06918","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c06918","url":null,"abstract":"The decarboxylation of bio-originated <span>l</span>-lysine to cadaverine provided a sustainable pathway for the production of bionylon 5X materials due to the low cost and overcapacity of <span>l</span>-lysine. A photocatalytic approach was designed to produce cadaverine using Pt/TiO<sub>2</sub> as an effective photocatalyst under mild conditions (UV light, 30 °C, and 0.1 MPa H<sub>2</sub>). The Pt cocatalyst was utilized to promote the effective separation of photogenerated electrons and holes in the semiconductor TiO<sub>2</sub>. After Pt doping, the bandgap width of TiO<sub>2</sub> was narrowed from 3.12 to 2.88 eV, promoting the generation of photogenerated electrons and holes. With the synergistic effect of Pt, TiO<sub>2</sub>, and oxygen vacancies, the selectivity of cadaverine increased to 86% under optimal conditions. At a molecular level, FT-IR spectra showed that <span>l</span>-lysine was adsorbed vertically via the coordination of −COOH on Pt/TiO<sub>2</sub>. It was then directed to be oxidized by photogenerated holes to form (NH<sub>2</sub>)<sub>2</sub>(CH<sub>2</sub>)<sub>4</sub>CH· radicals, as proven by the in situ FT-IR investigation. Alkyl radical intermediates formed on holes then readily coupled with hydrogen species to yield a high selectivity of cadaverine. This work sheds new light on the effective and green high-value conversion of biomass.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"31 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055418","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}