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A Cage Structural Hollow-Mesoporous Microreactor Confining Extractant for Lithium Recovery from Salt-Lake Brine. 笼形结构中空-介孔微反应器约束萃取剂用于盐湖卤水锂回收。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-23 DOI: 10.1002/cssc.202500818
Enze Li, Yudi Gong, Zelong Li, Qiancheng Xia, Guandao Gao, Zihe Pan, Zhaozan Xu, Fangqin Cheng
{"title":"A Cage Structural Hollow-Mesoporous Microreactor Confining Extractant for Lithium Recovery from Salt-Lake Brine.","authors":"Enze Li, Yudi Gong, Zelong Li, Qiancheng Xia, Guandao Gao, Zihe Pan, Zhaozan Xu, Fangqin Cheng","doi":"10.1002/cssc.202500818","DOIUrl":"10.1002/cssc.202500818","url":null,"abstract":"<p><p>The sustainable and efficient lithium supply can effectively support the global energy transformation toward decarbonization and the development of electrified industries. However, current established solvent extraction technology suffers from extractant dissolution and low efficiency. Herein, a stable cage structural hollow-mesoporous microreactor with the confinement of lithium extractant, Na[FeCl<sub>4</sub>·2TBP], in the hollow cavity is developed for enhancing lithium separation from salt-lake brine. Resultantly, the confinement effect can compartmentalize extractant into micron-sized droplets and prevent its dissolution into aqueous phase. The obtained hollow-mesoporous microreactor exerts outstanding separation performance of Li<sup>+</sup> from brine, even at Mg/Li mass ratio up to 100:1, with high cyclic stability, adsorption quantity of 34.6 mg g<sup>-1</sup>, and Li<sup>+</sup>/Mg<sup>2+</sup> selectivity of nearly 1000 which is about six times higher than that for conventional extraction by Na[FeCl<sub>4</sub>·2TBP]. The mesopores within shells serve as Li<sup>+</sup> transport channels before reaction with the extractant confined in the hollow cavity. In this article, it is propose that the interfacial electric field generated by surface charges of mesopores can enhance Li<sup>+</sup> dehydration and diffusion, which synergize with stronger binding capacity of Li<sup>+</sup> with [FeCl<sub>4</sub>·2TBP]<sup>-</sup> to enhance the selectivity of Li<sup>+</sup>. These results constitute a novel perspective to design new approaches for lithium recovery from lithium-containing aqueous solutions.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500818"},"PeriodicalIF":7.5,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144473465","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Organic Solvent-Regulated Supramolecular Adhesives with Robust yet Reversible Adhesion. 有机溶剂调节的超分子粘合剂,具有坚固而可逆的粘附性。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-23 DOI: 10.1002/cssc.202501027
Shuning Li, Mengnan Lai, Qiuyu Wang, Bin Zhu, Qiqi Huang, Peirou Wang, Yuqian Huang, Qiufeng Li, Zhan Chen, Yaokang Zhang, Xuechang Zhou
{"title":"Organic Solvent-Regulated Supramolecular Adhesives with Robust yet Reversible Adhesion.","authors":"Shuning Li, Mengnan Lai, Qiuyu Wang, Bin Zhu, Qiqi Huang, Peirou Wang, Yuqian Huang, Qiufeng Li, Zhan Chen, Yaokang Zhang, Xuechang Zhou","doi":"10.1002/cssc.202501027","DOIUrl":"https://doi.org/10.1002/cssc.202501027","url":null,"abstract":"<p><p>Reversible adhesives are crucial for enabling high-strength, eco-friendly bonding with on-demand detachment, yet achieving fully sustainable adhesives with high-strength and reliable detachment remains a challenge. Here, we present a supramolecular adhesive derived from natural materials, namely supramolecular adhesive tailored by organic solvents (SATO), comprising tannic acid, β-cyclodextrin, and organic solvents (DMSO, ethylene glycol, or glycerol) integrated through dynamic hydrogen-bond networks. The optimized SATO achieves robust interfacial adhesion strength up to 4.1 MPa, with retained adhesion (~0.8 MPa) even after 30 repeated bonding-debonding cycles. The adhesive demonstrates humidity-sensitive adhesion and exceptional freeze resistance, retaining ~96% of its initial adhesion strength after 7 days storage at -50 °C. When used to fabricate sand columns, SATO achieves compressive strengths of >11 MPa while enabling rapid on-demand disintegration within 2 s via water exposure. By synergizing eco-friendliness, high mechanical performance, and reversible adhesion, SATO holds promise for applications in arid environment and temporary structural engineering.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202501027"},"PeriodicalIF":7.5,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144473524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Carbon-Coated Silver Nanoparticles for Highly Robust Chloride Capture in Electrochemical Desalination and Lithium Recovery. 碳包覆银纳米粒子在电化学脱盐和锂回收中的高鲁棒氯化物捕获。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-21 DOI: 10.1002/cssc.202500267
Seoni Kim, Sung Pil Hong, Hwajoo Joo, Chanhyeong Lee, Yung-Eun Sung, Jeyong Yoon, Jin Soo Kang
{"title":"Carbon-Coated Silver Nanoparticles for Highly Robust Chloride Capture in Electrochemical Desalination and Lithium Recovery.","authors":"Seoni Kim, Sung Pil Hong, Hwajoo Joo, Chanhyeong Lee, Yung-Eun Sung, Jeyong Yoon, Jin Soo Kang","doi":"10.1002/cssc.202500267","DOIUrl":"10.1002/cssc.202500267","url":null,"abstract":"<p><p>In recent years, electrochemical desalination and resource recovery processes have gained significant attention as means of utilizing waters, wherein the majority of anionic species are chloride ions. There have been research efforts to develop high-performance electrode materials for the chloride uptake. Silver with extremely fast kinetics is an ideal option, but the cost and stability issues are yet to be resolved. Herein, silver nanoparticles with nitrogen-doped carbon (NC) shells are developed for electrochemical Cl<sup>-</sup> capture in desalination and lithium recovery processes. Starting from commercial Ag powders, nanosized particles are obtained by the chlorination to AgCl, which is followed by the polydopamine coating and thermal annealing. Interestingly, dopamine polymerization can be coupled with the dechlorination of the AgCl, enabling the simultaneous polymeric shell formation and AgCl-to-Ag conversion. This NC-coated Ag nanoparticles (N-Ag@NC) manifest superior capacity and cyclic stability in electrochemical Cl<sup>-</sup> capture, when compared with those of Ag particles without NC shells or with a larger (microscale) size. The enhanced performance is attributable to the small particle sizes and the NC shells, which result in a higher Ag utilization and tolerance to the volume changes accompanying the chlorination/dechlorination.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500267"},"PeriodicalIF":7.5,"publicationDate":"2025-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144339711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
A Telescoped Strategy for the Preparation of Five-Membered Hetero- and Carbocycles via Hydrogen Atom Transfer Photocatalysis in Flow. 流动中氢原子转移光催化制备五元杂环和碳环的缩合策略。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-20 DOI: 10.1002/cssc.202501012
Filippo Sacchelli, Elena Quadri, Luna Raineri, Alexandra Jorea, Marzia Pessina, Anna Lo Presti, Nicola Della Ca', Davide Ravelli, Luca Capaldo
{"title":"A Telescoped Strategy for the Preparation of Five-Membered Hetero- and Carbocycles via Hydrogen Atom Transfer Photocatalysis in Flow.","authors":"Filippo Sacchelli, Elena Quadri, Luna Raineri, Alexandra Jorea, Marzia Pessina, Anna Lo Presti, Nicola Della Ca', Davide Ravelli, Luca Capaldo","doi":"10.1002/cssc.202501012","DOIUrl":"10.1002/cssc.202501012","url":null,"abstract":"<p><p>Five-membered heterocycles such as pyrroles and thiophenes, along with cyclopentenones, are key scaffolds in pharmaceutical chemistry. However, the synthesis of these motifs via diversity oriented synthesis is hindered by the limited accessibility of unsymmetrical 1,4-diketones. Herein, a practical and sustainable flow protocol is presented for the telescoped synthesis of pyrroles, thiophenes, and cyclopentenones. The process begins with decatungstate-photocatalyzed hydrogen atom transfer from aldehydes to generate acyl radicals, which undergo regioselective addition to functionalized enones. The resulting diketones are then fed into a second reactor-tubular or packed-bed-to undergo Paal-Knorr or Hunsdiecker condensation reactions. This modular strategy enables rapid access to densely substituted, biorelevant hetero- and carbocycles with unconventional substitution patterns, as demonstrated by the synthesis of tri-, tetra-, and pentasubstituted pyrroles and thiophenes, and mono-, di-, and trisubstituted cyclopentenones.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2501012"},"PeriodicalIF":7.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144332195","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Hierarchical Microstructured K3V2(PO4)3/C-Composite Electrode for Potassium-Ion Batteries through Scalable Spray-Drying Approach. 分级微结构K3V2(PO4)3/ c复合钾离子电池电极的喷雾干燥研究
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-20 DOI: 10.1002/cssc.202501111
Andreas Heyn, Celine Röder, Holger Geßwein, Ali Ahmadian, Martin Velazquez-Rizo, Nicole Bohn, Fabian Jeschull, Joachim R Binder
{"title":"Hierarchical Microstructured K<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>/C-Composite Electrode for Potassium-Ion Batteries through Scalable Spray-Drying Approach.","authors":"Andreas Heyn, Celine Röder, Holger Geßwein, Ali Ahmadian, Martin Velazquez-Rizo, Nicole Bohn, Fabian Jeschull, Joachim R Binder","doi":"10.1002/cssc.202501111","DOIUrl":"10.1002/cssc.202501111","url":null,"abstract":"<p><p>Potassium vanadium phosphate K<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> (KVP) is a promising polyanionic cathodic material for potassium-ion batteries. As many other polyanionic materials KVP suffers from low electronic conductivity and shows just limited electrochemical performance. To overcome this limitation and improve the electrochemical performance, an easily scalable spray-drying process is developed to create hierarchically structured KVP/C composites. The spray-drying process leads to spherical and open porous granules of KVP particles wrapped in a carbon matrix, formed by the decomposition of sucrose and β-lactose. The influence of different carbon sources (sucrose and β-lactose) onto the granules' microstructure is systematically studied and correlated it with the electrochemical performance of the KVP/C. The best-performing composition is employed to study different electrolyte additives with the aim to improve the electrolyte stability at high potentials in potassium half-cells.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2501111"},"PeriodicalIF":7.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144332196","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
How to Produce Green Hydrogen from Olivine and Seawater? By Ultrasound. 如何从橄榄石和海水中生产绿色氢?通过超声波。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-20 DOI: 10.1002/cssc.202500627
Sergey I Nikitenko, Tony Chave
{"title":"How to Produce Green Hydrogen from Olivine and Seawater? By Ultrasound.","authors":"Sergey I Nikitenko, Tony Chave","doi":"10.1002/cssc.202500627","DOIUrl":"10.1002/cssc.202500627","url":null,"abstract":"<p><p>Green hydrogen is a pillar for achieving global decarbonization and the reduction of greenhouse gas emissions. Here, a new, nature-inspired process for green hydrogen production using virtually unlimited natural resources is reported. Olivine, the most abundant mineral in the Earth's upper mantle, is key to this process. It is found that 20 kHz ultrasound accelerates hydrogen production from olivine suspensions in seawater under near-ambient conditions by almost 3000 times compared to the hydrothermal process. Strong mechanical stirring does not lead to hydrogen evolution in the temperature range of 40-90 °C. The striking effect of ultrasound is attributed to acoustic cavitation, which provides depassivation of the olivine surface, fragmentation of olivine particles, and local transient heating caused by collapsing bubbles. In principle, ultrasonic activation of the olivine/seawater system enables on-demand hydrogen production.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500627"},"PeriodicalIF":7.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144332197","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Microfluidic-Assisted Evolution of a Robust NAD+-Dependent Enzyme with Improved Isobutanol Tolerance at Elevated Temperatures. 一种在高温下具有提高异丁醇耐受性的稳健NAD+依赖酶的微流体辅助进化。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-20 DOI: 10.1002/cssc.202501120
Mariko Teshima, Robert Genth, Tenuun Bayaraa, Manuel Döring, Barbara Beer, Gerhard Schenk, Volker Sieber
{"title":"Microfluidic-Assisted Evolution of a Robust NAD<sup>+</sup>-Dependent Enzyme with Improved Isobutanol Tolerance at Elevated Temperatures.","authors":"Mariko Teshima, Robert Genth, Tenuun Bayaraa, Manuel Döring, Barbara Beer, Gerhard Schenk, Volker Sieber","doi":"10.1002/cssc.202501120","DOIUrl":"10.1002/cssc.202501120","url":null,"abstract":"<p><p>Prompted by the thermostability issue identified in recent work on enzyme discovery/engineering and its application, the directed evolution of an NAD<sup>+</sup>-dependent aldehyde dehydrogenase (ALDH) with improved thermostability and isobutanol tolerance at 50 °C, properties required for its successful implementation in cell-free isobutanol biosynthesis, is described herein. ALDH not only plays an important role in multienzyme cascades for the production of platform chemicals but also represents a bottleneck due to its modest stability. Using a custom-built absorbance-activated droplet sorter, ultrahigh-throughput microfluidic screening of a randomized library of 63,000 members is performed, leading to the discovery of a variant with a 250-fold prolonged half-life at 50 °C without significant loss of activity. Subsequently, the most promising mutations are distributed on designer templates in the combinatorial staggered extension process library to create a new generation of variants. One of these variants shows a threefold increase in k<sub>cat</sub> K<sub>m</sub> <sup>-1</sup>. Another shows significantly higher stability in 3% v/v isobutanol, retaining ≈50% of its initial activity after 6 h of incubation at 50 °C. Finally, a cell-free multienzymatic cascade using the ultimate variant demonstrates its superior stability in 4% v/v isobutanol at 50 °C, highlighting the success of engineering to overcome the cofactor-related challenge of establishing cascade balance.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2501120"},"PeriodicalIF":7.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144332199","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Improving the Economics of Sustainable Aviation Fuels: System-Level Analyses and Perspective. 提高可持续航空燃料的经济性:系统级分析和观点。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-20 DOI: 10.1002/cssc.202500878
Sungil Yun, Bomin Choe, Heeseung Na, Byeongchan Ahn, Hyungtae Cho, Young-Ju Kim, Wangyun Won
{"title":"Improving the Economics of Sustainable Aviation Fuels: System-Level Analyses and Perspective.","authors":"Sungil Yun, Bomin Choe, Heeseung Na, Byeongchan Ahn, Hyungtae Cho, Young-Ju Kim, Wangyun Won","doi":"10.1002/cssc.202500878","DOIUrl":"10.1002/cssc.202500878","url":null,"abstract":"<p><p>The transportation sector is becoming more electrified in accordance with the energy transition to renewable energy. However, aviation is challenging to decarbonize due to the low energy density of batteries. Specifically, it is difficult to store large-scale batteries in aircraft because there are stringent limitations on weight and space. Therefore, sustainable aviation fuel (SAF) should serve as a bridge to battery-powered aircraft untilbattery technology matures to lower transportation-related carbon emissions. It is imperative to produce SAF in a techno-economically feasible manner. Nevertheless, the successful commercialization of SAF is being hampered by the shortcomings of the SAF production processes, such as low efficiency. Therefore, a coproduction strategy is employed to build a new process addressing uncompetitive economics and low carbon efficiency of the SAF production process. The developed process coproduces valuable biochemicals, adipic acid, and furfural, with butene oligomer (i.e., SAF) using lignocellulosic biomass. In this article, comprehensive evaluations including tech no-economic analysis and life-cycle assessment are conducted to demonstrate the benefits of the proposed process. The findings reveal that the proposed approach not only improves the process economics by ≈2.7% but also significantly enhances the environmental sustainability of the process, achieving a reduction of 15.75 kg CO<sub>2</sub> eq kg<sup>-1</sup> SAF.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500878"},"PeriodicalIF":7.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144332198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
A High-Throughput Investigation of the Binding Specificity of Carbohydrate-Binding Modules for Synthetic and Natural Polymers. 碳水化合物结合模块对合成和天然聚合物结合特异性的高通量研究。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-19 DOI: 10.1002/cssc.202500468
Andrew Philip Rennison, Jaime Fernandez-Macgregor, Julie Melot, Fabien Durbesson, Tobias Tandrup, Peter Westh, Renaud Vincentelli, Marie Sofie Møller
{"title":"A High-Throughput Investigation of the Binding Specificity of Carbohydrate-Binding Modules for Synthetic and Natural Polymers.","authors":"Andrew Philip Rennison, Jaime Fernandez-Macgregor, Julie Melot, Fabien Durbesson, Tobias Tandrup, Peter Westh, Renaud Vincentelli, Marie Sofie Møller","doi":"10.1002/cssc.202500468","DOIUrl":"10.1002/cssc.202500468","url":null,"abstract":"<p><p>Carbohydrate-binding modules (CBMs) are noncatalytic domains that enhance enzyme binding to substrates. Type A CBMs show potential for engineering plastic-degrading enzymes due to their affinity for synthetic polymers. This study presents a high-throughput screening pipeline for characterizing the affinity and specificity of type A CBMs towards the synthetic polymers polyethylene terephthalate (PET), polystyrene (PS), and polyethylene (PE), and the polysaccharides cellulose, chitin, and starch. ≈800 CBMs from the families CBM2, CBM3, CBM10, and CBM64 are expressed as green fluorescent protein (GFP)-fusion proteins and tested for binding using a modified holdup assay, which produced up to 10 000 data points per day. The screening identifies ≈150 binders for PET and PE, around 250 for PS, and demonstrates family-specific binding patterns for avicel, chitin, and starch. To demonstrate practical utility, four CBMs with high PET affinity are fused to the PET hydrolase LCC<sup>ICCG</sup>, enhancing activity on PET powder by around 5-fold. These CBM-enzyme fusions mitigate competitive binding to plastic impurities, improving performance in mixed plastic assays. This work significantly expands the repertoire of CBMs binding to synthetic polymers, advances our understanding of CBM-substrate interactions, and provides knowledge for engineering enzymes to tackle plastic pollution, particularly where mixed plastics pose significant challenges.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500468"},"PeriodicalIF":7.5,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144323966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Crystallinity-Enhanced CO2 Adsorption by Sodium Poly(Heptazine Imide) Frameworks. 聚七嗪亚胺钠框架对CO2的结晶增强吸附。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-06-19 DOI: 10.1002/cssc.202500775
Pedro Ouro, Álvaro Cuevas, Johannes Liessem, Dariusz Mitoraj, Radim Beranek, Eva Díaz, Salvador Ordóñez, Ildefonso Marin-Montesinos, Daniel Pereira, Mariana Sardo, Igor Krivtsov, Luís Mafra, Marina Ilkaeva
{"title":"Crystallinity-Enhanced CO<sub>2</sub> Adsorption by Sodium Poly(Heptazine Imide) Frameworks.","authors":"Pedro Ouro, Álvaro Cuevas, Johannes Liessem, Dariusz Mitoraj, Radim Beranek, Eva Díaz, Salvador Ordóñez, Ildefonso Marin-Montesinos, Daniel Pereira, Mariana Sardo, Igor Krivtsov, Luís Mafra, Marina Ilkaeva","doi":"10.1002/cssc.202500775","DOIUrl":"10.1002/cssc.202500775","url":null,"abstract":"<p><p>This work presents sodium poly(heptazine imide) (NaPHI)-based materials, synthesized in a NaCl medium, as highly effective platforms for CO<sub>2</sub> capture. High crystallinity-an often-overlooked aspect in PHI frameworks-is identified as a key factor governing CO<sub>2</sub> adsorption capacity in microporous structures. Thermogravimetric analysis and manometric studies reveal a CO<sub>2</sub> uptake of ≈3.8 mmol g<sup>-1</sup>, at 1 bar and 25 °C, surpassing most reported PHI-based adsorbents under similar conditions. Exchanging Na<sup>+</sup> with K<sup>+</sup> or Rb<sup>+</sup> preserves CO<sub>2</sub> adsorption performance, whereas Cs<sup>+</sup> incorporation induces structural distortion, greatly reducing CO<sub>2</sub> adsorption capacity in PHI. These materials exhibit excellent cyclic stability (20 cycles) without degradation and CO<sub>2</sub> adsorption capacity loss. Notably, at flue gas-relevant temperature (100 °C), NaPHI attains a CO<sub>2</sub> capacity of 2.1 mmol g<sup>-1</sup>, doubling the performance of benchmark Zeolite 13X (1.1 mmol g<sup>-1</sup>). Ideal Adsorbed Solution Theory confirms remarkable CO<sub>2</sub>/N<sub>2</sub> selectivity (≈3.8 mmol g<sup>-1</sup> vs typical N<sub>2</sub> adsorption of 0.3 mmol g<sup>-1</sup>), a critical property for postcombustion CO<sub>2</sub> capture. These findings position PHI-based materials as a disruptive platform for CO<sub>2</sub> adsorption, offering 1) straightforward synthesis from readily available precursors, 2) promising scalability, and 3) outstanding performance.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500775"},"PeriodicalIF":7.5,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144323968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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