Global warming caused primarily by excessive emissions of CO2 has attracted worldwide attention. Herein, three 2-hydroxypyridium ionic liquids (ILs) based task-specific deep eutectic solvents (DESs) were synthesized to absorb CO2 and physical properties including density, viscosity, and melting points were measured to explore the effect on CO2 absorption. The CO2 absorption capacities of the ILs-based task-specific DESs were investigated at different pressures and temperatures, which showed that the maximum absorption capacity of the DES was up to 1.48 molCO2·molDES−1 or 0.233 gCO2·gDES−1 at the atmospheric pressure and 25 °C. The plausible absorption mechanism was also proposed by a combination of 1:1 and 2:1 stoichiometric reactions of CO2 and the IL-based task-specific DES via multiple-site absorption, which was confirmed by 13C and 1H nuclear magnetic resonance (NMR), Fourier transform infrared (FT-IR) spectroscopy, quantum chemical calculation, and reaction equilibrium thermodynamic modeling. The thermodynamic properties, including absorption Gibbs free energy, absorption enthalpy, and absorption entropy were rationally deduced and explained. Furthermore, the excellent CO2 absorption capacity and regenerability of multiple-site task-specific DES make it a new environmentally eco-friendly choice for highly efficient CO2 absorption and subsequent CO2 transformation.
{"title":"Multiple-site absorption of CO2 in 2-hydroxypyridium ionic liquids based task-specific deep eutectic solvents","authors":"Xinzi Wu, Jiawei Ruan, Ke Wang, Xiaoyi Zhang, Mingfeng Ma, Lifang Chen, Zhiwen Qi","doi":"10.1016/j.gce.2024.09.005","DOIUrl":"10.1016/j.gce.2024.09.005","url":null,"abstract":"<div><div>Global warming caused primarily by excessive emissions of CO<sub>2</sub> has attracted worldwide attention. Herein, three 2-hydroxypyridium ionic liquids (ILs) based task-specific deep eutectic solvents (DESs) were synthesized to absorb CO<sub>2</sub> and physical properties including density, viscosity, and melting points were measured to explore the effect on CO<sub>2</sub> absorption. The CO<sub>2</sub> absorption capacities of the ILs-based task-specific DESs were investigated at different pressures and temperatures, which showed that the maximum absorption capacity of the DES was up to 1.48 mol<sub>CO2</sub>·mol<sub>DES</sub><sup>−1</sup> or 0.233 g<sub>CO2</sub>·g<sub>DES</sub><sup>−1</sup> at the atmospheric pressure and 25 °C. The plausible absorption mechanism was also proposed by a combination of 1:1 and 2:1 stoichiometric reactions of CO<sub>2</sub> and the IL-based task-specific DES <em>via</em> multiple-site absorption, which was confirmed by <sup>13</sup>C and <sup>1</sup>H nuclear magnetic resonance (NMR), Fourier transform infrared (FT-IR) spectroscopy, quantum chemical calculation, and reaction equilibrium thermodynamic modeling. The thermodynamic properties, including absorption Gibbs free energy, absorption enthalpy, and absorption entropy were rationally deduced and explained. Furthermore, the excellent CO<sub>2</sub> absorption capacity and regenerability of multiple-site task-specific DES make it a new environmentally eco-friendly choice for highly efficient CO<sub>2</sub> absorption and subsequent CO<sub>2</sub> transformation.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 1","pages":"Pages 38-50"},"PeriodicalIF":7.6,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145420216","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2024-10-05DOI: 10.1016/j.gce.2024.09.011
Yang Liu , Yuxiang Chen , Chuanlei Liu , Yupeng Cui , Qiyue Zhao , Guanchu Guo , Hao Jiang , Qiumin Wu , Haiyang Wen , Fahai Cao , Benxian Shen , Hui Sun
Machine learning (ML) algorithms are playing increasingly important roles in exploring solvents for wide industrial applications. However, most ML strategies for solvent screening neglect the contributions of intermolecular interactions among solvent components, resulting in reduced prediction accuracy for the solubilities of solvent mixtures. In this study, we propose an efficient method combining feature-based transfer learning and a hybrid Henry's law constant (HLC) calculation method to assist the exploration of promising solvent mixtures to remove organic sulfides. The incorporation of predicted HLC values from established models as features significantly enhances the prediction accuracy for various organic sulfides. In the case of 2-propanethiol, the prediction shows a R2test of 0.91, RMSE of 0.0166, and MAE of 0.0118. The hybrid HLC calculation method, which incorporates non-ideal interactions between two solvent components, outperforms both the conductor-like screening models for real solvents (COSMO-RS) and ideal solution methods in predicting experimental HLC values. The present method successfully predicts a hybrid solvent for methanethiol (MeSH) removal. Both static and dynamic absorption experiments confirm that this designed solvent mixture has the lowest HLC of 370.48 kPa and the highest removal rate of 80.38% for MeSH.
{"title":"Prediction of organic sulfur solubility in mixed solvent using feature-based transfer learning and a hybrid Henry's law constant calculation method","authors":"Yang Liu , Yuxiang Chen , Chuanlei Liu , Yupeng Cui , Qiyue Zhao , Guanchu Guo , Hao Jiang , Qiumin Wu , Haiyang Wen , Fahai Cao , Benxian Shen , Hui Sun","doi":"10.1016/j.gce.2024.09.011","DOIUrl":"10.1016/j.gce.2024.09.011","url":null,"abstract":"<div><div>Machine learning (ML) algorithms are playing increasingly important roles in exploring solvents for wide industrial applications. However, most ML strategies for solvent screening neglect the contributions of intermolecular interactions among solvent components, resulting in reduced prediction accuracy for the solubilities of solvent mixtures. In this study, we propose an efficient method combining feature-based transfer learning and a hybrid Henry's law constant (HLC) calculation method to assist the exploration of promising solvent mixtures to remove organic sulfides. The incorporation of predicted HLC values from established models as features significantly enhances the prediction accuracy for various organic sulfides. In the case of 2-propanethiol, the prediction shows a R<sup>2</sup><sub>test</sub> of 0.91, RMSE of 0.0166, and MAE of 0.0118. The hybrid HLC calculation method, which incorporates non-ideal interactions between two solvent components, outperforms both the conductor-like screening models for real solvents (COSMO-RS) and ideal solution methods in predicting experimental HLC values. The present method successfully predicts a hybrid solvent for methanethiol (MeSH) removal. Both static and dynamic absorption experiments confirm that this designed solvent mixture has the lowest HLC of 370.48 kPa and the highest removal rate of 80.38% for MeSH.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 1","pages":"Pages 109-120"},"PeriodicalIF":7.6,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145420207","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2024-10-09DOI: 10.1016/j.gce.2024.10.002
Atul A. Pawar , S. Anuradha Jabasingh , Shimelis Kebede Kassahun , Hern Kim
The direct conversion of carbon dioxide (CO2) and propylene oxide (PO) into propylene carbonate (PC) offers a green way to utilize anthropogenic CO2. However, this reaction is limited by low conversion of PO and harsh reaction conditions. In this study, we solve this problem using ionic liquids (ILs)/metal oxide composites (ILs@MAO). The catalytic activity of MAO-500 (500 = annealing temperature) is poor evidenced by its low conversion of PO (24.94%). However, ILs@MAO-500 has a high conversion of PO (97.54%) under similar reaction conditions (2 h at 1.5 MPa CO2 pressure, 90 °C, and 0.85 g catalyst). The ILs consist of imidazolium cation with weak coordinated [NTf2]– anion leading to outward movement of anion resulting in the formation of “heterodinuclear complex”. This complex generates an amorphous-crystalline intermediate with balanced acid-base sites that activate PO and stabilize the catalytic intermediate. In large part, the high PO conversion is theorized to be primarily due to the abundant reactive sites in the ILs that are covalently immobilized on the MAO-500 carrier. Furthermore, even after multiple recycling, ILs@MAO-500 remains stable and exhibits high yield and selectivity. The proposed solvent-free catalytic system is mild, kinetically fast, and naturally safe for coupling CO2 and PO into PC synthesis.
{"title":"Incorporation of Mg/Al metal oxide into ionic liquids for CO2 capture and conversion into cyclic carbonate under solvent-free conditions: effect of coordination ability, recyclability, and catalytic study","authors":"Atul A. Pawar , S. Anuradha Jabasingh , Shimelis Kebede Kassahun , Hern Kim","doi":"10.1016/j.gce.2024.10.002","DOIUrl":"10.1016/j.gce.2024.10.002","url":null,"abstract":"<div><div>The direct conversion of carbon dioxide (CO<sub>2</sub>) and propylene oxide (PO) into propylene carbonate (PC) offers a green way to utilize anthropogenic CO<sub>2</sub>. However, this reaction is limited by low conversion of PO and harsh reaction conditions. In this study, we solve this problem using ionic liquids (ILs)/metal oxide composites (ILs@MAO). The catalytic activity of MAO-500 (500 = annealing temperature) is poor evidenced by its low conversion of PO (24.94%). However, ILs@MAO-500 has a high conversion of PO (97.54%) under similar reaction conditions (2 h at 1.5 MPa CO<sub>2</sub> pressure, 90 °C, and 0.85 g catalyst). The ILs consist of imidazolium cation with weak coordinated [NTf<sub>2</sub>]<sup>–</sup> anion leading to outward movement of anion resulting in the formation of “heterodinuclear complex”. This complex generates an amorphous-crystalline intermediate with balanced acid-base sites that activate PO and stabilize the catalytic intermediate. In large part, the high PO conversion is theorized to be primarily due to the abundant reactive sites in the ILs that are covalently immobilized on the MAO-500 carrier. Furthermore, even after multiple recycling, ILs@MAO-500 remains stable and exhibits high yield and selectivity. The proposed solvent-free catalytic system is mild, kinetically fast, and naturally safe for coupling CO<sub>2</sub> and PO into PC synthesis.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 1","pages":"Pages 121-130"},"PeriodicalIF":7.6,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145420214","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2024-09-30DOI: 10.1016/j.gce.2024.09.012
Junfa Yuan , Jinshu Huang , Joseph VL. Ruatpuia , Jiasheng Chen , Huan Wang , Samuel Lalthazuala Rokhum , Hu Li
Deep eutectic solvent (DES) pretreatment is attractive for the delignification of lignocellulosic biomass, while unable to circumvent the trenchant demand for the higher-temperature operating conditions. Herein, an electro-assisted DES (choline chloride/ethylene glycol = 1:2) strategy was developed for wheat straw pretreatment at room temperature. The rate of lignin removal, hemicellulose removal, cellulose recovery, and cellulose saccharification reached 68.1%, 60.8%, 95.1%, and 82.5%, respectively, which were comparable or superior to the reported efficiency of traditional DES pretreatment methods. The destruction of lignin by electricity and in-situ dissolution of released lignin components with DES enabled effectively the separation of the full components. Notably, the evolution rate of hydrogen in-situ produced during electro-driven DES pretreatment of wheat straw was 50 μmol cm−2 h−1, and 4.6 g/100 g lipids could be obtained with Trichosporon cutaneum grown on the fractionated cellulose and hemicellulose components. The electro-assisted DES process offers a potential platform for lignocellulosic biomass fractionation at ambient conditions. According to the life cycle cost analysis (LCCA), the estimated cost of producing hydrogen from 100 g of wheat straw is only $37.24, demonstrating its potential for commercial viability.
{"title":"Electro-driven deep eutectic solvent pretreatment of wheat straw with enhancive component fractionation and hydrogen evolution at room temperature","authors":"Junfa Yuan , Jinshu Huang , Joseph VL. Ruatpuia , Jiasheng Chen , Huan Wang , Samuel Lalthazuala Rokhum , Hu Li","doi":"10.1016/j.gce.2024.09.012","DOIUrl":"10.1016/j.gce.2024.09.012","url":null,"abstract":"<div><div>Deep eutectic solvent (DES) pretreatment is attractive for the delignification of lignocellulosic biomass, while unable to circumvent the trenchant demand for the higher-temperature operating conditions. Herein, an electro-assisted DES (choline chloride/ethylene glycol = 1:2) strategy was developed for wheat straw pretreatment at room temperature. The rate of lignin removal, hemicellulose removal, cellulose recovery, and cellulose saccharification reached 68.1%, 60.8%, 95.1%, and 82.5%, respectively, which were comparable or superior to the reported efficiency of traditional DES pretreatment methods. The destruction of lignin by electricity and <em>in-situ</em> dissolution of released lignin components with DES enabled effectively the separation of the full components. Notably, the evolution rate of hydrogen <em>in</em><em>-</em><em>situ</em> produced during electro-driven DES pretreatment of wheat straw was 50 μmol cm<sup>−2</sup> h<sup>−1</sup>, and 4.6 g/100 g lipids could be obtained with <em>Trichosporon cutaneum</em> grown on the fractionated cellulose and hemicellulose components. The electro-assisted DES process offers a potential platform for lignocellulosic biomass fractionation at ambient conditions. According to the life cycle cost analysis (LCCA), the estimated cost of producing hydrogen from 100 g of wheat straw is only $37.24, demonstrating its potential for commercial viability.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 1","pages":"Pages 83-93"},"PeriodicalIF":7.6,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145420210","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Incorporating high valence dopants, such as W6+ and Mo6+ has been verified to be effective for tuning the microstructure and grain boundary of polycrystal Ni-rich cathode. However, the hindered consolidation of primary particles induced by dopants during lithiation calcination limits the utilization of those dopants to crystalize single-crystal Ni-rich cathodes with stabilized lattice and surface. Herein, high performance single crystal LiNi0.84Co0.11Mn0.05O2 cathode with Al3+ and W6+ regulated lattice and boundary phase was construed based on commercial process with two-step calcination process containing separated lithiation and crystallization. The introduction of appropriate amount of Al3+ in the first lithiation calcination of 6 h endows the bulk of crystalline with enhanced lattice stability, while the incorporation of W6+ with stoichiometrical LiOH in the secondary crystallization calcination of 6 h renders uniformly distributed surface layer without hampering the growth of single-crystal. With the Al3+ doped bulk lattice, W6+ doped subsurface region and hetero-epitaxially grown Li2WO4, the cathode infused by two-step calcination exhibits high discharge capacity, rate performance, and cycling stability. Specifically, the modified LiNi0.84Co0.11Mn0.05O2 exhibits exceptional capacity retention, maintaining 88.98% of its initial capacity after 200 cycles at a rate of 1 C within a voltage window of 2.7–4.3 V at a temperature of 25 °C in half-cell. This performance is markedly superior to the capacity retention of 72.96% observed for pristine cathode. Even when subjected to a stringent test after 200 cycles at the same rate, the modified cathode sustains an impressive capacity retention of 82.41% at an elevated cut-off voltage of 4.5 V and a temperature of 30 °C.
{"title":"High-performance single crystal Ni-rich cathode with regulated lattice and interface constructed by separated lithiation and crystallization calcination","authors":"Siqi Chen , Xin Zhou , Shuo Wang , Ping Zhang , Wenbin Wu , Xiaohong Liu , Guilin Feng , Bin Zhang , Wangyan Xing , Meihua Zuo , Ping Zhang , Wei Xiang","doi":"10.1016/j.gce.2024.09.004","DOIUrl":"10.1016/j.gce.2024.09.004","url":null,"abstract":"<div><div>Incorporating high valence dopants, such as W<sup>6+</sup> and Mo<sup>6+</sup> has been verified to be effective for tuning the microstructure and grain boundary of polycrystal Ni-rich cathode. However, the hindered consolidation of primary particles induced by dopants during lithiation calcination limits the utilization of those dopants to crystalize single-crystal Ni-rich cathodes with stabilized lattice and surface. Herein, high performance single crystal LiNi<sub>0.84</sub>Co<sub>0.11</sub>Mn<sub>0.05</sub>O<sub>2</sub> cathode with Al<sup>3+</sup> and W<sup>6+</sup> regulated lattice and boundary phase was construed based on commercial process with two-step calcination process containing separated lithiation and crystallization. The introduction of appropriate amount of Al<sup>3+</sup> in the first lithiation calcination of 6 h endows the bulk of crystalline with enhanced lattice stability, while the incorporation of W<sup>6+</sup> with stoichiometrical LiOH in the secondary crystallization calcination of 6 h renders uniformly distributed surface layer without hampering the growth of single-crystal. With the Al<sup>3+</sup> doped bulk lattice, W<sup>6+</sup> doped subsurface region and hetero-epitaxially grown Li<sub>2</sub>WO<sub>4</sub>, the cathode infused by two-step calcination exhibits high discharge capacity, rate performance, and cycling stability. Specifically, the modified LiNi<sub>0.84</sub>Co<sub>0.11</sub>Mn<sub>0.05</sub>O<sub>2</sub> exhibits exceptional capacity retention, maintaining 88.98% of its initial capacity after 200 cycles at a rate of 1 C within a voltage window of 2.7–4.3 V at a temperature of 25 °C in half-cell. This performance is markedly superior to the capacity retention of 72.96% observed for pristine cathode. Even when subjected to a stringent test after 200 cycles at the same rate, the modified cathode sustains an impressive capacity retention of 82.41% at an elevated cut-off voltage of 4.5 V and a temperature of 30 °C.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 1","pages":"Pages 51-60"},"PeriodicalIF":7.6,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145420212","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-01Epub Date: 2025-06-03DOI: 10.1016/j.gce.2025.05.010
Yunze Zhang , Jian Wang
The cathode-electrolyte interphase (CEI) plays a pivotal role in determining the energy density and cycling stability of lithium-ion batteries. However, its complex formation mechanisms, dynamic evolution, and interplay with battery components pose significant challenges for a fundamental understanding and targeted regulation. While prior research has focused on modifying bulk electrolyte solvation structures and applying inert cathode coatings, this perspective analyzes the mechanisms of CEI formation and stabilization, with particular emphasis on cathode pre-interphase engineering, near-surface electric double-layer modulation, and functional coating design. Future research prospects are outlined, highlighting the advanced in situ characterization techniques with high spatiotemporal resolution to probe transient interfacial processes, along with innovative strategies for constructing CEI architectures.
{"title":"Stabilizing the cathode-electrolyte interphase for superior Li-ion batteries","authors":"Yunze Zhang , Jian Wang","doi":"10.1016/j.gce.2025.05.010","DOIUrl":"10.1016/j.gce.2025.05.010","url":null,"abstract":"<div><div>The cathode-electrolyte interphase (CEI) plays a pivotal role in determining the energy density and cycling stability of lithium-ion batteries. However, its complex formation mechanisms, dynamic evolution, and interplay with battery components pose significant challenges for a fundamental understanding and targeted regulation. While prior research has focused on modifying bulk electrolyte solvation structures and applying inert cathode coatings, this perspective analyzes the mechanisms of CEI formation and stabilization, with particular emphasis on cathode pre-interphase engineering, near-surface electric double-layer modulation, and functional coating design. Future research prospects are outlined, highlighting the advanced <em>in situ</em> characterization techniques with high spatiotemporal resolution to probe transient interfacial processes, along with innovative strategies for constructing CEI architectures.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 4","pages":"Pages 447-455"},"PeriodicalIF":7.6,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144917210","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-01Epub Date: 2025-08-30DOI: 10.1016/S2666-9528(25)00064-0
{"title":"OFC: Outside Front Cover","authors":"","doi":"10.1016/S2666-9528(25)00064-0","DOIUrl":"10.1016/S2666-9528(25)00064-0","url":null,"abstract":"","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 4","pages":"Page OFC"},"PeriodicalIF":7.6,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144917741","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-01Epub Date: 2025-05-10DOI: 10.1016/j.gce.2025.04.005
Yongheng Ren , Xiaohua Liu , Genggeng Dai , Lu Zhang , Hongwei Chen , Pengcheng Yang , Ye Li , Xinyue Yu , Yang Chen , Xiufeng Shi , Peng Lin , Jiangfeng Yang , Jinping Li , Libo Li
Efficient trace radioactive krypton isotopes (85Kr) capture from air under humid conditions is a critical challenge for nuclear safety and environmental protection. Commercial zeolites suffer from low Kr/N2 selectivity due to cation-induced interactions that strengthen nitrogen (N2) adsorption, while their hydrophilicity triggers severe water competition. Herein, we proposed utilizing the smooth pore surface in pure-silica zeolites to weaken the N2 adsorption and mitigate water competition. The pure silica ZSM-11 exhibited significant Kr/N2 selectivity (4.8) and Kr uptake of 12.8 cm3/g at 298 K and 1 bar, superior to the commercial zeolites. Its intersecting ten-membered ring (10-MR) channels facilitated optimal Kr interactions and distribution, as corroborated by Grand Canonical Monte Carlo (GCMC) simulations, which revealed preferential multisite Kr···O interactions with significantly higher Kr densities than N2. Dynamic breakthrough experiments demonstrated that pure silica zeolites, particularly ZSM-11, achieved superior Kr capturing performance and cycling stability under humid conditions (relative humidity (RH) = 72.6%), realizing a leap from ppm levels to high purity (> 80%) Kr. This work demonstrated the rational design of pore surface and topologies in zeolite for inert gases capture provided an effective technological route for radioactive krypton isotopes separation under humid conditions.
{"title":"Smooth pore surface in zeolites for krypton capture under humid conditions","authors":"Yongheng Ren , Xiaohua Liu , Genggeng Dai , Lu Zhang , Hongwei Chen , Pengcheng Yang , Ye Li , Xinyue Yu , Yang Chen , Xiufeng Shi , Peng Lin , Jiangfeng Yang , Jinping Li , Libo Li","doi":"10.1016/j.gce.2025.04.005","DOIUrl":"10.1016/j.gce.2025.04.005","url":null,"abstract":"<div><div>Efficient trace radioactive krypton isotopes (<sup>85</sup>Kr) capture from air under humid conditions is a critical challenge for nuclear safety and environmental protection. Commercial zeolites suffer from low Kr/N<sub>2</sub> selectivity due to cation-induced interactions that strengthen nitrogen (N<sub>2</sub>) adsorption, while their hydrophilicity triggers severe water competition. Herein, we proposed utilizing the smooth pore surface in pure-silica zeolites to weaken the N<sub>2</sub> adsorption and mitigate water competition. The pure silica ZSM-11 exhibited significant Kr/N<sub>2</sub> selectivity (4.8) and Kr uptake of 12.8 cm<sup>3</sup>/g at 298 K and 1 bar, superior to the commercial zeolites. Its intersecting ten-membered ring (10-MR) channels facilitated optimal Kr interactions and distribution, as corroborated by Grand Canonical Monte Carlo (GCMC) simulations, which revealed preferential multisite Kr···O interactions with significantly higher Kr densities than N<sub>2</sub>. Dynamic breakthrough experiments demonstrated that pure silica zeolites, particularly ZSM-11, achieved superior Kr capturing performance and cycling stability under humid conditions (relative humidity (RH) = 72.6%), realizing a leap from ppm levels to high purity (> 80%) Kr. This work demonstrated the rational design of pore surface and topologies in zeolite for inert gases capture provided an effective technological route for radioactive krypton isotopes separation under humid conditions.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 4","pages":"Pages 431-438"},"PeriodicalIF":7.6,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144917208","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alcohol industry residues (AIRs) are protein-rich lignocellulosic biowastes from a major industry, having the dual traits of renewable biomass and organic waste. They mainly consist of Brewer's spent grains (BSG) and Baijiu distiller's grains (BDG), with annual production totaling tens of millions of tons. Recycling these residues effectively is crucial for the environment, society, and industry. Given their unique characteristic of concentrated carbon and nitrogen sources, valorizing AIRs into biocarbon products through thermochemistry is the most sustainable method for waste management, resource recycling, and green ecology. In this review, the preparation and properties of AIRs-derived biocarbon products are systematically discussed. Recent advancements in the green thermochemical valorization of AIRs into biocarbon products for various applications like thermal utilization, environmental remediation, and energy storage are comprehensively reviewed. It is suggested that hydrothermal carbonization, coupled with necessary chemical functionalization (e.g., using metal oxides and oxysalts), would be a preferable strategy for producing desired functionalized biocarbon for use as carbon adsorbents (for wastewater treatment) and carbon fertilizers (for soil conservation). The yield and quality of functionalized biocarbon can be ensured through the directional regulation of the migration of essential elements like carbon and nitrogen. The co-generation of nitrogen-doped biochar and nitrogen-enriched liquid fertilizer using innovative hydrothermal strategies is identified as a potential research avenue to achieve the full and cascading utilization of AIRs. This review aims to provide an overview and insights into thermochemically valorizing AIRs alongside other light industrial residues for relevant researchers.
{"title":"Thermochemical valorization of alcohol industry residues into biocarbon for energy and environmental applications: a review","authors":"Hao Zhan , Tianle Xu , Hao Jiang , Mingjie Chen , Zonghao Lai , Wenjian Zhao , Lijian Leng , Zhiyong Zeng , Xinming Wang","doi":"10.1016/j.gce.2024.11.001","DOIUrl":"10.1016/j.gce.2024.11.001","url":null,"abstract":"<div><div>Alcohol industry residues (AIRs) are protein-rich lignocellulosic biowastes from a major industry, having the dual traits of renewable biomass and organic waste. They mainly consist of Brewer's spent grains (BSG) and Baijiu distiller's grains (BDG), with annual production totaling tens of millions of tons. Recycling these residues effectively is crucial for the environment, society, and industry. Given their unique characteristic of concentrated carbon and nitrogen sources, valorizing AIRs into biocarbon products through thermochemistry is the most sustainable method for waste management, resource recycling, and green ecology. In this review, the preparation and properties of AIRs-derived biocarbon products are systematically discussed. Recent advancements in the green thermochemical valorization of AIRs into biocarbon products for various applications like thermal utilization, environmental remediation, and energy storage are comprehensively reviewed. It is suggested that hydrothermal carbonization, coupled with necessary chemical functionalization (<em>e.g.</em>, using metal oxides and oxysalts), would be a preferable strategy for producing desired functionalized biocarbon for use as carbon adsorbents (for wastewater treatment) and carbon fertilizers (for soil conservation). The yield and quality of functionalized biocarbon can be ensured through the directional regulation of the migration of essential elements like carbon and nitrogen. The co-generation of nitrogen-doped biochar and nitrogen-enriched liquid fertilizer using innovative hydrothermal strategies is identified as a potential research avenue to achieve the full and cascading utilization of AIRs. This review aims to provide an overview and insights into thermochemically valorizing AIRs alongside other light industrial residues for relevant researchers.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 4","pages":"Pages 456-472"},"PeriodicalIF":7.6,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144917211","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-01Epub Date: 2025-05-16DOI: 10.1016/j.gce.2025.05.002
Ariel Riofrio , Miguel A. Bañares , Zhenlei Zhang , Xiangping Zhang , King Lun Yeung
The increasing demand for sustainable energy has intensified interest in hydrogen production from renewable sources. Although catalytic steam reforming of methane and other feedstocks has been extensively investigated, research on utilizing fats, oils, and grease (FOG) remains limited and dispersed. This study offers a comprehensive analysis of steam reforming catalysts for FOG conversion, concentrating on nickel-based, noble metal, and metal oxide-supported catalysts initially developed for methane, waste cooking oil, and glycerol. Catalyst performance is assessed in terms of activity, stability, cost, and environmental impact, addressing sustainable catalyst design and recycling principles. FOG management strategies are also explored, with a particular emphasis on Hong Kong, where FOG interception is crucial due to infrastructure constraints. Unlike cities where food waste is ground and flushed through extensive sewer systems, Hong Kong necessitates localized FOG removal to prevent costly blockages and environmental harm. A techno-economic analysis demonstrated the feasibility of producing H2 at a selling price as low as USD 3/kg H2, with a carbon capture potential of 0.40 kg CO2-eq/kg H2. Life cycle assessment (LCA) further confirmed environmental benefits, indicating the potential to capture 0.14 kg CO2 per kg of FOG processed. Additionally, the study identifies opportunities for cost reduction through more efficient FOG acquisition and valorization, which can enhance carbon savings and economic viability. Overall, this work underscores the potential of FOG as a renewable feedstock and delineates key research directions for catalyst development and integrated waste-to-hydrogen systems.
{"title":"A perspective on transforming fats, oil, and grease (FOG) into hydrogen: insights on steam reforming catalysts and the case study of Hong Kong using techno-economic analysis and life cycle assessment","authors":"Ariel Riofrio , Miguel A. Bañares , Zhenlei Zhang , Xiangping Zhang , King Lun Yeung","doi":"10.1016/j.gce.2025.05.002","DOIUrl":"10.1016/j.gce.2025.05.002","url":null,"abstract":"<div><div>The increasing demand for sustainable energy has intensified interest in hydrogen production from renewable sources. Although catalytic steam reforming of methane and other feedstocks has been extensively investigated, research on utilizing fats, oils, and grease (FOG) remains limited and dispersed. This study offers a comprehensive analysis of steam reforming catalysts for FOG conversion, concentrating on nickel-based, noble metal, and metal oxide-supported catalysts initially developed for methane, waste cooking oil, and glycerol. Catalyst performance is assessed in terms of activity, stability, cost, and environmental impact, addressing sustainable catalyst design and recycling principles. FOG management strategies are also explored, with a particular emphasis on Hong Kong, where FOG interception is crucial due to infrastructure constraints. Unlike cities where food waste is ground and flushed through extensive sewer systems, Hong Kong necessitates localized FOG removal to prevent costly blockages and environmental harm. A techno-economic analysis demonstrated the feasibility of producing H<sub>2</sub> at a selling price as low as USD 3/kg H<sub>2</sub>, with a carbon capture potential of 0.40 kg CO<sub>2</sub>-eq/kg H<sub>2</sub>. Life cycle assessment (LCA) further confirmed environmental benefits, indicating the potential to capture 0.14 kg CO<sub>2</sub> per kg of FOG processed. Additionally, the study identifies opportunities for cost reduction through more efficient FOG acquisition and valorization, which can enhance carbon savings and economic viability. Overall, this work underscores the potential of FOG as a renewable feedstock and delineates key research directions for catalyst development and integrated waste-to-hydrogen systems.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 4","pages":"Pages 473-493"},"PeriodicalIF":7.6,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144917212","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}