Green ChemistryPub Date : 2026-06-29Epub Date: 2026-02-24DOI: 10.1039/d6gc00784h
Lori Gonnet , Cameron B. Lennox , Tristan H. Borchers , Mohammad S. Askari , Alexander Wahrhaftig-Lewis , Stefan G. Koenig , Karthik Nagapudi , Tomislav Friščić
{"title":"Establishing parameters for resonant acoustic mixing (RAM) chemistry using Buchwald–Hartwig amination as a model","authors":"Lori Gonnet , Cameron B. Lennox , Tristan H. Borchers , Mohammad S. Askari , Alexander Wahrhaftig-Lewis , Stefan G. Koenig , Karthik Nagapudi , Tomislav Friščić","doi":"10.1039/d6gc00784h","DOIUrl":"10.1039/d6gc00784h","url":null,"abstract":"<div><div>While Resonant Acoustic Mixing (RAM) has been proposed as a scalable methodology for environmentally-friendly synthesis, notably media-free mechanochemical synthesis, the underlying reaction environment and the parameters that govern reaction control, optimization, and scale-up remain poorly understood. Using the Buchwald–Hartwig amination as a model system, this study provides insight into the RAM reaction environment and establishes design parameters through a combination of systematic screening and multimodal, real-time <em>in situ</em> monitoring of reaction progress, temperature evolution, and the transformations of crystalline and non-crystalline bulk phases. The simultaneous application of benchtop infrared thermography, and fingerprint- and terahertz-region Raman (THz-Raman) spectroscopy enables the direct correlation of reactivity, thermal behaviour, and phase evolution. Specifically, this work identifies the filling ratio (<em>φ</em>), acceleration, and the amount of liquid additive (<em>η</em>) as critical parameters to design tunable and scalable (at least 100 mmol) reactivity under RAM conditions, in short timeframes. Real-time monitoring reveals that rapid Buchwald–Hartwig reactivity is associated with autogenous heating, and that <em>φ</em> and acceleration serve as parameters that can be used to control reaction kinetics and temperature evolution. By identifying experimentally accessible reaction control parameters and presenting a benchtop-only design for the simultaneous monitoring of temperature, reaction progress and evolution of transient bulk phases, this work provides a foundation for the rational design, control, and safety of chemistry under RAM conditions.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10434-10446"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336674","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}
Green ChemistryPub Date : 2026-06-29Epub Date: 2026-06-09DOI: 10.1039/d6gc02757a
Nina Klos , Christopher Weike , Philipp Demling , Andreas Sebastian Klein , Giancarlo Franciò , Lars M. Blank , Walter Leitner , Dörte Rother
{"title":"Concatenating microorganisms, chemical catalysts, and enzymes for the synthesis of ethyl formate from renewables","authors":"Nina Klos , Christopher Weike , Philipp Demling , Andreas Sebastian Klein , Giancarlo Franciò , Lars M. Blank , Walter Leitner , Dörte Rother","doi":"10.1039/d6gc02757a","DOIUrl":"10.1039/d6gc02757a","url":null,"abstract":"<div><div>Alternative chemical synthesis routes and the (re)utilization of CO<sub>2</sub> are crucial for the development of a circular bioeconomy. To establish sustainable production methods, concatenating various catalysts allows for leveraging the unique advantages of each catalyst type. During process development, however, the reaction conditions must be harmonized, the catalyst compatibility must be examined, bottlenecks must be identified, and thus the operating window for the best process mode must be found. Here, we present ethyl formate synthesis from glucose, which is achieved by concatenating three catalysts: the yeast <em>Saccharomyces cerevisiae</em>, a ruthenium catalyst, and a lipase in an immobilized enzyme formulation. This study identifies the parameters that require investigation when combining different catalyst types and integrating CO<sub>2</sub> as an alternative raw material. Parameters such as product stability across different reaction systems, product distribution in a two-phase system using different organic solvents, and catalyst compatibility were studied. <em>Candida antarctica</em> lipase B was identified as a suitable biocatalyst for the enzymatic esterification of formic acid and ethanol. The catalyst compatibility is shown. However, the aqueous phase, necessary for yeasts, conflicts with product stability and catalyst activity. The desired one-pot, one-step process could not be realized. As a consequence, the process can only be efficiently performed in two steps, because in a one-pot, one-step reaction, the product yield was low. The concept of a concatenated ruthenium-catalyzed hydrogenation and lipase reaction can also be adapted to other formate esters starting from CO<sub>2</sub>.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10570-10579"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336705","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}
Green ChemistryPub Date : 2026-06-29Epub Date: 2026-06-05DOI: 10.1039/d6gc01294a
Jingnan Wang , Wenqi Ma , Yuxuan Xin , Jiayi Cui , Feng Guo , Yujia Jiang , Wankui Jiang , Fengxue Xin , Wenming Zhang , Min Jiang
{"title":"Multidimensional engineering of Komagataella phaffii for efficient synthesis of retinal","authors":"Jingnan Wang , Wenqi Ma , Yuxuan Xin , Jiayi Cui , Feng Guo , Yujia Jiang , Wankui Jiang , Fengxue Xin , Wenming Zhang , Min Jiang","doi":"10.1039/d6gc01294a","DOIUrl":"10.1039/d6gc01294a","url":null,"abstract":"<div><div>Retinal is a fundamental molecule in the visual system and a critical regulator of skin health and cellular physiology. The sustainable production of retinal <em>via</em> engineered microbial cell factories offers a promising alternative to chemical synthesis. In this study, we established the biosynthetic pathway in <em>Komagataella phaffii</em>, providing the first experimental demonstration of the membrane-associated nature of β-carotene 15,15′-mono(di)oxygenase (BCMO). To maximize productivity, we implemented a multi-layered engineering strategy, including the amplification of key gene dosages, the balancing of NADPH cofactor supply, and the augmentation of precursor availability. Leveraging the unique sub-cellular architecture of <em>K. phaffii</em>, an anchoring motif from the peroxin PEX15 was used to achieve peroxisome surface display of BCMO. This spatial scaffolding effectively achieved <em>in vivo</em> enzyme immobilization, significantly enhancing catalytic activity. To harmonize cellular fitness with the oxygen-dependent requirements of BCMO, heterologous expression of <em>Vitreoscilla</em> hemoglobin (VHb) led to a 58.13% increase in biomass and a 17.32% improvement in retinal titer. In addition, we identified the Pdr5 transporter as a key mediator for retinal efflux, thereby alleviating intracellular cytotoxicity. The integration of surfactants facilitated the recovery of over 90% of intracellular retinal into the extracellular space, substantially reducing downstream processing complexity. Finally, utilizing glucose and methanol as carbon sources, the engineered strain achieved retinal titers of 764.22 mg L<sup>−1</sup> and 1406.69 mg L<sup>−1</sup> in a 5 L bioreactor, respectively. The methanol-derived titer represents the highest reported to date, underscoring the potential of <em>K. phaffii</em> as a versatile one-carbon biomanufacturing platform for industrial terpenoid biosynthesis.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10580-10595"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336706","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}
Green ChemistryPub Date : 2026-06-29Epub Date: 2026-06-12DOI: 10.1039/d6gc02132h
Shaoyan Huang , Shuling Liu , Sha Fan , Rui Su , Deliang Tian , Zili Deng , Jinbao Li , Jianbo Tong
{"title":"Dual-functional SnS2–CuS heterostructure for zinc anode protection and conversion-type anode toward advanced aqueous zinc-ion batteries","authors":"Shaoyan Huang , Shuling Liu , Sha Fan , Rui Su , Deliang Tian , Zili Deng , Jinbao Li , Jianbo Tong","doi":"10.1039/d6gc02132h","DOIUrl":"10.1039/d6gc02132h","url":null,"abstract":"<div><div>Aqueous zinc-ion batteries (AZIBs) face critical challenges including poor cycling stability, zinc dendrite growth, and low zinc utilization. To address these issues, a multifunctional SnS<sub>2</sub>–CuS heterostructure is proposed, serving both as a zinc anode protective layer in conventional AZIBs and a metal-free anode in rocking-chair zinc-ion batteries (RCZIBs). In AZIBs, the SnS<sub>2</sub>–CuS heterostructure generates a synergistic effect between different phases. This effect improves interfacial charge transfer efficiency, guides the oriented deposition of Zn<sup>2+</sup> along the (001) crystal plane of SnS<sub>2</sub>, and optimizes Zn<sup>2+</sup> migration kinetics. When deployed as the anode for RCZIBs, the elaborate heterostructure construction efficiently alleviates the severe volume expansion of CuS during repeated charge–discharge cycling, while interfacial charge polarization derived from heterogeneous coupling further accelerates the electrochemical reaction kinetics. To clarify the electrochemical mechanism, <em>in situ</em> XRD, <em>in situ</em> EIS, DRT analysis, and <em>ex situ</em> XPS are used to track phase transitions and interfacial dynamic processes. Density functional theory calculations also theoretically verify that the SnS<sub>2</sub>–CuS heterostructure significantly enhances Zn<sup>2+</sup> storage capability. Electrochemical tests show that the assembled RCZIB delivers a discharge specific capacity of 179.03 mAh g<sup>−1</sup> at 0.2 A g<sup>−1</sup>, retaining 114.51 mAh g<sup>−1</sup> after 200 cycles. Moreover, it maintains 83.6% of its initial capacity after 1000 cycles at 1 A g<sup>−1</sup>, demonstrating outstanding cycling stability. This study achieves the compatible application of the SnS<sub>2</sub>–CuS heterostructure in both AZIBs and RCZIBs and highlights its considerable potential for next-generation high-performance energy storage systems.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10616-10630"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336648","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}
Green ChemistryPub Date : 2026-06-29Epub Date: 2026-06-09DOI: 10.1039/d6gc01624c
Yangyang Jiang , Yuxin Liu , Yuanli Qi , Yurou Shao , Dong Wang , Benshuai Guo , Jingyan Zhao , Zhibin Zhou , Yuntao Lei , Lili Jin
{"title":"Novel benzenesulfonamide-based ionic liquids for energy-efficient CO2 capture and conversion","authors":"Yangyang Jiang , Yuxin Liu , Yuanli Qi , Yurou Shao , Dong Wang , Benshuai Guo , Jingyan Zhao , Zhibin Zhou , Yuntao Lei , Lili Jin","doi":"10.1039/d6gc01624c","DOIUrl":"10.1039/d6gc01624c","url":null,"abstract":"<div><div>The capture and utilization of carbon dioxide (CO<sub>2</sub>) from the post-combustion of fossil fuels has been identified as a highly effective strategy for reducing carbon emissions. Herein, a series of novel substituted benzenesulfonamide ionic liquids (BSA-ILs) were designed and synthesized <em>via</em> facile acid–base neutralization reactions for the purpose of achieving reversible CO<sub>2</sub> capture and catalyzing CO<sub>2</sub> chemical fixation. Addressing the inherently high viscosity of neat BSA-ILs (551.2–7785.7 mPa s), propylene carbonate (PC), a green product derived from CO<sub>2</sub> chemical fixation, was selected as a diluent to form BSA-IL mixed absorbents (BSA-IL-MAs). The optimized system exhibited a high CO<sub>2</sub> uptake capacity of 1.38 mol of CO<sub>2</sub> per mol BSA-IL, an excellent CO<sub>2</sub>/N<sub>2</sub> selectivity of 18.36, and a remarkable 99.0% conversion of epichlorohydrin under mild, solvent-free, metal-free, halogen-free, co-catalyst-free and atmospheric pressure conditions. Meanwhile, the findings demonstrated a certain positive correlation between the CO<sub>2</sub> uptake capacity/conversion and the p<em>K</em><sub>a</sub> of the substituted BSA. Notably, the BSA-IL system retained nearly intact CO<sub>2</sub> capture performance and catalytic activity after five consecutive absorption–desorption and catalytic cycles, with an extremely low <em>E</em>-factor of 0.11. Spectroscopic characterization confirmed the formation of a new carbonyl moiety peak in CO<sub>2</sub>-saturated BSA-ILs, indicating that chemisorption dominated the CO<sub>2</sub> uptake process. NMR investigations and DFT calculations further elucidated the interactions between BSA-ILs, CO<sub>2</sub> and epoxide substrates, validating the feasibility of the proposed reaction pathways. This work provides a sustainable, efficient and industrially feasible integrated platform for CO<sub>2</sub> capture and utilization, offering a paradigm for low-carbon catalytic conversion systems.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10496-10509"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336691","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}
Green ChemistryPub Date : 2026-06-29Epub Date: 2026-06-04DOI: 10.1039/d6gc02039a
Weizhi Huang , Xiaoqi Ding , Sha Ao , Huaqiang Cao , Jia Hu , Xiaoqing Han , Shilin Liu
{"title":"Integrating compartmentalized catalysis with low-energy recovery via a magneto-responsive water-in-water Pickering emulsion platform for sustainable biomanufacturing of 4-methyl-5-thiazoleethanol","authors":"Weizhi Huang , Xiaoqi Ding , Sha Ao , Huaqiang Cao , Jia Hu , Xiaoqing Han , Shilin Liu","doi":"10.1039/d6gc02039a","DOIUrl":"10.1039/d6gc02039a","url":null,"abstract":"<div><div>Simultaneously achieving compartmentalized catalysis and low-energy recovery remains a significant challenge in conventional liquid fermentation. To address this issue, citrate-functionalized Fe<sub>3</sub>O<sub>4</sub> nanoparticles were utilized to construct a water/water (W/W) Pickering emulsion system. A recombinant <em>Bacillus amyloliquefaciens</em> strain was engineered for 4-methyl-5-thiazoleethanol (MTE) biosynthesis through competing pathway knockout (<em>ΔylmB</em>) and site-directed mutagenesis of TenA (Y113A/F169A). In liquid fermentation, the engineered strain (<em>ΔylmB</em>/pHY-BaTenA<sup>Y113A/F169A</sup>) achieved a 6.80-fold increase in MTE production (from 273.67 mg·L<sup>−1</sup> to 1862.05 mg·L<sup>−1</sup>). When cultivated in the magneto-responsive W/W Pickering emulsion under optimized conditions, the MTE yield was increased to 3061.14 mg·L<sup>−1</sup>, representing a 20.47% improvement over the Fe<sub>3</sub>O<sub>4</sub> nanoparticle-free control. This enhancement was attributed to the stable compartmentalized micro-environment of the aqueous two-phase system, which promoted bacterial proliferation and sustained catalytic activity. Notably, the interfacial Fe<sub>3</sub>O<sub>4</sub> nanoparticles enabled gentle magnetic separation, achieving supernatant clarification (OD<sub>600</sub> = 0.27 ± 0.04) comparable to that of high-speed centrifugation (0.20 ± 0.02). Magnetically harvested bacteria readily resumed normal growth in fresh media, and the nanoparticles could be reused for two cycles, retaining 47.80% of their saturation magnetization and supporting a sustained MTE yield of 2968.88 mg·L<sup>−1</sup>. A magneto-responsive aqueous two-phase system was developed to couple compartmentalized biosynthesis with low-energy bacterial recovery. This integrated platform would provide a circular and sustainable strategy for biomanufacturing high-value compounds.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10510-10522"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336692","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}
Green ChemistryPub Date : 2026-06-29Epub Date: 2026-06-04DOI: 10.1039/d6gc02196d
Huilin Li , Xuechong Ding , Teng Zhou
{"title":"Greening water-lean solvents for CO2 capture: replacing toxic 1-methyl-2-pyrrolidone with high-performance eco-friendly cosolvents","authors":"Huilin Li , Xuechong Ding , Teng Zhou","doi":"10.1039/d6gc02196d","DOIUrl":"10.1039/d6gc02196d","url":null,"abstract":"<div><div>Water-lean solvents are promising alternatives to aqueous amines for post-combustion CO<sub>2</sub> capture due to their lower regeneration energy. However, the majority of state-of-the-art water-lean solvents rely on 1-methyl-2-pyrrolidone (NMP) as the organic cosolvent, whose reproductive toxicity poses a serious barrier to large-scale deployment. This study proposes a systematic strategy to identify green, low-toxicity replacements for NMP in water-lean solvents. Based on COSMO-RS σ-profile similarity calculation, 20 high-potential candidates were first identified from 2562 organic solvents. Subsequent environmental, health, and safety (EHS) evaluations, combined with physicochemical property filtering, narrowed the selection to two green cosolvents: methylaminoacetaldehyde dimethyl acetal (MAADMA) and 3-methoxy-1-butanol (MOB). These two candidates and NMP were then experimentally validated in combination with three representative amines (EMEA, DMEDA, and DMPDA) at 5 wt% water content. Among all tested systems, the EM-A-5H solvent (30% EMEA/65% MAADMA/5% H<sub>2</sub>O) showed the best performance, with a remarkable cyclic capacity of 0.86 mol CO<sub>2</sub> per mol amine and a regeneration efficiency of 93.6%. Importantly, EM-A-5H achieved a total regeneration energy of 2.20 GJ per t CO<sub>2</sub>, 41% lower than conventional 30 wt% MEA and 15% lower than the NMP-based counterpart solvent. It also exhibited an excellent stability and satisfactory viscosity over seven absorption–desorption cycles without performance degradation. This work offers a systematic and practical approach for the rational design of eco-friendly, high-performance water-lean solvents for CO<sub>2</sub> capture.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10537-10547"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336694","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}
Green ChemistryPub Date : 2026-06-29Epub Date: 2026-06-09DOI: 10.1039/d6gc00989a
Sungkwon Yoon , Charlie Bateman , James J. C. Busfield , Peter J. Martin , Biqiong Chen
{"title":"A green versatile platform for synthesising renewable ether-based thermoplastic elastomers","authors":"Sungkwon Yoon , Charlie Bateman , James J. C. Busfield , Peter J. Martin , Biqiong Chen","doi":"10.1039/d6gc00989a","DOIUrl":"10.1039/d6gc00989a","url":null,"abstract":"<div><div>Ether-based polymers are commonly used in diverse applications. However, it is challenging to synthesise polyethers with more than five methylene groups in their repeating units from cyclic ethers, which limits the molecular design of ether-based polymers. Creating a new synthesis pathway to enabling green chemistry and flexible design of their molecular structures is, therefore, highly desired. Here, a green versatile platform is presented for synthesising renewable ether-based thermoplastic elastomers (TPEs) with broad and tuneable properties. An organic acid catalyst is used to synthesise a long-chain polyether diol from a fatty acid diol <em>via</em> a S<sub>N</sub>2 reaction. This biobased, renewable polyether diol then serves as a universal platform for the synthesis of a wide spectrum of TPEs including thermoplastic polyurethanes, poly(urethane urea)s and poly(ether ester) elastomers, with controllable mechanical properties, excellent transparency and chemical resistance. The structure–property relationships, processability, and sustainability of these TPEs are also reported. The synthesis of these biobased TPEs can be readily scaled up, and different types of products are manufactured from the elastomers. This work provides a viable synthesis strategy to overcoming the limitations of the molecular design facing existing ether-based polymers, while enabling the sustainable manufacture of renewable ether-based TPE materials and products.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10699-10711"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336716","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}
Green ChemistryPub Date : 2026-06-29Epub Date: 2026-06-12DOI: 10.1039/d6gc02278b
Jiajia Li , Yulu Liu , Manhua Chen , Keke Cao , Rongqiang Zhang , Nan Zhang , Zhi Li , Qi Qiang , Yuping Tang , Qizhao Wang
{"title":"An AE/Fe-MOF/PVDF heterojunction self-cleaning photocatalytic membrane for rapid electron transfer to enhance photo-Fenton degradation of tannic acid","authors":"Jiajia Li , Yulu Liu , Manhua Chen , Keke Cao , Rongqiang Zhang , Nan Zhang , Zhi Li , Qi Qiang , Yuping Tang , Qizhao Wang","doi":"10.1039/d6gc02278b","DOIUrl":"10.1039/d6gc02278b","url":null,"abstract":"<div><div>As the traditional Chinese medicine (TCM) industry develops at a fast pace, its wastewater discharge has become an increasingly severe environmental problem. Membrane technology has been applied in the treatment of TCM wastewater; however, the high concentration of macromolecular organics, such as tannic acid, pectin, and protein, readily triggers severe pore blockage and fouling of polyvinylidene fluoride (PVDF) separation membranes. To address these challenges, this study innovatively integrates the natural photosensitizer aloe-emodin (AE) with an Fe-MOF to construct an AE/Fe-MOF type-I heterojunction photocatalyst directly immobilized onto a PVDF membrane substrate. Under visible-light irradiation with H<sub>2</sub>O<sub>2</sub>, the fabricated AE/Fe-MOF/PVDF membrane achieves 87.29% degradation efficiency toward tannic acid (TA) within 90 minutes. It also exhibits excellent removal performance for simulated TCM wastewater derived from <em>Rheum officinale</em> Baill. and <em>Polygonum cuspidatum</em> Sieb. et Zucc., achieving chemical oxygen demand (COD) removal rates of 74.44% and 96.61%, respectively. Furthermore, the AE/Fe-MOF/PVDF membrane demonstrates remarkable self-cleaning capability, achieving a flux recovery ratio (FRR) of up to 96.5% following <em>in situ</em> photo-Fenton degradation, which is far superior to conventional hydraulic cleaning (65.7%). Stable filtration performance is maintained across multiple filtration–cleaning cycles. Mechanistic investigations reveal that the AE/Fe-MOF type-I heterojunction enhances the spatial separation of photoinduced carriers and accelerates the Fe<sup>3+</sup>/Fe<sup>2+</sup> redox cycle, thereby synergistically driving a sustained and efficient photo-Fenton process that enables simultaneous pollutant degradation and <em>in situ</em> membrane fouling mitigation. This work not only provides a novel heterojunction-based self-cleaning photocatalytic membrane for the efficient treatment of TCM wastewater but also deepens the understanding of the synergistic mechanism between charge transfer and the iron cycle in natural photosensitizer and MOF hybrid systems.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10642-10657"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336650","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}
Green ChemistryPub Date : 2026-06-29Epub Date: 2026-05-12DOI: 10.1039/d6gc01231k
Assya Bellaadem , Roland Kalb , Blaž Likozar , Filipa A. Vicente
{"title":"Towards safe and sustainable ionic liquids: a critical outlook on industrial and pharmaceutical integration","authors":"Assya Bellaadem , Roland Kalb , Blaž Likozar , Filipa A. Vicente","doi":"10.1039/d6gc01231k","DOIUrl":"10.1039/d6gc01231k","url":null,"abstract":"<div><div>Ionic liquids (ILs) have emerged over the past three decades as highly versatile and tunable solvents whose physicochemical properties can be precisely adjusted by selecting appropriate combinations of cations and anions. In pharmaceuticals, ILs serve as solvents, excipients, and active pharmaceutical ingredients (API-ILs), addressing challenges such as poor solubility, limited bioavailability, and polymorphism. Despite rapid scientific progress, the transition of ILs from laboratory research to industrial application remains slow. Significant knowledge gaps persist in toxicity, biocompatibility, biodegradability, scalability, and long-term safety, while life-cycle assessment (LCA), techno-economic analysis (TEA), and social LCA remain limited. These gaps are further exacerbated by the structural diversity of ILs, which hinders standardised testing and predictive modelling. Addressing these challenges requires early integration of Safe and Sustainable by Design (SSbD) principles, improved computational and screening tools, and the development of protocols tailored to IL diversity. Incorporating green chemistry and circular economy approaches can streamline the identification of safer and more sustainable ILs while reducing experimental and economic burdens. This review therefore brings together environmental, economic, social, and industrial considerations, including LCA, TEA, toxicity, scalability, and current pharmaceutical applications, to provide a unified perspective on the opportunities and barriers associated with IL development. By consolidating these aspects, it aims to guide more responsible, efficient, and sustainable implementation of ILs, with relevance to API-ILs and their potential future in the pharmaceutical industry.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 25","pages":"Pages 10350-10382"},"PeriodicalIF":10.6,"publicationDate":"2026-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336664","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}