Emerging per- and polyfluoroalkyl substances (PFAS) are highly toxic chemicals with extraodinary stability in the aquatic environment. Highly efficient adsorbents are in urgent need to address the environmental challenges caused by PFAS. Herein, we developed a novel aminated foam adsorbent with high affinity for PFAS adsorption through polymerization, amination and pyrolyzation. For initial 1 μg/L perfluorooctanoic acid (PFOA) solution, more than 97.9 % removal efficiency could be obatined with a rapid equilibration time of ∼ 15 min. The elevated adsorption efficiency could be explained by the synergetic effect of electrostatic/hydrogen bonding and hydrophobic interaction, while the increase of specific surface area (SSA) also has a positive effect on PFOA adsorption. Furthermore, the sythesized polyacrylamide-polyaniline material (pyrolyzed at 301℃, PAM-PANI-2) exhibited high adaptability to different environmental influencing factors, including pH and co-existed organic matters, and presented excellent adsorption removal ability for other common PFAS except for PFOA. Moreover, it is worth noting that this foam material has advantages in regeneration compared to traditional powder adsorbents, without complicated procedures such as centrifugation and filtration. These results indicate that aminated PAM polymers are promising adsorbents in remediations of trace PFAS-contaminated water, which can give new insights to the design and application of novel polymer materials of PFAS treatments.
{"title":"Efficient separation of per- and polyfluoroalkyl substances (PFAS) from water by aminated polyacrylamide hydrogel foam","authors":"Yichen Xu, Xueru Yu, Xinhao Wang, Yiqian Song, Wenran Wang, Ming Zhang, Deyang Kong, Zhanghao Chen, Cheng Gu","doi":"10.1016/j.cej.2024.157833","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157833","url":null,"abstract":"Emerging per- and polyfluoroalkyl substances (PFAS) are highly toxic chemicals with extraodinary stability in the aquatic environment. Highly efficient adsorbents are in urgent need to address the environmental challenges caused by PFAS. Herein, we developed a novel aminated foam adsorbent with high affinity for PFAS adsorption through polymerization, amination and pyrolyzation. For initial 1 μg/L perfluorooctanoic acid (PFOA) solution, more than 97.9 % removal efficiency could be obatined with a rapid equilibration time of ∼ 15 min. The elevated adsorption efficiency could be explained by the synergetic effect of electrostatic/hydrogen bonding and hydrophobic interaction, while the increase of specific surface area (SSA) also has a positive effect on PFOA adsorption. Furthermore, the sythesized polyacrylamide-polyaniline material (pyrolyzed at 301℃, PAM-PANI-2) exhibited high adaptability to different environmental influencing factors, including pH and co-existed organic matters, and presented excellent adsorption removal ability for other common PFAS except for PFOA. Moreover, it is worth noting that this foam material has advantages in regeneration compared to traditional powder adsorbents, without complicated procedures such as centrifugation and filtration. These results indicate that aminated PAM polymers are promising adsorbents in remediations of trace PFAS-contaminated water, which can give new insights to the design and application of novel polymer materials of PFAS treatments.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"15 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673740","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-20DOI: 10.1016/j.cej.2024.157853
Yuanyi Shao, Bingnan Mu, Lan Xu, Yiqi Yang
For the first time, artificial fibers from proteins, mainly kafirin and glutelin, from sorghum distillers grains (SDG) have been developed. SDG is difficult to digest due to dense cystine crosslinkages, therefore, is a poor animal feed with much lower value than corn distillers grains. However, dense cystine crosslinkages are an advantage for fiber properties, such as mechanical properties and wet stability. Also, fibers are much more expensive than feed, hence, can add higher values to sorghum industry. Previously, only kafirin was extracted from SDG using traditional solvents for plant proteins, such as alcohol/water, acetic acid, and formic acid. However, these solvents provided kafirin with poor or no spinnability. Glutelin, another major protein in SDG, about 35% of total, had not been used for industrial applications. We developed a green and sustainable water-based system that dissolved sorghum proteins including both kafirin and glutelin and achieved desirable fiber spinnability. We also developed the green aqueous coagulation and oxidation systems to effectively solidify protein fibers after wet spinning from our aqueous spinning solution and recovered cystine crosslinkages between sorghum protein molecules. The artificial sorghum protein fibers from our total aqueous and green spinning system have mechanical properties better than soy protein fibers and regenerated feather keratin fibers. We also used the sustainable sucrose-derived aldehydes to chemically crosslink sorghum proteins. With only 2% of the crosslinker based on weight of fibers, our artificial sorghum protein fibers have mechanical properties better than that of wool.
{"title":"A green and sustainable technology for the development of artificial protein fibers from sorghum distillers grains for industrialization","authors":"Yuanyi Shao, Bingnan Mu, Lan Xu, Yiqi Yang","doi":"10.1016/j.cej.2024.157853","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157853","url":null,"abstract":"For the first time, artificial fibers from proteins, mainly kafirin and glutelin, from sorghum distillers grains (SDG) have been developed. SDG is difficult to digest due to dense cystine crosslinkages, therefore, is a poor animal feed with much lower value than corn distillers grains. However, dense cystine crosslinkages are an advantage for fiber properties, such as mechanical properties and wet stability. Also, fibers are much more expensive than feed, hence, can add higher values to sorghum industry. Previously, only kafirin was extracted from SDG using traditional solvents for plant proteins, such as alcohol/water, acetic acid, and formic acid. However, these solvents provided kafirin with poor or no spinnability. Glutelin, another major protein in SDG, about 35% of total, had not been used for industrial applications. We developed a green and sustainable water-based system that dissolved sorghum proteins including both kafirin and glutelin and achieved desirable fiber spinnability. We also developed the green aqueous coagulation and oxidation systems to effectively solidify protein fibers after wet spinning from our aqueous spinning solution and recovered cystine crosslinkages between sorghum protein molecules. The artificial sorghum protein fibers from our total aqueous and green spinning system have mechanical properties better than soy protein fibers and regenerated feather keratin fibers. We also used the sustainable sucrose-derived aldehydes to chemically crosslink sorghum proteins. With only 2% of the crosslinker based on weight of fibers, our artificial sorghum protein fibers have mechanical properties better than that of wool.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"74 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679086","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-20DOI: 10.1016/j.cej.2024.157838
Ke Kong, Jun Liang, Fangling Cui, Ying Zhang, Daqiang Yuan, Ruihu Wang
The development of porous adsorbents for removal of concomitant perfluorooctane sulfonate (PFOS) and dichromate pollutants is pivotal and challenging in wastewater remediation. Herein, we presented a leaf-inspired artificial cleaning system based on an ionic polymer (ImIP-6) with high local density of imidazolium moieties and charge-balanced chloride for efficiently simultaneous removal of PFOS and dichromate. ImIP-6 exhibits fast kinetics and ultrahigh uptake capacities with maximum adsorption values of 2606 mg g−1 for PFOS and 247 mg g−1 for Cr(VI), which are far superior to many porous sorbents. The mechanism studies have evidenced that ImIP-6 possesses two types of domains for PFOS and dichromate adsorption, in which the imidazolium-based cationic surface induces PFOS enrichment and subsequent formation of micelles on the outer surfaces without significantly interfering the adsorption of dichromate in the interior pores. This work provides one new approach based on biomimetic systems with hierarchical adsorption domains for wastewater remediation.
{"title":"Novel hierarchical ionic polymers for removal of perfluorooctane sulfonate and dichromate","authors":"Ke Kong, Jun Liang, Fangling Cui, Ying Zhang, Daqiang Yuan, Ruihu Wang","doi":"10.1016/j.cej.2024.157838","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157838","url":null,"abstract":"The development of porous adsorbents for removal of concomitant perfluorooctane sulfonate (PFOS) and dichromate pollutants is pivotal and challenging in wastewater remediation. Herein, we presented a leaf-inspired artificial cleaning system based on an ionic polymer (ImIP-6) with high local density of imidazolium moieties and charge-balanced chloride for efficiently simultaneous removal of PFOS and dichromate. ImIP-6 exhibits fast kinetics and ultrahigh uptake capacities with maximum adsorption values of 2606 mg g<sup>−1</sup> for PFOS and 247 mg g<sup>−1</sup> for Cr(VI), which are far superior to many porous sorbents. The mechanism studies have evidenced that ImIP-6 possesses two types of domains for PFOS and dichromate adsorption, in which the imidazolium-based cationic surface induces PFOS enrichment and subsequent formation of micelles on the outer surfaces without significantly interfering the adsorption of dichromate in the interior pores. This work provides one new approach based on biomimetic systems with hierarchical adsorption domains for wastewater remediation.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"11 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-19DOI: 10.1016/j.cej.2024.157762
Yipengchen Yin, Li Zhu, Tiaoyan Jiang, Rong Chai, Ya Zhang, Tianyu Li, Kai Wang, Sheng Wang, Qin Zhang
Radiotherapy (RT) is a critical clinical treatment for cancer. However, radioresistance often hampers its effectiveness, leading to local recurrence and therapeutic failure. Ferroptosis has been regarded as a natural barrier to tumor progression and plays a significant role in RT-mediated anticancer effects. Therefore, the simultaneous activation of ferroptosis and RT is of great significance for cancer therapy. Herein, we engineered the tumor-releasing nanozymes (BMBs), combining manganese oxide as the ferroptosis inducer and two-dimensional bismuthene with high-Z effect for augmented ferroptotic RT in a triple-enzyme-like radiosensitization manner. The nanozymes BMBs depleted glutathione (GSH) and nicotinamide adenine dinucleotide phosphate (NADPH) in the tumor microenvironment to exhibit glutathione peroxidase (GPX)-like activity and NADPH dehydrogenase (NDH)-like activity, accompanied by aberrant reactive oxygen species (ROS) production exhibiting peoxidase (POD)-like activity. In addition, the nanozymes BMBs simultaneously inactivate ferroptosis defensive system: glutathione peroxidase 4 (GPX4) and ferroptosis suppressor protein 1 (FSP1) to induce ferroptosis. The strong oxidative stress induced cascade enzyodynamic effect and ferroptosis, which synergized with the two-dimensional bismuthene-mediated radiosensitization to improve the efficacy of RT. Both in vitro and in vivo experiments substantiated the excellent radiotherapeutic response of the nanozymes by enhancing RT and ferroptosis. Therefore, this work demonstrates that the rational combination of nanozymes with POD/GPX/NDH-like activity and GPX4/FSP1 suppressing ability to induce ferroptosis for synergistic radiosensitization provides a viable and promising strategy for cancer treatment.
{"title":"Engineered multienzyme-mimicking 2D bismuthene catalytic nanotriggers enable cascade enzyodynamic-boosted and synergistic GPX4/FSP1-mediated ferroptosis amplification for cancer radiosensitization","authors":"Yipengchen Yin, Li Zhu, Tiaoyan Jiang, Rong Chai, Ya Zhang, Tianyu Li, Kai Wang, Sheng Wang, Qin Zhang","doi":"10.1016/j.cej.2024.157762","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157762","url":null,"abstract":"Radiotherapy (RT) is a critical clinical treatment for cancer. However, radioresistance often hampers its effectiveness, leading to local recurrence and therapeutic failure. Ferroptosis has been regarded as a natural barrier to tumor progression and plays a significant role in RT-mediated anticancer effects. Therefore, the simultaneous activation of ferroptosis and RT is of great significance for cancer therapy. Herein, we engineered the tumor-releasing nanozymes (BMBs), combining manganese oxide as the ferroptosis inducer and two-dimensional bismuthene with high-Z effect for augmented ferroptotic RT in a triple-enzyme-like radiosensitization manner. The nanozymes BMBs depleted glutathione (GSH) and nicotinamide adenine dinucleotide phosphate (NADPH) in the tumor microenvironment to exhibit glutathione peroxidase (GPX)-like activity and NADPH dehydrogenase (NDH)-like activity, accompanied by aberrant reactive oxygen species (ROS) production exhibiting peoxidase (POD)-like activity. In addition, the nanozymes BMBs simultaneously inactivate ferroptosis defensive system: glutathione peroxidase 4 (GPX4) and ferroptosis suppressor protein 1 (FSP1) to induce ferroptosis. The strong oxidative stress induced cascade enzyodynamic effect and ferroptosis, which synergized with the two-dimensional bismuthene-mediated radiosensitization to improve the efficacy of RT. Both <em>in vitro</em> and <em>in vivo</em> experiments substantiated the excellent radiotherapeutic response of the nanozymes by enhancing RT and ferroptosis. Therefore, this work demonstrates that the rational combination of nanozymes with POD/GPX/NDH-like activity and GPX4/FSP1 suppressing ability to induce ferroptosis for synergistic radiosensitization provides a viable and promising strategy for cancer treatment.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"99 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671085","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-19DOI: 10.1016/j.cej.2024.157764
Xiaran Su, Yuming Dong, Yongfa Zhu, Haifeng Shi
Polyethylene terephthalate plastic is widely used and poses challenges in degradation, highlighting the importance of finding efficient degradation methods. In this study, MIL-125-NH2/BNQDs composites were synthesized to degrade polyethylene terephthalate plastic in the peroxymonosulfate-activated persistent photocatalysis system. The results showed that MIL-125-NH2/2BNQDs exhibited the best degradation effect on polyethylene terephthalate plastic activated by peroxymonosulfate under light conditions, with a degradation efficiency of 95.71 % achieved by adding 3 mM peroxymonosulfate, which was 3.01 times that of MIL-125-NH2 alone. Furthermore, all composite samples retained persistent catalytic activity under dark conditions after light irradiation. After visible light irradiation, the polyethylene terephthalate degradation efficiency achieved 90.23 % when MIL-125-NH2/2BNQDs activated by peroxymonosulfate were used under dark conditions. The mechanism of action of reactive radicals in the polyethylene terephthalate degradation process was revealed by scavenger experiments. In-situ X-ray photoelectron spectroscopy analysis demonstrated that MIL-125-NH2/2BNQDs induce Ti4+ to Ti3+ transition through electron transfer, resulting in higher efficiency of peroxymonosulfate activation. The composites achieve improved electron storage capacity and enhanced peroxymonosulfate activation efficiency. Furthermore, the alteration of valence in transition metals (from Ti4+ to Ti3+) triggers photochromism, which amplifies the ability to absorb light. This study provides new insights for the development of novel photocatalysts for environmentally friendly degradation of polyethylene terephthalate plastics, contributing to the removal of plastic waste and the promotion of resource sustainability
{"title":"MIL-125-NH2/BNQDs persistent photocatalyst enhanced peroxymonosulfate activation for efficient PET plastics removal","authors":"Xiaran Su, Yuming Dong, Yongfa Zhu, Haifeng Shi","doi":"10.1016/j.cej.2024.157764","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157764","url":null,"abstract":"Polyethylene terephthalate plastic is widely used and poses challenges in degradation, highlighting the importance of finding efficient degradation methods. In this study, MIL-125-NH<sub>2</sub>/BNQDs composites were synthesized to degrade polyethylene terephthalate plastic in the peroxymonosulfate-activated persistent photocatalysis system. The results showed that MIL-125-NH<sub>2</sub>/2BNQDs exhibited the best degradation effect on polyethylene terephthalate plastic activated by peroxymonosulfate under light conditions, with a degradation efficiency of 95.71 % achieved by adding 3 mM peroxymonosulfate, which was 3.01 times that of MIL-125-NH<sub>2</sub> alone. Furthermore, all composite samples retained persistent catalytic activity under dark conditions after light irradiation. After visible light irradiation, the polyethylene terephthalate degradation efficiency achieved 90.23 % when MIL-125-NH<sub>2</sub>/2BNQDs activated by peroxymonosulfate were used under dark conditions. The mechanism of action of reactive radicals in the polyethylene terephthalate degradation process was revealed by scavenger experiments. In-situ X-ray photoelectron spectroscopy analysis demonstrated that MIL-125-NH<sub>2</sub>/2BNQDs induce Ti<sup>4+</sup> to Ti<sup>3+</sup> transition through electron transfer, resulting in higher efficiency of peroxymonosulfate activation. The composites achieve improved electron storage capacity and enhanced peroxymonosulfate activation efficiency. Furthermore, the alteration of valence in transition metals (from Ti<sup>4+</sup> to Ti<sup>3+</sup>) triggers photochromism, which amplifies the ability to absorb light. This study provides new insights for the development of novel photocatalysts for environmentally friendly degradation of polyethylene terephthalate plastics, contributing to the removal of plastic waste and the promotion of resource sustainability","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"503 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671088","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-19DOI: 10.1016/j.cej.2024.157816
Mingda Che, Jingzhe Xiao, Shuya Zhang, Cancan Shan, Ze Zhao, Renliang Huang, Yitong Zhou, Mei Cui, Wei Qi, Rongxin Su
Nanoscale zero-valent iron (nZVI) is a promising reductant for the degradation of chlorinated hydrocarbons in contaminated groundwater. However, the inherent iron oxide shell limits its dechlorination reactivity. Here, a preparation strategy was proposed to enhance the Kirkendall effect of nZVI, aiming to alleviate the diffusion limitation of Fe atoms. Specifically, sulfidation and cellulose nanofibers (CNF) were employed to alter the shell composition, inducing radial nanocrack formation on S-nZVI@CNF. The type and content of surface groups on CNF are crucial to the nanocrack density, which in turn influences the number of dechlorination sites on S-nZVI@CNF. For the degradation of trichloroethylene (TCE) using carboxylated CNF-modified S-nZVI (S-nZVI@TOCNF), the radial nanocracks enhance its electron-donating capacity, while sulfidation suppresses the side reaction of H2 evolution. Compared with nZVI, S-nZVI@TOCNF demonstrates higher dechlorination reactivity (km = 0.0098 L.g−1.min−1) and selectivity (εe = 19.6 %), thereby accelerating TCE degradation through the β-elimination pathway. Additionally, S-nZVI@TOCNF shows resistance to interference, adaptability across a wide pH range (3.0–11.0), recyclability, and stability. Notably, 92.2 % of TCE from real groundwater was removed. This study employed a Kirkendall strategy to achieve the precise customization of nZVI with varied dechlorination capabilities, enhancing its potential for chlorinated hydrocarbon remediation in groundwater.
{"title":"A Kirkendall strategy for the efficient degradation of trichloroethylene from groundwater using cellulose nanofiber-supported sulfidated nZVI","authors":"Mingda Che, Jingzhe Xiao, Shuya Zhang, Cancan Shan, Ze Zhao, Renliang Huang, Yitong Zhou, Mei Cui, Wei Qi, Rongxin Su","doi":"10.1016/j.cej.2024.157816","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157816","url":null,"abstract":"Nanoscale zero-valent iron (nZVI) is a promising reductant for the degradation of chlorinated hydrocarbons in contaminated groundwater. However, the inherent iron oxide shell limits its dechlorination reactivity. Here, a preparation strategy was proposed to enhance the Kirkendall effect of nZVI, aiming to alleviate the diffusion limitation of Fe atoms. Specifically, sulfidation and cellulose nanofibers (CNF) were employed to alter the shell composition, inducing radial nanocrack formation on S-nZVI@CNF. The type and content of surface groups on CNF are crucial to the nanocrack density, which in turn influences the number of dechlorination sites on S-nZVI@CNF. For the degradation of trichloroethylene (TCE) using carboxylated CNF-modified S-nZVI (S-nZVI@TOCNF), the radial nanocracks enhance its electron-donating capacity, while sulfidation suppresses the side reaction of H<sub>2</sub> evolution. Compared with nZVI, S-nZVI@TOCNF demonstrates higher dechlorination reactivity (k<sub>m</sub> = 0.0098 L.g<sup>−1</sup>.min<sup>−1</sup>) and selectivity (ε<sub>e</sub> = 19.6 %), thereby accelerating TCE degradation through the β-elimination pathway. Additionally, S-nZVI@TOCNF shows resistance to interference, adaptability across a wide pH range (3.0–11.0), recyclability, and stability. Notably, 92.2 % of TCE from real groundwater was removed. This study employed a Kirkendall strategy to achieve the precise customization of nZVI with varied dechlorination capabilities, enhancing its potential for chlorinated hydrocarbon remediation in groundwater.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"54 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671089","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Epigenetic drugs have been used in the treatment of many diseases. Unfortunately, however, epigenetic drugs are not targeted, which makes the action of epigenetic drugs often systemic. This systemic epigenetic alteration can lead to a host of unwanted side effects. To improve delivery targeting and enhance the efficacy of drugs, the application of novel drug carriers in the field of epigenetic drug delivery becomes very important. We summarize the types of materials that have been used in the field of epigenetic drug delivery, such as liposomes, micelles, inorganic materials, framework materials, and so on (mainly in cancer therapy). We also describe some of the biocompatible or condition-responsive modifications commonly used in the field of drug nano-delivery based on the properties of different materials. Finally, we also draw inspiration from other drug delivery materials and reveal more materials that are still not used for epigenetic drug delivery, such as HOFs, Janus particles, molecular cage-like materials, etc., and discuss the current challenges and the way forward, which will provide more ideas for researchers.
{"title":"Perspectives on materials: Reality and potential of epigenetic drug nano-delivery","authors":"Yunxiang Zhang, Derui Xu, Xinmiao Hou, Xiaohui Wang, Siyu Zhao, Xinghua Jin","doi":"10.1016/j.cej.2024.157746","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157746","url":null,"abstract":"Epigenetic drugs have been used in the treatment of many diseases. Unfortunately, however, epigenetic drugs are not targeted, which makes the action of epigenetic drugs often systemic. This systemic epigenetic alteration can lead to a host of unwanted side effects. To improve delivery targeting and enhance the efficacy of drugs, the application of novel drug carriers in the field of epigenetic drug delivery becomes very important. We summarize the types of materials that have been used in the field of epigenetic drug delivery, such as liposomes, micelles, inorganic materials, framework materials, and so on (mainly in cancer therapy). We also describe some of the biocompatible or condition-responsive modifications commonly used in the field of drug nano-delivery based on the properties of different materials. Finally, we also draw inspiration from other drug delivery materials and reveal more materials that are still not used for epigenetic drug delivery, such as HOFs, Janus particles, molecular cage-like materials, etc., and discuss the current challenges and the way forward, which will provide more ideas for researchers.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"99 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The construction of aqueous rechargeable ammonium-iodine batteries (AIBs) must be eye-catching by combining the unique properties of ammonium ion (NH4+) and the special redox mechanism of iodine. Polyaniline (PANI) as a conductive polymer is a potential cathode material for aqueous NH4+ batteries. However, the proton (H+) escape of amino group (─NH─) in the oxidation process of PANI cannot realize the reversible reduction reaction from full-oxidized imine (─N═) to ─NH─. In this work, polyaniline with H+ reservoirs (PANI-H+) was successfully prepared by electrodeposition for the NH4+ and I3−/I2 storage. Interestingly, ─SO3−H+ groups as H+ reservoirs in 1, 5-Naphthalenedisulfonic acid (1, 5-NDSA) can provide H+ for the reduction of ═N─ to ─NH─, thus achieving the reversible redox process of PANI-H+. Therefore, PANI-H+ electrode exhibited excellent discharge capacity (299.3 mAh/g and 126.7mAh/g at the current density of 1 A/g and 10 A/g, respectively), and good stability of long-term cycles (≈100 % capacity retention after 1000 cycles at the current density of 10 A/g) in (NH4)2SO4 + I3− electrolyte. A series of spectroscopy analyses indicated the dual storage mechanism of NH4+ (de)intercalation and interfacial redox of I3−/I2. Finally, aqueous ammonium-iodine full cell (PTCDA|(NH4)2SO4 + I3−|PANI-H+) was constructed and presented satisfactory electrochemical performances. This work provides guidance to construct promising AIBs.
{"title":"A type of polyaniline with H+ reservoirs for dual-mechanism NH4+ and I3−/I2 storage","authors":"Xiaodong Zhi, Jiuzeng Jin, Ruiying Zhang, Jia Zheng, Changwei Li, Zhongmin Feng, Yun Wang, Ting Sun","doi":"10.1016/j.cej.2024.157804","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157804","url":null,"abstract":"The construction of aqueous rechargeable ammonium-iodine batteries (AIBs) must be eye-catching by combining the unique properties of ammonium ion (NH<sub>4</sub><sup>+</sup>) and the special redox mechanism of iodine. Polyaniline (PANI) as a conductive polymer is a potential cathode material for aqueous NH<sub>4</sub><sup>+</sup> batteries. However, the proton (H<sup>+</sup>) escape of amino group (─NH─) in the oxidation process of PANI cannot realize the reversible reduction reaction from full-oxidized imine (─N═) to ─NH─. In this work, polyaniline with H<sup>+</sup> reservoirs (PANI-H<sup>+</sup>) was successfully prepared by electrodeposition for the NH<sub>4</sub><sup>+</sup> and I<sub>3</sub><sup>−</sup>/I<sub>2</sub> storage. Interestingly, ─SO<sub>3</sub><sup>−</sup>H<sup>+</sup> groups as H<sup>+</sup> reservoirs in 1, 5-Naphthalenedisulfonic acid (1, 5-NDSA) can provide H<sup>+</sup> for the reduction of ═N─ to ─NH─, thus achieving the reversible redox process of PANI-H<sup>+</sup>. Therefore, PANI-H<sup>+</sup> electrode exhibited excellent discharge capacity (299.3 mAh/g and 126.7mAh/g at the current density of 1 A/g and 10 A/g, respectively), and good stability of long-term cycles (≈100 % capacity retention after 1000 cycles at the current density of 10 A/g) in (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> + I<sub>3</sub><sup>−</sup> electrolyte. A series of spectroscopy analyses indicated the dual storage mechanism of NH<sub>4</sub><sup>+</sup> (de)intercalation and interfacial redox of I<sub>3</sub><sup>−</sup>/I<sub>2</sub>. Finally, aqueous ammonium-iodine full cell (PTCDA|(NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> + I<sub>3</sub><sup>−</sup>|PANI-H<sup>+</sup>) was constructed and presented satisfactory electrochemical performances. This work provides guidance to construct promising AIBs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"11 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670935","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-19DOI: 10.1016/j.cej.2024.157806
Qi Wang, Aoxiang Liu, Bo Shen, Xin Ma, Yanling Wu, Xiaojia jiang, Jun Li, Chunjuan Li, Xiujuan Tang, Derek Hao, Huayue Zhu, Hao Du
In-situ Fenton like process was highly promising and energy-efficient for treating emerging organic contaminants. However, the challenge in the production and activation of H2O2 faces its practical application. Herein, a photoelectro-Fenton-like (PEF) system was successfully fabricated with BiVO4 thin-film, graphite (C) and PhC2Cu as photoanode, cathode and photocathode, respectively. The ternary system was applied for visible-light degradation of Tetracycline (TC) at a low potential of 0.5 V·H2O2 was generated at the graphite cathode and then activated to produce •OH by Cu(Ⅰ) from PhC2Cu photocathode. The photo-generated electrons accelerated the Cu(Ⅰ)/Cu(Ⅱ) cycle to achieve sustainable PEF reactions. After 150 min of illumination, 97 % TC was degraded in BiVO4|C|PCu system, superior to BiVO4|C and BiVO4|PCu systems. The outstanding stability and reusability of this PEF system was proved by 10 cycles. Moreover, the vulnerable atomic sites of TC molecule were predicated by the Fukui function. Both inhibition zone tests of bacteria and wheat seeds cultivation experiments proved that the constructed PEF system displayed outstanding performance in hampering TC eco-toxicity. For example, the Fv/Fm fluorescence image map demonstrated that the constructed PEF system not only degraded organic pollutants but also lowered their toxicity. Finally, the mechanism of in-situ generation and activation of H2O2 was proposed based on the results of quenching experiments, PL spectra and ESR technique. Overall, this study provides a promising pathway to remediate environmental pollution through constructing a PEF system based on dual cathodes.
{"title":"Sustainable dual-cathode photoelectro-Fenton-like system at a wide pH range for rapid degradation of emerging pollutants","authors":"Qi Wang, Aoxiang Liu, Bo Shen, Xin Ma, Yanling Wu, Xiaojia jiang, Jun Li, Chunjuan Li, Xiujuan Tang, Derek Hao, Huayue Zhu, Hao Du","doi":"10.1016/j.cej.2024.157806","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157806","url":null,"abstract":"In-situ Fenton like process was highly promising and energy-efficient for treating emerging organic contaminants. However, the challenge in the production and activation of H<sub>2</sub>O<sub>2</sub> faces its practical application. Herein, a photoelectro-Fenton-like (PEF) system was successfully fabricated with BiVO<sub>4</sub> thin-film, graphite (C) and PhC<sub>2</sub>Cu as photoanode, cathode and photocathode, respectively. The ternary system was applied for visible-light degradation of Tetracycline (TC) at a low potential of 0.5 V·H<sub>2</sub>O<sub>2</sub> was generated at the graphite cathode and then activated to produce •OH by Cu(Ⅰ) from PhC<sub>2</sub>Cu photocathode. The photo-generated electrons accelerated the Cu(Ⅰ)/Cu(Ⅱ) cycle to achieve sustainable PEF reactions. After 150 min of illumination, 97 % TC was degraded in BiVO<sub>4</sub>|C|PCu system, superior to BiVO<sub>4</sub>|C and BiVO<sub>4</sub>|PCu systems. The outstanding stability and reusability of this PEF system was proved by 10 cycles. Moreover, the vulnerable atomic sites of TC molecule were predicated by the Fukui function. Both inhibition zone tests of bacteria and wheat seeds cultivation experiments proved that the constructed PEF system displayed outstanding performance in hampering TC eco-toxicity. For example, the Fv/Fm fluorescence image map demonstrated that the constructed PEF system not only degraded organic pollutants but also lowered their toxicity. Finally, the mechanism of in-situ generation and activation of H<sub>2</sub>O<sub>2</sub> was proposed based on the results of quenching experiments, PL spectra and ESR technique. Overall, this study provides a promising pathway to remediate environmental pollution through constructing a PEF system based on dual cathodes.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"106 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670802","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-19DOI: 10.1016/j.cej.2024.157834
Yi Han, Si Yang, Gang Guo, Jing Chen, Xiaohui Wu, Feixiang Zan
Anaerobic digestion (AD) frequently encounters challenges such as acidification under high organic loadings, leading to system instability or failure. This study demonstrates that biogas stirring (RB) effectively mitigates acidification during the AD of FW (FW), outperforming traditional mechanical stirring (RM). The RB system sustained stable methane production, reaching 249.1 mL CH4/g VSadded/d, whereas the RM system encountered significant acidification, with a pH dropping to 5.0 ± 0.2, impeding methanogenesis. For sludge characteristics, biogas stirring in the RB system significantly decreased particle size to 78 μm, which were anticipated to facilitate mass transfer and substrate conversion. Focus on the microbial communities evolution, employing biogas stirring facilitated a rational microbial collaboration with the enhanced capability for volatile fatty acids (VFAs) conversion and methane production. In addition, Methanobacterium, a typical methanogen for hydrogenotrophic methanogenesis (HM), was predominant in RB, occupying in an important position (Centrality = 0.9232) in the microbial network. Furthermore, the increased H2 partial pressure enriched the concentration of F420 by 63.1 %, facilitating its uptake and supporting the growth syntrophic acetate-oxidizing (SAO) bacteria. The consequent activation of the SAO-HM pathway is key to rapidly restoring methane production post-acidification. The findings of this study revealed the underlying role of biogas stirring for SAO-HM pathway and provided a potential strategy to facilitate acidification alleviation in AD.
{"title":"Strengthening the syntrophic pathway for acetate oxidation-hydrogenotrophic methanogenesis by biogas stirring for effectively mitigating acidification in anaerobic digestion","authors":"Yi Han, Si Yang, Gang Guo, Jing Chen, Xiaohui Wu, Feixiang Zan","doi":"10.1016/j.cej.2024.157834","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157834","url":null,"abstract":"Anaerobic digestion (AD) frequently encounters challenges such as acidification under high organic loadings, leading to system instability or failure. This study demonstrates that biogas stirring (RB) effectively mitigates acidification during the AD of FW (FW), outperforming traditional mechanical stirring (RM). The RB system sustained stable methane production, reaching 249.1 mL CH<sub>4</sub>/g VS<sub>added</sub>/d, whereas the RM system encountered significant acidification, with a pH dropping to 5.0 ± 0.2, impeding methanogenesis. For sludge characteristics, biogas stirring in the RB system significantly decreased particle size to 78 μm, which were anticipated to facilitate mass transfer and substrate conversion. Focus on the microbial communities evolution, employing biogas stirring facilitated a rational microbial collaboration with the enhanced capability for volatile fatty acids (VFAs) conversion and methane production. In addition, <em>Methanobacterium</em>, a typical methanogen for hydrogenotrophic methanogenesis (HM), was predominant in RB, occupying in an important position (Centrality = 0.9232) in the microbial network. Furthermore, the increased H<sub>2</sub> partial pressure enriched the concentration of F<sub>420</sub> by 63.1 %, facilitating its uptake and supporting the growth syntrophic acetate-oxidizing (SAO) bacteria. The consequent activation of the SAO-HM pathway is key to rapidly restoring methane production post-acidification. The findings of this study revealed the underlying role of biogas stirring for SAO-HM pathway and provided a potential strategy to facilitate acidification alleviation in AD.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"15 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673778","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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