The surface modification of transparent conductive oxides with self-assembled monolayers (SAM) based on carbazole has been demonstrated to be a workable strategy for the formation of efficient hole-selective contacts, thus significantly enhancing the power conversion efficiency (PCE) and stability of p-i-n perovskite solar cells (PSCs). While the inherent monolayer nature of SAM offers unique advantages, the buried interface poses a significant challenge to synergistic regulation for both perovskite (PVK) and SAM. In this study, an interfacial layer composed of an ionic compound, 3-(methylthio) propylamine hydroiodide (3MTPAI), is introduced between the PVK and SAM layers to enhance the photovoltaic performance of PSCs. 3MTPAI has been demonstrated to enhance the ion–dipole interactions of the SAM, facilitating a better-matched energy level between the PVK and hole transport layer (HTL). This, in turn, improves hole extraction/transport from the PVK layer to the HTL and reduces carrier recombination of the PSCs. Consequently, the PCE of the PSCs modified with 3MTPAI increases from 23.90 % to 25.30 %. Furthermore, devices treated with 3MTPAI exhibit enhanced stability, maintaining 90 % of the original PCE after 1000 h under conditions of 55 ± 5 % RH. Therefore, the buried interface modification strategy employing dual-role 3MTPAI molecules emerges as a viable approach to enhance the efficiency and stability of PSCs.
{"title":"Gradient layer arrangement for modulating the buried interface of inverted perovskite solar cells","authors":"Wenjing Miao, Ran Yin, Rongfei Wu, Weiwei Sun, Yansheng Sun, Kexiang Wang, Tingting You, Weichang Hao, Penggang Yin","doi":"10.1016/j.cej.2025.162942","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162942","url":null,"abstract":"The surface modification of transparent conductive oxides with self-assembled monolayers (SAM) based on carbazole has been demonstrated to be a workable strategy for the formation of efficient hole-selective contacts, thus significantly enhancing the power conversion efficiency (PCE) and stability of p-i-n perovskite solar cells (PSCs). While the inherent monolayer nature of SAM offers unique advantages, the buried interface poses a significant challenge to synergistic regulation for both perovskite (PVK) and SAM. In this study, an interfacial layer composed of an ionic compound, 3-(methylthio) propylamine hydroiodide (3MTPAI), is introduced between the PVK and SAM layers to enhance the photovoltaic performance of PSCs. 3MTPAI has been demonstrated to enhance the ion–dipole interactions of the SAM, facilitating a better-matched energy level between the PVK and hole transport layer (HTL). This, in turn, improves hole extraction/transport from the PVK layer to the HTL and reduces carrier recombination of the PSCs. Consequently, the PCE of the PSCs modified with 3MTPAI increases from 23.90 % to 25.30 %. Furthermore, devices treated with 3MTPAI exhibit enhanced stability, maintaining 90 % of the original PCE after 1000 h under conditions of 55 ± 5 % RH. Therefore, the buried interface modification strategy employing dual-role 3MTPAI molecules emerges as a viable approach to enhance the efficiency and stability of PSCs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"21 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862775","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 : 2025-04-22DOI: 10.1016/j.cej.2025.162977
Wei Liu, Chen Dai, Linheng He, Xingyu Liu, Zhiyang Zhao, Wenqian Yan, Man Yuan, Zihao Song, Sheng Cui
Water pollution has become one of the major environmental challenges due to the rapid development of industry and human activities. Heavy metals, oil, pesticides, antibiotics, and radionuclides have caused serious water pollution. Adsorption is a fast and simple method to remove these pollutants. Careful design and optimization of material properties is the key to improving adsorption efficiency. Biomass aerogels are manufactured from biomass materials, as a three-dimensional porous material, they exhibit high specific surface area, abundant active sites, low cost, and environmental friendliness. Therefore, it has attracted great attention in the field of water pollution treatment. Therefore, this paper summarizes the material types, preparation methods, adsorption properties, and adsorption mechanisms of biomass aerogels, highlights the modification methods of aerogels that adapt to the expected application of different pollutants, presents the recent progress of biomass aerogels in pollutant removal from different water bodies, and discusses the future potential of aerogels in water treatment applications.
{"title":"Biomass aerogel: An emerging eco-friendly material for adsorbing pollutants in water","authors":"Wei Liu, Chen Dai, Linheng He, Xingyu Liu, Zhiyang Zhao, Wenqian Yan, Man Yuan, Zihao Song, Sheng Cui","doi":"10.1016/j.cej.2025.162977","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162977","url":null,"abstract":"Water pollution has become one of the major environmental challenges due to the rapid development of industry and human activities. Heavy metals, oil, pesticides, antibiotics, and radionuclides have caused serious water pollution. Adsorption is a fast and simple method to remove these pollutants. Careful design and optimization of material properties is the key to improving adsorption efficiency. Biomass aerogels are manufactured from biomass materials, as a three-dimensional porous material, they exhibit high specific surface area, abundant active sites, low cost, and environmental friendliness. Therefore, it has attracted great attention in the field of water pollution treatment. Therefore, this paper summarizes the material types, preparation methods, adsorption properties, and adsorption mechanisms of biomass aerogels, highlights the modification methods of aerogels that adapt to the expected application of different pollutants, presents the recent progress of biomass aerogels in pollutant removal from different water bodies, and discusses the future potential of aerogels in water treatment applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"7 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862838","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 authors regret, Fig. 5 and Fig. 7 in addition with the captions of Fig. 4 and Fig. 6 in this article.
{"title":"Corrigendum to “A dual lubricating and antibacterial hydrogel coating containing hyperbranched polylysine with excellent biocompatibility for surface modification of central venous catheters” [Chem. Eng. J. 509 (2025) 161402]","authors":"Bohui Shao, Xuelong Wang, Lei Huang, Xiaowei Liu, Liming Wang, Weiwei Zheng, Changyou Gao","doi":"10.1016/j.cej.2025.162383","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162383","url":null,"abstract":"The authors regret, <strong>Fig. 5</strong> and <strong>Fig. 7</strong> in addition with the captions of <strong>Fig. 4</strong> and <strong>Fig. 6</strong> in this article.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"108 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857878","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}
Lithium-sulfur batteries (LSBs) face substantial performance limitations, primarily due to the slow kinetics of conversion and the detrimental shuttling effect of lithium polysulfides (LiPSs). In this study, cobalt single-atom catalysts were synthesized on nitrogen-doped hollow carbon spheres through the impregnation adsorption method. The combination of atomically dispersed Co sites with hollow carbon spheres enables the formation of nitrogen-doped hollow carbon spheres loaded with cobalt single-atom catalysts (NHCS@CoSAs), which act as efficient sulfur hosts. While being employed as a bifunctional electrocatalyst, the Co-N4 catalytic sites not only inhibit the detrimental shuttle effect by adsorbing LiPSs but also accelerate their interfacial redox conversion, promoting faster conversion kinetics. This results in LSBs achieving a stable cycling life exceeding 2000 cycles, with a capacity fade of just 0.026 % per cycle at 2C. In addition, Li-S pouch cells featuring NHCS@CoSAs exhibit a remarkable initial capacity of 972.2 mAh g−1 at a rate of 0.1C, even under a high sulfur loading of 4.16 mg cm−2. This study could offer fresh perspectives on developing high-performance sulfur-based cathodes for LSBs.
{"title":"Atomically dispersed cobalt sites on nitrogen-doped hollow carbon spheres as efficient electrocatalysts for high performance lithium-sulfur batteries","authors":"Xunli Guo, Mingzhi Yang, Jiahao Hou, Hongyun Li, Zhewen Liu, Yuheng Cui, Dong Shi, Haixiao Hu, Baoguo Zhang, Yongliang Shao, Yongzhong Wu, Xiaopeng Hao","doi":"10.1016/j.cej.2025.162955","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162955","url":null,"abstract":"Lithium-sulfur batteries (LSBs) face substantial performance limitations, primarily due to the slow kinetics of conversion and the detrimental shuttling effect of lithium polysulfides (LiPSs). In this study, cobalt single-atom catalysts were synthesized on nitrogen-doped hollow carbon spheres through the impregnation adsorption method. The combination of atomically dispersed Co sites with hollow carbon spheres enables the formation of nitrogen-doped hollow carbon spheres loaded with cobalt single-atom catalysts (NHCS@CoSAs), which act as efficient sulfur hosts. While being employed as a bifunctional electrocatalyst, the Co-N<sub>4</sub> catalytic sites not only inhibit the detrimental shuttle effect by adsorbing LiPSs but also accelerate their interfacial redox conversion, promoting faster conversion kinetics. This results in LSBs achieving a stable cycling life exceeding 2000 cycles, with a capacity fade of just 0.026 % per cycle at 2C. In addition, Li-S pouch cells featuring NHCS@CoSAs exhibit a remarkable initial capacity of 972.2 mAh g<sup>−1</sup> at a rate of 0.1C, even under a high sulfur loading of 4.16 mg cm<sup>−2</sup>. This study could offer fresh perspectives on developing high-performance sulfur-based cathodes for LSBs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"51 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857880","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 : 2025-04-22DOI: 10.1016/j.cej.2025.162943
Di Zhao, Xu Sun, Ziyuan Chai, Chengcheng Chi, Xiaobiao Zuo, Lei Jiang, Liping Heng
Ice formation in harsh weather conditions poses a significant challenge across various sectors, including transportation, energy, and infrastructure. Researchers have recently developed a variety of solar-driven photothermal super-wetting interfaces for deicing applications, showcasing excellent anti-icing and de-icing capabilities. However, these interfaces often suffer from low solar efficiency and require high operating temperatures, primarily due to suboptimal photothermal layer design, hindering their broad application. To address these issues, we developed a hierarchically structured photothermal solid slippery interface (P/HPC), consisting of paraffin, polydimethylsiloxane (PDMS), and carbon black, using a double-template method. The unique micro/nano hierarchical porous structure of the photothermal layer promotes multiple internal reflections of sunlight, thereby enhancing solar absorption and exhibiting superior photothermal properties. Under 1.0 kW/m2 light intensity, this composite interface demonstrates exceptional anti-/de-icing properties, even at temperatures as low as −50 Moreover, the interface demonstrates outstanding light-triggered self-healing abilities and stability under harsh conditions, offering a promising solution for anti-/de-icing applications in a variety of extreme environments.
{"title":"Hierarchically-structured light-thermal solid slippery interface for anti-/de-icing","authors":"Di Zhao, Xu Sun, Ziyuan Chai, Chengcheng Chi, Xiaobiao Zuo, Lei Jiang, Liping Heng","doi":"10.1016/j.cej.2025.162943","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162943","url":null,"abstract":"Ice formation in harsh weather conditions poses a significant challenge across various sectors, including transportation, energy, and infrastructure. Researchers have recently developed a variety of solar-driven photothermal super-wetting interfaces for deicing applications, showcasing excellent anti-icing and de-icing capabilities. However, these interfaces often suffer from low solar efficiency and require high operating temperatures, primarily due to suboptimal photothermal layer design, hindering their broad application. To address these issues, we developed a hierarchically structured photothermal solid slippery interface (P/HPC), consisting of paraffin, polydimethylsiloxane (PDMS), and carbon black, using a double-template method. The unique micro/nano hierarchical porous structure of the photothermal layer promotes multiple internal reflections of sunlight, thereby enhancing solar absorption and exhibiting superior photothermal properties. Under 1.0 kW/m<sup>2</sup> light intensity, this composite interface demonstrates exceptional anti-/de-icing properties, even at temperatures as low as −50 Moreover, the interface demonstrates outstanding light-triggered self-healing abilities and stability under harsh conditions, offering a promising solution for anti-/de-icing applications in a variety of extreme environments.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"69 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862844","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 : 2025-04-22DOI: 10.1016/j.cej.2025.162970
Yanan Li, Jie Yang, Jiaqi Wang, Zhuo Feng, Kangjian Jing, Weiqin Wu, Meijing Yao, Xiaona Liu
The extensive use of fluoroquinolone antibiotics (FQs) and their low degradation efficiency pose significant threats to aquatic ecosystems and human health. However, the species-specific reactions and the key reaction mechanisms underlying their degradation by ferrate (Fe(VI)) based on density functional theory (DFT) calculations remain unclear. This study systematically examines the oxidation mechanisms of four FQs (enoxacin (ENO), ofloxacin (OFL), gatifloxacin (GAT), and fleroxacin (FLE)) by Fe(VI), through combined experimental and DFT methods. The results showed that the oxidation of FQs by Fe(VI) conformed to secondary reaction kinetics with second-order reaction rate constants following FLE (1.57 mM−1·min−1) > GAT (0.99 mM−1·min−1) > OFL (0.96 mM−1·min−1) > ENO (0.79 mM−1·min−1). While Fe(VI) species dominated the reaction, specific contributions from Fe(V)/Fe(IV) and hydroxyl radicals (·OH) were quantitatively verified, and DFT further proved that FeO42-, as the predominant Fe(VI) species, governed the reaction at pH 8.0, the optimum reaction pH. Instrumental analysis detected the main products, and DFT predicted the reactive active sites, suggesting that the quinolone and piperazine rings cleavage on the FQs molecules was achieved through hydroxylation, decarboxylation, and other reactions, with the intermediates tending to be harmless. Both methods identified three distinct reaction mechanisms: ·OH attack, single-oxygen transfer (SOT), and double-oxygen transfer, with ·OH attack the most likely to occur and SOT the main reaction mechanism. This study combines DFT calculations with experimental observations to identify the mechanisms of Fe(VI)-mediated FQs degradation at the molecular structural level, and provide new insights into the treatment of FQs.
{"title":"Oxidative degradation of fluoroquinolone antibiotics by ferrate(VI): Kinetics, reaction mechanism, and theoretical calculations","authors":"Yanan Li, Jie Yang, Jiaqi Wang, Zhuo Feng, Kangjian Jing, Weiqin Wu, Meijing Yao, Xiaona Liu","doi":"10.1016/j.cej.2025.162970","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162970","url":null,"abstract":"The extensive use of fluoroquinolone antibiotics (FQs) and their low degradation efficiency pose significant threats to aquatic ecosystems and human health. However, the species-specific reactions and the key reaction mechanisms underlying their degradation by ferrate (Fe(VI)) based on density functional theory (DFT) calculations remain unclear. This study systematically examines the oxidation mechanisms of four FQs (enoxacin (ENO), ofloxacin (OFL), gatifloxacin (GAT), and fleroxacin (FLE)) by Fe(VI), through combined experimental and DFT methods. The results showed that the oxidation of FQs by Fe(VI) conformed to secondary reaction kinetics with second-order reaction rate constants following FLE (1.57 mM<sup>−1</sup>·min<sup>−1</sup>) > GAT (0.99 mM<sup>−1</sup>·min<sup>−1</sup>) > OFL (0.96 mM<sup>−1</sup>·min<sup>−1</sup>) > ENO (0.79 mM<sup>−1</sup>·min<sup>−1</sup>). While Fe(VI) species dominated the reaction, specific contributions from Fe(V)/Fe(IV) and hydroxyl radicals (·OH) were quantitatively verified, and DFT further proved that FeO<sub>4</sub><sup>2-</sup>, as the predominant Fe(VI) species, governed the reaction at pH 8.0, the optimum reaction pH. Instrumental analysis detected the main products, and DFT predicted the reactive active sites, suggesting that the quinolone and piperazine rings cleavage on the FQs molecules was achieved through hydroxylation, decarboxylation, and other reactions, with the intermediates tending to be harmless. Both methods identified three distinct reaction mechanisms: ·OH attack, single-oxygen transfer (SOT), and double-oxygen transfer, with ·OH attack the most likely to occur and SOT the main reaction mechanism. This study combines DFT calculations with experimental observations to identify the mechanisms of Fe(VI)-mediated FQs degradation at the molecular structural level, and provide new insights into the treatment of FQs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"32 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862773","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 : 2025-04-22DOI: 10.1016/j.cej.2025.162971
Junghoon Mok, Amadeu K. Sum
To reach carbon neutrality, Carbon Capture and Storage (CCS) technology has emerged as a critical solution. This research introduces an innovative and groundbreaking approach to gas capture, the “gas hydrate condensation” method specifically applied to CO2 capture. We demonstrate that water vapor, efficiently supplied through controlled convection, can directly co-condense with CO2 on cold surfaces to form gas hydrates. This novel method bypasses the mass/heat transfer limitations inherent in traditional approaches that utilize bulk water for gas hydrate formation, which is further enhanced with liquid CO2 condensation/vaporization. In this context, condensed liquid CO2 serves dual purpose: as a refrigerant, facilitating the transport of cold energy, and as a water carrier, significantly accelerating the gas hydrate condensation process. This enhanced method is shown to improve CO2 capture rates by more than three-fold compared to conventional gas hydrate condensation strategies. Moreover, this work details the distribution and morphology of the gas hydrates formed, laying the groundwork for development and scale-up of this technology. These findings represent a significant advancement in the realm of gas hydrate-based CCS technologies, introducing a versatile, efficient and sustainable strategy for capturing CO2 and other greenhouse gases.
{"title":"An efficient and sustainable method for improved CO2 capture based on gas hydrate condensation","authors":"Junghoon Mok, Amadeu K. Sum","doi":"10.1016/j.cej.2025.162971","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162971","url":null,"abstract":"To reach carbon neutrality, Carbon Capture and Storage (CCS) technology has emerged as a critical solution. This research introduces an innovative and groundbreaking approach to gas capture, the “gas hydrate condensation” method specifically applied to CO<sub>2</sub> capture. We demonstrate that water vapor, efficiently supplied through controlled convection, can directly co-condense with CO<sub>2</sub> on cold surfaces to form gas hydrates. This novel method bypasses the mass/heat transfer limitations inherent in traditional approaches that utilize bulk water for gas hydrate formation, which is further enhanced with liquid CO<sub>2</sub> condensation/vaporization. In this context, condensed liquid CO<sub>2</sub> serves dual purpose: as a refrigerant, facilitating the transport of cold energy, and as a water carrier, significantly accelerating the gas hydrate condensation process. This enhanced method is shown to improve CO<sub>2</sub> capture rates by more than three-fold compared to conventional gas hydrate condensation strategies. Moreover, this work details the distribution and morphology of the gas hydrates formed, laying the groundwork for development and scale-up of this technology. These findings represent a significant advancement in the realm of gas hydrate-based CCS technologies, introducing a versatile, efficient and sustainable strategy for capturing CO<sub>2</sub> and other greenhouse gases.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"21 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862836","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 development of highly active and selective cathode materials is important for the in-situ synthesis of hydrogen peroxide (H2O2) and its activation to radicals for the degradation of emerging contaminants. In this paper, a nitrogen-doped carbon bilayer catalyst based on transition metal single atoms (Co2-NC/Fe3-C3N4) was developed to construct a flow-through electrocatalytic membrane system as the cathode for the efficient removal of ibuprofen (IBP) from wastewater. The active sites of high-density transition metal single atoms and heteroatoms N synergistically enhanced O2 adsorption and *OOH desorption to promote H2O2 generation. The results showed that the actual contents of Fe and Co single atoms in the catalysts were 6.0 wt% and 4.2 wt%, which were higher than that of common single atoms < 3 wt%. The degradation rate of IBP in the Co2-NC/Fe3-C3N4 bilayer electrocatalytic membrane system could reach 93.1 % at 60 min under optimal conditions. The Fe3-C3N4 layer produced H2O2 and further activated to hydroxyl radical (•OH) mainly through the three electron oxygen reduction reaction (3e--ORR), whereas the Co2-NC layer produced H2O2 through the 2e--ORR to provide the precursors for the Fe3-C3N4 layer for reactive oxygen species generation. The contribution of •OH was as high as 86.49 %, which was the main ROS for degrading IBP. The susceptible reaction sites of IBP were O9, O10, C1, and C11, and there were two main degradation pathways, and the toxicity of the degraded intermediates was reduced, which decreased the environmental risk generated by IBP.
{"title":"Nitrogen-doped carbon bilayer flow-through electrocatalytic membrane based on transition metal single atoms: Simultaneous generation and activation of H2O2 for ibuprofen degradation","authors":"Xiangting Hou, Hui Wang, Lumeng Jia, Mengxue Li, Wenchao Yu, Zhaoyong Bian","doi":"10.1016/j.cej.2025.162950","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162950","url":null,"abstract":"The development of highly active and selective cathode materials is important for the in-situ synthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) and its activation to radicals for the degradation of emerging contaminants. In this paper, a nitrogen-doped carbon bilayer catalyst based on transition metal single atoms (Co<sub>2</sub>-NC/Fe<sub>3</sub>-C<sub>3</sub>N<sub>4</sub>) was developed to construct a flow-through electrocatalytic membrane system as the cathode for the efficient removal of ibuprofen (IBP) from wastewater. The active sites of high-density transition metal single atoms and heteroatoms N synergistically enhanced O<sub>2</sub> adsorption and *OOH desorption to promote H<sub>2</sub>O<sub>2</sub> generation. The results showed that the actual contents of Fe and Co single atoms in the catalysts were 6.0 wt% and 4.2 wt%, which were higher than that of common single atoms < 3 wt%. The degradation rate of IBP in the Co<sub>2</sub>-NC/Fe<sub>3</sub>-C<sub>3</sub>N<sub>4</sub> bilayer electrocatalytic membrane system could reach 93.1 % at 60 min under optimal conditions. The Fe<sub>3</sub>-C<sub>3</sub>N<sub>4</sub> layer produced H<sub>2</sub>O<sub>2</sub> and further activated to hydroxyl radical (•OH) mainly through the three electron oxygen reduction reaction (3e<sup>-</sup>-ORR), whereas the Co<sub>2</sub>-NC layer produced H<sub>2</sub>O<sub>2</sub> through the 2e<sup>-</sup>-ORR to provide the precursors for the Fe<sub>3</sub>-C<sub>3</sub>N<sub>4</sub> layer for reactive oxygen species generation. The contribution of •OH was as high as 86.49 %, which was the main ROS for degrading IBP. The susceptible reaction sites of IBP were O9, O10, C1, and C11, and there were two main degradation pathways, and the toxicity of the degraded intermediates was reduced, which decreased the environmental risk generated by IBP.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"9 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862837","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 : 2025-04-22DOI: 10.1016/j.cej.2025.162966
Jun Wu, Chengdeng Wang, Jiamao Hao, Zhi Wang, Lu Yang, Zhiming Bai, Xiaoqin Yan, Yousong Gu
Fluorides are considered potential replacements for intercalation electrodes in high-performance lithium-ion batteries (LIBs), owing to the high energy density achieved through conversion reactions for lithium storage. However, their practical application is hindered by severe polarization effects due to sluggish charge transport and electrochemical kinetics of LiF reactions. Herein, a dual-conductivity-enhanced Ni-CoF2@CNT electrode is developed through CNT modulation and in situ reduction of CoxNiyF2 solid solutions. Electrochemical characterizations and XPS confirm the irreversible transformation of NiF2 into metallic Ni. Kinetic analyses reveal that the composite electrode exhibits low interfacial impedance, rapid interfacial charge transfer, and a lithium-ion diffusion coefficient three times than that of pristine CoF2. Morphological regulation promotes Faradaic reactions into pseudocapacitance, mitigating diffusion limitations under high-rate conditions. Notably, density functional theory (DFT) calculations and ex situ XPS demonstrate that the Ni(111) crystal plane catalyzes LiF cleavage during charging, reducing the energy barrier from 3.620 eV for direct cleavage to 0.871 eV. The designed electrode exhibits outstanding cycling stability and rate performance, retaining a capacity of 405 mAh g−1 with 94 % retention after 1000 cycles at 1 A g−1. This study presents a straightforward and effective in situ reduction strategy for incorporating metallic phases into fluorides, providing a promising pathway for high-performance conversion electrodes.
{"title":"In situ Ni matrix for kinetic enhancement and Li-F cleavage catalysis enabled high-performance conversion fluoride electrodes","authors":"Jun Wu, Chengdeng Wang, Jiamao Hao, Zhi Wang, Lu Yang, Zhiming Bai, Xiaoqin Yan, Yousong Gu","doi":"10.1016/j.cej.2025.162966","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162966","url":null,"abstract":"Fluorides are considered potential replacements for intercalation electrodes in high-performance lithium-ion batteries (LIBs), owing to the high energy density achieved through conversion reactions for lithium storage. However, their practical application is hindered by severe polarization effects due to sluggish charge transport and electrochemical kinetics of LiF reactions. Herein, a dual-conductivity-enhanced Ni-CoF<sub>2</sub>@CNT electrode is developed through CNT modulation and in situ reduction of Co<sub>x</sub>Ni<sub>y</sub>F<sub>2</sub> solid solutions. Electrochemical characterizations and XPS confirm the irreversible transformation of NiF<sub>2</sub> into metallic Ni. Kinetic analyses reveal that the composite electrode exhibits low interfacial impedance, rapid interfacial charge transfer, and a lithium-ion diffusion coefficient three times than that of pristine CoF<sub>2</sub>. Morphological regulation promotes Faradaic reactions into pseudocapacitance, mitigating diffusion limitations under high-rate conditions. Notably, density functional theory (DFT) calculations and ex situ XPS demonstrate that the Ni(111) crystal plane catalyzes LiF cleavage during charging, reducing the energy barrier from 3.620 eV for direct cleavage to 0.871 eV. The designed electrode exhibits outstanding cycling stability and rate performance, retaining a capacity of 405 mAh g<sup>−1</sup> with 94 % retention after 1000 cycles at 1 A g<sup>−1</sup>. This study presents a straightforward and effective in situ reduction strategy for incorporating metallic phases into fluorides, providing a promising pathway for high-performance conversion electrodes.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"50 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862846","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}
Periodate (PI, IO4−)-based advanced oxidation processes (AOPs) have recently received increasing attention in water treatment. The activation of PI to generate different reactive species is crucial for decontaminants in PI-AOPs. This review provides a comprehensive experimental data and analysis information in metal-activated PI processes for the contaminant degradation. Various categories of metals for PI activation, including single metal and bimetals with their activation mechanisms were discussed. Among them, manganese (Mn) and iron (Fe) were the two dominant activators in PI activation. Noble metals including ruthenium (Ru), osmium (Os) and metal-complexes also showed promising prospects in PI activation, which was first noticed in this review. The importance of external and internal metal complexes in metal-activated PI activation was perceived for the first time, especially distinct production pathways of reactive species (i.e high-valent manganese-oxygen species and generated reactive complexes) produced by different metal complex sources. The identification of various reactive species was defined in details. Besides, the potential risks and strategies for iodine-containing disinfection by-products (I-DBPs) reduction were summarized for the first time. Ultimately, the challenges, knowledge gaps and future development are proposed to facilitate the metal-activated PI technology to take a step further for practical application.
{"title":"Metal-based activation of periodate as an advanced oxidation process for water decontamination: A critical review","authors":"Yun Shen, Jinjing Huang, Junlian Qiao, Jiabin Chen, Egshiglen Batjargal, Baigal-Amar Tuulaikhuu, Yajie Qian, Xuefei Zhou, Yalei Zhang","doi":"10.1016/j.cej.2025.162949","DOIUrl":"https://doi.org/10.1016/j.cej.2025.162949","url":null,"abstract":"Periodate (PI, IO<sub>4</sub><sup>−</sup>)-based advanced oxidation processes (AOPs) have recently received increasing attention in water treatment. The activation of PI to generate different reactive species is crucial for decontaminants in PI-AOPs. This review provides a comprehensive experimental data and analysis information in metal-activated PI processes for the contaminant degradation. Various categories of metals for PI activation, including single metal and bimetals with their activation mechanisms were discussed. Among them, manganese (Mn) and iron (Fe) were the two dominant activators in PI activation. Noble metals including ruthenium (Ru), osmium (Os) and metal-complexes also showed promising prospects in PI activation, which was first noticed in this review. The importance of external and internal metal complexes in metal-activated PI activation was perceived for the first time, especially distinct production pathways of reactive species (i.e high-valent manganese-oxygen species and generated reactive complexes) produced by different metal complex sources. The identification of various reactive species was defined in details. Besides, the potential risks and strategies for iodine-containing disinfection by-products (I-DBPs) reduction were summarized for the first time. Ultimately, the challenges, knowledge gaps and future development are proposed to facilitate the metal-activated PI technology to take a step further for practical application.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"6 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857883","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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