Pub Date : 2024-11-19DOI: 10.1016/j.cej.2024.157824
Pan Huang, Charley Huang, Yongxiang Sun, Ziqian Zhao, Lin Yang, Haoyu Yang, Lu Gong, Wenshuai Yang, Hongbo Zeng
Engineering solar evaporators with Janus structures is crucial for facilitating water transition and heat localization to enhance water evaporation efficiency. However, the fragile discontinuous bilayer structures and unavoidable surface fouling significantly hinder their application. Herein, inspired by the Janus structure of Black Amanita mushrooms, we designed a robust solar evaporator with an integrated wood-like and Janus structure using directional freeze-casting and magnetically induced self-assembly of polypyrrole-coated Fe3O4 particles as a build-in photothermal top layer within a hydrophilic matrix, followed by covering it with an additional hydrophobic fluorine layer to simultaneously regulate surface wettability and antifouling properties. Incorporating the hydrophobic fluorine layer onto the solar evaporator not only enhances its water evaporation efficiency via thermal localization effects, but also prevents fouling, salt, and dust scaling accumulation on its surface, facilitating water transportation, thus achieving a groundbreaking performance with the evaporation rate of 2.13 kg m−2h−1 under one sun irradiation. Moreover, the mechanical performance of the as-prepared solar evaporator can be further optimized by precisely modulating supramolecular interactions within its structure, achieving Young’s modulus over 4 MPa and maintaining structural integrity after the peel-off tests. The fabricated solar evaporator enables highly efficient water purification from artificial seawater, oil-in-water emulsions, and industrial wastewater, providing a rational strategy for designing high-yield solar evaporation systems for wastewater containing complex contaminants
{"title":"Bio-inspired magnetically induced self-assembling Janus solar evaporator with antifouling and antiscaling properties","authors":"Pan Huang, Charley Huang, Yongxiang Sun, Ziqian Zhao, Lin Yang, Haoyu Yang, Lu Gong, Wenshuai Yang, Hongbo Zeng","doi":"10.1016/j.cej.2024.157824","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157824","url":null,"abstract":"Engineering solar evaporators with Janus structures is crucial for facilitating water transition and heat localization to enhance water evaporation efficiency. However, the fragile discontinuous bilayer structures and unavoidable surface fouling significantly hinder their application. Herein, inspired by the Janus structure of Black Amanita mushrooms, we designed a robust solar evaporator with an integrated wood-like and Janus structure using directional freeze-casting and magnetically induced self-assembly of polypyrrole-coated Fe<sub>3</sub>O<sub>4</sub> particles as a build-in photothermal top layer within a hydrophilic matrix, followed by covering it with an additional hydrophobic fluorine layer to simultaneously regulate surface wettability and antifouling properties. Incorporating the hydrophobic fluorine layer onto the solar evaporator not only enhances its water evaporation efficiency via thermal localization effects, but also prevents fouling, salt, and dust scaling accumulation on its surface, facilitating water transportation, thus achieving a groundbreaking performance with the evaporation rate of 2.13 kg m<sup>−2</sup>h<sup>−1</sup> under one sun irradiation. Moreover, the mechanical performance of the as-prepared solar evaporator can be further optimized by precisely modulating supramolecular interactions within its structure, achieving Young’s modulus over 4 MPa and maintaining structural integrity after the peel-off tests. The fabricated solar evaporator enables highly efficient water purification from artificial seawater, oil-in-water emulsions, and industrial wastewater, providing a rational strategy for designing high-yield solar evaporation systems for wastewater containing complex contaminants","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":"142670934","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.2024.157796
Xinling Yang, Zhou Chen, Jingjing Tan, Yuanna Zhang, Jinglei Cui, Changzhen Wang, Li Fang, Yulei Zhu, Long Huang, Hu Shi, Yongzhao Wang
Identifying the active sites and synergistic catalytic effect for Cu-based catalysts remains challenging due to the evolving structures of Cu0 and Cu+ species during the hydrogenation reaction process. In this study, Cu/t-ZrO2 catalysts prepared by the oxalic acid complex precipitation method were explored for the hydrogenation of furfural to understand the catalytic functions of Cu0 and Cu+ during the reaction. The catalyst calcined at 300°C (Cu/t-ZrO2-300) exhibited a superior catalytic efficiency in furfural hydrogenation to furfuryl alcohol. A 100 % yield of furfuryl alcohol together with a high TOF of 24.2 h−1 was achieved at 120°C. Extensive characterization, including in-situ FTIR, in-situ XPS, EPR, and Raman, substantiated that the excellent catalytic performance of the catalysts was assigned to the synergistic catalysis Cu+, Cu0 and oxygen vacancies. Among them, Cu+ and oxygen vacancies in the catalyst were favorable to the adsorption and activation of the carbonyl group, where sites were more preferred to adsorb CO and formed a stable complex compared to Cu0 active sites. Furthermore, the DFT calculations verified that these abundant oxygen vacancies in the Cu-ZrO2 interface induced a reverse of charge transfer from Zr to Cu atoms in the catalyst, resulting in a downshift of the d-band center for Cu, which was beneficial to the adsorption and activation of furfural and the desorption of active H*. Meanwhile, the results corroborated that more oxygen vacancies in the catalyst can regulate the adsorption configuration of furfural on the catalyst surface. This study elucidated the catalytic mechanism of complex active sites in Cu-based catalysts for furfural hydrogenation, and which will offer a valuable reference for the design of efficient catalysts for biomass platform conversion.
由于在氢化反应过程中 Cu0 和 Cu+ 物种的结构不断变化，因此确定 Cu 基催化剂的活性位点和协同催化效应仍具有挑战性。本研究探讨了草酸络合沉淀法制备的 Cu/t-ZrO2 催化剂在糠醛加氢反应中的应用，以了解 Cu0 和 Cu+ 在反应过程中的催化功能。在 300°C 煅烧的催化剂（Cu/t-ZrO2-300）在糠醛氢化成糠醇的过程中表现出卓越的催化效率。在 120°C 时，糠醇的产率达到 100%，TOF 达到 24.2 h-1。包括原位傅立叶变换红外光谱、原位 XPS、EPR 和拉曼光谱在内的广泛表征证实，催化剂的优异催化性能归功于 Cu+、Cu0 和氧空位的协同催化作用。其中，催化剂中的 Cu+ 和氧空位有利于羰基的吸附和活化，与 Cu0 活性位点相比，Cu+ 和氧空位更有利于吸附 CO 并形成稳定的复合物。此外，DFT 计算还验证了 Cu-ZrO2 界面中这些丰富的氧空位诱导了催化剂中电荷从 Zr 原子向 Cu 原子的反向转移，导致 Cu 的 d 带中心下移，有利于糠醛的吸附和活化以及活性 H* 的解吸。同时，研究结果也证实了催化剂中更多的氧空位可以调节糠醛在催化剂表面的吸附构型。该研究阐明了铜基催化剂中复杂活性位点对糠醛加氢的催化机理，为设计高效的生物质平台转化催化剂提供了宝贵的参考。
{"title":"Understanding the synergistic catalysis of balanced Cu0-Cu+ sites and oxygen vacancies in Cu/ZrO2 catalysts for the efficient hydrogenation of furfural","authors":"Xinling Yang, Zhou Chen, Jingjing Tan, Yuanna Zhang, Jinglei Cui, Changzhen Wang, Li Fang, Yulei Zhu, Long Huang, Hu Shi, Yongzhao Wang","doi":"10.1016/j.cej.2024.157796","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157796","url":null,"abstract":"Identifying the active sites and synergistic catalytic effect for Cu-based catalysts remains challenging due to the evolving structures of Cu<sup>0</sup> and Cu<sup>+</sup> species during the hydrogenation reaction process. In this study, Cu/t-ZrO<sub>2</sub> catalysts prepared by the oxalic acid complex precipitation method were explored for the hydrogenation of furfural to understand the catalytic functions of Cu<sup>0</sup> and Cu<sup>+</sup> during the reaction. The catalyst calcined at 300°C (Cu/t-ZrO<sub>2</sub>-300) exhibited a superior catalytic efficiency in furfural hydrogenation to furfuryl alcohol. A 100 % yield of furfuryl alcohol together with a high TOF of 24.2 h<sup>−1</sup> was achieved at 120°C. Extensive characterization, including <em>in-situ</em> FTIR, <em>in-situ</em> XPS, EPR, and Raman, substantiated that the excellent catalytic performance of the catalysts was assigned to the synergistic catalysis Cu<sup>+</sup>, Cu<sup>0</sup> and oxygen vacancies. Among them, Cu<sup>+</sup> and oxygen vacancies in the catalyst were favorable to the adsorption and activation of the carbonyl group, where sites were more preferred to adsorb CO and formed a stable complex compared to Cu<sup>0</sup> active sites. Furthermore, the DFT calculations verified that these abundant oxygen vacancies in the Cu-ZrO<sub>2</sub> interface induced a reverse of charge transfer from Zr to Cu atoms in the catalyst, resulting in a downshift of the <em>d</em>-band center for Cu, which was beneficial to the adsorption and activation of furfural and the desorption of active H*. Meanwhile, the results corroborated that more oxygen vacancies in the catalyst can regulate the adsorption configuration of furfural on the catalyst surface. This study elucidated the catalytic mechanism of complex active sites in Cu-based catalysts for furfural hydrogenation, and which will offer a valuable reference for the design of efficient catalysts for biomass platform conversion.","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":"142670800","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}
In this work, inspired by the biological structure of shellfish, a bio-based bilayer smart packaging film was developed for real-time visual monitoring of meat freshness. Specifically, the bilayer smart packaging film consisted of a protective outer layer and a functional inner layer. The protective outer layer had a shell-like “brick and mortar” microstructure, consisting of a hard substance (mica powder) and a bio-based soft substance (polylactic acid), which provided the film with improved water resistance and gas barrier properties (WVP = 5.38–6.05 g·m−1·s−1·Pa−1). The functional inner layer consisted of a composite polysaccharide matrix (guar gum, sodium alginate and carboxylated cellulose nanofibers) and three natural indicators (black rice extract, curcumin and their composite indicator), which provided the film with enhanced light barrier property (T600: from 61.6 to 4.0 %), antioxidant capacity and pH-responsive property. Notably, this bilayer smart packaging film prepared by the shellfish bionic strategy demonstrated universal applicability of freshness monitoring for three typical meats (chicken, pork and shrimp). In brief, this work provides promising and feasible results based on an aquatic organism biomimetic strategy for the preparation of sustainable and high-performance bio-based smart packaging materials, which has potential applications in the field of food quality maintenance and food safety monitoring.
{"title":"Engineering a shellfish-inspired bio-based double-layered smart packaging material with enhanced water resistance and barrier performance for universally applicable meat freshness monitoring","authors":"Zitian Liu, Qiying Wang, Ligang Lin, Qingrun Liu, Wensong Ma, Qi Cheng, Jing Yang, Fengling Tang, Meina Xu, Xu Yang, Huiyang Shang, Hao Wu","doi":"10.1016/j.cej.2024.157808","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157808","url":null,"abstract":"In this work, inspired by the biological structure of shellfish, a bio-based bilayer smart packaging film was developed for real-time visual monitoring of meat freshness. Specifically, the bilayer smart packaging film consisted of a protective outer layer and a functional inner layer. The protective outer layer had a shell-like “brick and mortar” microstructure, consisting of a hard substance (mica powder) and a bio-based soft substance (polylactic acid), which provided the film with improved water resistance and gas barrier properties (WVP = 5.38–6.05 g·m<sup>−1</sup>·s<sup>−1</sup>·Pa<sup>−1</sup>). The functional inner layer consisted of a composite polysaccharide matrix (guar gum, sodium alginate and carboxylated cellulose nanofibers) and three natural indicators (black rice extract, curcumin and their composite indicator), which provided the film with enhanced light barrier property (T<sub>600</sub>: from 61.6 to 4.0 %), antioxidant capacity and pH-responsive property. Notably, this bilayer smart packaging film prepared by the shellfish bionic strategy demonstrated universal applicability of freshness monitoring for three typical meats (chicken, pork and shrimp). In brief, this work provides promising and feasible results based on an aquatic organism biomimetic strategy for the preparation of sustainable and high-performance bio-based smart packaging materials, which has potential applications in the field of food quality maintenance and food safety monitoring.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"69 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671084","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.2024.157815
Fanlong Kong, Deliang Chen, Tianyu Zhai, Wenpeng Wang, Guoxian Yang, Yile Dai, Yuqian Cui, Boyang Wei, Sen Wang
Acetamiprid (Ace) and cadmium (Cd) in paddy fields had caused serious impact on natural ecosystems and human health. In this study, Fe-Mn-BC ternary micro-electrolysis filler was successfully prepared and used to remove Ace and Cd in situ in paddy fields via constructing “Fe-Mn-BC micro-electrolysis-microorganism” system. The adsorption capacity of Fe-Mn-BC on Cd and Ace were 62.92 mg/g and 236.18 mg/kg, which were twice and six times than those of zeolites, respectively. In the laboratory simulated experiments, the removal efficiencies of Ace and Cd in CW with Fe-Mn-BC were around 85.0 %. The Ace was decomposed into macromolecular substances by electron transfer in the anodic oxidation process by Fe-Mn-BC and then degraded to water and carbon dioxide by microorganism, while Cd was mainly removed through adsorption of filler and microorganism and the coprecipitation with OH– form cathode and Fen+ from anode to form CdXFe(1-X)(OH)2. The introduce of Fe-Mn-BC promoted the production of microbial extracellular polymeric substances (mainly protein), favorable for Cd and Ace adsorption. Metagenomic sequencing results showed that the Fe-Mn-BC enriched the microorganism related to Ace degradation such as Streptomyces, Nonomuraea, Pseudonocardia, and Nocardia, and enhanced the relative abundances of Cd resistance genes (ABC.CD.P, ABC-2.A and ABC-2.P), and the Ace degradation genes (mcp, pht5, etbAa, TENA_E, and ylmB), promoting the removal of Ace and Cd. This study proposed a multi-functional and easy-operated way for the removal of Ace and Cd from soil and water in paddy fields.
稻田中的啶虫脒（Ace）和镉（Cd）对自然生态系统和人类健康造成了严重影响。本研究成功制备了Fe-Mn-BC三元微电解填料，并通过构建 "Fe-Mn-BC微电解-微生物 "系统，用于原位去除水稻田中的啶虫脒（Ace）和镉（Cd）。Fe-Mn-BC对镉和Ace的吸附量分别为62.92 mg/g和236.18 mg/kg，分别是沸石的2倍和6倍。在实验室模拟实验中，Fe-Mn-BC 对 CW 中 Ace 和 Cd 的去除率约为 85.0%。Ace在Fe-Mn-BC的阳极氧化过程中通过电子传递分解成大分子物质，然后被微生物降解为水和二氧化碳；而Cd主要通过填料和微生物的吸附以及与阴极的OH-和阳极的Fen+共沉淀形成CdXFe(1-X)(OH)2而被去除。Fe-Mn-BC的引入促进了微生物胞外聚合物物质（主要是蛋白质）的产生，有利于Cd和Ace的吸附。元基因组测序结果表明，Fe-Mn-BC富集了链霉菌、野村菌、假丝酵母菌和诺卡氏菌等与Ace降解相关的微生物，提高了抗镉基因（ABC.CD.P、ABC-2.A和ABC-2.P）和Ace降解基因（mcp、pht5、etbAa、TENA_E和ylmB）的相对丰度，促进了Ace和镉的去除。本研究提出了一种多功能、易操作的去除稻田土壤和水中的 Ace 和 Cd 的方法。
{"title":"Enhanced simultaneous removal of acetamiprid and cadmium from soil and water in paddy fields by Fe-Mn-BC ternary micro-electrolysis: Performance, mechanism and pathway","authors":"Fanlong Kong, Deliang Chen, Tianyu Zhai, Wenpeng Wang, Guoxian Yang, Yile Dai, Yuqian Cui, Boyang Wei, Sen Wang","doi":"10.1016/j.cej.2024.157815","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157815","url":null,"abstract":"Acetamiprid (Ace) and cadmium (Cd) in paddy fields had caused serious impact on natural ecosystems and human health. In this study, Fe-Mn-BC ternary micro-electrolysis filler was successfully prepared and used to remove Ace and Cd in situ in paddy fields via constructing “Fe-Mn-BC micro-electrolysis-microorganism” system. The adsorption capacity of Fe-Mn-BC on Cd and Ace were 62.92 mg/g and 236.18 mg/kg, which were twice and six times than those of zeolites, respectively. In the laboratory simulated experiments, the removal efficiencies of Ace and Cd in CW with Fe-Mn-BC were around 85.0 %. The Ace was decomposed into macromolecular substances by electron transfer in the anodic oxidation process by Fe-Mn-BC and then degraded to water and carbon dioxide by microorganism, while Cd was mainly removed through adsorption of filler and microorganism and the coprecipitation with OH<sup>–</sup> form cathode and Fe<sup>n+</sup> from anode to form Cd<sub>X</sub>Fe<sub>(1-X)</sub>(OH)<sub>2</sub>. The introduce of Fe-Mn-BC promoted the production of microbial extracellular polymeric substances (mainly protein), favorable for Cd and Ace adsorption. Metagenomic sequencing results showed that the Fe-Mn-BC enriched the microorganism related to Ace degradation such as <em>Streptomyces</em>, <em>Nonomuraea</em>, <em>Pseudonocardia</em>, and <em>Nocardia</em>, and enhanced the relative abundances of Cd resistance genes (<span><span><em>ABC.CD</em></span><svg aria-label=\"Opens in new window\" focusable=\"false\" height=\"20\" viewbox=\"0 0 8 8\"><path d=\"M1.12949 2.1072V1H7V6.85795H5.89111V2.90281L0.784057 8L0 7.21635L5.11902 2.1072H1.12949Z\"></path></svg></span><em>.P, ABC-2.A</em> and <em>ABC-2.P</em>), and the Ace degradation genes (<em>mcp, pht5, etbAa, TENA_E</em>, and <em>ylmB</em>), promoting the removal of Ace and Cd. This study proposed a multi-functional and easy-operated way for the removal of Ace and Cd from soil and water in paddy fields.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"35 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670748","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}
Based on Vacuum UV (VUV) in situ cracking water to generate reactive oxygen species (ROS) and promote Fe2+/Fe3+ redox cycle, a novel oxidant-free VUV/Fe2+/oxalate (Ox) homogeneous oxidation process was built to efficiently degrade norfloxacin (NOR). The performance and synergistic mechanism of VUV/Fe2+/Ox for NOR degradation under near-neutral conditions were investigated. Compared with sub-processes, VUV/Fe2+/Ox obviously accelerated NOR oxidation and reduced energy consumption, and its synergistic factor of NOR removal was 2.32. Effects of operating parameters Fe2+, Ox dose and solution pH on VUV/Fe2+/Ox and their mechanisms were analyzed. Synergistic mechanisms of NOR degradation via VUV/Fe2+/Ox, such as in situ generation of H2O2, Fe2+/Fe3+ redox cycle, ROS characterization and contribution analysis, NOR degradation pathways and its toxicity changes were also investigated. Through the use of ROS fluorescence characterizations and quenching experiments, hydroxyl radical and superoxide radical were identified as primary ROS in VUV/Fe2+/Ox, and their contributions to NOR degradation were 73.17 % and 20.91 %, respectively. Besides, synergistic mechanisms of VUV/Fe2+/Ox process, which mainly included the respective roles of VUV irradiation, Fe2+ and Ox, were also recommended. Furthermore, effects of chelators and water matrices on NOR degradation via VUV/Fe2+/Ox were also researched. VUV/Fe2+/Ox process showed satisfactory NOR degradation effects in actual waters, indicating its practical application potential. The degradation of NOR by novel VUV/Fe2+/Ox process significantly reduced its environmental and health hazards.
基于真空紫外（VUV）原位裂解水产生活性氧（ROS）并促进 Fe2+/Fe3+ 氧化还原循环的原理，建立了一种新型的无氧化剂 VUV/Fe2+/草酸盐（Ox）均相氧化工艺，用于高效降解诺氟沙星（NOR）。研究了紫外/Fe2+/Ox 在近中性条件下降解 NOR 的性能和协同机制。与其他子过程相比，紫外/Fe2+/Ox明显加速了NOR的氧化，降低了能耗，其去除NOR的协同系数为2.32。分析了操作参数 Fe2+、Ox 剂量和溶液 pH 对紫外/Fe2+/Ox 的影响及其机理。此外，还研究了紫外/Fe2+/Ox 降解 NOR 的协同机制，如原位生成 H2O2、Fe2+/Fe3+ 氧化还原循环、ROS 特征和贡献分析、NOR 降解途径及其毒性变化。通过 ROS 荧光表征和淬灭实验，确定羟自由基和超氧自由基是紫外/Fe2+/Ox 中的主要 ROS，它们对 NOR 降解的贡献率分别为 73.17 % 和 20.91 %。此外，还提出了紫外/Fe2+/Ox 过程的协同机制，主要包括紫外辐照、Fe2+ 和 Ox 各自的作用。此外，还研究了螯合剂和水基质对紫外/Fe2+/Ox 降解 NOR 的影响。紫外/Fe2+/Ox 工艺在实际水体中显示出令人满意的 NOR 降解效果，表明其具有实际应用潜力。新型紫外/Fe2+/氧化工艺对 NOR 的降解大大降低了其对环境和健康的危害。
{"title":"Novel oxidant-free VUV/Fe2+/oxalate process for high-efficiency removal of norfloxacin: Oxidation performance and synergistic mechanism","authors":"Chuang Wang, Xiaohui Wang, Jinying Du, Renjian Deng, Bozhi Ren, Wenhao Wang, Baolin Hou, Bingzhi Liu, Zhiwei Zhao","doi":"10.1016/j.cej.2024.157779","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157779","url":null,"abstract":"Based on Vacuum UV (VUV) in situ cracking water to generate reactive oxygen species (ROS) and promote Fe<sup>2+</sup>/Fe<sup>3+</sup> redox cycle, a novel oxidant-free VUV/Fe<sup>2+</sup>/oxalate (Ox) homogeneous oxidation process was built to efficiently degrade norfloxacin (NOR). The performance and synergistic mechanism of VUV/Fe<sup>2+</sup>/Ox for NOR degradation under near-neutral conditions were investigated. Compared with sub-processes, VUV/Fe<sup>2+</sup>/Ox obviously accelerated NOR oxidation and reduced energy consumption, and its synergistic factor of NOR removal was 2.32. Effects of operating parameters Fe<sup>2+</sup>, Ox dose and solution pH on VUV/Fe<sup>2+</sup>/Ox and their mechanisms were analyzed. Synergistic mechanisms of NOR degradation via VUV/Fe<sup>2+</sup>/Ox, such as in situ generation of H<sub>2</sub>O<sub>2</sub>, Fe<sup>2+</sup>/Fe<sup>3+</sup> redox cycle, ROS characterization and contribution analysis, NOR degradation pathways and its toxicity changes were also investigated. Through the use of ROS fluorescence characterizations and quenching experiments, hydroxyl radical and superoxide radical were identified as primary ROS in VUV/Fe<sup>2+</sup>/Ox, and their contributions to NOR degradation were 73.17 % and 20.91 %, respectively. Besides, synergistic mechanisms of VUV/Fe<sup>2+</sup>/Ox process, which mainly included the respective roles of VUV irradiation, Fe<sup>2+</sup> and Ox, were also recommended. Furthermore, effects of chelators and water matrices on NOR degradation via VUV/Fe<sup>2+</sup>/Ox were also researched. VUV/Fe<sup>2+</sup>/Ox process showed satisfactory NOR degradation effects in actual waters, indicating its practical application potential. The degradation of NOR by novel VUV/Fe<sup>2+</sup>/Ox process significantly reduced its environmental and health hazards.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"174 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670847","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.2024.157769
Huazeng Yang, Rui Zhang, Zhiyuan Liu, Xin Xu, Yishuo Teng, Ming Hou, Guangshuai Zhang, Yongzhao Hou, Guangwu Wen, Dong Wang
Developing carbonaceous materials with low cost and high chloride ions capture ability is highly desired but great challenging for the practical application of capacitive deionization (CDI). Herein, we use cheap petroleum coke as precursors to synthesize N-doped activated porous carbon (N-a4pC), which exhibited excellent Cl- capture capability. The N-a4pC electrode possesses a larger capacitance and more pronounced pseudocapacitive characteristics. We then assemble N-a4pC//activated carbon (AC) cell with N-a4pC as the anode and AC as the cathode, and the N-a4pC(Cl-)//AC(Na+) cell demonstrated high desalination capability of 38.1 mg g−1, which is significantly higher than the desalination capability of the AC(Cl-)//AC(Na+) and AC(Cl-)//N-a4pC(Na+) cells. Density functional theory (DFT) calculations show that N-containing graphene structures have a greater adsorption energy for Cl-, and the differential charge density maps indicate that N facilitate the accumulation of weak positive charges. Moreover, CDI cell as desalted batteries to light one light-emitting diode (LED) shows a continuous and stable discharge process. The desorption voltage of the N-a4pC(Cl-)//AC(Na+) cell is influenced by the adsorption voltage and the concentration of the NaCl. Meanwhile, the desorption voltage increases proportionally with the number of cells, demonstrating the stability as a desalting battery. This work demonstrates the significant potential of industrial waste in the development of low cost carbon electrodes, reveals the mechanism behind the enhanced Cl- capture capability due to N-doping and pore structure optimization, and systematically showcases the desalting battery performance using a CDI cell during the desorption process.
开发具有低成本和高氯离子捕获能力的碳质材料是电容式去离子（CDI）实际应用中的一大挑战。在此，我们以廉价的石油焦为前驱体，合成了掺杂 N 的活性多孔碳（N-a4pC），该材料具有优异的氯离子捕获能力。N-a4pC 电极具有更大的电容和更明显的伪电容特性。以 N-a4pC 为阳极、AC 为阴极组装成 N-a4pC// 活性炭（AC）电池，N-a4pC（Cl-）//AC（Na+）电池的脱盐能力高达 38.1 mg g-1，明显高于 AC（Cl-）//AC（Na+）和 AC（Cl-）//N-a4pC（Na+）电池的脱盐能力。密度泛函理论（DFT）计算表明，含 N 的石墨烯结构对 Cl- 有更大的吸附能，而差分电荷密度图表明 N 有助于弱正电荷的积累。此外，CDI 电池作为脱盐电池点亮一个发光二极管（LED）的过程显示出连续稳定的放电过程。N-a4pC(Cl-)//AC(Na+) 电池的解吸电压受吸附电压和 NaCl 浓度的影响。同时，解吸电压随着电池数量的增加而成正比增加，这证明了其作为脱盐电池的稳定性。这项研究证明了工业废料在开发低成本碳电极方面的巨大潜力，揭示了由于 N 掺杂和孔隙结构优化而增强 Cl- 捕获能力的机制，并系统地展示了在解吸过程中使用 CDI 电池的脱盐电池性能。
{"title":"Unraveling the chloride ion capture capability of nitrogen-doped porous carbon for capacitive deionization and desalination battery","authors":"Huazeng Yang, Rui Zhang, Zhiyuan Liu, Xin Xu, Yishuo Teng, Ming Hou, Guangshuai Zhang, Yongzhao Hou, Guangwu Wen, Dong Wang","doi":"10.1016/j.cej.2024.157769","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157769","url":null,"abstract":"Developing carbonaceous materials with low cost and high chloride ions capture ability is highly desired but great challenging for the practical application of capacitive deionization (CDI). Herein, we use cheap petroleum coke as precursors to synthesize N-doped activated porous carbon (N-a<sub>4</sub>pC), which exhibited excellent Cl<sup>-</sup> capture capability. The N-a<sub>4</sub>pC electrode possesses a larger capacitance and more pronounced pseudocapacitive characteristics. We then assemble N-a<sub>4</sub>pC//activated carbon (AC) cell with N-a<sub>4</sub>pC as the anode and AC as the cathode, and the N-a<sub>4</sub>pC(Cl<sup>-</sup>)//AC(Na<sup>+</sup>) cell demonstrated high desalination capability of 38.1 mg g<sup>−1</sup>, which is significantly higher than the desalination capability of the AC(Cl<sup>-</sup>)//AC(Na<sup>+</sup>) and AC(Cl<sup>-</sup>)//N-a<sub>4</sub>pC(Na<sup>+</sup>) cells. Density functional theory (DFT) calculations show that N-containing graphene structures have a greater adsorption energy for Cl<sup>-</sup>, and the differential charge density maps indicate that N facilitate the accumulation of weak positive charges. Moreover, CDI cell as desalted batteries to light one light-emitting diode (LED) shows a continuous and stable discharge process. The desorption voltage of the N-a<sub>4</sub>pC(Cl<sup>-</sup>)//AC(Na<sup>+</sup>) cell is influenced by the adsorption voltage and the concentration of the NaCl. Meanwhile, the desorption voltage increases proportionally with the number of cells, demonstrating the stability as a desalting battery. This work demonstrates the significant potential of industrial waste in the development of low cost carbon electrodes, reveals the mechanism behind the enhanced Cl<sup>-</sup> capture capability due to N-doping and pore structure optimization, and systematically showcases the desalting battery performance using a CDI cell during the desorption process.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"35 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670755","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}
Autologous tumor cells hold great promise as personalized therapeutic vaccines. Nevertheless, the metabolic competition between tumor cells and the functional immune cells limits patient responses to autologous vaccine via fostering immunosuppressive microenvironment and facilitating immune escape. Herein, the STING-activating Photo-vaccination Inducer (BMA) is developed which can shift in immunological state from “cold” to “hot” by tumor metabolic reprogramming and the release of autologous tumor vaccines. BMA can form into peroxidase mimics in situ upon external energy stimulation, enabling continuous production of reactive oxygen species (ROS) through photodynamic effects and photosensitizer recycling. Tumor metabolic reprogramming with continually ROS generation facilitates maturation of dendritic cells (DCs) and reeducation of tumor immune landscape due to spatiotemporally cascading mitochondrial and nucleus dysfunction, leading to in situ nucleic acid vaccine release and stimulator of the interferon genes (STING) pathway activation. As anticipated, results from Cytometry by Time-Of-Flight (CyTOF) results indicate that the tumor landscape has been altered, effectively eradicating primary tumors and inducing beneficial “Abscopal Effects” that counteract checkpoint blockade (ICB) resistance. Our work for the first time leverages a universal and novel strategy of free radical therapy and personalized therapeutic vaccine for tumor immunoscape re-education thereby enhancing αPD-L1 blockade, presenting a rational way to surmount immunotherapy barriers to available clinical treatments.
{"title":"Six birds with one stone: STING-activating photo-vaccination with glutamine metabolism reprogramming and cascade mitochondrial dysfunction for robust immune landscape remodeling","authors":"Luyao Tian, Xia Li, Lanping Guo, Luqi Huang, Wenyuan Gao","doi":"10.1016/j.cej.2024.157744","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157744","url":null,"abstract":"Autologous tumor cells hold great promise as personalized therapeutic vaccines. Nevertheless, the metabolic competition between tumor cells and the functional immune cells limits patient responses to autologous vaccine via fostering immunosuppressive microenvironment and facilitating immune escape. Herein, the STING-activating Photo-vaccination Inducer (BMA) is developed which can shift in immunological state from “cold” to “hot” by tumor metabolic reprogramming and the release of autologous tumor vaccines. BMA can form into peroxidase mimics <em>in situ</em> upon external energy stimulation,<!-- --> <!-- -->enabling continuous production of reactive oxygen species (ROS) through photodynamic effects and photosensitizer recycling. Tumor metabolic reprogramming with continually ROS generation facilitates maturation of dendritic cells (DCs) and reeducation of tumor immune landscape<!-- --> <!-- -->due to<!-- --> <!-- -->spatiotemporally<!-- --> <!-- -->cascading mitochondrial and nucleus dysfunction, leading to <em>in situ</em> nucleic acid vaccine release and stimulator of the interferon genes (STING) pathway activation. As anticipated, results from Cytometry by Time-Of-Flight (CyTOF) results indicate that the tumor landscape has been altered, effectively eradicating primary tumors and inducing beneficial “Abscopal Effects” that counteract checkpoint blockade (ICB) resistance. Our work for the first time leverages a universal and novel strategy of free radical therapy and personalized therapeutic vaccine for tumor immunoscape re-education thereby enhancing αPD-L1 blockade, presenting a rational way to surmount immunotherapy barriers to available clinical treatments.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"67 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670799","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 reduction of fossil fuel resources and the ongoing surge in global energy demand have captured the interest of researchers worldwide, prompting a focus on developing renewable energy sources. For this reason, biomass conversion has emerged as a crucial pathway for renewable fuel production. Lignin, constituting 10–35% of woody biomass, represents a significant and largely untapped sustainable feedstock. Despite the potential of lignin, a substantial portion of this lignocellulosic residue remains unused, with approximately 60% considered waste. This study addresses the challenge of underutilized lignin by introducing an innovative approach to its hydrogenolysis. Despite their potential, existing hydrogenolysis methods face obstacles such as complexity, high cost, and the need for high temperatures or pressures. Herein we report a noncatalytic nonthermal hydrogen plasma method for lignin hydrogenolysis, conducted under ambient temperature and pressure conditions. Our method proves to be highly effective in breaking lignin bonds, achieving complete conversion, and generating valuable gaseous and bio-oil products including methane and aromatic dimers and monomers obtained from guaiacyl and syringyl units within the lignin structure. Our results showed an increase in gaseous products, especially methane, and aromatic monomer yields, as well as a reduction in total bio-oil and biochar yields and lignin functional groups by increasing reaction time, input power, and H2 partial pressure. This research confirms the considerable promise of utilizing noncatalytic nonthermal hydrogen plasma-assisted hydrogenolysis as an effective technique for producing gaseous and liquid fuels from lignin.
{"title":"Nonthermal hydrogen plasma-enabled ambient, fast lignin hydrogenolysis to valuable chemicals and bio-oils","authors":"Parsa Pishva, Jialu Li, Rongxuan Xie, Jinyao Tang, Prangan Nandy, Tanvir Farouk, Jinghua Guo, Zhenmeng Peng","doi":"10.1016/j.cej.2024.157776","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157776","url":null,"abstract":"The reduction of fossil fuel resources and the ongoing surge in global energy demand have captured the interest of researchers worldwide, prompting a focus on developing renewable energy sources. For this reason, biomass conversion has emerged as a crucial pathway for renewable fuel production. Lignin, constituting 10–35% of woody biomass, represents a significant and largely untapped sustainable feedstock. Despite the potential of lignin, a substantial portion of this lignocellulosic residue remains unused, with approximately 60% considered waste. This study addresses the challenge of underutilized lignin by introducing an innovative approach to its hydrogenolysis. Despite their potential, existing hydrogenolysis methods face obstacles such as complexity, high cost, and the need for high temperatures or pressures. Herein we report a noncatalytic nonthermal hydrogen plasma method for lignin hydrogenolysis, conducted under ambient temperature and pressure conditions. Our method proves to be highly effective in breaking lignin bonds, achieving complete conversion, and generating valuable gaseous and bio-oil products including methane and aromatic dimers and monomers obtained from guaiacyl and syringyl units within the lignin structure. Our results showed an increase in gaseous products, especially methane, and aromatic monomer yields, as well as a reduction in total bio-oil and biochar yields and lignin functional groups by increasing reaction time, input power, and H<sub>2</sub> partial pressure. This research confirms the considerable promise of utilizing noncatalytic nonthermal hydrogen plasma-assisted hydrogenolysis as an effective technique for producing gaseous and liquid fuels from lignin.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"1 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670978","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 widespread application of Lithium-ion Batteries (LIBs) has led to a significant increase in the number of spent LIBs. Consequently, the recycling and utilization of spent LIBs have become an inevitable choice for recovering valuable resources and protecting the environment, aligning with the principles of sustainable development. This study reports an iron air battery recycling system that is capable of recovering both Li/Co and energy from spent LiCoO2 cathode materials and the separation reaction is completely spontaneous. Meanwhile, lithium and cobalt were successfully recovered from the powdered leach solution of spent LiCoO2 cathode material, and it was preliminarily demonstrated that spent iron could be used as a sacrificial anode for the system. Several key parameters affecting recovery are optimized, including anode solution pH, discharge current density, and concentration of the solution to be recovered. Under the conditions of anode solution pH of 1.8, discharge current density of 0.1 mA cm−2, and concentration of recovery solution of 0.15 mol/L, the system can be operated stably for more than 24 h, and the recoveries of Li+ and Co2+ can be up to 1.49 mg h−1 and 18.75 mg h−1 respectively, and the output energy can reach 75.15 kJ/mol. This research not only provides a sustainable and cost-effective method of disposing of used lithium-ion batteries, but also offers up new possibilities for the disposal of scrap iron.
{"title":"Recovery of Li/Co from spent lithium-ion battery through iron-air batteries","authors":"Chuhan Tang, Wei Shan, YiRan Zheng, Liang Zhang, Yuxin Liu, Bin Liao, HeDong Chen, Xianhua Hou","doi":"10.1016/j.cej.2024.157578","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157578","url":null,"abstract":"The widespread application of Lithium-ion Batteries (LIBs) has led to a significant increase in the number of spent LIBs. Consequently, the recycling and utilization of spent LIBs have become an inevitable choice for recovering valuable resources and protecting the environment, aligning with the principles of sustainable development. This study reports an iron air battery recycling system that is capable of recovering both Li/Co and energy from spent LiCoO<sub>2</sub> cathode materials and the separation reaction is completely spontaneous. Meanwhile, lithium and cobalt were successfully recovered from the powdered leach solution of spent LiCoO<sub>2</sub> cathode material, and it was preliminarily demonstrated that spent iron could be used as a sacrificial anode for the system. Several key parameters affecting recovery are optimized, including anode solution pH, discharge current density, and concentration of the solution to be recovered. Under the conditions of anode solution pH of 1.8, discharge current density of 0.1 mA cm<sup>−2</sup>, and concentration of recovery solution of 0.15 mol/L, the system can be operated stably for more than 24 h, and the recoveries of Li<sup>+</sup> and Co<sup>2+</sup> can be up to 1.49 mg h<sup>−1</sup> and 18.75 mg h<sup>−1</sup> respectively, and the output energy can reach 75.15 kJ/mol. This research not only provides a sustainable and cost-effective method of disposing of used lithium-ion batteries, but also offers up new possibilities for the disposal of scrap iron.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"251 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673775","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.2024.157787
Yiqi Fan, Mei Chen, Guoneng Li
As a result of the affinity and inadequate ability to regulate Li+, Li metal tends to accumulate on the surface of substrate materials, which reduces space utilization and promotes dendrite growth. Especially since the flow of Li+ toward the substrate’s bottom can be tricky to control, high mass-loading is a challenge for the traditional framework design. Herein, inspired by a tree root network, a cellulose-based gradient framework was designed for the Li metal anode. Bacterial cellulose-doping carbon-coated zinc oxide (ZnO@C) nanoparticles are used for decorating the top, and ZnO@C nanoparticles placed on Cu foil decorate the bottom. Owing to the gradient conductivity, Li deposition can be directed from the bottom to up to obtain sufficient unoccupied space accommodating volume changes and fully utilize the entire frame to achieve high mass-loading. Moreover, the transportation of Li+ is facilitated by the spontaneous formation of the LiF/Li2CO3/LiOH-enriched SEI layer, which has an exceptional ability to conduct ions. As a result, a 3000 h lifespan with an average coulombic efficiency of 98 % was achieved. Notably, LiFePO4 full cell exhibits excellent cycling stability and high energy density (102 mAh/g) under realistic conditions (negative to positive capacity ratio as 1.75).
{"title":"Multilayered conductive gradient framework for stability high Mass-Loading Lithium metal battery","authors":"Yiqi Fan, Mei Chen, Guoneng Li","doi":"10.1016/j.cej.2024.157787","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157787","url":null,"abstract":"As a result of the affinity and inadequate ability to regulate Li<sup>+</sup>, Li metal tends to accumulate on the surface of substrate materials, which reduces space utilization and promotes dendrite growth. Especially since the flow of Li<sup>+</sup> toward the substrate’s bottom can be tricky to control, high mass-loading is a challenge for the traditional framework design. Herein, inspired by a tree root network, a cellulose-based gradient framework was designed for the Li metal anode. Bacterial cellulose-doping carbon-coated zinc oxide (ZnO@C) nanoparticles are used for decorating the top, and ZnO@C nanoparticles placed on Cu foil decorate the bottom. Owing to the gradient conductivity, Li deposition can be directed from the bottom to up to obtain sufficient unoccupied space accommodating volume changes and fully utilize the entire frame to achieve high mass-loading. Moreover, the transportation of Li<sup>+</sup> is facilitated by the spontaneous formation of the LiF/Li<sub>2</sub>CO<sub>3</sub>/LiOH-enriched SEI layer, which has an exceptional ability to conduct ions. As a result, a 3000 h lifespan with an average coulombic efficiency of 98 % was achieved. Notably, LiFePO<sub>4</sub> full cell exhibits excellent cycling stability and high energy density (102 mAh/g) under realistic conditions (negative to positive capacity ratio as 1.75).","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"13 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670936","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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