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Efficient capture of gaseous, aqueous iodine, near-sunlight white light emission and iodine sensing in 12-connected and [Pb6]-cluster based MOFs
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158782
Ya-Nan Yu, Wei-Min Ma, Jia-Xin Wu, Qian Zhang, Jie Zhou, Ke-Ke Jiang, Dan-Dan Wang, Yong-Kang Li, Yang-Min Ma, Zheng Yin
{"title":"Efficient capture of gaseous, aqueous iodine, near-sunlight white light emission and iodine sensing in 12-connected and [Pb6]-cluster based MOFs","authors":"Ya-Nan Yu, Wei-Min Ma, Jia-Xin Wu, Qian Zhang, Jie Zhou, Ke-Ke Jiang, Dan-Dan Wang, Yong-Kang Li, Yang-Min Ma, Zheng Yin","doi":"10.1016/j.cej.2024.158782","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158782","url":null,"abstract":"The radioactive iodine as highly harmful fission waste from nuclear power production features fifteen-million years radiation period and easy diffusion, yet its efficient treatment and sensing is greatly challenged by the operation concentration as low as several ppm in gaseous and aqueous medium. A (3,12)-connected and [Pb<sub>6</sub>(<em>µ</em><sub>4</sub>-O)<sub>2</sub>(COO)<sub>8</sub>] based MOFs of [Pb<sub>6</sub>(<em>μ</em><sub>4</sub>-O)<sub>2</sub>(pia)<sub>4</sub>]·4DMF (<strong>1</strong>) was rationally constructed as a multifunctional materials for iodine capture and sensing, which possesses the highest void fraction of 34.4 % among all known cluster based Pb-MOFs. Microwave-assistant solvothermal reaction facilitates gram-scale synthesis of <strong>1</strong> with yield of 82 % within 4 h. The 1D round channels sized at 1.0 nm coupled with high structure stability of the MOFs contribute to accommodate iodine. <strong>1</strong> can rapidly capture iodine vapor at 70 °C in 6 h with fully utilized nanopores, resulting in a high iodine packing density of 3.52 g cm<sup>−3</sup> closely matching that of iodine single crystal. Particularly, the MOFs of <strong>1</strong> exhibits long-lasting adsorption to iodine vapor at extremely low concentration of 120 ppm, as well as efficient capture of I<sub>2</sub> in 1.0 × 10<sup>-4</sup> M aqueous solution with removal percentages of 67.1 % in only 20 min, driven by synergistic host–guest interactions. The MOFs is further discovered as a single-phase white-emitting phosphor with quite broad fluorescence spectrum covering the entire visible region, benefited from the multiple Pb···Pb interactions and change-transfer between the metal and ligand. White light emitting diodes can be created by coating commercial blue LEDs with phosphor <strong>1</strong>, generating pure white chromaticity coordinates of (0.313, 0.338), a near daylight color temperature of 6420 K, a high color rendering index of 85 and light maintenance up to 120 °C. The migration of iodine into the channels of <strong>1</strong> led to obvious fluorescence quenching. As the combined result, <strong>1</strong> presents a rare and instructive multifunctional MOFs that exhibiting efficient capture to low-concentration iodine in gaseous/aqueous condition and fluorescent detection to iodine.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"261 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857744","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}
引用次数: 0
Stepwise chemical-electrochemical cycles for decoupling modular biomass oxidation and hydrogen evolution
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158764
Shih-Wei Lin, Song-Chi Chen, Ying-Rui Lu, Chih-Jung Chen
{"title":"Stepwise chemical-electrochemical cycles for decoupling modular biomass oxidation and hydrogen evolution","authors":"Shih-Wei Lin, Song-Chi Chen, Ying-Rui Lu, Chih-Jung Chen","doi":"10.1016/j.cej.2024.158764","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158764","url":null,"abstract":"Electrochemical biomass oxidation offers a sustainable method for producing high-value chemicals using green electricity, along with the coproduction of H<sub>2</sub> fuel through the hydrogen evolution reaction (HER). Typically conducted in alkaline electrolytes to enhance efficiency, this medium actually leads to significant side reactions in biomass molecules, such as the Cannizzaro disproportionation and self-polymerization. Besides, the negative impact of cathode on biomass during HER, which causes substantial carbon loss, has frequently been overlooked. Our study introduced the utilization of redox reservoirs (RRs) to effectively decouple the half-reactions, allowing for their independent operation. Characterized by a highly positive formal potential, the RR spontaneously performed the 5-hydroxymethylfurfural oxidation reaction (HMFOR) in water (without supporting electrolyte) under open circuit conditions. This approach not only eliminated the need for subsequent purification of final products but also significantly avoided side reactions, even with highly concentrated reactants. <em>In-situ</em> X-ray absorption spectroscopy revealed Ni<sup>3+</sup> species within RRs as the active sites for water-based HMFOR, following first-order kinetics. Moreover, the flexibility of RRs was demonstrated by the successful oxidation of furfural, indicating their wide applicability for various organic substrates","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"31 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857817","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}
引用次数: 0
Alkali metal ion-doped GaN for ultrafast electrochemical capacitor: Doping mechanism, structural adjustment, and structure–performance relationship
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158761
Yuzhou Zhu, Kai Zhou, Wanting Liu, Weisheng Fu, Jinlin Zhang, Benkang Chen, Haihui Jiang, Libin Liu, Ligang Gai
{"title":"Alkali metal ion-doped GaN for ultrafast electrochemical capacitor: Doping mechanism, structural adjustment, and structure–performance relationship","authors":"Yuzhou Zhu, Kai Zhou, Wanting Liu, Weisheng Fu, Jinlin Zhang, Benkang Chen, Haihui Jiang, Libin Liu, Ligang Gai","doi":"10.1016/j.cej.2024.158761","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158761","url":null,"abstract":"Microstructure adjustment plays a crucial role in improving the surface reactivity of materials. However, surface reactivity improved by alkali metal doping for electrode materials applied in energy storage is usually overlooked by researchers. Herein, we report on facile synthesis of Li<sup>+</sup>/Na<sup>+</sup>-doped GaN microcrystals and their structure–electrochemical performance relationship. The dosage concentration is optimized, and the doping mechanism is proposed in terms of the metathesis reaction of Li<sub>2</sub>O/Na<sub>2</sub>O with GaN under carbothermal reduction conditions using LiNO<sub>3</sub>/NaNO<sub>3</sub> as the dopants. Both macro- and microstructures of GaN can be tuned through Li<sup>+</sup>/Na<sup>+</sup> doping. In addition to the increased specific surface area and total pore volume, the reduced <em>d</em> band center and band gap caused by Li<sup>+</sup>/Na<sup>+</sup> doping present an anti-<em>d</em> band center phenomenon and contribute to enhanced ion storage and transport, leading to excellent electrochemical performance of the target materials. In addition, symmetric electrochemical capacitors with the target materials can deliver output voltage of 2.4, 1.5, and 1.0 V at –60, 25, and 120 °C by using phosphoric acid–water–dimethyl sulfoxide mixed solution as the electrolyte. The symmetric electrochemical capacitors with Na<sup>+</sup>-doped GaN can deliver specific energy of 45.9 mW h cm<sup>−3</sup> at 344 mW cm<sup>−3</sup> and –60 °C, 36.1 mW h cm<sup>−3</sup> at 215 mW cm<sup>−3</sup> and 25 °C, and 16.7 mW h cm<sup>−3</sup> at 287 mW cm<sup>−3</sup> and 120 °C, respectively, holding considerable promise for practice in all-temperature environment.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"264 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858217","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}
引用次数: 0
Biomimetic robust polymeric interphase facilitating stable Zn metal anode
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158787
Duo Chen, Wentong Shen, Zixuan Dai, Yuanhang Wang, Tengyu Yao, Sikan Wang, Yiming Zhang, Chenglin Miao, Yicheng Tan, Laifa Shen
{"title":"Biomimetic robust polymeric interphase facilitating stable Zn metal anode","authors":"Duo Chen, Wentong Shen, Zixuan Dai, Yuanhang Wang, Tengyu Yao, Sikan Wang, Yiming Zhang, Chenglin Miao, Yicheng Tan, Laifa Shen","doi":"10.1016/j.cej.2024.158787","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158787","url":null,"abstract":"Rampant dendrite growth and hydrogen evolution reaction of Zn anode severely hinder the practical application of aqueous zinc-ion batteries (AZIBs). Traditional surface modifying layers tend to have distinct interface with the Zn plate, which readily results in detachment and failure of the modification under repeated cycling. Herein, inspired by mussel adhesive proteins, a uniform and dense polydopamine (PDA) layer is introduced on Zn surface by a Cu<sup>2+</sup>-assisted minute-level in-situ polymerization method. The robust polymeric interphase can improve the zincophilicity and wettability of Zn surface, reducing the energy barrier for Zn nucleation to facilitate homogenous dendrite-free deposition. Importantly, the PDA layer can promote the desolvation process of hydrated Zn<sup>2+</sup> by abundant –NH<sub>2</sub> and –OH groups, and effectively suppress side reactions associated with H<sub>2</sub>O, such as hydrogen evolution reaction, and Zn corrosion, ensuring the long-term cycling stability of the Zn anode. As a result, the PDA modified Zn anode achieves prolonged cycling stability of 840 h under high deposition capacity of 5 mAh cm<sup>–2</sup> and current density of 5mA cm<sup>–2</sup>. Moreover, the pouch-type cell based on the PDA modified Zn anode delivers impressive reversible lifespan for 500 cycles at 0.5 A g<sup>–1</sup>, demonstrating the potential application prospect for this biomimetic interphase in AZIBs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"11 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857822","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}
引用次数: 0
Supramolecular flame retardants enabled fire-extinguishing polycarbonate with enhanced thermal stability and reduced smoke release
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158762
Qingyao Gao, Menghe Zhu, Jihang Wang, Jianhao Zhu, Xinliang Liu, Chuanxin Xie, Xilei Chen, Lei Liu, Pingan Song
{"title":"Supramolecular flame retardants enabled fire-extinguishing polycarbonate with enhanced thermal stability and reduced smoke release","authors":"Qingyao Gao, Menghe Zhu, Jihang Wang, Jianhao Zhu, Xinliang Liu, Chuanxin Xie, Xilei Chen, Lei Liu, Pingan Song","doi":"10.1016/j.cej.2024.158762","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158762","url":null,"abstract":"The creation of mechanically robust, thermostable, and flame-retardant polycarbonate (PC) is highly desirable in the industry. Unfortunately, achieving such a comprehensive performance portfolio remains challenging due to their different governing mechanisms. Most flame retardants provide satisfactory fire retardancy at the expense of other properties. Herein, we rationally design three novel supramolecular flame retardants (PAPZ@Co, PAPZ@La, PAPZ@Fe) containing phosphorus, nitrogen, and transition metal elements based on ionic and metal–ligand coordination interactions. Benefiting from the π-π stacking and ionic interactions, these supramolecular flame retardants show high thermal stability and good compactivity with PC, thus maintaining the good tensile strength of the matrix. Particularly, PAPZ@Fe enhances the thermal stability of PC by improving the initial degradation temperature by 8 °C and char yields by 36.8 % at 800 °C. The addition of 1.5 wt% PAPZ@Fe enables PC to achieve a desirable UL-94 V0 rating and a high limiting oxygen index of 31.6 %, in combination with a 36.3 % decrease in the peak heat release rate. This work offers a facile strategy for creating high-performance PC for practical application in industry.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"25 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857824","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}
引用次数: 0
Rapid in situ photochemical synthesis of carbon dots in polymer coating by infrared CO2 laser writing for color tunable fluorescent patterning
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158749
Yuanyuan Guo, Yixun Gao, Yao Wang, Yi-Kuen Lee, Patrick J. French, Ahmad M. Umar Siddiqui, Hao Li, Guofu Zhou
{"title":"Rapid in situ photochemical synthesis of carbon dots in polymer coating by infrared CO2 laser writing for color tunable fluorescent patterning","authors":"Yuanyuan Guo, Yixun Gao, Yao Wang, Yi-Kuen Lee, Patrick J. French, Ahmad M. Umar Siddiqui, Hao Li, Guofu Zhou","doi":"10.1016/j.cej.2024.158749","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158749","url":null,"abstract":"The significant <em>in situ</em> multicolored patterning without changing printing tools nor substrate media still remains challenging, especially toward practical applications for anti-counterfeiting. This research invented a unique universal approach for the laser-induced <em>in situ</em> synthesis of colorful fluorescent patterns (from blue: CIE 0.15, 0.18 to red orange: CIE 0.36, 0.39) through the controlled formation of N, S doped carbon dots (CDs) in solid composite polymer films or hydrogel with a hierarchical and physically unclonable microsurface architecture for anti-counterfeiting. The <em>in situ</em> patterning approach, coupled with multi-layer technique, yielding designable blue, yellow, orange, and red orange color under 365 nm in the same pattern. A 5 cm<sup>2</sup> colorful pattern can be efficiently finished within 5 min without changing substrate and the line width accuracy can be up to 300 μm. The absolute quantum efficiency of the blue pattern reached as high as 23 %. The fluorescent patterns can be survived at indoor for 24 months. The hydrogen bonding interactions between the CDs precursor and polymer facilitated the generation, uniform dispersion and stabilization of CDs during the laser irradiation. The hypothesis that laser irradiation induced photochemical reactions of CD precursors within a polymer matrix was supported by thermodynamic assessments. The universality of <em>in situ</em> fluorescent patterning strategy was demonstrated by developing fluorescent patterns on both solid polymer films, hydrogel, pharmaceutical packaging and textile","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"7 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849645","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}
引用次数: 0
Phototunable phosphorescence energy transfer based on photodimerization of coumarin-12-crown-4 accelerated by γ-cyclodextrin
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158772
Hui-Juan Wang, Yan-Tao Li, Ming-Che Shao, Chang-Shuo Yu, Jin-Yao Yang, Lingyang Liu, Suna Wang, Jianmin Dou
{"title":"Phototunable phosphorescence energy transfer based on photodimerization of coumarin-12-crown-4 accelerated by γ-cyclodextrin","authors":"Hui-Juan Wang, Yan-Tao Li, Ming-Che Shao, Chang-Shuo Yu, Jin-Yao Yang, Lingyang Liu, Suna Wang, Jianmin Dou","doi":"10.1016/j.cej.2024.158772","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158772","url":null,"abstract":"Herein, we designed and synthesized water-soluble coumarin-12-crown-4 (<strong>C12C4</strong>) which can be encapsulated by γ-cyclodextrin (γ-CD) with 2:1 ratio forming psuedorotaxane, accompanying the morphology from nanotubes to regular nanosheets with a range of edge lengths (2–10 μm) and a range of thicknesses (200–500 nm). With α-CD, β-CD as references, the encapsulation by γ-CD could promote the photodimerization process of <strong>C12C4</strong> after irradiation with 365 nm light. Meanwhile, the morphology of pseudorotaxane <strong>C12C4</strong>⊂γ-CD changed into a chapped surface. By virtue of this, the pseudorotaxane <strong>C12C4</strong>⊂γ-CD was doped into poly (vinyl alcohol) (PVA) and a phosphorescence emission at 515 nm (τ = 458.80 ms) appeared and showed green afterglow for 3 s. Further doping commercial dye rhodamine B (RhB) into <strong>C12C4</strong>⊂γ-CD@PVA, a highly efficient triplet-to-singlet Förster-resonance energy transfer (TS-FRET) system was obtained with multicolor afterglows. More interestingly, both the phosphorescence of <strong>C12C4</strong>⊂γ-CD@PVA and the delayed fluorescence of <strong>C12C4</strong>⊂γ-CD + RhB@PVA could be tuned by 365 nm light irradiation. Finally, the photo-controlled phosphorescence smart materials were used to constructed INHIBIT logic gate, logic operation of INHIBIT + AND and time resolved anti-counterfeiting.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"23 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857741","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}
引用次数: 0
Interaction mechanisms of coal macerals during pyrolysis: Insights from TG and Py-GC/MS experiments combined with ReaxFF MD simulations
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158768
Yufan Wei, Ying Wu, Zhenyi Du, Xin Zhang, Jun Xu, Kai Xu, Long Jiang, Yi Wang, Sheng Su, Song Hu, Jun Xiang
{"title":"Interaction mechanisms of coal macerals during pyrolysis: Insights from TG and Py-GC/MS experiments combined with ReaxFF MD simulations","authors":"Yufan Wei, Ying Wu, Zhenyi Du, Xin Zhang, Jun Xu, Kai Xu, Long Jiang, Yi Wang, Sheng Su, Song Hu, Jun Xiang","doi":"10.1016/j.cej.2024.158768","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158768","url":null,"abstract":"The mechanisms of interaction among coal macerals during pyrolysis processes remain uncertain. This study investigates the interactions between vitrinite and inertinite in three Chinese coals of varying ranks using Thermogravimetric Analysis (TGA), Pyrolysis–gas chromatography/mass spectrometry (Py-GC/MS), and reactive force field molecular dynamics (ReaxFF MD) simulations. Experimental results show that the interactions between vitrinite and inertinite consistently inhibit volatile matter release and increase pyrolysis activation energy across different coal types and mixing ratios. Furthermore, these interactions reduce the yield of polycyclic aromatic compounds while promoting the formation of light volatiles. ReaxFF MD simulations further reveal that the interactions between vitrinite and inertinite significantly enhance polycondensation reactions. The key mechanism involves larger inertinite molecules possessing numerous and persistent binding sites due to steric hindrance. These molecules can fix substantial amounts of smaller vitrinite fragments, particularly polycyclic aromatic molecules, resulting in reduced aromatic product yields. Further analysis reveals that interaction strength decreases with increasing coal rank. At equivalent coal ranks, the 1:1 mixing ratio exhibits stronger interactions compared to other ratios. Additionally, different mixing ratios demonstrate distinct interaction patterns across various temperature ranges. Subsequently, an interaction strength index and a comprehensive coal property index were developed for quantitative characterization. The results show a good positive correlation between the two indices, establishing that interaction strength is fundamentally governed by both coal rank and structural heterogeneity. This study provides new insights into complex coal pyrolysis mechanisms and offers valuable guidance for optimizing industrial pyrolysis processes.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"71 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857746","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}
引用次数: 0
Atomically dispersed iron & iron clusters synergistically accelerate electrocatalytic ammonia synthesis
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158785
Haoran Zhang, Yuelong Liu, Sanshuang Gao, Haijian Wang, Rui Bai, Yan Zhao, Yingtang Zhou, Guangzhi Hu, Xue Zhao
{"title":"Atomically dispersed iron & iron clusters synergistically accelerate electrocatalytic ammonia synthesis","authors":"Haoran Zhang, Yuelong Liu, Sanshuang Gao, Haijian Wang, Rui Bai, Yan Zhao, Yingtang Zhou, Guangzhi Hu, Xue Zhao","doi":"10.1016/j.cej.2024.158785","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158785","url":null,"abstract":"Green energy-driven electrochemical-nitrate-reduction-reaction (eNitRR) provides an alternative pathway for sustainable ammonia synthesis, but there is still a lack of reliable catalyst. Herein, through the combination of coordination confinement and spatial confinement, single-atom Fe and Fe clusters were simultaneously embedded on nitrogen-doped-hollow-carbon-tubes (Fe/NHCTs) to cooperatively promote the highly selective conversion of nitrate to ammonia in complex water environments. The ammonia yield rate reached 45595.63 μg h<sup>−1</sup> mg<sup>−1</sup> with Faradaic efficiency close to 100 %. The Zn-nitrate battery with Fe/NHCTs as the core has a high open circuit voltage and power density, and can output electric energy for a long time while highly selective synthesis of ammonia. The pathway and hydrogenation mechanism of nitrate evolution to ammonia were revealed using the <em>in-situ</em> attenuated total reflection Fourier-transform infrared, online differential-electrochemical-mass-spectrometry and density functional theory calculations, the intermodulation of electrons between single-atom Fe and Fe clusters synergistically accelerates the conversion of nitrate to ammonia.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"22 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857814","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}
引用次数: 0
Stretchable electroluminescent fibers based on liquid metal compensation strategy
IF 15.1 1区 工程技术
Chemical Engineering Journal Pub Date : 2024-12-19 DOI: 10.1016/j.cej.2024.158783
Zhaosen Yuan, Zhuquan Zhou, Bohao Jin, Nan Li, Zheng Jiang, Minghui Guo, Qian Wang
{"title":"Stretchable electroluminescent fibers based on liquid metal compensation strategy","authors":"Zhaosen Yuan, Zhuquan Zhou, Bohao Jin, Nan Li, Zheng Jiang, Minghui Guo, Qian Wang","doi":"10.1016/j.cej.2024.158783","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158783","url":null,"abstract":"Electroluminescent devices, particularly in fiber form, demand highly transparent and conductive materials as external electrodes to maintain high brightness during stretching. As a result, materials with poor conductivity but good transparency, or good conductivity but poor transparency, are restricted in their applicability. Addressing this challenge, we introduce a compensation strategy for external electrodes designed to compensate for the shortcomings of two conductive materials used in the preparation of stretchable electroluminescent fibers. Specifically, by introducing liquid metal as a compensatory conductive layer into the poly(3,4-ethylenedioxythiophene)–polystyrene sulfonate film on the fiber surface, the maximum brightness of the fiber can be achieved at 125.71 cd·m<sup>−2</sup>. Furthermore, the fiber can be stretched to 253 % of its original length while still maintaining excellent luminescent brightness. After undergoing 100 cycles of stretching and recovery at 200 % of its original length, the brightness of the ACEL fiber exhibited a decrease of less than 5 %. The fiber also exhibits tunable luminescent color characteristics under varying voltages and frequencies, shifting from green to blue. Furthermore, after encapsulation, the fiber can operate underwater for extended periods. This strategy significantly broadens the range of electrode material options, and opens up a new research idea for the application of more conductive materials as electroluminescent fibers in smart textiles and wearable devices.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"52 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857743","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}
引用次数: 0
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