Langmuir最新文献_第3页

Mechanism of High Hydrocarbon-Fuel-Gelation Performance of Ultralow-Concentration Bis-urea-Based Gellants

IF 3.9 2区化学

Langmuir Pub Date : 2025-02-02 DOI: 10.1021/acs.langmuir.4c05128

Yan Xu, Kang Xue, Yi Chen, Chongjun Li, Huaiyu Li, Xiaolei Guo, Ruijie Gao, Chengxiang Shi, Xiangwen Zhang, Ji-Jun Zou, Lun Pan

{"title":"Mechanism of High Hydrocarbon-Fuel-Gelation Performance of Ultralow-Concentration Bis-urea-Based Gellants","authors":"Yan Xu, Kang Xue, Yi Chen, Chongjun Li, Huaiyu Li, Xiaolei Guo, Ruijie Gao, Chengxiang Shi, Xiangwen Zhang, Ji-Jun Zou, Lun Pan","doi":"10.1021/acs.langmuir.4c05128","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c05128","url":null,"abstract":"Bis-urea-based gellants have garnered considerable attention due to their capacity to form all kinds of gels in solvents for multiple applications. Nevertheless, the range of applicable solvents is limited, and the synthesis process is complicated. Herein, we report a one-step synthesis process of bis-urea-based gellants (Bu(n)) for gelling nonpolar organic solvents, including high-energy fuels. Importantly, the critical gelation concentration (CGC) of Bu(n) decreases with the increase of alkyl chain length, and that of Bu18 is lower than 0.1 wt % in various hydrocarbon fuels. The discrepant gelation performance of gellants in solvents was investigated by molecular dynamics simulation and spectral characterizations. The results indicate that the electrostatic interaction between urea groups is vital to constructing a gellant framework, and the wide van der Waals (vdW) surface provided by alkyl groups helps to immobilize solvents. The nonbonding interactions between gellant molecules facilitate the formation of a 3D fibrous network structure, which further accumulates into a cambium layer structure. Due to the excellent gelation performance of gellants in fuels, the gel fuels perform the rheological characteristics of shear thinning and thixotropic recovering with calorific value remaining, thus demonstrating potential for application.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"38 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077097","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Paintable, Scalable, and Durable Zwitterionic Hydrogel Coating for Enhanced Marine Antifouling Applications

IF 3.9 2区化学

Langmuir Pub Date : 2025-02-02 DOI: 10.1021/acs.langmuir.4c04595

Boyi Song, Ershuai Zhang, Yuanjie Shi, Hui Zhu, Wei Wang, Sheu-Jane Gallagher, Zhiqiang Cao

{"title":"A Paintable, Scalable, and Durable Zwitterionic Hydrogel Coating for Enhanced Marine Antifouling Applications","authors":"Boyi Song, Ershuai Zhang, Yuanjie Shi, Hui Zhu, Wei Wang, Sheu-Jane Gallagher, Zhiqiang Cao","doi":"10.1021/acs.langmuir.4c04595","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04595","url":null,"abstract":"Marine biofouling has been a severe challenge since the increase of maritime trade, significantly impacting the efficiency of ships by increasing drag, fuel consumption, hull corrosion, and even problems related to navigational safety and biological invasions. Commercial antifouling coatings have been developed for many years, but a satisfactory solution has yet to be found due to problems, such as high toxicity, environmental pollution, or high costs. Zwitterionic materials, with their superhydrophilic properties, demonstrate excellent resistance to nonspecific adhesion alongside good biocompatibility, making them promising candidates for marine antifouling applications. However, their superhydrophilic nature makes it difficult to anchor onto hydrophobic substrates, limiting their use. In this study, we presented a paintable, scalable, and durable antifouling coating system made by zwitterionic hydrogel (PSDA-Z), which was covalently attached to substrates through an acrylated epoxy resin primer coat and maintained antifouling performance even after 3 months of high-speed water shearing, high-pressure sandpaper abrasion, and sharp scratching. This PSDA-Z could also easily be applied on various substrates without specific treatments, including epoxy resin, poly(vinyl chloride) (PVC), polyurethane (PU), and wood. More importantly, this coating system achieved excellent antifouling performance comparable to self-polishing coatings (SPCs), the current industry standard in marine antifouling coating, in the Atlantic Ocean field tests for 3 months, suggesting its promise as an effective and ecofriendly alternative for marine antifouling applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"23 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077048","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Engineering Protein-Based Lipid-Binding Nanovesicles via Catechol-Amine-Derived Coacervation with Their Underlying Interfacial Mechanisms 通过儿茶酚--氨产生的共凝作用及其潜在的界面机制设计蛋白型脂质结合纳米囊泡

IF 3.9 2区化学

Langmuir Pub Date : 2025-02-02 DOI: 10.1021/acs.langmuir.4c03941

Haibing Yang, Yao Song, Qiang Zhang, Moran Wang, Tianqi Jia, Qing Pan, Kanda Sun, Xiang Guan, Mingfei Pan, Feng Chen, Bin Yan

{"title":"Engineering Protein-Based Lipid-Binding Nanovesicles via Catechol-Amine-Derived Coacervation with Their Underlying Interfacial Mechanisms","authors":"Haibing Yang, Yao Song, Qiang Zhang, Moran Wang, Tianqi Jia, Qing Pan, Kanda Sun, Xiang Guan, Mingfei Pan, Feng Chen, Bin Yan","doi":"10.1021/acs.langmuir.4c03941","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03941","url":null,"abstract":"The development of nonphospholipid nanovesicles has garnered tremendous attention as a viable alternative to traditional liposomal nanovesicles. Protein/peptide-based nanovesicles have demonstrated their potential to reduce immunogenicity while enhancing bioactivity. However, a fundamental understanding of how proteinaceous vesicles interact with lipids and cell membranes remains elusive. In this study, we engineered a series of protamine-based nonphospholipid nanovesicles by modulating intramolecular catechol–amine interactions. By grafting trihydroxybenzene (GA) and catechol (CA) groups onto the protamine (Prot), a salt-triggered coacervation was observed in an alkaline environment with the size of as-prepared vesicles ranging from 200 to 1200 nm. The bonding affinity to lipid interfaces followed the order of Prot-CA-Fe3+(25 μM) > Prot-CA-Fe3+(10 μM) > Prot-CA > original Prot with the underlying nanomechanics investigated by the lipid bubble force measurement. Direct quantification of interactions between the nanovesicles and living human gingival fibroblasts was performed by using surface charge difference mapping. Introducing trace amounts of Fe3+ (at 10 and 25 μM) enhanced vesicle–lipid interactions via the synergy of catechol–amine interactions and Fe3+-induced complexation. This work provides improved valuable insights into the interactions between nanovesicles and cell membranes, offering an energetic paradigm for modulating cell-target delivery processes via intramolecular short-range interactions.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"13 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077386","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Molecular Effects of Zwitterionic Peptide on Monolayer Lipid Membranes upon Enzyme-Catalyzed Degradation

IF 3.9 2区化学

Langmuir Pub Date : 2025-02-02 DOI: 10.1021/acs.langmuir.4c04426

Bailin Feng, Shiyu Du, Yiqing Yang, Yuli Zhu, Nash McKeague, Binhua Lin, Wei Bu, Gang Cheng, Ying Liu

{"title":"Molecular Effects of Zwitterionic Peptide on Monolayer Lipid Membranes upon Enzyme-Catalyzed Degradation","authors":"Bailin Feng, Shiyu Du, Yiqing Yang, Yuli Zhu, Nash McKeague, Binhua Lin, Wei Bu, Gang Cheng, Ying Liu","doi":"10.1021/acs.langmuir.4c04426","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04426","url":null,"abstract":"Secretory phospholipase A2 (sPLA2), an enzyme overexpressed in numerous diseases, has been used to trigger structural transformations in lipid-based drug delivery systems, enabling payload release at target sites. Zwitterionic peptides are known for their superior antifouling properties, often outperforming poly(ethylene glycol) (PEG) surface modification by resisting protein adsorption. In this study, we examined lipid monolayers at the water–vapor interface on a Langmuir trough, incorporating varying molar fractions of zwitterionic peptide-conjugated lipids or PEG-conjugated lipids. Synchrotron X-ray surface techniques, including X-ray reflectivity and grazing incidence X-ray diffraction, were employed to analyze molecular packing, enzyme adsorption, enzyme-catalyzed lipid degradation, and metabolite reorganization at the interface, and microscopy was used to observe domain morphologies. The results demonstrate that zwitterionic peptides exhibit a significantly greater efficiency than PEG in stabilizing the interfacial monolayer packing structure against enzyme-catalyzed lipid degradation. However, contrary to most studies reporting strong resistance of zwitterionic materials to nonspecific protein absorption, enzyme absorption to the interface, which is interfacial and phospholipids specific, was not impeded by the presence of zwitterionic peptides at low molar ratios (≤10 mol %).","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"3 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077046","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Approach to Enantiomer Recognition during Adsorption by Different Adsorption Rates on Zeotype Borophosphate LiCu2[BP2O8(OH)2] with Spontaneously Emerged Chirality

IF 3.9 2区化学

Langmuir Pub Date : 2025-02-02 DOI: 10.1021/acs.langmuir.4c04695

Zhanna D. Uteeva, Elina R. Mansurova, Yuliya F. Sharafutdinova, Diana O. Bagdanova, Marat R. Agliullin, Timur A. Mukhametzyanov, Vladimir Yu Guskov

{"title":"Approach to Enantiomer Recognition during Adsorption by Different Adsorption Rates on Zeotype Borophosphate LiCu2[BP2O8(OH)2] with Spontaneously Emerged Chirality","authors":"Zhanna D. Uteeva, Elina R. Mansurova, Yuliya F. Sharafutdinova, Diana O. Bagdanova, Marat R. Agliullin, Timur A. Mukhametzyanov, Vladimir Yu Guskov","doi":"10.1021/acs.langmuir.4c04695","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04695","url":null,"abstract":"Zeotype borophosphates are porous adsorbents with a 3D open framework. The unique feature of borophosphates is noncentrosymmetric or even chiral structures. The chirality emerged as an asymmetrical arrangement of atoms in crystals and can be referred to the supramolecular, not molecular, chirality hierarchy level. In this work, the zeotype copper borophosphate LiCu2[BP2O8(OH)2] was studied as a promising adsorbent for enantiomer separation. LiCu2[BP2O8(OH)2] has a rare feature: without any external source of chirality, crystals with only [CD(−)284] and [CD(−)760] Cotton effects are synthesized. Tryptophan enantiomer adsorption on LiCu2[BP2O8(OH)2] was studied. At almost all tryptophan concentrations, enantioselectivity was observed. At nonequilibrium conditions, enantioselectivity coefficients were higher than at adsorption equilibrium. In some cases, chiral recognition was not observed at equilibrium but occurred before equilibrium. In a nonequilibrium area of amount of adsorbed substance vs adsorption time curve, a phenomenon of very high enantioselectivity was discovered. The enantioselectivity coefficient values were 3–5, and even 11.8. Such extremely high enantioselectivity values were caused by the nontrivial kinetic curve for l-tryptophan. A far from the equilibrium, a plateau was observed on the curve. At the end of the plateau, the maximal enantioselectivity was observed. This mechanism of enantioselectivity enhancement can be useful for chromatographic separations, chemical sensors, and catalysts.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"207 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077049","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Magnetic Capture of Functionalized Nanoscale Zerovalent Iron for Soil Remediation: A Feasibility Study on Transport Control

IF 3.9 2区化学

Langmuir Pub Date : 2025-02-02 DOI: 10.1021/acs.langmuir.4c04720

Wei Ming Ng, Wai Hong Chong, Ahmad Zuhairi Abdullah, JitKang Lim

{"title":"Magnetic Capture of Functionalized Nanoscale Zerovalent Iron for Soil Remediation: A Feasibility Study on Transport Control","authors":"Wei Ming Ng, Wai Hong Chong, Ahmad Zuhairi Abdullah, JitKang Lim","doi":"10.1021/acs.langmuir.4c04720","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04720","url":null,"abstract":"Nanoscale zerovalent iron (nZVI) has been proposed as a promising nanomaterial for soil remediation. However, injecting nZVI into contaminated sites to target and treat pollutant sources may pose potential environmental risks due to its colloidal stability and mobility in the environment. In this regard, this study assessed the feasibility of implementing magnetic capture of surface-functionalized nZVI in soil environments under the influence of the convective flow current. Here, functionalized nZVI particles were prepared by introducing carboxymethyl cellulose (CMC) as a stabilizing agent during the synthesis of nZVI by using the liquid-phase reduction method. The functionalized nZVI particles were then injected into a two-dimensional flow column containing a sand matrix with a high gradient magnetic trap (HGMT) embedded within the system. Particle transports in both the absence and presence of a magnetic field were recorded by using a digital camera, and the breakthrough curves were generated from the data collected spectrophotometrically. The results showed that the relative breakthrough concentration of nZVI decreased from 0.92 to nearly zero, with a delayed breakthrough time as the applied magnetic field strength increased from zero (no magnetic field) to 0.093 T, demonstrating a 100% capture efficiency. It was found that the magnetic capture for the nZVI particles was contributed by two mechanisms: (1) low gradient magnetic separation (LGMS), driven by the penetrating magnetic field from the permanent magnets, and (2) high gradient magnetic separation (HGMS), which occurred near the wire surfaces within the HGMT section magnetized by the permanent magnets. Findings in this work have proven the feasibility of magnetic separation as a control strategy for nanoparticle applications in environmental remediation.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"22 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077050","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Nonaqueous G-Quadruplex Ionogels

IF 3.9 2区化学

Langmuir Pub Date : 2025-02-02 DOI: 10.1021/acs.langmuir.4c04810

Zeyi Wang, Yuzhen Qian, Guozhen Wang, Xinyu Sun, Jingcheng Hao

{"title":"Nonaqueous G-Quadruplex Ionogels","authors":"Zeyi Wang, Yuzhen Qian, Guozhen Wang, Xinyu Sun, Jingcheng Hao","doi":"10.1021/acs.langmuir.4c04810","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04810","url":null,"abstract":"Supramolecular ionogels, as an emerging class of materials, utilize the intriguing properties of ionic liquids (ILs) and offer a promising method for constructing functional materials in anhydrous solvents. G-Quadruplex, assembled from guanine-rich nucleic acid building blocks, is an important structure closely associated with life and leads to the gelation for constructing versatile materials, such as the electrolytes of supercapacitors. Herein, we design and fabricate G-quadruplex ionogels using an unreported cation. Among the metal acetylacetonates under investigation, iron(III) acetylacetonate is distinctive in its capacity to stabilize G-quadruplexes through a reaction with the solvent ethylammonium nitrate (EAN), resulting in the formation of Fe(acac)2+. The ionogel displays high ionic conductivity (6.43 mS·cm–1), a wide electrochemical stability window (2.86 V), and self-healing properties. The supercapacitor based on the G-quadruplex ionogel electrolyte delivers a gravimetric capacitance of 91.8 F·g–1, a high energy density of 32.6 W h/kg, and a power density of 319.8 W/kg at a current density of 0.2A·g–1. Therefore, the present findings have important implications for deepening the understanding of G-quadruplex structures and metal acetylacetonate complexes and provide an approach to fabricating ionogel electrolytes for high-performance supercapacitors.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"35 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077051","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Achieving Fast Ionic Transport and High Mechanical Properties of Cellulose-Based Solid-State Electrolyte via a Cationic Chain-Extended Effect for Zinc Metal Batteries

IF 3.9 2区化学

Langmuir Pub Date : 2025-02-02 DOI: 10.1021/acs.langmuir.4c04556

Tianyun Zhang, Yu Li, Tian Zhang, Yanci Wang, Jiaojiao Wu, Fen Ran

{"title":"Achieving Fast Ionic Transport and High Mechanical Properties of Cellulose-Based Solid-State Electrolyte via a Cationic Chain-Extended Effect for Zinc Metal Batteries","authors":"Tianyun Zhang, Yu Li, Tian Zhang, Yanci Wang, Jiaojiao Wu, Fen Ran","doi":"10.1021/acs.langmuir.4c04556","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04556","url":null,"abstract":"In recent years, rechargeable aqueous zinc metal batteries have ushered in rapid development, but their large-scale industrial application is hindered by zinc anode dendrite formation and hydrogen evolution reaction. Using a solid-state polymer electrolyte is one of the strategies to solve this problem. Herein, by introducing the chain-expanding effect of zinc salts on oxidized bacterial cellulose, cellulose-based polymer electrolytes with excellent strength and ionic conductivity are prepared. According to the thermogravimetric calculations, the bound water content in prepared electrolytes greatly increases, which slows down the occurrence of side reactions. More importantly, the expanding distance between the fiber chains provides more space for the movement of Zn2+. The obtained solid-state electrolyte displays a high ionic conductivity (38.26 mS cm–1) and good mechanical properties (tensile stress is 592 kPa and tensile strain is 381%). Due to the properties of the solid electrolyte itself, its electrochemical window is expanded to 2.58 V. The assembled Zn∥Zn symmetrical battery maintains an ultralong cycle lifespan over 980 h of 0.5 mA cm–2. The Zn∥NH4V10O10 battery provides the specific capacity (363.1 mAh g–1 at 0.1 A g–1) and shows a satisfactory rate performance.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"60 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077047","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Alumina-Supported Porphyrin Zinc as a Carbonic Anhydrase Mimic: Enhanced CO₂ Hydration Catalysis.

IF 3.7 2区化学

Langmuir Pub Date : 2025-01-31 DOI: 10.1021/acs.langmuir.4c04431

Yuchen Zhou, Zezhi Chen, Huijuan Gong, Donglin Jiang, Huiqiang Yu, Lu Chen

{"title":"Alumina-Supported Porphyrin Zinc as a Carbonic Anhydrase Mimic: Enhanced CO2 Hydration Catalysis.","authors":"Yuchen Zhou, Zezhi Chen, Huijuan Gong, Donglin Jiang, Huiqiang Yu, Lu Chen","doi":"10.1021/acs.langmuir.4c04431","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04431","url":null,"abstract":"Zinc porphyrin is a promising carbonic anhydrase (CA) mimic for promoting CO2 absorption, but its application is hindered by poor dispersibility in absorption solutions. To address these challenges, we developed a strategy to impregnate zinc porphyrin on an γ-Al2O3 carrier. The hydrophilic surface groups and porous structure of γ-Al2O3 were expected to enhance both the hydrophilicity and stability of zinc porphyrin. To verify its feasibility, zinc tetraphenylporphyrin (ZnTPP) was chosen as the representative to synthesize ZnTPP/Al2O3. Characterizations showed that ZnTPP could be loaded into the pores of γ-Al2O3 in a highly dispersed state. Also, ZnTPP/Al2O3 could be uniformly dispersed in the absorption liquid, effectively exposing the Zn2+ active sites and reducing diffusion resistance. CO2 absorption experiments revealed that ZnTPP/Al2O3 significantly enhanced CO2 absorption in water, 20 wt % K2CO3, and 20 wt % monoethanolamine (MEA) solutions, far outperforming original ZnTPP. Density functional theory (DFT) calculations further elucidated the interaction mechanisms, showing that oxygen atoms on γ-Al2O3 stabilize ZnTPP by forming van der Waals and coordination bonds with Zn2+ active sites. Additionally, these oxygen atoms donate electrons to Zn2+, enhancing its catalytic activity. These findings highlight the effectiveness of this strategy and provide a promising pathway for optimizing other CA-mimics for CO2 capture applications.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":" ","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143070750","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Study on the Photoelectrocatalytic Performance of Ti/Ti-W-O Coating Photoelectrodes Prepared by the Microarc Oxidation Method.

IF 3.7 2区化学

Langmuir Pub Date : 2025-01-31 DOI: 10.1021/acs.langmuir.4c04794

Qian Zhang, Yujia Wu, Guowen Wang, Xinxin Zhang, Dedong Sun, Hongchao Ma

{"title":"Study on the Photoelectrocatalytic Performance of Ti/Ti-W-O Coating Photoelectrodes Prepared by the Microarc Oxidation Method.","authors":"Qian Zhang, Yujia Wu, Guowen Wang, Xinxin Zhang, Dedong Sun, Hongchao Ma","doi":"10.1021/acs.langmuir.4c04794","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c04794","url":null,"abstract":"Photoinduced cathodic protection is an environmentally friendly, economical, and sustainable technology that has been widely used in the corrosion protection of alloy materials. In this study, the corrosion-resistant Ti/Ti-W-O ceramic coatings are prepared by changing the concentration of additives, microarc oxidation voltage, pulse frequency, and time using titanium alloy (TC4) as the substrate and sodium tungstate (Na2WO4) as the main additive via the microarc oxidation (MAO) method. The optimum parameters were determined as follows: concentration of added salt (Na2WO4): 0.05 mol/L; reaction conditions: anode voltage 300 V, cathode voltage 30 V, duty cycle 1:1 (50%), frequency 800 Hz, and reaction time 5 min. They were evaluated from two perspectives: photocathodic protection and photocatalysis, respectively. The test results show that the composite coatings have more negative conduction band potentials, narrower band gaps, higher photocurrent densities, and smaller impedance arc radii under the same conditions as those analyzed in the electrochemical workstation test. In addition, the optimized Ti/Ti-W-O composite photoelectrode coupled with 304 stainless steel showed the largest negative shift in corrosion potential (447 mV vs) and improved degradation efficiency of the dyeing wastewater (improved by ∼20%). The above results demonstrate that the composite electrodes in this study exhibit good performance in photocathodic protection and photovoltaic synergy.","PeriodicalId":50,"journal":{"name":"Langmuir","volume":" ","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143070752","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0