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Delamination of NiFe layered double hydroxides into perforated monolayers for efficient water splitting
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-29 DOI: 10.1016/j.jcis.2025.137478
Huanran Li , Hong Pang , Wei Ma , Dai-Ming Tang , Nobuyuki Sakai , Nattapol Ma , Emmanuel Picheau , Wipakorn Jevasuwan , Naoki Fukata , Yoshiyuki Sugahara , Takayoshi Sasaki , Renzhi Ma
The introduction of vacancies can significantly change the coordination and valence states of the catalytic active sites, thereby modulating the electronic structure to promote the oxygen evolution reaction (OER). However, atomic-level vacancy engineering on low-dimensional layered double hydroxides (LDHs) has not been achieved, which could be due to the significant structural damage and/or carbonate (CO32−) contamination occurring during the vacancy creating process. In this study, atomic-scale cation vacancies were generated in LDHs without apparent structure damage and carbonate contamination. Perforated monolayer nanosheets with an utmost exposure of active sites were successfully obtained through a subsequent exfoliation in formamide. Compared to bulk LDHs, the flocculated vacancy-containing nanosheets exhibit a small overpotential of 245 mV at a current density of 10 mA cm−2 and maintain excellent stability at a high current density of 500 mA cm−2. Density functional theory (DFT) calculations indicate that introducing cation vacancies on monolayer NiFe-LDH nanosheets and creating unsaturated Ni-Fe sites can effectively reduce the Gibbs free energy of the OER process. The two-electrode electrolyzer assembled with commercial Pt/C for overall water splitting can operate at a cell voltage as low as 1.50 V to yield a current density of 10 mA cm−2. It also demonstrates long-term stability of 50 h at a large current density of 500 mA cm−2. The current strategy of atomic cation vacancy engineering on monolayer LDHs provides important insights into the design of low-cost LDH-based catalysts toward efficient alkaline water electrolysis and other energy-related applications.
{"title":"Delamination of NiFe layered double hydroxides into perforated monolayers for efficient water splitting","authors":"Huanran Li ,&nbsp;Hong Pang ,&nbsp;Wei Ma ,&nbsp;Dai-Ming Tang ,&nbsp;Nobuyuki Sakai ,&nbsp;Nattapol Ma ,&nbsp;Emmanuel Picheau ,&nbsp;Wipakorn Jevasuwan ,&nbsp;Naoki Fukata ,&nbsp;Yoshiyuki Sugahara ,&nbsp;Takayoshi Sasaki ,&nbsp;Renzhi Ma","doi":"10.1016/j.jcis.2025.137478","DOIUrl":"10.1016/j.jcis.2025.137478","url":null,"abstract":"<div><div>The introduction of vacancies can significantly change the coordination and valence states of the catalytic active sites, thereby modulating the electronic structure to promote the oxygen evolution reaction (OER). However, atomic-level vacancy engineering on low-dimensional layered double hydroxides (LDHs) has not been achieved, which could be due to the significant structural damage and/or carbonate (CO<sub>3</sub><sup>2−</sup>) contamination occurring during the vacancy creating process. In this study, atomic-scale cation vacancies were generated in LDHs without apparent structure damage and carbonate contamination. Perforated monolayer nanosheets with an utmost exposure of active sites were successfully obtained through a subsequent exfoliation in formamide. Compared to bulk LDHs, the flocculated vacancy-containing nanosheets exhibit a small overpotential of 245 mV at a current density of 10 mA cm<sup>−2</sup> and maintain excellent stability at a high current density of 500 mA cm<sup>−2</sup>. Density functional theory (DFT) calculations indicate that introducing cation vacancies on monolayer NiFe-LDH nanosheets and creating unsaturated Ni-Fe sites can effectively reduce the Gibbs free energy of the OER process. The two-electrode electrolyzer assembled with commercial Pt/C for overall water splitting can operate at a cell voltage as low as 1.50 V to yield a current density of 10 mA cm<sup>−2</sup>. It also demonstrates long-term stability of 50 h at a large current density of 500 mA cm<sup>−2</sup>. The current strategy of atomic cation vacancy engineering on monolayer LDHs provides important insights into the design of low-cost LDH-based catalysts toward efficient alkaline water electrolysis and other energy-related applications.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137478"},"PeriodicalIF":9.4,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143768365","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Boosting catalytic reduction of hexavalent chromium over PdNi alloy by electron injection into unoccupied Pd d-band
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-28 DOI: 10.1016/j.jcis.2025.137465
Wenxin Du, Xujia Cao, Yuan Lin, Yunyun Gui, Lijun Liu
Hexavalent chromium (Cr(VI)) in industrial wastewater presents a severe environmental threat. Using formic acid for Cr(VI) reduction offers an efficient and sustainable chromium remediation. While Pd reduces the energy barrier for formic acid dissociation to produce H*, the formation of strong PdH bonds hinders subsequent Cr(VI) reduction due to elevated energy levels and an increased proportion of unoccupied states in the Pd 4d bands. To address this challenge, we developed a PdNi/TiO2 nanofibrous catalyst designed to optimize hydrogen adsorption through intermetallic electron transfer within the alloy. Experimental and theoretical results confirm that electrons from Ni are injected into the unoccupied portion of the Pd d-band, downshifting the d-band center upon alloy formation. This electron injection optimizes the electronic states of the Pd active sites, lowering the energy barrier for formic acid dissociation while weakening the PdH interaction, thereby facilitating the release of H* species. The optimized Pd6Ni4/TiO2 achieves an improved turnover frequency (TOF) of 164.8 min−1 for Cr(VI) reduction, outperforming most previous Pd-based catalysts.
{"title":"Boosting catalytic reduction of hexavalent chromium over PdNi alloy by electron injection into unoccupied Pd d-band","authors":"Wenxin Du,&nbsp;Xujia Cao,&nbsp;Yuan Lin,&nbsp;Yunyun Gui,&nbsp;Lijun Liu","doi":"10.1016/j.jcis.2025.137465","DOIUrl":"10.1016/j.jcis.2025.137465","url":null,"abstract":"<div><div>Hexavalent chromium (Cr(VI)) in industrial wastewater presents a severe environmental threat. Using formic acid for Cr(VI) reduction offers an efficient and sustainable chromium remediation. While Pd reduces the energy barrier for formic acid dissociation to produce H*, the formation of strong Pd<img>H bonds hinders subsequent Cr(VI) reduction due to elevated energy levels and an increased proportion of unoccupied states in the Pd 4<em>d</em> bands. To address this challenge, we developed a PdNi/TiO<sub>2</sub> nanofibrous catalyst designed to optimize hydrogen adsorption through intermetallic electron transfer within the alloy. Experimental and theoretical results confirm that electrons from Ni are injected into the unoccupied portion of the Pd <em>d</em>-band, downshifting the <em>d</em>-band center upon alloy formation. This electron injection optimizes the electronic states of the Pd active sites, lowering the energy barrier for formic acid dissociation while weakening the Pd<img>H interaction, thereby facilitating the release of H* species. The optimized Pd<sub>6</sub>Ni<sub>4</sub>/TiO<sub>2</sub> achieves an improved turnover frequency (TOF) of 164.8 min<sup>−1</sup> for Cr(VI) reduction, outperforming most previous Pd-based catalysts.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"691 ","pages":"Article 137465"},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759707","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
High-rate LiFe0.75Mn0.25PO4/C cathode material for lithium-ion battery was prepared by oriented growth of precursor crystal plane
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-28 DOI: 10.1016/j.jcis.2025.137436
Yu Zhang , Rong Li , Qi Guo , Fangxiang Song , Kang Kai , Qianlin Chen
The emergence of the lithium-ion battery as a subject of intense research interest has propelled of high-energy–density LiFexMn1-xPO4(LFMP) becoming a prominent area of investigation. However, the material suffers from inherently low electronic conductivity due to its olivine structure, which imposes severe constraints on electron transport kinetics, thus adversely impacting both charge–discharge rates and overall electrochemical performance. We propose an innovative protocol for high-precision reaction mechanism modulation. By employing Fe3(PO4)2·8H2O with strategically enhanced (020) crystal plane exposure as a pivotal precursor, we synthesized LiFe0.75Mn0.25PO4/C cathode material featuring a shorter ion diffusion path. Comprehensive characterization coupled with electrochemical validation revealed that the resultant cathode material exhibits a smaller particle size and more uniform morphology, along with a superior rate performance and cycle stability. The discharge specific capacity is 144.1 mAh g−1 and the capacity retention reaches 96.1 % over 1000 cycles at a 1C rate. The findings demonstrate that the regulation of the growth trajectory of the precursor Fe3(PO4)2·8H2O crystal plane can markedly enhance the electronic conductivity and Li+ mobility of the cathode material, thereby optimising the electrochemical performance.
{"title":"High-rate LiFe0.75Mn0.25PO4/C cathode material for lithium-ion battery was prepared by oriented growth of precursor crystal plane","authors":"Yu Zhang ,&nbsp;Rong Li ,&nbsp;Qi Guo ,&nbsp;Fangxiang Song ,&nbsp;Kang Kai ,&nbsp;Qianlin Chen","doi":"10.1016/j.jcis.2025.137436","DOIUrl":"10.1016/j.jcis.2025.137436","url":null,"abstract":"<div><div>The emergence of the lithium-ion battery as a subject of intense research interest has propelled of high-energy–density LiFe<sub>x</sub>Mn<sub>1-x</sub>PO<sub>4</sub>(LFMP) becoming a prominent area of investigation. However, the material suffers from inherently low electronic conductivity due to its olivine structure, which imposes severe constraints on electron transport kinetics, thus adversely impacting both charge–discharge rates and overall electrochemical performance. We propose an innovative protocol for high-precision reaction mechanism modulation. By employing Fe<sub>3</sub>(PO<sub>4</sub>)<sub>2</sub>·8H<sub>2</sub>O with strategically enhanced (020) crystal plane exposure as a pivotal precursor, we synthesized LiFe<sub>0.75</sub>Mn<sub>0.25</sub>PO<sub>4</sub>/C cathode material featuring a shorter ion diffusion path. Comprehensive characterization coupled with electrochemical validation revealed that the resultant cathode material exhibits a smaller particle size and more uniform morphology, along with a superior rate performance and cycle stability. The discharge specific capacity is 144.1 mAh g<sup>−1</sup> and the capacity retention reaches 96.1 % over 1000 cycles at a 1C rate. The findings demonstrate that the regulation of the growth trajectory of the precursor Fe<sub>3</sub>(PO<sub>4</sub>)<sub>2</sub>·8H<sub>2</sub>O crystal plane can markedly enhance the electronic conductivity and Li<sup>+</sup> mobility of the cathode material, thereby optimising the electrochemical performance.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"691 ","pages":"Article 137436"},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143760215","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Engineered cell nanovesicle antagonists for androgen deprivation therapy of melanoma
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-28 DOI: 10.1016/j.jcis.2025.137468
Yu Zhao , Yichuan Ma , Qingqing Leng , Qi Zhang , Yuanhang Li , Mengmeng Ji , Hua Yang , Xiaoya Li , Guang Jia , Zhenhua Li , Huifang Liu , Jinchao Zhang
Epidemiological studies on melanoma have revealed significant gender disparities, with the incidence and mortality rates being higher in males than in females. Recent studies indicate that androgen contributing to T cell exhaustion and promoting cancer cell proliferation. While clinical androgen deprivation therapies (ADT),particularly the use of androgen receptor (AR) antagonists to block AR signaling, has been employed in clinical settings to reduce androgen levels, antiandrogen drugs often encounter challenges such as poor targeting and selectivity, increased toxicity, low stability, short half-life and the emergence of drug resistance. Here, we establish a nanoantagonists for efficient AR signaling blockade by arming antigen-activated dendritic cells (DCs) nanovesicles with AR antibodies (aAR-NVOVA). This innovative approach demonstrates dual therapeutic efficacy: aAR-NVOVA effectively disrupts androgen-AR interactions in both melanoma cells and T cells, simultaneously inhibiting tumor proliferation and reversing T cell exhaustion. Furthermore, aAR-NVOVA retains the inherent immunostimulatory properties of DCs, facilitating T cell activation and enhancing cytotoxic T lymphocyte infiltration within tumor tissues. As a result, a synergistic effect has been observed in boosting T cell-based immunotherapy by simultaneously enhancing T cell activity and reducing its exhaustion. Our study using aAR-NVOVA to antagonize androgen effects offers a promising new strategy for enhancing melanoma immunotherapy.
{"title":"Engineered cell nanovesicle antagonists for androgen deprivation therapy of melanoma","authors":"Yu Zhao ,&nbsp;Yichuan Ma ,&nbsp;Qingqing Leng ,&nbsp;Qi Zhang ,&nbsp;Yuanhang Li ,&nbsp;Mengmeng Ji ,&nbsp;Hua Yang ,&nbsp;Xiaoya Li ,&nbsp;Guang Jia ,&nbsp;Zhenhua Li ,&nbsp;Huifang Liu ,&nbsp;Jinchao Zhang","doi":"10.1016/j.jcis.2025.137468","DOIUrl":"10.1016/j.jcis.2025.137468","url":null,"abstract":"<div><div>Epidemiological studies on melanoma have revealed significant gender disparities, with the incidence and mortality rates being higher in males than in females. Recent studies indicate that androgen contributing to T cell exhaustion and promoting cancer cell proliferation. While clinical androgen deprivation therapies (ADT),particularly the use of androgen receptor (AR) antagonists to block AR signaling, has been employed in clinical settings to reduce androgen levels, antiandrogen drugs often encounter challenges such as poor targeting and selectivity, increased toxicity, low stability, short half-life and the emergence of drug resistance. Here, we establish a nanoantagonists for efficient AR signaling blockade by arming antigen-activated dendritic cells (DCs) nanovesicles with AR antibodies (aAR-NV<sub>OVA</sub>). This innovative approach demonstrates dual therapeutic efficacy: aAR-NV<sub>OVA</sub> effectively disrupts androgen-AR interactions in both melanoma cells and T cells, simultaneously inhibiting tumor proliferation and reversing T cell exhaustion. Furthermore, aAR-NV<sub>OVA</sub> retains the inherent immunostimulatory properties of DCs, facilitating T cell activation and enhancing cytotoxic T lymphocyte infiltration within tumor tissues. As a result, a synergistic effect has been observed in boosting T cell-based immunotherapy by simultaneously enhancing T cell activity and reducing its exhaustion. Our study using aAR-NV<sub>OVA</sub> to antagonize androgen effects offers a promising new strategy for enhancing melanoma immunotherapy.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"691 ","pages":"Article 137468"},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759712","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Atomic spin engineering of Fe-N-C by axial chlorine-ligand modulation for lightweight and efficient electromagnetic wave absorption
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-28 DOI: 10.1016/j.jcis.2025.137464
Qi Wei, Pan Zhang, Xinyu Guo, Weiqing Jiang, Xiaoma Tao, Pei Kang Shen, Zhi Qun Tian
Introducing atomic magnetic factors to regulate the electromagnetic parameters of graphene is essential to achieving new-generation electromagnetic wave (EMW) absorbing materials. Herein, a new strategy of endowing graphene with atomic magnetic moments was developed by implanting high-spin FeN4 moieties with axial Cl ligands into 3D N-doped graphene (Cl-Fe-NG). The design facilitates the multi-reflection loss, dielectric loss and magnetic loss of EMW at ultra-low filling. Its minimum reflective loss (RL) is up to −65.9 dB with the biggest effective absorption bandwidth (EAB) of up to 5.5 GHz in the thin thickness of 1.9 mm and a low filler loading of 5 wt%. Meanwhile, a waterborne polyurethane wave-absorbing coating filled with 5 wt% Cl-Fe-NG demonstrates its high absorption performance with a dominant absorption loss of 90 %. Additionally, theory calculations reveal that introducing axial Cl-ligand FeN4 moiety with high-spin Fe into graphene not only generates additional electric dipoles but also induces an atomic magnetic moment, effectively enhancing the dielectric and magnetic loss of graphene for EMW absorption. This work provides a new approach to designing graphene with atomic magnetic moments for developing EMW absorbing materials with “thin, wide, light, and strong” characteristics instead of the conventional route of graphene with magnetic nanoparticles.
引入原子磁因子来调节石墨烯的电磁参数对于实现新一代电磁波(EMW)吸收材料至关重要。在此,我们通过在三维 N 掺杂石墨烯(Cl-Fe-NG)中植入带有轴向 Cl 配体的高自旋 FeN4 分子,开发了一种赋予石墨烯原子磁矩的新策略。这种设计有助于在超低填充下实现电磁波的多重反射损耗、介电损耗和磁损耗。其最小反射损耗(RL)高达 -65.9 dB,在厚度为 1.9 mm 的薄层和 5 wt% 的低填充量条件下,最大有效吸收带宽(EAB)高达 5.5 GHz。同时,填充了 5 wt% Cl-Fe-NG 的水性聚氨酯吸波涂层也表现出了很高的吸波性能,主要吸波损耗为 90%。此外,理论计算显示,在石墨烯中引入具有高自旋 Fe 的轴向 Cl 配体 FeN4 分子不仅会产生额外的电偶极子,还会诱发原子磁矩,从而有效提高石墨烯在电磁波吸收方面的介电损耗和磁损耗。这项工作为设计具有原子磁矩的石墨烯提供了一种新的方法,以开发具有 "薄、宽、轻、强 "特性的电磁波吸收材料,而不是传统的石墨烯与磁性纳米粒子的结合。
{"title":"Atomic spin engineering of Fe-N-C by axial chlorine-ligand modulation for lightweight and efficient electromagnetic wave absorption","authors":"Qi Wei,&nbsp;Pan Zhang,&nbsp;Xinyu Guo,&nbsp;Weiqing Jiang,&nbsp;Xiaoma Tao,&nbsp;Pei Kang Shen,&nbsp;Zhi Qun Tian","doi":"10.1016/j.jcis.2025.137464","DOIUrl":"10.1016/j.jcis.2025.137464","url":null,"abstract":"<div><div>Introducing atomic magnetic factors to regulate the electromagnetic parameters of graphene is essential to achieving new-generation electromagnetic wave (EMW) absorbing materials. Herein, a new strategy of endowing graphene with atomic magnetic moments was developed by implanting high-spin FeN<sub>4</sub> moieties with axial Cl ligands into 3D <em>N</em>-doped graphene (Cl-Fe-NG). The design facilitates the multi-reflection loss, dielectric loss and magnetic loss of EMW at ultra-low filling. Its minimum reflective loss (RL) is up to −65.9 dB with the biggest effective absorption bandwidth (EAB) of up to 5.5 GHz in the thin thickness of 1.9 mm and a low filler loading of 5 wt%. Meanwhile, a waterborne polyurethane wave-absorbing coating filled with 5 wt% Cl-Fe-NG demonstrates its high absorption performance with a dominant absorption loss of 90 %. Additionally, theory calculations reveal that introducing axial Cl-ligand FeN<sub>4</sub> moiety with high-spin Fe into graphene not only generates additional electric dipoles but also induces an atomic magnetic moment, effectively enhancing the dielectric and magnetic loss of graphene for EMW absorption. This work provides a new approach to designing graphene with atomic magnetic moments for developing EMW absorbing materials with “thin, wide, light, and strong” characteristics instead of the conventional route of graphene with magnetic nanoparticles.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137464"},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759925","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Structure and phase engineering afforded gradient manganese dioxide composites for impedance matching toward electromagnetic wave absorption
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-28 DOI: 10.1016/j.jcis.2025.137445
Lulu Song , Caixia Sun , Yongqiang Wang , Zhenyi Huang , Yongpeng Zhao , Shengling Yuan , Yahong Zhang , Wenzhen Xia
Impedance mismatch severely limits the performance of electromagnetic (EM) microwave absorber materials. Aiming at addressing this issue, this study proposes a strategy combining structure and phase engineering to design gradient manganese dioxide (MnO2) core@shell composites. The core of the composites comprises cadmium (Cd)-doped α-MnO2 nanowires, synthesized via a self-assembly process achieved using the hydrothermal method, which possess remarkable dielectric attenuation capability that can effectively consume EM energy. The shell comprised α-MnO2 nanosheets, which serve as a matching layer and introduce interfaces and defects that further enhance EM energy attenuation; notably, these α-MnO2 nanosheets are formed through calcination-induced phase transition of δ-MnO2 nanosheets grown on the core nanowire surface. The uniform growth of nanosheets on nanowires is facilitated by the low lattice mismatch between α-MnO2 and δ-MnO2. The resulting Cd-doped α-MnO2 nanowire@α-MnO2 nanosheet composites deliver remarkable absorption performance; the minimum reflection loss can reach − 50.50 dB and effective absorption bandwidth reaches 5.44 GHz in the Ku band, which are attributed to optimized synergy between attenuation and impedance matching, dipole polarization enhancement through heteroatom doping, and interfacial polarization at the core–shell interface. This study provides a novel approach to designing advanced EM absorption materials.
{"title":"Structure and phase engineering afforded gradient manganese dioxide composites for impedance matching toward electromagnetic wave absorption","authors":"Lulu Song ,&nbsp;Caixia Sun ,&nbsp;Yongqiang Wang ,&nbsp;Zhenyi Huang ,&nbsp;Yongpeng Zhao ,&nbsp;Shengling Yuan ,&nbsp;Yahong Zhang ,&nbsp;Wenzhen Xia","doi":"10.1016/j.jcis.2025.137445","DOIUrl":"10.1016/j.jcis.2025.137445","url":null,"abstract":"<div><div>Impedance mismatch severely limits the performance of electromagnetic (EM) microwave absorber materials. Aiming at addressing this issue, this study proposes a strategy combining structure and phase engineering to design gradient manganese dioxide (MnO<sub>2</sub>) core@shell composites. The core of the composites comprises cadmium (Cd)-doped α-MnO<sub>2</sub> nanowires, synthesized via a self-assembly process achieved using the hydrothermal method, which possess remarkable dielectric attenuation capability that can effectively consume EM energy. The shell comprised α-MnO<sub>2</sub> nanosheets, which serve as a matching layer and introduce interfaces and defects that further enhance EM energy attenuation; notably, these α-MnO<sub>2</sub> nanosheets are formed through calcination-induced phase transition of δ-MnO<sub>2</sub> nanosheets grown on the core nanowire surface. The uniform growth of nanosheets on nanowires is facilitated by the low lattice mismatch between α-MnO<sub>2</sub> and δ-MnO<sub>2</sub>. The resulting Cd-doped α-MnO<sub>2</sub> nanowire@α-MnO<sub>2</sub> nanosheet composites deliver remarkable absorption performance; the minimum reflection loss can reach − 50.50 dB and effective absorption bandwidth reaches 5.44 GHz in the Ku band, which are attributed to optimized synergy between attenuation and impedance matching, dipole polarization enhancement through heteroatom doping, and interfacial polarization at the core–shell interface. This study provides a novel approach to designing advanced EM absorption materials.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"691 ","pages":"Article 137445"},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143738583","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Pre-carbonization-mediated construction of urchin-like NiFe2O4 superparticles with enhanced CNT growth for efficient oxygen evolution
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-28 DOI: 10.1016/j.jcis.2025.137463
Junjie Qiu , Xiangyun Xi , Shuoran Zheng , Tongtao Li , Yajun Wang , Xiaomeng Ren , Angang Dong
In this study, we report the rational design and synthesis of carbonized NiFe2O4 superparticles (CarSPs) hierarchically integrated with densely aligned carbon nanotube (CNT) architectures, hereafter denoted as CarSP-CNTs, which exhibit a biomimetic urchin-like morphology. Through exploitation of the colloidal self-assembly and catalytic functionalities inherent to NiFe2O4 nanoparticles (NPs), we achieve seamless integration of one-dimensional CNT arrays with three-dimensional superstructural frameworks. Systematic investigation reveals that the pre-carbonization of surface-bound organic ligands coupled with subsequent CNT growth induces synergistic interplay between conductive carbon matrices and active spinel oxide phases. This structural optimization confers CarSP-CNTs with enhanced charge transfer kinetics and catalytically robust interfaces, as evidenced by their superior electrocatalytic performance for the oxygen evolution reaction (OER) in alkaline electrolyte (1 M KOH). The optimized CarSP-CNTs exhibit a minimal overpotential of 307 mV to deliver a current density of 10 mA cm−2, alongside remarkable operational stability exceeding 20 h of continuous electrolysis. These findings establish a paradigm for the rational design of hierarchically structured, multi-component electrocatalysts through coordinated nanoscale engineering, offering a versatile platform for advancing energy conversion technologies.
{"title":"Pre-carbonization-mediated construction of urchin-like NiFe2O4 superparticles with enhanced CNT growth for efficient oxygen evolution","authors":"Junjie Qiu ,&nbsp;Xiangyun Xi ,&nbsp;Shuoran Zheng ,&nbsp;Tongtao Li ,&nbsp;Yajun Wang ,&nbsp;Xiaomeng Ren ,&nbsp;Angang Dong","doi":"10.1016/j.jcis.2025.137463","DOIUrl":"10.1016/j.jcis.2025.137463","url":null,"abstract":"<div><div>In this study, we report the rational design and synthesis of carbonized NiFe<sub>2</sub>O<sub>4</sub> superparticles (CarSPs) hierarchically integrated with densely aligned carbon nanotube (CNT) architectures, hereafter denoted as CarSP-CNTs, which exhibit a biomimetic urchin-like morphology. Through exploitation of the colloidal self-assembly and catalytic functionalities inherent to NiFe<sub>2</sub>O<sub>4</sub> nanoparticles (NPs), we achieve seamless integration of one-dimensional CNT arrays with three-dimensional superstructural frameworks. Systematic investigation reveals that the pre-carbonization of surface-bound organic ligands coupled with subsequent CNT growth induces synergistic interplay between conductive carbon matrices and active spinel oxide phases. This structural optimization confers CarSP-CNTs with enhanced charge transfer kinetics and catalytically robust interfaces, as evidenced by their superior electrocatalytic performance for the oxygen evolution reaction (OER) in alkaline electrolyte (1 M KOH). The optimized CarSP-CNTs exhibit a minimal overpotential of 307 mV to deliver a current density of 10 mA cm<sup>−2</sup>, alongside remarkable operational stability exceeding 20 h of continuous electrolysis. These findings establish a paradigm for the rational design of hierarchically structured, multi-component electrocatalysts through coordinated nanoscale engineering, offering a versatile platform for advancing energy conversion technologies.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"691 ","pages":"Article 137463"},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745787","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Spinning microrods in a rotating electric field with tunable hodograph
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-28 DOI: 10.1016/j.jcis.2025.137456
Sofia A. Korsakova , Nikita P. Kryuchkov , Egor V. Yakovlev , Daniil A. Bystrov , Fabian Hagemans , Ivan V. Simkin , Pavel A. Libet , Jérôme J. Crassous , Stanislav O. Yurchenko

Hypothesis

In external high-frequency rotational electric fields, the polarization of rod-like colloidal particles experiences a slight temporal delay relative to the field, resulting in a torque that acts upon the particles. This torque depends on the hodograph of the external rotating electric field (the spatial curve traced by the tip of the electric field vector as it changes over time), enabling control over the rotational dynamics of rod-like colloidal particles.

Experiments

The experiments were conducted using synthesized monodisperse silica microrods with average size of 3.29×1.12×1.12μm3 dispersed in deionized water, at a mass fraction of 0.2%. The external electric field was generated using an 8-electrode system, and it rotated within the system's plane along an elliptical hodograph at a frequency of 30 kHz. We used an optical microscope with magnification objective of equipped with a CCD-camera (Thorlabs). The experimental data were processed using Fiji software.

Findings

The external high-frequency rotational electric field allows for controlled imposition of three types of rotational dynamics onto rod-like colloidal particles: (i) asynchronous continuous rotation – tunable spinners, (ii) oscillations around a certain direction with sporadic rod flips – rotational jumpers with enhanced directional ordering, and (iii) a regime of “arrested” particle orientation along the principal axes of field anisotropy.
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引用次数: 0
Interface-engineering enhanced photocatalytic conversion of CO2 into solar fuels over S-type Co-Bi2WO6@Ce-MOF heterostructured photocatalysts
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-27 DOI: 10.1016/j.jcis.2025.137452
Jiale Ren , Qianfei Ma , Xiaofeng Sun , Shifa Wang , Guorong Liu , Hua Yang
Development of excellent photocatalysts for efficient conversion CO2 into renewable fuels is vital to alleviate the problems of greenhouse effect and energy crisis. In this study, we have developed new S-type Codoped-Bi2WO6@Ce-MOF heterostructured photocatalysts by in-situ growing Ce-MOF (cerium metal–organic framework) nanoparticles on the surface of Co-doped Bi2WO6 (BWO) hierarchical microflowers. Experimental and theoretical studies demonstrate the formation of S-type heterojunction in the Co-BWO@Ce-MOF hybrids, and the S-type electron transfer from the conduction band of Ce-MOF to the valence band of Co-BWO enables more photoelectrons in the Co-BWO conduction band to participate in the CO2 photoreduction reactions. Simultaneously, the Co doping reinforces the chemical bonding between Co-BWO and Ce-MOF and enhances the interface electric field, thus promoting the photocarrier transfer. The Co doping also creates abundant oxygen vacancies in Ce-MOF, which are beneficial to the visible-light absorption and photocarrier separation/transfer. Moreover, the Co doping enhances the adsorption/activation of CO2, promotes electron transfer from the photocatalyst to CO2 and reduces the energy barriers for the CO2 reduction through engineering the interface electronic configuration. Owing to these factors, the Co-BWO@Ce-MOF heterostructures are endowed with excellent CO2 photoreduction activity. Particularly, the Co1BWO@25CM photocatalytically induces the CO/CH4 yield rates of 77.1/11.4 μmol g−1 h−1, which are increased by 2.0/1.3 times over those for Co1BWO and 8.7/8.8 times over those for Ce-MOF. This study highlights that the S-type charge transfer and interface engineering synergistically enhance the CO2 photoreduction performance of heterojunction photocatalysts.
要缓解温室效应和能源危机问题,就必须开发出能将二氧化碳高效转化为可再生燃料的优秀光催化剂。在这项研究中,我们通过在钴掺杂的 Bi2WO6(BWO)分层微流体表面原位生长 Ce-MOF(铈金属有机框架)纳米粒子,开发出了新型 S 型 Codoped-Bi2WO6@Ce-MOF 异质结构光催化剂。实验和理论研究证明,Co-BWO@Ce-MOF 杂化物中形成了 S 型异质结,S 型电子从 Ce-MOF 的导带转移到 Co-BWO 的价带,使 Co-BWO 导带中更多的光电子参与 CO2 光还原反应。同时,Co 的掺杂加强了 Co-BWO 和 Ce-MOF 之间的化学键,增强了界面电场,从而促进了光载流子的转移。Co 掺杂还在 Ce-MOF 中产生了大量的氧空位,有利于可见光吸收和光载流子分离/转移。此外,掺 Co 还能增强对 CO2 的吸附/活化,促进光催化剂向 CO2 的电子转移,并通过界面电子构型工程降低 CO2 还原的能量障碍。由于这些因素,Co-BWO@Ce-MOF 异质结构具有优异的二氧化碳光还原活性。特别是 Co1BWO@25CM 光催化诱导的 CO/CH4 产率为 77.1/11.4 μmol g-1 h-1,比 Co1BWO 提高了 2.0/1.3 倍,比 Ce-MOF 提高了 8.7/8.8 倍。这项研究表明,S 型电荷转移和界面工程可协同提高异质结光催化剂的二氧化碳光还原性能。
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引用次数: 0
Schottky-mediated porphyrin-metal-organic framework/Ti3C2-MXene heterojunction for water decontamination via photonic-thermal-enzyme synergistic catalysis
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-27 DOI: 10.1016/j.jcis.2025.137462
Shuo Li , Jinhe Li , Wei Ren , Ying Xu , Qinqin Liu
The inherent limitations of single-modal photocatalytic systems in complex wastewater treatment motivate the development of multifunctional catalysts to overcome restricted reaction kinetics and narrow activation spectra. In this study, we engineered a photo-thermal-enzyme triply synergistic catalyst by constructing an interfacial Schottky junction between porphyrinic metal–organic frameworks (PCN-224) and Ti3C2-MXene via a solvothermal synthesis. Scanning electron microscopy unveiled that PCN-224 cubes were anchored onto MXene’s delaminated sheets. This design uniquely integrated three complementary merits, including high photothermal conversion efficiency endowed by MXene, high charge separation enabled by Schottky-junction, and enzyme-mimetic activity through PCN-224 integration. Mechanistic studies combining first principles calculations, photoelectrochemical characterization, and operando infrared thermography revealed that the Schottky-junction optimized carrier utilization while localized heating favored to reduce activation energy of water and oxygen. The enzymatic oxidation of 3,3′,5,5′-testhylbenzidine was employed to evidence the peroxidase-like activity of the PCN-224/Mxene. This optimized composite achieved 91.2 % tetracycline (50 mg/L) and 97.4 % Rhodamine B (50 mg/L) degradation within 60 min, alongside 99.99 % and 99.92 % inactivation of methicillin-resistant Staphylococcus aureus and Escherichia coli, respectively. This work establishes a paradigm for multimechanistic synergy in environmental catalysis, demonstrating how rational catalysis engineering can simultaneously leverage photonic, thermal, and enzymatic activation pathways to overcome fundamental limitations in conventional systems. The demonstrated approach provides a scalable strategy for advanced water treatment technologies requiring high efficiency under real-world conditions.
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引用次数: 0
期刊
Journal of Colloid and Interface Science
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