Rational construction of core@shell heterostructured photocatalysts is the key to realize efficient hydrogen production from water splitting attributing to the accelerated photoinduced charges separation/transfer and enhanced light absorption ability. In this work, two-dimensional (2D) ZnIn2S4 (ZIS) nanosheets were in-situ grown on phosphorus doped MnCo2O4.5 (P-MnCo2O4.5) nanospheres to construct P-MnCo2O4.5@ZIS heterostructured photocatalysts for efficient photocatalytic hydrogen production. The optimized 6 wt% P-MnCo2O4.5@ZIS composite presents remarkable photocatalytic hydrogen evolution rate of 4197 µmol g−1 h−1 (8 times of single ZIS) along with excellent cycling stability, which is comparable to most previous reported ZnIn2S4-based or even noble-metal involved catalysts. The improved photocatalytic performance is resulted from the distinguished heterostructure and components of P-MnCo2O4.5@ZIS, in which the close contact interface facilitates the separation/transfer and inhibits the recombination of charges, and the uniform distribution of ZIS nanosheets on P-MnCo2O4.5 increases the active sites and fortifies the light absorption. The present work comes up with a prospective method for establishing core@shell ZIS-based heterostructured photocatalysts for efficient hydrogen generation.
{"title":"Constructing core–shell phosphorus doped MnCo2O4.5@ZIS for efficient photocatalytic hydrogen production from water splitting","authors":"Yueru Yan, Yuanyuan Zhao, Yun Lou, Yafei Zhao, Huishan Shang, Yinze Yang, Dan Wang, Bing Zhang","doi":"10.1016/j.jcis.2024.11.052","DOIUrl":"10.1016/j.jcis.2024.11.052","url":null,"abstract":"<div><div>Rational construction of core@shell heterostructured photocatalysts is the key to realize efficient hydrogen production from water splitting attributing to the accelerated photoinduced charges separation/transfer and enhanced light absorption ability. In this work, two-dimensional (2D) ZnIn<sub>2</sub>S<sub>4</sub> (ZIS) nanosheets were in-situ grown on phosphorus doped MnCo<sub>2</sub>O<sub>4.5</sub> (P-MnCo<sub>2</sub>O<sub>4.5</sub>) nanospheres to construct P-MnCo<sub>2</sub>O<sub>4.5</sub>@ZIS heterostructured photocatalysts for efficient photocatalytic hydrogen production. The optimized 6 wt% P-MnCo<sub>2</sub>O<sub>4.5</sub>@ZIS composite presents remarkable photocatalytic hydrogen evolution rate of 4197 µmol g<sup>−1</sup> h<sup>−1</sup> (8 times of single ZIS) along with excellent cycling stability, which is comparable to most previous reported ZnIn<sub>2</sub>S<sub>4</sub>-based or even noble-metal involved catalysts. The improved photocatalytic performance is resulted from the distinguished heterostructure and components of P-MnCo<sub>2</sub>O<sub>4.5</sub>@ZIS, in which the close contact interface facilitates the separation/transfer and inhibits the recombination of charges, and the uniform distribution of ZIS nanosheets on P-MnCo<sub>2</sub>O<sub>4.5</sub> increases the active sites and fortifies the light absorption. The present work comes up with a prospective method for establishing core@shell ZIS-based heterostructured photocatalysts for efficient hydrogen generation.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 965-975"},"PeriodicalIF":9.4,"publicationDate":"2024-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142643584","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}
Photothermal therapy (PTT) has gained significant attention as a non-invasive treatment in clinical oncology. However, the translation of PTT into clinical practice remains constrained by three fundamental limitations: acquired thermal tolerance in tumor cells, restricted light penetration depth in biological matrices, and insufficient therapeutic outcomes from single-modality treatment. To address these issues, a strategy for forming in situ complexes between near-infrared-II (NIR-II) photothermal agents and proteins is developed, aimed at damaging protein conformation and enhancing PTT effectiveness. We developed a nanoplatform called PCy-SF, consisting of the NIR-II photothermal polymer (PCy) and sorafenib (SF). PCy-SF responds to the tumor microenvironment (TME), specifically releasing Cy-CHO and sorafenib from the assemblies. The released Cy-CHO covalently binds to proteins, forming Cy-Protein complexes that activate NIR-II fluorescence, facilitating NIR-II imaging-guided photothermal therapy. Concurrently, the released SF intensifies microvascular damage, synergizing with PTT for enhanced therapeutic efficacy. Notably, PCy-SF induces a strong anticancer immune response, effectively suppressing tumor recurrence and metastasis. This study introduces a promising protein deactivation strategy for achieving mild-temperature PTT, offering broader applicability of PTT and insights for sensitizing tumors to photothermal therapy. Together, this innovative approach combining NIR-II photothermal agents with protein complexation and a responsive nanoplatform enhances PTT precision and efficacy, demonstrating significant potential in the field of cancer nanomedicine.
光热疗法（PTT）作为临床肿瘤学中的一种非侵入性治疗方法，已受到广泛关注。然而，将光热疗法转化为临床实践仍受到三个基本限制：肿瘤细胞获得性热耐受、光在生物基质中的穿透深度受限以及单一模式治疗的疗效不佳。为了解决这些问题，我们开发了一种在近红外-II（NIR-II）光热剂和蛋白质之间形成原位复合物的策略，旨在破坏蛋白质构象并提高 PTT 的有效性。我们开发了一种名为PCy-SF的纳米平台，由近红外光热聚合物（PCy）和索拉非尼（SF）组成。PCy-SF 可对肿瘤微环境（TME）做出反应，特异性地从组装体中释放 Cy-CHO 和索拉非尼。释放的Cy-CHO与蛋白质共价结合，形成Cy-蛋白质复合物，激活近红外-II荧光，促进近红外-II成像引导的光热疗法。同时，释放的 SF 会加剧微血管损伤，与 PTT 协同增强疗效。值得注意的是，PCy-SF 能诱导强烈的抗癌免疫反应，有效抑制肿瘤复发和转移。这项研究为实现低温 PTT 引入了一种前景广阔的蛋白质失活策略，为 PTT 提供了更广泛的适用性，并为肿瘤对光热疗法的敏感性提供了启示。这种创新方法将近红外-II光热制剂与蛋白质复合物和响应性纳米平台结合在一起，提高了PTT的精确性和疗效，显示了癌症纳米医学领域的巨大潜力。
{"title":"A tumor Microenvironment-triggered protein-binding Near-infrared-II Theranostic nanoplatform for Mild-Temperature photothermal therapy.","authors":"Wenlong Huang, Bo Jin, Haobing Gong, Nawab Ali, Duoduo Jiang, Tongtong Shan, Liangshun Zhang, Jia Tian, Weian Zhang","doi":"10.1016/j.jcis.2024.11.049","DOIUrl":"https://doi.org/10.1016/j.jcis.2024.11.049","url":null,"abstract":"<p><p>Photothermal therapy (PTT) has gained significant attention as a non-invasive treatment in clinical oncology. However, the translation of PTT into clinical practice remains constrained by three fundamental limitations: acquired thermal tolerance in tumor cells, restricted light penetration depth in biological matrices, and insufficient therapeutic outcomes from single-modality treatment. To address these issues, a strategy for forming in situ complexes between near-infrared-II (NIR-II) photothermal agents and proteins is developed, aimed at damaging protein conformation and enhancing PTT effectiveness. We developed a nanoplatform called PCy-SF, consisting of the NIR-II photothermal polymer (PCy) and sorafenib (SF). PCy-SF responds to the tumor microenvironment (TME), specifically releasing Cy-CHO and sorafenib from the assemblies. The released Cy-CHO covalently binds to proteins, forming Cy-Protein complexes that activate NIR-II fluorescence, facilitating NIR-II imaging-guided photothermal therapy. Concurrently, the released SF intensifies microvascular damage, synergizing with PTT for enhanced therapeutic efficacy. Notably, PCy-SF induces a strong anticancer immune response, effectively suppressing tumor recurrence and metastasis. This study introduces a promising protein deactivation strategy for achieving mild-temperature PTT, offering broader applicability of PTT and insights for sensitizing tumors to photothermal therapy. Together, this innovative approach combining NIR-II photothermal agents with protein complexation and a responsive nanoplatform enhances PTT precision and efficacy, demonstrating significant potential in the field of cancer nanomedicine.</p>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 Pt B","pages":"375-388"},"PeriodicalIF":9.4,"publicationDate":"2024-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142692296","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}
Pub Date : 2024-11-09DOI: 10.1016/j.jcis.2024.11.037
Chengzong Zeng , Xia Shen , Kun Shen , Linzhao Bao , Guangyin Liao , Jun Shen
The liquid metal (LM) composite is regarded as having potential and wide-ranging applications in electronic thermal management. Enhancing the thermal conductivity of LM is a crucial matter. Herein, a novel LM composite of eutectic gallium-indium (EGaIn)/diamond/graphite was developed. A highest thermal conductivity of 133 ± 3 W m−1 K−1 was achieved, 411 % higher than that of the matrix. The bonding mechanism reveals that the interfacial adsorption energy () of graphite and EGaIn can be effectively decreased by the functional groups of graphite (by −108 % for –OH and −125 % for −CO) and the oxide of EGaIn (by −64 %). Furthermore, the of diamond and EGaIn can be significantly reduced through the oxidation of EGaIn (by −83 %) and the H-terminal of diamond (by −187 %). The thermal conductance mechanism suggests that a 3 vol% graphite content in the EGaIn/40 vol% diamond/graphite composite can form an excellent thermal conductance bridge among diamond particles. However, the thermal conductivity of the composite significantly decreased when too much graphite was added due to the tendency of the graphite to coat the diamond particles. There was no significant change in the melting point of EGaIn after being mixed with diamond and graphite. The EGaIn/diamond/graphite composite also demonstrated excellent thermal management performance in LED lamps and CPU heat dissipation as a thermal interface material, particularly in high-power electronic devices. This work presents the potential to enhance the thermal conductivity of LM-based composite by bridging spheroidal particles with a flaky material.
液态金属（LM）复合材料被认为在电子热管理方面具有潜在而广泛的应用。提高液态金属的热导率是一个关键问题。在此，我们开发了一种新型的共晶镓铟 (EGaIn) / 金刚石/石墨液态金属复合材料。该复合材料的最高热导率为 133 ± 3 W m-1 K-1，比基体的热导率高出 411%。键合机理表明，石墨和 EGaIn 的界面吸附能（ΔE）可通过石墨的官能团（-OH 降低 108%，-CO 降低 125%）和 EGaIn 的氧化物（-64%）有效降低。此外，金刚石和 EGaIn 的 ΔE 可以通过 EGaIn 的氧化（-83%）和金刚石的 H 端（-187%）而显著降低。热传导机制表明，在 EGaIn/40 Vol% 金刚石/石墨复合材料中，3 Vol% 的石墨含量可在金刚石颗粒之间形成极佳的热传导桥。然而，当石墨添加过多时，复合材料的热导率会明显降低，原因是石墨容易包覆金刚石颗粒。EGaIn 与金刚石和石墨混合后，其熔点没有明显变化。作为一种热界面材料，EGaIn/金刚石/石墨复合材料在 LED 灯和 CPU 散热方面也表现出优异的热管理性能，尤其是在大功率电子设备中。这项研究通过将球形颗粒与片状材料桥接，展示了提高基于 LM 的复合材料导热性能的潜力。
{"title":"Boosted the thermal conductivity of liquid metal via bridging diamond particles with graphite","authors":"Chengzong Zeng , Xia Shen , Kun Shen , Linzhao Bao , Guangyin Liao , Jun Shen","doi":"10.1016/j.jcis.2024.11.037","DOIUrl":"10.1016/j.jcis.2024.11.037","url":null,"abstract":"<div><div>The liquid metal (LM) composite is regarded as having potential and wide-ranging applications in electronic thermal management. Enhancing the thermal conductivity of LM is a crucial matter. Herein, a novel LM composite of eutectic gallium-indium (EGaIn)/diamond/graphite was developed. A highest thermal conductivity of 133 ± 3 W m<sup>−1</sup> K<sup>−1</sup> was achieved, 411 % higher than that of the matrix. The bonding mechanism reveals that the interfacial adsorption energy (<span><math><mrow><mi>Δ</mi><mi>E</mi></mrow></math></span>) of graphite and EGaIn can be effectively decreased by the functional groups of graphite (by −108 % for –OH and −125 % for −C<img>O) and the oxide of EGaIn (by −64 %). Furthermore, the <span><math><mrow><mi>Δ</mi><mi>E</mi></mrow></math></span> of diamond and EGaIn can be significantly reduced through the oxidation of EGaIn (by −83 %) and the H-terminal of diamond (by −187 %). The thermal conductance mechanism suggests that a 3 vol% graphite content in the EGaIn/40 vol% diamond/graphite composite can form an excellent thermal conductance bridge among diamond particles. However, the thermal conductivity of the composite significantly decreased when too much graphite was added due to the tendency of the graphite to coat the diamond particles. There was no significant change in the melting point of EGaIn after being mixed with diamond and graphite. The EGaIn/diamond/graphite composite also demonstrated excellent thermal management performance in LED lamps and CPU heat dissipation as a thermal interface material, particularly in high-power electronic devices. This work presents the potential to enhance the thermal conductivity of LM-based composite by bridging spheroidal particles with a flaky material.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 643-656"},"PeriodicalIF":9.4,"publicationDate":"2024-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611308","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}
Pub Date : 2024-11-09DOI: 10.1016/j.jcis.2024.11.041
Xiaofeng Pan , Jian Guan , Shilin Cao , Xiaojuan Ma , Yonghao Ni , Qinhua Wang
To meet the stringent requirements of wearable and flexible electronics for functionality and comfort, it is urgent to develop green conductive, self-adhesive, and stretchable functional hydrogels. The chelates of transition metal ions and lignosulfonate sodium (LS) can impart multi-functionality to the hydrogel and significantly improve the hydrogel’s gelation speed. However, the presence of metal ions may weaken the adhesiveness of hydrogels by shielding the functional adhesive groups. Here, an oxidative metal ions-free lignin-catalyzed multifunctional polyacrylic acid (PAA) hydrogel is proposed. LS itself can undergo a redox reaction with the initiator to generate many free radicals, thereby catalyzing the rapid polymerization of polymer monomers at room temperature and subsequent gelation. Furthermore, LS can easily improve the hydrogels’ softness (compressive modulus: ∼7 kPa) and stretchability (maximum ∼2700 %). Interestingly, LS can simultaneously promote the hydrogel’s conductivity, adhesion, and UV blocking. Notably, the hydrogel integrating these advantageous features is suitable as non-invasive electronics in the human epidermis. We explored its ability to act as adhesive bioelectrodes to collect electrooculographic signals in patients with physical and language impairments. Bioelectrodes can recognize the patient’s eye movements. The displayed electrical signal can be output in 6 languages after being encoded. This provides a valuable case for LS-doped functional hydrogels in the medical field.
为满足可穿戴和柔性电子产品对功能性和舒适性的严格要求，迫切需要开发绿色导电、自粘性和可拉伸的功能性水凝胶。过渡金属离子螯合物和木质素磺酸钠（LS）可赋予水凝胶多功能性，并显著提高水凝胶的凝胶速度。然而，金属离子的存在可能会屏蔽功能性粘合基团，从而削弱水凝胶的粘合性。本文提出了一种不含氧化金属离子的木质素催化多功能聚丙烯酸（PAA）水凝胶。LS 本身可与引发剂发生氧化还原反应，生成许多自由基，从而催化聚合物单体在室温下快速聚合并随后凝胶化。此外，LS 还能轻松提高水凝胶的柔软度（压缩模量：∼7 kPa）和伸展性（最大值∼2700 %）。有趣的是，LS 还能同时提高水凝胶的导电性、粘附性和紫外线阻隔性。值得注意的是，集成了这些优势特性的水凝胶适合用作人体表皮的非侵入性电子器件。我们探索了水凝胶作为粘合生物电极的能力，以收集有身体和语言障碍的患者的脑电图信号。生物电极可以识别患者的眼球运动。显示的电信号经编码后可输出 6 种语言。这为掺杂 LS 的功能性水凝胶在医疗领域的应用提供了有价值的案例。
{"title":"An oxidative metal ions-free lignin-catalyzed multifunctional hydrogel bioelectronics for codable eye communication","authors":"Xiaofeng Pan , Jian Guan , Shilin Cao , Xiaojuan Ma , Yonghao Ni , Qinhua Wang","doi":"10.1016/j.jcis.2024.11.041","DOIUrl":"10.1016/j.jcis.2024.11.041","url":null,"abstract":"<div><div>To meet the stringent requirements of wearable and flexible electronics for functionality and comfort, it is urgent to develop green conductive, self-adhesive, and stretchable functional hydrogels. The chelates of transition metal ions and lignosulfonate sodium (LS) can impart multi-functionality to the hydrogel and significantly improve the hydrogel’s gelation speed. However, the presence of metal ions may weaken the adhesiveness of hydrogels by shielding the functional adhesive groups. Here, an oxidative metal ions-free lignin-catalyzed multifunctional polyacrylic acid (PAA) hydrogel is proposed. LS itself can undergo a redox reaction with the initiator to generate many free radicals, thereby catalyzing the rapid polymerization of polymer monomers at room temperature and subsequent gelation. Furthermore, LS can easily improve the hydrogels’ softness (compressive modulus: ∼7 kPa) and stretchability (maximum ∼2700 %). Interestingly, LS can simultaneously promote the hydrogel’s conductivity, adhesion, and UV blocking. Notably, the hydrogel integrating these advantageous features is suitable as non-invasive electronics in the human epidermis. We explored its ability to act as adhesive bioelectrodes to collect electrooculographic signals in patients with physical and language impairments. Bioelectrodes can recognize the patient’s eye movements. The displayed electrical signal can be output in 6 languages after being encoded. This provides a valuable case for LS-doped functional hydrogels in the medical field.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 753-761"},"PeriodicalIF":9.4,"publicationDate":"2024-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611298","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}
Pub Date : 2024-11-09DOI: 10.1016/j.jcis.2024.11.038
Muhammad Arif , Ayaz Mahsud , Haoran Xing , Abdul Hannan Zahid , Qian Liang , Muhammad Amjad Majeed , Amjad Ali , Xiazhang Li , Zhansheng Lu , Francis Leonard Deepak , Tahir Muhmood , Yinjuan Chen
The catalytic efficiency of heterogeneous photocatalytic CO2 reduction and photo-Fenton H2O2 activation is closely related to the local electron density of reaction center atoms. However, electron-hole recombination from random charge transfer significantly restricts the targeted electron delivery to the active center. Herein, Fe-C3N4/MoO3 heterojunction with interfacial coordination of atomically dispersed Fe-N4 sites with the O interface of MoO3 was synthesized by simple hydrothermal method. Based on the experimental results and density functional theory calculation (DFT), the heterojunction structure fosters accelerated interfacial electron transfer due to directional interfacial electric field (IEF) between Fe-CN and MoO heterogeneous interfaces, and the interfacial bond between Fe-N4 sites and O at the built-in interface regulates the local electron density of Fe-N4 active center. DFT further reveals that the interfacial electron flow and concentrated electron density at Fe-N4 sites result from the coordination between Fe-N4 and MoO3 interfaces. This directs electron flow towards the Fe center, significantly enhancing CO2 adsorption and H2O2 conversion efficiency. PDOS analysis shows that the dyz and dz2 orbitals of the isolated Fe atom in Fe-CN overlap with the pz orbital of the O atom in MoO3, playing a pivotal role in CO2 adsorption. Consequently, the Fe-CN/MoO3 heterojunction demonstrated highly efficient photocatalytic CO2 reduction to CH4, coupled with benzyl alcohol oxidation and photo-Fenton tetracycline degradation. These findings offer a promising multifunctional catalyst strategy for the development of energy conversion and environmental remediation.
异相光催化二氧化碳还原和光-芬顿 H2O2 活化的催化效率与反应中心原子的局部电子密度密切相关。然而，随机电荷转移产生的电子-空穴重组极大地限制了电子向活性中心的定向输送。本文采用简单的水热法合成了Fe-C3N4/MoO3异质结，其原子分散的Fe-N4位点与MoO3的O界面相互配位。根据实验结果和密度泛函理论（DFT）计算，异质结结构促进了Fe-CN和MoO异质界面之间的定向界面电场（IEF）所导致的加速界面电子转移，而Fe-N4位点与内置界面上的O之间的界面键调节了Fe-N4活性中心的局部电子密度。DFT 进一步揭示，Fe-N4 位点上的界面电子流和集中的电子密度来自于 Fe-N4 和 MoO3 界面之间的配位。这引导电子流向 Fe 中心，显著提高了 CO2 吸附和 H2O2 转化效率。PDOS 分析表明，Fe-CN 中孤立的 Fe 原子的 dyz 和 dz2 轨道与 MoO3 中 O 原子的 pz 轨道重叠，在吸附 CO2 的过程中起着关键作用。因此，Fe-CN/MoO3 异质结表现出了高效的光催化 CO2 还原成 CH4 的能力，同时还具有苯甲醇氧化和光 Fenton 降解四环素的能力。这些发现为开发能源转换和环境修复提供了一种前景广阔的多功能催化剂策略。
{"title":"Modulating the local electron density at built-in interface iron single sites in Fe-CN/MoO3 heterostructure for enhanced CO2 reduction to CH4 and photo-Fenton reaction","authors":"Muhammad Arif , Ayaz Mahsud , Haoran Xing , Abdul Hannan Zahid , Qian Liang , Muhammad Amjad Majeed , Amjad Ali , Xiazhang Li , Zhansheng Lu , Francis Leonard Deepak , Tahir Muhmood , Yinjuan Chen","doi":"10.1016/j.jcis.2024.11.038","DOIUrl":"10.1016/j.jcis.2024.11.038","url":null,"abstract":"<div><div>The catalytic efficiency of heterogeneous photocatalytic CO<sub>2</sub> reduction and photo-Fenton H<sub>2</sub>O<sub>2</sub> activation<!--> <!-->is<!--> <!-->closely related to the local electron density of reaction center atoms. However, electron-hole recombination from random charge transfer significantly restricts the targeted electron delivery to the active center. Herein, Fe-C<sub>3</sub>N<sub>4</sub>/MoO<sub>3</sub> heterojunction with interfacial coordination of atomically dispersed Fe-N<sub>4</sub> sites with the O interface of MoO<sub>3</sub> was synthesized by simple hydrothermal method. Based on the experimental results and density functional theory calculation (DFT), the heterojunction structure fosters accelerated interfacial electron transfer due to directional interfacial electric field (IEF) between Fe-CN and MoO heterogeneous interfaces, and the interfacial bond between Fe-N<sub>4</sub> sites and O at the built-in interface regulates the local electron density of Fe-N<sub>4</sub> active center. DFT further reveals that the interfacial electron flow and concentrated electron density at Fe-N<sub>4</sub> sites result from the coordination between Fe-N<sub>4</sub> and MoO<sub>3</sub> interfaces. This directs electron flow towards the Fe center, significantly enhancing CO<sub>2</sub> adsorption and H<sub>2</sub>O<sub>2</sub> conversion efficiency. PDOS analysis shows that the <em>d</em><sub>yz</sub> and <em>d</em><sub>z</sub><sup>2</sup> orbitals of the isolated Fe atom in Fe-CN overlap with the <em>p</em><sub>z</sub> orbital of the O atom in MoO<sub>3</sub>, playing a pivotal role in CO<sub>2</sub> adsorption. Consequently, the Fe-CN/MoO<sub>3</sub> heterojunction demonstrated highly efficient photocatalytic CO<sub>2</sub> reduction to CH<sub>4</sub>, coupled with benzyl alcohol oxidation and photo-Fenton tetracycline degradation. These findings offer a promising multifunctional catalyst strategy for the development of energy conversion and environmental remediation.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 1053-1066"},"PeriodicalIF":9.4,"publicationDate":"2024-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142643636","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-09DOI: 10.1016/j.jcis.2024.11.044
Yameng Jiao , Qiang Song , Xu Yang , Ruimei Yuan , Di Zhao , Yuanxiao Zhao , Qingliang Shen , Hejun Li
Multifaceted balance makes the design of ceramics difficult but is urgently needed. This work purposes to grow uniform edge-rich graphene (ERG) on alumina (Al2O3/ERG) in-situ, then constructs a discontinuous conductive, strengthening and toughening network of crosslinked ERG by mixing Al2O3/ERG with Al2O3 and sintering. Under the guarantee of the tight-bound covalent interface, ERG and doping Al2O3 strengthen and toughen the ceramic by synergistic effect of weak and strong interface. And doping Al2O3 interrupts the conductive network of ERG to improve the impedance matching and endow material with moderate electromagnetic wave (EMW) loss capacity. The optimal flexural strength and fracture toughness of the composite ceramic reach 333.04 MPa and 12.43 MPa⋅m1/2, respectively. Meanwhile, it can absorb 80 % or more of the incident EMW in X-band with a matching thickness of 2 mm. This work takes full advantage of ERG to prepare load-bearing EMW absorbing ceramics, which expands the idea for material design.
{"title":"Strong and weak interface synergistic enhance the mechanical and microwave absorption properties of alumina","authors":"Yameng Jiao , Qiang Song , Xu Yang , Ruimei Yuan , Di Zhao , Yuanxiao Zhao , Qingliang Shen , Hejun Li","doi":"10.1016/j.jcis.2024.11.044","DOIUrl":"10.1016/j.jcis.2024.11.044","url":null,"abstract":"<div><div>Multifaceted balance makes the design of ceramics difficult but is urgently needed. This work purposes to grow uniform edge-rich graphene (ERG) on alumina (Al<sub>2</sub>O<sub>3</sub>/ERG) in-situ, then constructs a discontinuous conductive, strengthening and toughening network of crosslinked ERG by mixing Al<sub>2</sub>O<sub>3</sub>/ERG with Al<sub>2</sub>O<sub>3</sub> and sintering. Under the guarantee of the tight-bound covalent interface, ERG and doping Al<sub>2</sub>O<sub>3</sub> strengthen and toughen the ceramic by synergistic effect of weak and strong interface. And doping Al<sub>2</sub>O<sub>3</sub> interrupts the conductive network of ERG to improve the impedance matching and endow material with moderate electromagnetic wave (EMW) loss capacity. The optimal flexural strength and fracture toughness of the composite ceramic reach 333.04 MPa and 12.43 MPa⋅m<sup>1/2</sup>, respectively. Meanwhile, it can absorb 80 % or more of the incident EMW in X-band with a matching thickness of 2 mm. This work takes full advantage of ERG to prepare load-bearing EMW absorbing ceramics, which expands the idea for material design.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 1007-1015"},"PeriodicalIF":9.4,"publicationDate":"2024-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142643651","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}
Hydrogels hold great potential for use in intelligent packaging, yet they often suffer from limited functionality and inadequate mechanical strength when applied to anticounterfeiting and freshness monitoring. In this study, we present a straightforward method to create a multifunctional hydrogel by in-situ polymerizing acrylic acid (PAA) within a gelatin-Al3+ system. The resulting hydrogels exhibited an elongation at break of over 1200 %, a tensile stress of 1.20 MPa, and impressive toughness reaching 5.15 MJ/m3, significantly outperforming traditional gelatin-based hydrogels that typically achieve less than 800 % strain and below 1 MPa stress. These hydrogels also showed exceptional antifatigue and tear resistance, with a tearing energy of 5200 J/m2, greatly exceeding the 1000 J/m2 standard of typical double network hydrogels, and were capable of supporting weights 1560 times their own mass. The strong hydrogen bonding between the –COOH groups of PAA and the –NH2 groups of gelatins contributed to an upper critical solution temperature above 40°C, with adaptable PAA content allowing for anticounterfeiting applications. The hydrogel could encode information such as self-erasing numbers, QR codes, and ASCII binary codes, changing its encoded data with temperature shifts and erasing at room temperature to enhance data security. Additionally, it exhibited potent antibacterial properties against S. aureus and E. coli, immobilized anthocyanin as an ammonia-responsive indicator, and accurately tracked salmon spoilage by correlating color changes with total volatile basic nitrogen content. These characteristics make the hydrogel highly suitable for smart packaging applications within the food industry.
{"title":"Polyacrylic Acid-Reinforced gelatin hydrogels with enhanced mechanical properties, temperature-responsiveness and antimicrobial activity for smart encryption and salmon freshness monitoring","authors":"Siyao Luo, Chang-Ying Hu, Shiqing Huang, Xiaowen Xu","doi":"10.1016/j.jcis.2024.11.048","DOIUrl":"10.1016/j.jcis.2024.11.048","url":null,"abstract":"<div><div>Hydrogels hold great potential for use in intelligent packaging, yet they often suffer from limited functionality and inadequate mechanical strength when applied to anticounterfeiting and freshness monitoring. In this study, we present a straightforward method to create a multifunctional hydrogel by in-situ polymerizing acrylic acid (PAA) within a gelatin-Al<sup>3+</sup> system. The resulting hydrogels exhibited an elongation at break of over 1200 %, a tensile stress of 1.20 MPa, and impressive toughness reaching 5.15 MJ/m<sup>3</sup>, significantly outperforming traditional gelatin-based hydrogels that typically achieve less than 800 % strain and below 1 MPa stress. These hydrogels also showed exceptional antifatigue and tear resistance, with a tearing energy of 5200 J/m<sup>2</sup>, greatly exceeding the 1000 J/m<sup>2</sup> standard of typical double network hydrogels, and were capable of supporting weights 1560 times their own mass. The strong hydrogen bonding between the –COOH groups of PAA and the –NH<sub>2</sub> groups of gelatins contributed to an upper critical solution temperature above 40°C, with adaptable PAA content allowing for anticounterfeiting applications. The hydrogel could encode information such as self-erasing numbers, QR codes, and ASCII binary codes, changing its encoded data with temperature shifts and erasing at room temperature to enhance data security. Additionally, it exhibited potent antibacterial properties against <em>S. aureus</em> and <em>E. coli</em>, immobilized anthocyanin as an ammonia-responsive indicator, and accurately tracked salmon spoilage by correlating color changes with total volatile basic nitrogen content. These characteristics make the hydrogel highly suitable for smart packaging applications within the food industry.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 725-741"},"PeriodicalIF":9.4,"publicationDate":"2024-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611400","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}
Pub Date : 2024-11-09DOI: 10.1016/j.jcis.2024.11.034
Yuxuan Shao , Junjie Ni , Jie Yin , Xinqing Liu , Yulai Song , Yue Xu , Shuai Guo , Laima Luo
The construction of heterojunctions between non-noble-metal based compounds affords a scheme for accelerating the reaction kinetics of oxygen evolution reaction (OER) without using precious mental materials, which is extremely important but remains challenging. Herein, the heterogeneous structure between Fe60Co10Ni10Cr10Mn10 medium-entropy alloy (MEA) and FeS2 is developed by a mechanical alloying approach. The resulting MEA-30 wt%FeS2 delivers a high OER activity with a low overpotential of 261.6 mV at 10 mA/cm2, along with Tafel slope of 52.7 mV/dec in 1.0 mol/L KOH solution, superior to the commercial RuO2. The combination of detailed characterization techniques and density functional theory (DFT) calculation reveals that the heterojunctions between Fe-based MEA and FeS2 generates the synergistic effect on the activation and formation steps of OOH*, thus promoting the OER reaction kinetics. Furthermore, the abundant active sites provided by the reconstructions of MEA-30 wt%FeS2 during OER process also contributes to the catalytic performance. This work greatly expands the application scope of medium-entropy materials and provides a new method for the fabrication of novel heterogeneous electrocatalyst of Fe-based MEA and FeS2.
在非贵金属基化合物之间构建异质结提供了一种在不使用贵金属材料的情况下加速氧进化反应（OER）反应动力学的方案，这一点极为重要，但仍然具有挑战性。本文通过机械合金化方法，在 Fe60Co10Ni10Cr10Mn10 中熵合金（MEA）和 FeS2 之间建立了异质结构。由此得到的 MEA-30 wt%FeS2 具有很高的 OER 活性，在 10 mA/cm2 的条件下过电位低至 261.6 mV，在 1.0 mol/L KOH 溶液中的 Tafel 斜坡为 52.7 mV/dec，优于商用 RuO2。结合详细的表征技术和密度泛函理论（DFT）计算发现，铁基 MEA 和 FeS2 之间的异质结对 OOH* 的活化和形成步骤产生了协同效应，从而促进了 OER 反应动力学。此外，在 OER 过程中，MEA-30 wt%FeS2 重构所提供的丰富活性位点也有助于提高催化性能。这项工作大大拓展了中等熵材料的应用范围，并为制备新型铁基 MEA 和 FeS2 异质电催化剂提供了一种新方法。
{"title":"Heterogeneous electrocatalyst of nanoscale Fe-based medium-entropy alloy and sulfide for oxygen evolution reaction","authors":"Yuxuan Shao , Junjie Ni , Jie Yin , Xinqing Liu , Yulai Song , Yue Xu , Shuai Guo , Laima Luo","doi":"10.1016/j.jcis.2024.11.034","DOIUrl":"10.1016/j.jcis.2024.11.034","url":null,"abstract":"<div><div>The construction of heterojunctions between non-noble-metal based compounds affords a scheme for accelerating the reaction kinetics of oxygen evolution reaction (OER) without using precious mental materials, which is extremely important but remains challenging. Herein, the heterogeneous structure between Fe<sub>60</sub>Co<sub>10</sub>Ni<sub>10</sub>Cr<sub>10</sub>Mn<sub>10</sub> medium-entropy alloy (MEA) and FeS<sub>2</sub> is developed by a mechanical alloying approach. The resulting MEA-30 wt%FeS<sub>2</sub> delivers a high OER activity with a low overpotential of 261.6 mV at 10 mA/cm<sup>2</sup>, along with Tafel slope of 52.7 mV/dec in 1.0 mol/L KOH solution, superior to the commercial RuO<sub>2</sub>. The combination of detailed characterization techniques and density functional theory (DFT) calculation reveals that the heterojunctions between Fe-based MEA and FeS<sub>2</sub> generates the synergistic effect on the activation and formation steps of OOH*, thus promoting the OER reaction kinetics. Furthermore, the abundant active sites provided by the reconstructions of MEA-30 wt%FeS<sub>2</sub> during OER process also contributes to the catalytic performance. This work greatly expands the application scope of medium-entropy materials and provides a new method for the fabrication of novel heterogeneous electrocatalyst of Fe-based MEA and FeS<sub>2</sub>.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 742-752"},"PeriodicalIF":9.4,"publicationDate":"2024-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611366","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}
Pub Date : 2024-11-09DOI: 10.1016/j.jcis.2024.11.039
Yuecen Zhao , Hengzhen Feng , Wenzhong Lou , Li Li , Quansheng Wang , Guifu Ding , Congchun Zhang
Thermal barrier coatings (TBCs) have garnered significant attention as crucial protective components for turbine blades. However, the current use of TBCs is limited by their singular functionality and the inability to accurately obtain the temperature gradient distribution within the coatings. Addressing the aforementioned issues, this paper proposes an intelligent thermal barrier coating embedded with thin-film thermocouples. This method not only provides effective thermal protection but also facilitates the precise measurement of the internal temperature gradient within the coating. To mitigate the thermal mismatch in TBCs under high-temperature environments, which can compromise their lifespan, this study employs multi-objective optimization of structural parameters to design an optimal coating thickness. This strategy ensures both superior thermal protection and extended service life. The intelligent temperature-sensing TBCs were fabricated using atmospheric plasma spraying and magnetron sputtering, followed by comprehensive characterization. To validate the performance of the intelligent temperature-sensing TBCs, static tests were conducted in a muffle furnace. The results demonstrated that the sensors exhibit excellent repeatability and high-temperature durability. Furthermore, a test platform replicating the thermal shock conditions of an engine environment was developed. This platform confirmed that the intelligent temperature-sensing TBCs are capable of accurately measuring the internal temperature gradient within the coating under engine-like conditions, offering a novel methodology for engine monitoring and diagnostics.
{"title":"Intelligent temperature measuring thermal spray multilayer thermal barrier coatings based on embedded thin film thermocouples","authors":"Yuecen Zhao , Hengzhen Feng , Wenzhong Lou , Li Li , Quansheng Wang , Guifu Ding , Congchun Zhang","doi":"10.1016/j.jcis.2024.11.039","DOIUrl":"10.1016/j.jcis.2024.11.039","url":null,"abstract":"<div><div>Thermal barrier coatings (TBCs) have garnered significant attention as crucial protective components for turbine blades. However, the current use of TBCs is limited by their singular functionality and the inability to accurately obtain the temperature gradient distribution within the coatings. Addressing the aforementioned issues, this paper proposes an intelligent thermal barrier coating embedded with thin-film thermocouples. This method not only provides effective thermal protection but also facilitates the precise measurement of the internal temperature gradient within the coating. To mitigate the thermal mismatch in TBCs under high-temperature environments, which can compromise their lifespan, this study employs multi-objective optimization of structural parameters to design an optimal coating thickness. This strategy ensures both superior thermal protection and extended service life. The intelligent temperature-sensing TBCs were fabricated using atmospheric plasma spraying and magnetron sputtering, followed by comprehensive characterization. To validate the performance of the intelligent temperature-sensing TBCs, static tests were conducted in a muffle furnace. The results demonstrated that the sensors exhibit excellent repeatability and high-temperature durability. Furthermore, a test platform replicating the thermal shock conditions of an engine environment was developed. This platform confirmed that the intelligent temperature-sensing TBCs are capable of accurately measuring the internal temperature gradient within the coating under engine-like conditions, offering a novel methodology for engine monitoring and diagnostics.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 1042-1052"},"PeriodicalIF":9.4,"publicationDate":"2024-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142643623","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}
Pub Date : 2024-11-08DOI: 10.1016/j.jcis.2024.11.040
Ge Bai , Chunhua Niu , Xuexue Liang , Lan Li , Yulong Feng , Zhong Wei , Kai Chen , Klemen Bohinc , Xuhong Guo
Calcium peroxide (CaO2) is commonly used as a hydrogen peroxide (H2O2) donor to eliminate bacterial infections. However, the rapid dissociation of CaO2 and the explosive release of H2O2 have limited the development of CaO2 in the antibacterial field. Therefore, a series of silver nanoparticles (AgNPs) functionalized bacteria-triggered smart hydrogels (CSA-H) that integrate sustained release of nanoparticles and localized chemodynamic sterilization were constructed. The pH-responsive hydrogel formed through the Schiff base reaction enables the responsive release of CaO2 nanoparticles while simultaneously regulating the concentration of H2O2 within the bacterial infection microenvironment. AgNPs are capable of reacting with H2O2 under mildly acidic conditions to produce hydroxyl radicals with enhanced antimicrobial activity. The antimicrobial results demonstrated that AgNPs functionalized silicon dioxide-coated calcium peroxide (CaO2@SiO2/AgNPs) nanoparticles exhibited enhanced bactericidal activity compared to AgNPs or CaO2 alone. Furthermore, CSA-H hydrogels exhibited significant antibacterial activity against S. aureus and E. coli under the dual effect of AgNPs and pH-driven Fenton-like reactions. This chemodynamic antibacterial platform is environmentally responsive and provides a promising strategy for creating multifunctional hydrogels loaded with nano-enzymes, thus advancing the development of AgNPs in chemodynamic-antibacterial related applications.
{"title":"Engineering Robust Silver-Decorated calcium peroxide Nano-Antibacterial Platforms for chemodynamic enhanced sterilization","authors":"Ge Bai , Chunhua Niu , Xuexue Liang , Lan Li , Yulong Feng , Zhong Wei , Kai Chen , Klemen Bohinc , Xuhong Guo","doi":"10.1016/j.jcis.2024.11.040","DOIUrl":"10.1016/j.jcis.2024.11.040","url":null,"abstract":"<div><div>Calcium peroxide (CaO<sub>2</sub>) is commonly used as a hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) donor to eliminate bacterial infections. However, the rapid dissociation of CaO<sub>2</sub> and the explosive release of H<sub>2</sub>O<sub>2</sub> have limited the development of CaO<sub>2</sub> in the antibacterial field. Therefore, a series of silver nanoparticles (AgNPs) functionalized bacteria-triggered smart hydrogels (CSA-H) that integrate sustained release of nanoparticles and localized chemodynamic sterilization were constructed. The pH-responsive hydrogel formed through the Schiff base reaction enables the responsive release of CaO<sub>2</sub> nanoparticles while simultaneously regulating the concentration of H<sub>2</sub>O<sub>2</sub> within the bacterial infection microenvironment. AgNPs are capable of reacting with H<sub>2</sub>O<sub>2</sub> under mildly acidic conditions to produce hydroxyl radicals with enhanced antimicrobial activity. The antimicrobial results demonstrated that AgNPs functionalized silicon dioxide-coated calcium peroxide (CaO<sub>2</sub>@SiO<sub>2</sub>/AgNPs) nanoparticles exhibited enhanced bactericidal activity compared to AgNPs or CaO<sub>2</sub> alone. Furthermore, CSA-H hydrogels exhibited significant antibacterial activity against <em>S. aureus</em> and <em>E. coli</em> under the dual effect of AgNPs and pH-driven Fenton-like reactions. This chemodynamic antibacterial platform is environmentally responsive and provides a promising strategy for creating multifunctional hydrogels loaded with nano-enzymes, thus advancing the development of AgNPs in chemodynamic-antibacterial related applications.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 684-695"},"PeriodicalIF":9.4,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142611328","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}
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