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Adsorption suppression and viscosity transition in semidilute PEO/silica nanoparticle mixtures under the protein limit
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137377
Saki Kusakabe , Xiang Li , Koichi Mayumi , Takuya Katashima , Ichiro Sakuma , Yuki Akagi
Understanding the interplay between polymer adsorption and colloidal interactions is essential for designing advanced materials with tailored properties. This study investigates the adsorption-driven aggregation and rheological transitions in semidilute mixtures of silica nanoparticles and high-molecular-weight poly(ethylene oxide) (PEO) in the protein limit, where the polymer’s size exceeds that of the particles. By systematically varying the ratio of the particle hydrodynamic size to the polymer’s hydrodynamic screening length (Rh,silica/ξh,PEO), distinct regimes of adsorption suppression, aggregation onset, and saturation were identified. Below Rh,silica/ξh,PEO = 1, adsorption was suppressed due to the entropic penalty of polymer distortion, resulting in negligible viscosity changes and stable particle dispersions. Near Rh,silica/ξh,PEO = 1, the adsorption energy overcame the entropy loss, triggering rapid aggregation and a sharp increase in viscosity, accompanied by the emergence of a slow relaxation mode in dynamic light scattering. At higher ratios (Rh,silica/ξh,PEO > 2), adsorption saturated, forming dense PEO-silica aggregates, as confirmed by small-angle neutron scattering. These findings challenge conventional theories of polymer adsorption and emphasize the critical role of polymer conformational entropy and adsorption energy balance. This study provides a framework for understanding polymer-mediated colloidal interactions in semidilute regimes, with implications for the rational design of polymer-colloid composites in materials science, biophysics, and industrial formulations.
了解聚合物吸附与胶体相互作用之间的相互作用对于设计具有定制特性的先进材料至关重要。本研究探讨了二氧化硅纳米粒子和高分子量聚环氧乙烷(PEO)半稀混合物在蛋白质极限下的吸附驱动聚集和流变转变。通过系统地改变颗粒的流体力学尺寸与聚合物的流体力学筛选长度之比(Rh,二氧化硅/ξh,PEO),确定了不同的吸附抑制、聚集开始和饱和状态。在 Rh,silica/ξh,PEO = 1 以下,由于聚合物变形的熵罚,吸附受到抑制,导致粘度变化可以忽略不计,颗粒分散稳定。在 Rh,silica/ξh,PEO = 1 附近,吸附能量超过了熵损失,引发了快速聚集和粘度的急剧增加,同时在动态光散射中出现了缓慢的弛豫模式。小角中子散射证实,在较高比率(Rh,二氧化硅/ξh,PEO >2)下,吸附饱和,形成致密的 PEO-二氧化硅聚集体。这些发现挑战了聚合物吸附的传统理论,强调了聚合物构象熵和吸附能量平衡的关键作用。这项研究为理解半稀释状态下聚合物介导的胶体相互作用提供了一个框架,对合理设计材料科学、生物物理学和工业配方中的聚合物-胶体复合材料具有重要意义。
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引用次数: 0
Co0.5CuP loaded Cd0.9Co0.1S hollow nanospheres with p-n heterojunction for photocatalytic hydrogen production
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137491
Qian Liu , Changdi Wang , Jianxiang Wang , Xiangjie Cui , Xingrong Zhang , Ruiyang Zhao , Jishu Han , Lei Wang
The development of efficient and stable composite photocatalysts is crucial for advancing the field of photocatalytic hydrogen production. In this paper, the Co0.5CuP/Cd0.9Co0.1S composite photocatalyst was synthesized by the template etching method and the in-situ growth method. The Co0.5CuP was tightly anchored on the surface of hollow structure Cd0.9Co0.1S nanospheres. The hydrogen production efficiency of the Co0.5CuP/Cd0.9Co0.1S composite photocatalyst was enhanced by adjusting the doping proportion of cobalt and the loading quantity of Co0.5CuP. Meanwhile, a p-n heterojunction was formed between Co0.5CuP and Cd0.9Co0.1S, which enhanced the separation of photoinduced charge carriers and further boosted the efficiency of photocatalytic hydrogen production. The results showed that the photocatalytic hydrogen evolution efficiency of Co0.5CuP/Cd0.9Co0.1S could reach 9.64 mmol·g−1·h−1. In addition, the photocatalytic reaction mechanism of the Co0.5CuP/Cd0.9Co0.1S composite photocatalyst was inferred based on the photoelectrochemical test and density functional theory calculation. This approach pioneers a novel pathway for the preparation of heterojunction photocatalysts by the combination of transition metal phosphide and hollow multi-metal sulfides.
{"title":"Co0.5CuP loaded Cd0.9Co0.1S hollow nanospheres with p-n heterojunction for photocatalytic hydrogen production","authors":"Qian Liu ,&nbsp;Changdi Wang ,&nbsp;Jianxiang Wang ,&nbsp;Xiangjie Cui ,&nbsp;Xingrong Zhang ,&nbsp;Ruiyang Zhao ,&nbsp;Jishu Han ,&nbsp;Lei Wang","doi":"10.1016/j.jcis.2025.137491","DOIUrl":"10.1016/j.jcis.2025.137491","url":null,"abstract":"<div><div>The development of efficient and stable composite photocatalysts is crucial for advancing the field of photocatalytic hydrogen production. In this paper, the Co<sub>0.5</sub>CuP/Cd<sub>0.9</sub>Co<sub>0.1</sub>S composite photocatalyst was synthesized by the template etching method and the in-situ growth method. The Co<sub>0.5</sub>CuP was tightly anchored on the surface of hollow structure Cd<sub>0.9</sub>Co<sub>0.1</sub>S nanospheres. The hydrogen production efficiency of the Co<sub>0.5</sub>CuP/Cd<sub>0.9</sub>Co<sub>0.1</sub>S composite photocatalyst was enhanced by adjusting the doping proportion of cobalt and the loading quantity of Co<sub>0.5</sub>CuP. Meanwhile, a p-n heterojunction was formed between Co<sub>0.5</sub>CuP and Cd<sub>0.9</sub>Co<sub>0.1</sub>S, which enhanced the separation of photoinduced charge carriers and further boosted the efficiency of photocatalytic hydrogen production. The results showed that the photocatalytic hydrogen evolution efficiency of Co<sub>0.5</sub>CuP/Cd<sub>0.9</sub>Co<sub>0.1</sub>S could reach 9.64 mmol·g<sup>−1</sup>·h<sup>−1</sup>. In addition, the photocatalytic reaction mechanism of the Co<sub>0.5</sub>CuP/Cd<sub>0.9</sub>Co<sub>0.1</sub>S composite photocatalyst was inferred based on the photoelectrochemical test and density functional theory calculation. This approach pioneers a novel pathway for the preparation of heterojunction photocatalysts by the combination of transition metal phosphide and hollow multi-metal sulfides.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137491"},"PeriodicalIF":9.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776929","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 loading of atomically exposed edge nickel sites embedded in hollow porous carbon nanofibers for enhanced methanol electrooxidation in direct methanol fuel cells
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137488
Fei Chen , Quan Zhou , Shuyan Yu , Shiquan Guo , Man Guo , Chong Zhang , Ziyu Guan , Haijiao Xie , Congju Li
The enhancement of catalytic activity and durability for atomically dispersed metal-nitrogen-carbon (M–N–C) catalysts in methanol oxidation reaction (MOR) anodes within direct methanol fuel cells presents a significant challenge. Here, we developed hollow porous nanofiber catalysts featuring edge Ni–N4 atomic sites through coaxial electrostatic spinning with domain-restricted Ni atoms embedded within a zeolitic imidazolium ester backbone, thereby increasing the exposure of accessible active sites (Ni: 4.96 %). The distinctive hollow porous fiber morphology and hierarchical structure facilitate convenient electronic conductivity and mass transport of reactants. Theoretical findings indicate that the surface adsorption of methanol at the edge Ni–N4 atomic sites exhibits negative free energy, promoting the adsorption and activation of reactants. Furthermore, the initial dehydrogenation step demonstrates a low free energy change, favoring reaction kinetics. The membrane electrode assembly achieved a power density of 42.2 mW cm−2 in single-cell application tests while displaying improved durability. This research provides valuable insights for future advancements in single-atom catalyst development for fuel cells or other energy applications.
在直接甲醇燃料电池的甲醇氧化反应(MOR)阳极中,如何提高原子分散金属氮碳(M-N-C)催化剂的催化活性和耐久性是一项重大挑战。在此,我们开发了中空多孔纳米纤维催化剂,通过同轴静电纺丝,将域受限的镍原子嵌入沸石咪唑鎓酯骨架中,从而增加了可触及活性位点(镍:4.96%)的暴露率,使其具有边缘镍-镍-碳原子位点。独特的中空多孔纤维形态和分层结构有利于电子传导和反应物的质量传输。理论研究结果表明,甲醇在 Ni-N4 原子位点边缘的表面吸附表现出负自由能,促进了反应物的吸附和活化。此外,最初的脱氢步骤显示出较低的自由能变化,有利于反应动力学。在单电池应用测试中,膜电极组件的功率密度达到了 42.2 mW cm-2,同时显示出更好的耐用性。这项研究为未来燃料电池或其他能源应用领域的单原子催化剂开发提供了宝贵的启示。
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引用次数: 0
Novel production of basalt nanosheets with ultrahigh aspect ratios and their assembly with nylon membranes for high-performance electrical insulating composite membranes
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137466
Dexian Ji , Shunxi Song , Xin Tong , Hao Sun , Cong Ma , Baolong Yuan , Yonghao Ni , Meiyun Zhang
The rapid advancement of modern electrical equipment has significantly increased the demand for advanced electrical insulating materials. Traditional silicate nanosheets are widely used as fillers in electrical insulating composites. However, their low aspect ratio restricts their effectiveness in high-performance electrical insulating applications. Here, a three-step liquid exfoliation strategy is proposed to prepare basalt nanosheets (BSNs) with an ultrahigh aspect ratio (up to 1397) from basalt scales (BS). This process involves cation exchange on BS to generate lamellar structures, serving as the basis for the preparation of lithium ion-exchanged BSNs (LBSNs). Next, oxalic acid/hydrogen peroxide treatment breaks the chemical bonds within the LBS sediment, producing chemically treated BSNs (CBSNs). Finally, BSNs are prepared by mixing LBSNs and CBSNs, followed by differential centrifugation to isolate BSNs with an ultrahigh aspect ratio (BSNs-1000). Subsequently, inspired by the overlapping structure of pangolin skin, BSNs-1000 are assembled onto nylon membranes, forming biomimetic nylon/BSNs-1000 (N/B-1000) composite membranes with an overlapping surface structure. This structure forms an effective physical barrier, impeding charge and crack propagation, thereby significantly enhancing their electrical insulating and mechanical properties. The novel exfoliation method and biomimetic strategy provide effective approaches for developing advanced electrical insulating membranes for high-performance electrical equipment.
{"title":"Novel production of basalt nanosheets with ultrahigh aspect ratios and their assembly with nylon membranes for high-performance electrical insulating composite membranes","authors":"Dexian Ji ,&nbsp;Shunxi Song ,&nbsp;Xin Tong ,&nbsp;Hao Sun ,&nbsp;Cong Ma ,&nbsp;Baolong Yuan ,&nbsp;Yonghao Ni ,&nbsp;Meiyun Zhang","doi":"10.1016/j.jcis.2025.137466","DOIUrl":"10.1016/j.jcis.2025.137466","url":null,"abstract":"<div><div>The rapid advancement of modern electrical equipment has significantly increased the demand for advanced electrical insulating materials. Traditional silicate nanosheets are widely used as fillers in electrical insulating composites. However, their low aspect ratio restricts their effectiveness in high-performance electrical insulating applications. Here, a three-step liquid exfoliation strategy is proposed to prepare basalt nanosheets (BSNs) with an ultrahigh aspect ratio (up to 1397) from basalt scales (BS). This process involves cation exchange on BS to generate lamellar structures, serving as the basis for the preparation of lithium ion-exchanged BSNs (LBSNs). Next, oxalic acid/hydrogen peroxide treatment breaks the chemical bonds within the LBS sediment, producing chemically treated BSNs (CBSNs). Finally, BSNs are prepared by mixing LBSNs and CBSNs, followed by differential centrifugation to isolate BSNs with an ultrahigh aspect ratio (BSNs-1000). Subsequently, inspired by the overlapping structure of pangolin skin, BSNs-1000 are assembled onto nylon membranes, forming biomimetic nylon/BSNs-1000 (N/B-1000) composite membranes with an overlapping surface structure. This structure forms an effective physical barrier, impeding charge and crack propagation, thereby significantly enhancing their electrical insulating and mechanical properties. The novel exfoliation method and biomimetic strategy provide effective approaches for developing advanced electrical insulating membranes for high-performance electrical equipment.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137466"},"PeriodicalIF":9.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759953","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
Cationic porphyrin-based covalent organic frameworks for enhanced phototherapy and targeted chemotherapy of bacterial infections
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137494
Jia-Jun Qian , Jing-Xuan Guo , Meng-Chao Wang , Li-Jian Chen , Xu Zhao , Xiu-Ping Yan
Bacterial infections significantly impede wound healing and threaten global public health. Porphyrin covalent organic frameworks (COFs) have shown promise as phototherapy antibacterial materials. However, the inherent π–π stacking interactions between the monomers also lead to aggregation and quenching of photosensitizers, thereby reducing the production of singlet oxygen (1O2) and compromising their antibacterial efficacy. Herein, we designed and prepared a novel cationic porphyrin-based COFs nanoplatform (TAPP-VIO), utilizing photosensitive TAPP and cationic VIO as structural units. This multifunctional nanoplatform is specifically tailored for targeted phototherapy and chemotherapy against bacterial infections. Upon irradiation, TAPP unit in TAPP-VIO generates heat and 1O2, which effectively disrupt bacterial structure and cause cell death. The incorporation of VIO unit introduces electrostatic repulsion between layers, mitigating π-π stacking effects and enhancing 1O2 production. Additionally, the positive charge imparted by the VIO unit enables TAPP-VIO to bind efficiently to negatively charged bacterial surfaces, immobilizing the bacteria and reducing their motility, thereby improving the overall efficacy of phototherapy. Under identical experimental conditions and concentrations, TAPP-VIO exhibits a 1O2 generation capacity that is 179% higher than that of nonionic porphyrin COF. Moreover, the temperature increase induced by TAPP-VIO is 85% of that observed with nonionic porphyrin COF (TAPP-MMA-Da), which is conducive to enhancing the phototherapeutic effects while minimizing heat-induced damage to healthy tissues. In summary, our study presents a straightforward approach to developing non-antibiotic antibacterial nanoagents, and the as-prepared TAPP-VIO is a promising candidate drug suitable for clinical trials in the future.
{"title":"Cationic porphyrin-based covalent organic frameworks for enhanced phototherapy and targeted chemotherapy of bacterial infections","authors":"Jia-Jun Qian ,&nbsp;Jing-Xuan Guo ,&nbsp;Meng-Chao Wang ,&nbsp;Li-Jian Chen ,&nbsp;Xu Zhao ,&nbsp;Xiu-Ping Yan","doi":"10.1016/j.jcis.2025.137494","DOIUrl":"10.1016/j.jcis.2025.137494","url":null,"abstract":"<div><div>Bacterial infections significantly impede wound healing and threaten global public health. Porphyrin covalent organic frameworks (COFs) have shown promise as phototherapy antibacterial materials. However, the inherent π–π stacking interactions between the monomers also lead to aggregation and quenching of photosensitizers, thereby reducing the production of singlet oxygen (<sup>1</sup>O<sub>2</sub>) and compromising their antibacterial efficacy. Herein, we designed and prepared a novel cationic porphyrin-based COFs nanoplatform (TAPP-VIO), utilizing photosensitive TAPP and cationic VIO as structural units. This multifunctional nanoplatform is specifically tailored for targeted phototherapy and chemotherapy against bacterial infections. Upon irradiation, TAPP unit in TAPP-VIO generates heat and <sup>1</sup>O<sub>2</sub>, which effectively disrupt bacterial structure and cause cell death. The incorporation of VIO unit introduces electrostatic repulsion between layers, mitigating π-π stacking effects and enhancing <sup>1</sup>O<sub>2</sub> production. Additionally, the positive charge imparted by the VIO unit enables TAPP-VIO to bind efficiently to negatively charged bacterial surfaces, immobilizing the bacteria and reducing their motility, thereby improving the overall efficacy of phototherapy<strong>.</strong> Under identical experimental conditions and concentrations, TAPP-VIO exhibits a <sup>1</sup>O<sub>2</sub> generation capacity that is 179% higher than that of nonionic porphyrin COF. Moreover, the temperature increase induced by TAPP-VIO is 85% of that observed with nonionic porphyrin COF (TAPP-MMA-Da), which is conducive to enhancing the phototherapeutic effects while minimizing heat-induced damage to healthy tissues. In summary, our study presents a straightforward approach to developing non-antibiotic antibacterial nanoagents, and the as-prepared TAPP-VIO is a promising candidate drug suitable for clinical trials in the future.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137494"},"PeriodicalIF":9.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776926","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
Enhancing the electrochemical conversion of carbon dioxide to value-added products on zinc oxide-MXene nanocomposite 在氧化锌-MXene 纳米复合材料上加强二氧化碳向增值产品的电化学转化
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137487
AbdulHakam Shafiu Abdullahi , Umar Mustapha , Omer Ahmed Taialla , Esraa Kotob , Ijaz Hussain , Khalid Alhooshani , Shehzada Muhammad Sajid Jillani , Saheed A. Ganiyu
Developing efficient and sustainable catalysts for CO2 electroreduction is critical to addressing the rising atmospheric CO2 levels and mitigating climate change. This study presents a novel ZnO-MXene (Ti2C) nanocomposite as a high-performance electrocatalyst for CO2 conversion, offering a strategic approach for generating valuable carbon-based feedstocks. The ZnO-MXene nanocomposites were synthesized via the wet impregnation method and comprehensively characterized using X-ray diffraction (XRD), energy-dispersive X-ray spectroscopy (EDS), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and Fourier transform infrared spectroscopy (FTIR). Electrochemical performance was assessed through linear sweep voltammetry (LSV), cyclic voltammetry (CV), and controlled potential coulometry, with gas chromatography employed for product quantification. ZnO-MX10 and ZnO-MX2.5 exhibited high selectivity for CH4 (79.3 % Faradaic efficiency, FE) at −0.56 VRHE and CO (76.8 % FE) at −0.78 VRHE, while significantly suppressing competing H2 evolution. The synergistic interaction between ZnO and MXene enhances charge transfer, increases active sites, and improves surface area, leading to superior electrochemical performance. Overall, this work introduces a novel ZnO-MXene nanocomposite with dual selectivity for CO and CH4, enhanced electroactive surface, and long-term stability. Unlike conventional Zn-based catalysts, which exhibit either limited selectivity or rapid degradation, our composite achieves 79.3 % Faradaic efficiency for CH4 and 76.8 % for CO, while suppressing H2 evolution. This unique tunability and stability make ZnO-MXene an attractive alternative to noble metal-based electrocatalysts.
开发高效、可持续的二氧化碳电还原催化剂对于解决大气中二氧化碳含量不断上升的问题和减缓气候变化至关重要。本研究提出了一种新型 ZnO-MXene (Ti2C) 纳米复合材料,作为二氧化碳转化的高性能电催化剂,为生成有价值的碳基原料提供了一种战略方法。ZnO-MXene 纳米复合材料是通过湿浸渍法合成的,并使用 X 射线衍射 (XRD)、能量色散 X 射线光谱 (EDS)、场发射扫描电子显微镜 (FESEM)、透射电子显微镜 (TEM) 和傅立叶变换红外光谱 (FTIR) 对其进行了全面表征。电化学性能通过线性扫描伏安法(LSV)、循环伏安法(CV)和受控电位库仑测定法进行评估,并采用气相色谱法进行产品定量。ZnO-MX10 和 ZnO-MX2.5 在-0.56 VRHE 条件下对 CH4(79.3 % Faradaic efficiency,FE)和 CO(76.8 % FE)在-0.78 VRHE 条件下表现出高选择性,同时显著抑制了竞争性 H2 的演化。氧化锌和 MXene 之间的协同作用增强了电荷转移、增加了活性位点并提高了表面积,从而实现了卓越的电化学性能。总之,这项研究推出了一种新型 ZnO-MXene 纳米复合材料,具有 CO 和 CH4 双选择性、增强的电活性表面和长期稳定性。传统的锌基催化剂要么选择性有限,要么会快速降解,而我们的复合材料与之不同,在抑制 H2 演化的同时,对 CH4 的法拉第效率达到 79.3%,对 CO 的法拉第效率达到 76.8%。这种独特的可调性和稳定性使 ZnO-MXene 成为贵金属电催化剂的一种极具吸引力的替代品。
{"title":"Enhancing the electrochemical conversion of carbon dioxide to value-added products on zinc oxide-MXene nanocomposite","authors":"AbdulHakam Shafiu Abdullahi ,&nbsp;Umar Mustapha ,&nbsp;Omer Ahmed Taialla ,&nbsp;Esraa Kotob ,&nbsp;Ijaz Hussain ,&nbsp;Khalid Alhooshani ,&nbsp;Shehzada Muhammad Sajid Jillani ,&nbsp;Saheed A. Ganiyu","doi":"10.1016/j.jcis.2025.137487","DOIUrl":"10.1016/j.jcis.2025.137487","url":null,"abstract":"<div><div>Developing efficient and sustainable catalysts for CO<sub>2</sub> electroreduction is critical to addressing the rising atmospheric CO<sub>2</sub> levels and mitigating climate change. This study presents a novel ZnO-MXene (Ti<sub>2</sub>C) nanocomposite as a high-performance electrocatalyst for CO<sub>2</sub> conversion, offering a strategic approach for generating valuable carbon-based feedstocks. The ZnO-MXene nanocomposites were synthesized via the wet impregnation method and comprehensively characterized using X-ray diffraction (XRD), energy-dispersive X-ray spectroscopy (EDS), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and Fourier transform infrared spectroscopy (FTIR). Electrochemical performance was assessed through linear sweep voltammetry (LSV), cyclic voltammetry (CV), and controlled potential coulometry, with gas chromatography employed for product quantification. ZnO-MX<sub>10</sub> and ZnO-MX<sub>2.5</sub> exhibited high selectivity for CH<sub>4</sub> (79.3 % Faradaic efficiency, FE) at −0.56 V<sub>RHE</sub> and CO (76.8 % FE) at −0.78 V<sub>RHE</sub>, while significantly suppressing competing H<sub>2</sub> evolution. The synergistic interaction between ZnO and MXene enhances charge transfer, increases active sites, and improves surface area, leading to superior electrochemical performance. Overall, this work introduces a novel ZnO-MXene nanocomposite with dual selectivity for CO and CH<sub>4</sub>, enhanced electroactive surface, and long-term stability. Unlike conventional Zn-based catalysts, which exhibit either limited selectivity or rapid degradation, our composite achieves 79.3 % Faradaic efficiency for CH<sub>4</sub> and 76.8 % for CO, while suppressing H<sub>2</sub> evolution. This unique tunability and stability make ZnO-MXene an attractive alternative to noble metal-based electrocatalysts.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137487"},"PeriodicalIF":9.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143783835","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
Enhancing CO tolerance via molecular trapping effect: Single-atom Pt anchored on Mo2C for efficient alkaline hydrogen oxidation reaction
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137489
Xiaokun Yang , Wenjie Yu , Yanfeng Zhang , Chuanpeng Qiao , Lili Liu , Yongfang Zhang , Qirui Li , Mengfei Mou , Rutao Wang , Xiangsen Yuan , Zhihao Wang , Liting Yan , Xuebo Zhao
Developing highly efficient, stable, and CO-tolerant electrocatalysts for hydrogen oxidation reaction (HOR) remains a critical challenge for practical proton/anion exchange membrane fuel cells. Here in, an atomically dispersed platinum (Pt) on Mo2C nanoparticles supported on nitrogen-doped carbon (PtSAMo2C-NC) with a unique yolk-shell structure is presented as a highly efficient and stable catalyst for HOR. The PtSAMo2C-NC catalyst demonstrates remarkable HOR performance, with a high exchange current density of 2.7 mA cm−2 and a mass activity of 2.15 A/mgPt at 50 mV (vs. RHE), which are 1.5 and 18 times greater than those of the 40 % commercial Pt/C catalyst, respectively. Furthermore, the unique PtSAMo2C-NC structure exhibits superior CO tolerance at H2/1,000 ppm CO, significantly outperforming commercial Pt/C catalysts. Density functional theory (DFT) calculations indicate that the introduction of Mo2C forms a strong electronic interaction with Pt, which decreases the electron density around the Pt atoms and shifts the d-band center away from the Fermi level. This results in a reduction of the *H adsorption energy and an optimization of the *OH adsorption energy in PtSAMo2C-NC. In addition, by calculating the CO adsorption energy, it was found that Mo2C exhibits strong CO adsorption ability, which generating a molecular trapping effect, thereby protecting the Pt active sites from poisoning. The strong metal-support electronic interaction significantly enhances the catalytic activity, stability, and CO tolerance of the material, providing a new strategy for developing catalysts with these desirable properties.
{"title":"Enhancing CO tolerance via molecular trapping effect: Single-atom Pt anchored on Mo2C for efficient alkaline hydrogen oxidation reaction","authors":"Xiaokun Yang ,&nbsp;Wenjie Yu ,&nbsp;Yanfeng Zhang ,&nbsp;Chuanpeng Qiao ,&nbsp;Lili Liu ,&nbsp;Yongfang Zhang ,&nbsp;Qirui Li ,&nbsp;Mengfei Mou ,&nbsp;Rutao Wang ,&nbsp;Xiangsen Yuan ,&nbsp;Zhihao Wang ,&nbsp;Liting Yan ,&nbsp;Xuebo Zhao","doi":"10.1016/j.jcis.2025.137489","DOIUrl":"10.1016/j.jcis.2025.137489","url":null,"abstract":"<div><div>Developing highly efficient, stable, and CO-tolerant electrocatalysts for hydrogen oxidation reaction (HOR) remains a critical challenge for practical proton/anion exchange membrane fuel cells. Here in, an atomically dispersed platinum (Pt) on Mo<sub>2</sub>C nanoparticles supported on nitrogen-doped carbon (Pt<sub>SA</sub>Mo<sub>2</sub>C-NC) with a unique yolk-shell structure is presented as a highly efficient and stable catalyst for HOR. The Pt<sub>SA</sub>Mo<sub>2</sub>C-NC catalyst demonstrates remarkable HOR performance, with a high exchange current density of 2.7 mA cm<sup>−2</sup> and a mass activity of 2.15 A/mg<sub>Pt</sub> at 50 mV (vs. RHE), which are 1.5 and 18 times greater than those of the 40 % commercial Pt/C catalyst, respectively. Furthermore, the unique Pt<sub>SA</sub>Mo<sub>2</sub>C-NC structure exhibits superior CO tolerance at H<sub>2</sub>/1,000 ppm CO, significantly outperforming commercial Pt/C catalysts. Density functional theory (DFT) calculations indicate that the introduction of Mo<sub>2</sub>C forms a strong electronic interaction with Pt, which decreases the electron density around the Pt atoms and shifts the d-band center away from the Fermi level. This results in a reduction of the *H adsorption energy and an optimization of the *OH adsorption energy in Pt<sub>SA</sub>Mo<sub>2</sub>C-NC. In addition, by calculating the CO adsorption energy, it was found that Mo<sub>2</sub>C exhibits strong CO adsorption ability, which generating a molecular trapping effect, thereby protecting the Pt active sites from poisoning. The strong metal-support electronic interaction significantly enhances the catalytic activity, stability, and CO tolerance of the material, providing a new strategy for developing catalysts with these desirable properties.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137489"},"PeriodicalIF":9.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759810","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
Metal effect boosts the photoelectric properties of two-dimentional Dion-Jacobson (3AMPY)(MA)3M4I13 perovskites
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137493
Gaoyin Wang , Haoyu Chu , Ken Deng , Jinfu Wu , Qin Ding , Ping-Ping Sun , Zhu-Zhu Sun , Chaoyuan Zeng , Weijie Chi
Two-Dimentional (2D) Dion-Jacobson (DJ) perovskites are emerging photovoltaic materials due to their excellent rigid structures and improved environmental stability compared to 2D Ruddlesden-Popper (RP) perovskites. Herein, we adopt 3-(aminomethyl)pyridine (3AMPY) as the divalent interlayer spacer to alleviate the toxicity of lead and explore more highly potential DJ alternatives, the optoelectronic and photovoltaic performance of lead-free DJ (3AMPY)(MA)3M4I13 perovskites are investigated by first-principles calculations, where the central metals are considered as Ba, Cd, Cu, Ge, Mg, Mn, Ni, Sn and Zn to replace Pb. Our findings reveal that introducing Mn, Cd, Ni, and Ge can effectively tune the bandgap within the optimal range of 0.90–1.60 eV for solar cell application. Notably, (3AMPY)(MA)3Ni4I13 exhibits the most favorable optical response capacity, with the light-harvesting efficiency maintaining 80 % in the UV–Vis range. (3AMPY)(MA)3Ge4I13 displays the most excellent carrier transport with electron mobility as high as 555.43 cm2 V−1 s−1, exhibiting a great advantage over 2D perovskites. The predicted photovoltaic performance shows that (3AMPY)(MA)3Mg4I13 possesses the largest open circuit voltage (VOC) (2.12 V), (3AMPY)(MA)3Ge4I13 has the highest short circuit current density (Jsc) (38.90 mA/cm2), and (3AMPY)(MA)3Mn4I13 is with the highest power conversion efficiency (PCE) of 22.55 %. The metal substitutions with Cd, Ni, and Ge show promoted photovoltaic potential over (3AMPY)(MA)3Pb4I13. These results form a basis for broadening the potential candidates of this 2D DJ series in photovoltaic perovskite solar cells (PSCs).
{"title":"Metal effect boosts the photoelectric properties of two-dimentional Dion-Jacobson (3AMPY)(MA)3M4I13 perovskites","authors":"Gaoyin Wang ,&nbsp;Haoyu Chu ,&nbsp;Ken Deng ,&nbsp;Jinfu Wu ,&nbsp;Qin Ding ,&nbsp;Ping-Ping Sun ,&nbsp;Zhu-Zhu Sun ,&nbsp;Chaoyuan Zeng ,&nbsp;Weijie Chi","doi":"10.1016/j.jcis.2025.137493","DOIUrl":"10.1016/j.jcis.2025.137493","url":null,"abstract":"<div><div>Two-Dimentional (2D) Dion-Jacobson (DJ) perovskites are emerging photovoltaic materials due to their excellent rigid structures and improved environmental stability compared to 2D Ruddlesden-Popper (RP) perovskites. Herein, we adopt 3-(aminomethyl)pyridine (3AMPY) as the divalent interlayer spacer to alleviate the toxicity of lead and explore more highly potential DJ alternatives, the optoelectronic and photovoltaic performance of lead-free DJ (3AMPY)(MA)<sub>3</sub>M<sub>4</sub>I<sub>13</sub> perovskites are investigated by first-principles calculations, where the central metals are considered as Ba, Cd, Cu, Ge, Mg, Mn, Ni, Sn and Zn to replace Pb. Our findings reveal that introducing Mn, Cd, Ni, and Ge can effectively tune the bandgap within the optimal range of 0.90–1.60 eV for solar cell application. Notably, (3AMPY)(MA)<sub>3</sub>Ni<sub>4</sub>I<sub>13</sub> exhibits the most favorable optical response capacity, with the light-harvesting efficiency maintaining 80 % in the UV–Vis range. (3AMPY)(MA)<sub>3</sub>Ge<sub>4</sub>I<sub>13</sub> displays the most excellent carrier transport with electron mobility as high as 555.43 cm<sup>2</sup> V<sup>−1</sup> s<sup>−1</sup>, exhibiting a great advantage over 2D perovskites. The predicted photovoltaic performance shows that (3AMPY)(MA)<sub>3</sub>Mg<sub>4</sub>I<sub>13</sub> possesses the largest open circuit voltage (<em>V</em><sub>OC</sub>) (2.12 V), (3AMPY)(MA)<sub>3</sub>Ge<sub>4</sub>I<sub>13</sub> has the highest short circuit current density (<em>J</em><sub>sc</sub>) (38.90 mA/cm<sup>2</sup>), and (3AMPY)(MA)<sub>3</sub>Mn<sub>4</sub>I<sub>13</sub> is with the highest power conversion efficiency (PCE) of 22.55 %. The metal substitutions with Cd, Ni, and Ge show promoted photovoltaic potential over (3AMPY)(MA)<sub>3</sub>Pb<sub>4</sub>I<sub>13</sub>. These results form a basis for broadening the potential candidates of this 2D DJ series in photovoltaic perovskite solar cells (PSCs).</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137493"},"PeriodicalIF":9.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759818","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
Broad-spectrum pathogenic bacteria SERS sensing with face-centered high-index facets Au CPNCs & microarray chips: A novel platform able to achieve dual-readout detection
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137485
Hao-yu Zhang , Jing-yuan Wang , Jian-jun Li , Jian Zhu , Guo-jun Weng , Ya-li Li , Jun-wu Zhao
Non-specificity and inadequate quantitative capability are the primary challenges faced by the surface-enhanced Raman scattering (SERS) technique, especially when it comes to detecting bacteria in real samples. Herein, a novel face-centered Au Convex Polyhedral Nanocrystal (Au CPNC) with high-index facets and its assembly Au CPNCs microarray chip were designed and fabricated to address these challenges, within the process where 4-mercaptophenylboronic acid (4-MPBA) was utilized as a multifunctional element. The as-prepared Au CPNC possesses anisotropic raised edges enjoying tunable localized surface plasmon resonance modes for SERS enhancement. Then we obtained long-region ordered Au CPNCs microarrays equipping even greater “hot spots” with a SERS enhancement factor (EF) up to 5.38 × 107. The constructed SERS probes excellently leveraged the outstanding SERS performance of Au CPNC and the superior functions of 4-MPBA, which enabled the differences among the bacterial “fingerprints” to be highlighted. Through partial least squares discriminant analysis (PLS-DA), we successfully identified Escherichia coli, Staphylococcus aureus, Pseudomonas aeruginosa and Listeria monocytogenes with achieving limits of detection (LODs) in spiked whole blood samples of 3, 1, 2, and 2 cfu/mL, respectively. Notably, the LODs for all samples by SERS mapping visual readout mode were as low as 10 cfu/mL. In practical applications, our method demonstrated its efficacy by 100 % accurately classifying (20 cases) of real blood samples. Altogether, the theoretical significance and application value of this study reside in providing fundamental insights and approaches for the development of pathogenic bacteria detection field.
{"title":"Broad-spectrum pathogenic bacteria SERS sensing with face-centered high-index facets Au CPNCs & microarray chips: A novel platform able to achieve dual-readout detection","authors":"Hao-yu Zhang ,&nbsp;Jing-yuan Wang ,&nbsp;Jian-jun Li ,&nbsp;Jian Zhu ,&nbsp;Guo-jun Weng ,&nbsp;Ya-li Li ,&nbsp;Jun-wu Zhao","doi":"10.1016/j.jcis.2025.137485","DOIUrl":"10.1016/j.jcis.2025.137485","url":null,"abstract":"<div><div>Non-specificity and inadequate quantitative capability are the primary challenges faced by the surface-enhanced Raman scattering (SERS) technique, especially when it comes to detecting bacteria in real samples. Herein, a novel face-centered Au Convex Polyhedral Nanocrystal (Au CPNC) with high-index facets and its assembly Au CPNCs microarray chip were designed and fabricated to address these challenges, within the process where 4-mercaptophenylboronic acid (4-MPBA) was utilized as a multifunctional element. The as-prepared Au CPNC possesses anisotropic raised edges enjoying tunable localized surface plasmon resonance modes for SERS enhancement. Then we obtained long-region ordered Au CPNCs microarrays equipping even greater “hot spots” with a SERS enhancement factor (EF) up to 5.38 × 10<sup>7</sup>. The constructed SERS probes excellently leveraged the outstanding SERS performance of Au CPNC and the superior functions of 4-MPBA, which enabled the differences among the bacterial “fingerprints” to be highlighted. Through partial least squares discriminant analysis (PLS-DA), we successfully identified <em>Escherichia coli, Staphylococcus aureus, Pseudomonas aeruginosa</em> and <em>Listeria monocytogenes</em> with achieving limits of detection (LODs) in spiked whole blood samples of 3, 1, 2, and 2 cfu/mL, respectively. Notably, the LODs for all samples by SERS mapping visual readout mode were as low as 10 cfu/mL. In practical applications, our method demonstrated its efficacy by 100 % accurately classifying (20 cases) of real blood samples. Altogether, the theoretical significance and application value of this study reside in providing fundamental insights and approaches for the development of pathogenic bacteria detection field.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137485"},"PeriodicalIF":9.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143807527","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-performance nitrogen-doped carbon catalyst with Co-Cu-CuxO interfaces via bimetallic ion exchange-carbonization: Synergistic Co/Cu interactions and nonradical activation mechanism for micropollutant removal
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-03-31 DOI: 10.1016/j.jcis.2025.137490
Xinqiang Cao , Yang Liu , Fucai Yang , Xianhang Huang , Wenfeng Qiu
Mono-metal active sites, with their restricted electron transfer ability, typically lead to lower redox reaction efficiency, which hampers peroxymonosulfate (PMS) activation and reduces antibiotic degradation effectiveness. In this work, a novel nitrogen-doped carbon catalyst with Co-Cu-CuxO interfaces was synthesized by pyrolyzing a Zn-based elliptical two-dimensional template through a Co2+/Cu2+ bimetallic ion exchange process. The synthesized samples were comprehensively characterized using a range of physicochemical analysis techniques. Furthermore, the catalytic performance was systematically evaluated under varying conditions, including peroxymonosulfate dosage, tetracycline concentration, solution pH, and the influence of co-existing ions and organic matter in water. The results indicated that the optimized 1:1–950 catalyst achieved over 96 % degradation of tetracycline (TC) through PMS activation, with a reaction rate constant (k) of 0.038 min−1, significantly outperforming both the mono-metal ion exchange group and the non-metal ion exchange group. This improvement was attributed to the synergistic effects of Co(II)/Co(III) and Cu(I)/Cu(II) redox reactions at the Co-Cu-CuxO interfaces. Quenching experiments, electron spin resonance (ESR), and electrochemical analyses revealed that non-radical reactive oxygen species (ROS), such as singlet oxygen (1O2) and high-valent metal-oxo species (e.g., Cu(III)-oxo and Co(IV)-oxo), played a key role in the degradation process. The degradation pathways for TC were proposed using high-performance liquid chromatography-mass spectrometry (HPLC-MS), and the environmental safety of the catalytic system was confirmed through physiological testing on mung bean growth. This work presents an efficient approach for PMS activation in TC degradation, using nitrogen-doped carbon catalysts with Co-Cu-CuxO interfaces synthesized via bimetallic ion exchange and carbonization strategy, with promising applications in advanced wastewater treatment.
{"title":"High-performance nitrogen-doped carbon catalyst with Co-Cu-CuxO interfaces via bimetallic ion exchange-carbonization: Synergistic Co/Cu interactions and nonradical activation mechanism for micropollutant removal","authors":"Xinqiang Cao ,&nbsp;Yang Liu ,&nbsp;Fucai Yang ,&nbsp;Xianhang Huang ,&nbsp;Wenfeng Qiu","doi":"10.1016/j.jcis.2025.137490","DOIUrl":"10.1016/j.jcis.2025.137490","url":null,"abstract":"<div><div>Mono-metal active sites, with their restricted electron transfer ability, typically lead to lower redox reaction efficiency, which hampers peroxymonosulfate (PMS) activation and reduces antibiotic degradation effectiveness. In this work, a novel nitrogen-doped carbon catalyst with Co-Cu-Cu<em>x</em>O interfaces was synthesized by pyrolyzing a Zn-based elliptical two-dimensional template through a Co<sup>2+</sup>/Cu<sup>2+</sup> bimetallic ion exchange process. The synthesized samples were comprehensively characterized using a range of physicochemical analysis techniques. Furthermore, the catalytic performance was systematically evaluated under varying conditions, including peroxymonosulfate dosage, tetracycline concentration, solution pH, and the influence of co-existing ions and organic matter in water. The results indicated that the optimized 1:1–950 catalyst achieved over 96 % degradation of tetracycline (TC) through PMS activation, with a reaction rate constant (<em>k</em>) of 0.038 min<sup>−1</sup>, significantly outperforming both the mono-metal ion exchange group and the non-metal ion exchange group. This improvement was attributed to the synergistic effects of <img>Co(II)/<img>Co(III) and <img>Cu(I)/<img>Cu(II) redox reactions at the Co-Cu-Cu<em>x</em>O interfaces. Quenching experiments, electron spin resonance (ESR), and electrochemical analyses revealed that non-radical reactive oxygen species (ROS), such as singlet oxygen (<sup>1</sup>O<sub>2</sub>) and high-valent metal-oxo species (e.g., <img>Cu(III)-oxo and <img>Co(IV)-oxo), played a key role in the degradation process. The degradation pathways for TC were proposed using high-performance liquid chromatography-mass spectrometry (HPLC-MS), and the environmental safety of the catalytic system was confirmed through physiological testing on mung bean growth. This work presents an efficient approach for PMS activation in TC degradation, using nitrogen-doped carbon catalysts with Co-Cu-Cu<em>x</em>O interfaces synthesized via bimetallic ion exchange and carbonization strategy, with promising applications in advanced wastewater treatment.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"692 ","pages":"Article 137490"},"PeriodicalIF":9.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143785560","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
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Journal of Colloid and Interface Science
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