Pub Date : 2025-11-04DOI: 10.26599/nr.2025.94908223
Xiaomeng She, Junxi Zhang, Huayue Yang, Han Tian, Weiwei Zhou, Yun Zhao, Song Zhang, Rong Tu, Guangxu Chen, Jian Peng
Electrocatalytic oxidation of biomass-derived 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid offers a sustainable route to high-value chemicals. Anion doping in cobalt-based catalysts can modulate catalytic performance by altering the coordination environment and electronic structure of active sites, thereby affecting surface reconstruction and reaction kinetics. Here, anion-modified cobalt hydroxysalts [Co(OH)2-x(Am-)x/m, A = CO32-, F-, Cl-] were synthesized to investigate anion-specific effects on electrooxidation of 5-hydroxymethylfurfural. The carbonate-incorporated nanowire catalyst exhibited outstanding performance, lowering the oxidation potential to 1.33 V at 50 mA cm-1 and increasing the active site density by 1.5 times relative to undoped Co(OH)2. In contrast, F- and Cl- doping led to redox potential shifts and reduced activity. In situ Raman spectroscopy revealed that the catalytic reaction was driven by active CoOOH species generated under anodic polarization. This process was accompanied by carbonate leaching and irreversible phase changes, which contributed to catalyst deactivation. This study provides insights into anion-controlled catalyst design for efficient and durable biomass electrooxidation.
电催化氧化生物质衍生的5-羟甲基糠醛为2,5-呋喃二羧酸提供了一条可持续的高价值化学品途径。在钴基催化剂中掺杂阴离子可以通过改变活性位点的配位环境和电子结构来调节催化性能，从而影响表面重构和反应动力学。本文合成了阴离子修饰的钴羟基盐[Co(OH)2-x(Am-)x/m, A = CO32-, F-, Cl-]，研究了阴离子对5-羟甲基糠醛电氧化的特异性影响。碳化物掺杂纳米线催化剂表现出优异的性能，在50 mA cm-1时氧化电位降至1.33 V，活性位点密度比未掺杂Co(OH)2提高1.5倍。相反，F-和Cl-掺杂导致氧化还原电位移位和活性降低。原位拉曼光谱显示，催化反应是由阳极极化下产生的活性CoOOH驱动的。这一过程伴随着碳酸盐浸出和不可逆的相变，导致催化剂失活。该研究为高效、持久的生物质电氧化提供了阴离子控制催化剂的设计思路。
{"title":"Carbonate-incorporated cobalt hydroxides for enhanced performance in the electrocatalytic oxidation of5-hydroxymethylfurfural","authors":"Xiaomeng She, Junxi Zhang, Huayue Yang, Han Tian, Weiwei Zhou, Yun Zhao, Song Zhang, Rong Tu, Guangxu Chen, Jian Peng","doi":"10.26599/nr.2025.94908223","DOIUrl":"https://doi.org/10.26599/nr.2025.94908223","url":null,"abstract":"Electrocatalytic oxidation of biomass-derived 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid offers a sustainable route to high-value chemicals. Anion doping in cobalt-based catalysts can modulate catalytic performance by altering the coordination environment and electronic structure of active sites, thereby affecting surface reconstruction and reaction kinetics. Here, anion-modified cobalt hydroxysalts [Co(OH)<sub>2-x</sub>(A<sup>m-</sup>)<sub>x/m</sub>, A = CO<sub>3</sub><sup>2-</sup>, F<sup>-</sup>, Cl<sup>-</sup>] were synthesized to investigate anion-specific effects on electrooxidation of 5-hydroxymethylfurfural. The carbonate-incorporated nanowire catalyst exhibited outstanding performance, lowering the oxidation potential to 1.33 V at 50 mA cm<sup>-1</sup> and increasing the active site density by 1.5 times relative to undoped Co(OH)<sub>2</sub>. In contrast, F<sup>-</sup> and Cl<sup>-</sup> doping led to redox potential shifts and reduced activity. <em>In situ</em> Raman spectroscopy revealed that the catalytic reaction was driven by active CoOOH species generated under anodic polarization. This process was accompanied by carbonate leaching and irreversible phase changes, which contributed to catalyst deactivation. This study provides insights into anion-controlled catalyst design for efficient and durable biomass electrooxidation.","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"19 3","pages":"94908223-94908223"},"PeriodicalIF":0.0,"publicationDate":"2025-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147333017","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Manipulating the organic counter cations, which serve as pore gatekeepers to selectively obstruct the channels in anionic metal-organic frameworks (MOFs), offers a highly effective strategy for optimizing the separation performance. Here, we report an yttrium-based MOF, Y-ebdc, featuring cage-type structures that accommodate protonated dimethylamine (DMA) as both counter cations and molecular sieving gates. Subsequent optimization of the adsorption separation performance for propylene/propane (C3H6/C3H8) was achieved through regulation of DMA’s thermal decomposition. The temperature dependence of DMA decomposition was elucidated using temperature-resolved in situ infrared spectroscopy and breakthrough studies. With approximately 70% of DMA removed, the expanded aperture window and increased pore volume remarkably enhance dynamic C3H6 uptake while simultaneously facilitating the direct production of polymer-grade (>99.5%) C3H6 in a single adsorption–desorption cycle. This study exemplifies how engineering the pore environment via co-existing counter cations within MOFs can effectively boost gas adsorption and separation performance.
{"title":"Pore engineering via controlled decomposition of counter cations in an anion-based metal-organic framework","authors":"Zongkai Liu, Bingquan Hua, Tianliang Lu, Guanying Dong, Jingwei Hou, Xiaoquan Feng, Yatao Zhang","doi":"10.26599/nr.2025.94908224","DOIUrl":"https://doi.org/10.26599/nr.2025.94908224","url":null,"abstract":"Manipulating the organic counter cations, which serve as pore gatekeepers to selectively obstruct the channels in anionic metal-organic frameworks (MOFs), offers a highly effective strategy for optimizing the separation performance. Here, we report an yttrium-based MOF, Y-ebdc, featuring cage-type structures that accommodate protonated dimethylamine (DMA) as both counter cations and molecular sieving gates. Subsequent optimization of the adsorption separation performance for propylene/propane (C<sub>3</sub>H<sub>6</sub>/C<sub>3</sub>H<sub>8</sub>) was achieved through regulation of DMA’s thermal decomposition. The temperature dependence of DMA decomposition was elucidated using temperature-resolved in situ infrared spectroscopy and breakthrough studies. With approximately 70% of DMA removed, the expanded aperture window and increased pore volume remarkably enhance dynamic C<sub>3</sub>H<sub>6</sub> uptake while simultaneously facilitating the direct production of polymer-grade (>99.5%) C<sub>3</sub>H<sub>6</sub> in a single adsorption–desorption cycle. This study exemplifies how engineering the pore environment via co-existing counter cations within MOFs can effectively boost gas adsorption and separation performance.","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"19 3","pages":"94908224-94908224"},"PeriodicalIF":0.0,"publicationDate":"2025-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147331571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-03DOI: 10.26599/nr.2025.94908222
Yangyang Dong, Dong Cai, Honglong Ning, Meiling Shu, Shuo Yang, Xuemei Zhou, Huagui Nie, Xingqiao Wu, Zhanshuang Jin, Zhi Yang
Designing tailored multifunctional catalysts that enhance lean-electrolyte sulfur redox kinetics is crucial for achieving high-energy-density lithium-sulfur batteries, however, still remains challenge. Motivated by the structural protection of active sites in natural enzymes, we implant natural glutathione (GSH) within the metal-organic framework MIL-47 (V) cavity for GSH@MIL-47 (V) biomimetic catalysts, thereby stabilizing and activating its thiol functionality. Quantification using DTNB as a probe confirmed successful GSH incorporation, revealing that GSH@MIL-47 (V) enables a continuous and stable catalytic reaction cycle. Moreover, in-situ and ex-situ spectroscopies indicate thiol-driven S-S bond breakage that lowers the reaction energy barrier and concurrently promote LiTFSI decomposition. As a result, GSH@MIL-47 (V) cells, at 6 C rate, deliver a discharge capacity of 733.1 mAh g-1 and maintain 573.0 mAh g-1 after 750 cycles. Even under an electrolyte-to-sulfur ratio of 5.5 μL mg-1, it maintains 867.2 mAh g-1 at a high-rate of 0.5 C. This strategy highlights the potential of enzyme-inspired catalysts for enhancing lithium-sulfur batteries.
然而，为了实现高能量密度的锂硫电池，设计定制的多功能催化剂来提高贫电解质硫氧化还原动力学是至关重要的。受天然酶活性位点结构保护的激励，我们将天然谷胱甘肽（GSH）植入金属-有机框架MIL-47 (V)腔中，用于GSH@MIL-47 (V)仿生催化剂，从而稳定和激活其硫醇功能。使用DTNB作为探针的定量证实了GSH的成功结合，表明GSH@MIL-47 (V)能够实现连续稳定的催化反应循环。此外，原位和原位光谱表明，硫醇驱动的S-S键断裂降低了反应能垒，同时促进了LiTFSI的分解。因此，GSH@MIL-47 (V)电池在6℃的倍率下，放电容量为733.1 mAh g-1，并在750次循环后保持573.0 mAh g-1。即使在5.5 μL mg-1的电解硫比下，它在0.5 c的高倍率下也能保持867.2 mAh g-1。这一策略突出了酶激发催化剂在增强锂硫电池方面的潜力。
{"title":"Thiol centric enzyme mimetic catalysis within MIL-47 (V) accelerates sulfur redox and enhances stability for lean electrolyte lithium–sulfur batteries","authors":"Yangyang Dong, Dong Cai, Honglong Ning, Meiling Shu, Shuo Yang, Xuemei Zhou, Huagui Nie, Xingqiao Wu, Zhanshuang Jin, Zhi Yang","doi":"10.26599/nr.2025.94908222","DOIUrl":"https://doi.org/10.26599/nr.2025.94908222","url":null,"abstract":"Designing tailored multifunctional catalysts that enhance lean-electrolyte sulfur redox kinetics is crucial for achieving high-energy-density lithium-sulfur batteries, however, still remains challenge. Motivated by the structural protection of active sites in natural enzymes, we implant natural glutathione (GSH) within the metal-organic framework MIL-47 (V) cavity for GSH@MIL-47 (V) biomimetic catalysts, thereby stabilizing and activating its thiol functionality. Quantification using DTNB as a probe confirmed successful GSH incorporation, revealing that GSH@MIL-47 (V) enables a continuous and stable catalytic reaction cycle. Moreover, <em>in-situ</em> and <em>ex-situ</em> spectroscopies indicate thiol-driven S-S bond breakage that lowers the reaction energy barrier and concurrently promote LiTFSI decomposition. As a result, GSH@MIL-47 (V) cells, at 6 C rate, deliver a discharge capacity of 733.1 mAh g<sup>-1</sup> and maintain 573.0 mAh g<sup>-1</sup> after 750 cycles. Even under an electrolyte-to-sulfur ratio of 5.5 μL mg<sup>-1</sup>, it maintains 867.2 mAh g<sup>-1</sup> at a high-rate of 0.5 C. This strategy highlights the potential of enzyme-inspired catalysts for enhancing lithium-sulfur batteries.","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"19 2","pages":"94908222-94908222"},"PeriodicalIF":0.0,"publicationDate":"2025-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147333771","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-01DOI: 10.26599/nr.2025.94908233
Chunguang Chen, Junkai Zhang, Yilei Ding, Zhenqian Liu, W. K. Liu, Zhi Zhu, Minhua Shao
Metal-organic frameworks (MOFs) are highly effective in activating peroxymonosulfate (PMS) for pollutant degradation, yet their practical application is limited by nanoparticle aggregation and poor recoverability. To address this, carbon nanotubes (CNTs) were employed as an ideal scaffold to host MOF-derived species. In this study, a Co-MOF@CNTs precursor was converted into a composite of Co nanoparticles embedded in defective porous carbon nanotubes (Co@CNTs-800). The resulting Co@CNTs-800/PMS system exhibited remarkable catalytic activity in the degradation of rhodamine B (RhB), achieving complete degradation within 4 minutes with a rate constant of 1.025 min-1. The material demonstrated excellent stability across a broad pH range (pH = 4~10) and exhibited high performance in the presence of common inorganic anions (Cl⁻ and NO₃⁻) as well as natural organic matter, with maintained stability over 6 cycles. Quenching assays and electron paramagnetic resonance (EPR) spectroscopy revealed that both free radical (SO4•–, •OH, and O2•–) and non-radical (1O2 and charge transfer) pathways contribute to the degradation process, with non-radical mechanisms dominated by 1O2. The degradation pathway of RhB was elucidated based on intermediates detected by liquid chromatography-mass spectrometry (LC-MS) and density functional theory (DFT) calculations. Additionally, the Co@CNTs-800/PMS system effectively removed other dyes, highlighting its potential for broader applications in advanced oxidation processes for water treatment.
{"title":"Ultrafast degradation of organic dyes via PMS activation by CNT-loaded MOF-derived Co nanoparticles","authors":"Chunguang Chen, Junkai Zhang, Yilei Ding, Zhenqian Liu, W. K. Liu, Zhi Zhu, Minhua Shao","doi":"10.26599/nr.2025.94908233","DOIUrl":"https://doi.org/10.26599/nr.2025.94908233","url":null,"abstract":"Metal-organic frameworks (MOFs) are highly effective in activating peroxymonosulfate (PMS) for pollutant degradation, yet their practical application is limited by nanoparticle aggregation and poor recoverability. To address this, carbon nanotubes (CNTs) were employed as an ideal scaffold to host MOF-derived species. In this study, a Co-MOF@CNTs precursor was converted into a composite of Co nanoparticles embedded in defective porous carbon nanotubes (Co@CNTs-800). The resulting Co@CNTs-800/PMS system exhibited remarkable catalytic activity in the degradation of rhodamine B (RhB), achieving complete degradation within 4 minutes with a rate constant of 1.025 min<sup>-1</sup>. The material demonstrated excellent stability across a broad pH range (pH = 4~10) and exhibited high performance in the presence of common inorganic anions (Cl⁻ and NO₃⁻) as well as natural organic matter, with maintained stability over 6 cycles. Quenching assays and electron paramagnetic resonance (EPR) spectroscopy revealed that both free radical (SO<sub>4</sub><sup>•–</sup>, <sup>•</sup>OH, and O<sub>2</sub><sup>•–</sup>) and non-radical (<sup>1</sup>O<sub>2</sub> and charge transfer) pathways contribute to the degradation process, with non-radical mechanisms dominated by <sup>1</sup>O<sub>2</sub>. The degradation pathway of RhB was elucidated based on intermediates detected by liquid chromatography-mass spectrometry (LC-MS) and density functional theory (DFT) calculations. Additionally, the Co@CNTs-800/PMS system effectively removed other dyes, highlighting its potential for broader applications in advanced oxidation processes for water treatment.","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147332144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-11-01DOI: 10.26599/nr.2025.94908229
Linghan Bai, Shijiao Zhang, Zhibiao Ma, Lvye Dou, Jianqiang Li
Wearable electronics devices face dual challenges of thermal failure and electromagnetic interference (EMI). While phase change materials (PCMs) offer efficient thermal management material, their inherent limitations-low thermal conductivity, rigidity, and limited electromagnetic loss hinder practical applications. Flexible composite PCMs (FCPCMs) with multifunctional integration present a promising solution. Herein, mimicking the lamellar “brick-and-mortar” architecture of natural nacre, a flexible phase-change composite film featuring a multi-dimensional hierarchical encapsulation structure is ingeniously engineered for synchronous thermal management and microwave absorption. This bioinspired design incorporates polyethylene glycol (PEG) within a robust scaffold of one-dimensional (1D) aramid nanofibers (ANFs), zero-dimensional (0D) nanodiamonds (NDs), and two-dimensional (2D) single-layer graphene (SG), bonded by waterborne polyurethane (WPU). The resulting nacre-mimetic, multi-dimensional architecture ensures exceptional encapsulation of PEG, effectively suppressing leakage while maintaining high phase-change cycling stability (>300 cycles). The optimized composite achieves synergistic performance: enhances thermal conductivity (1.13 W/(m·K)) strong microwave absorption performance (-41.36 dB), high phase-change enthalpy (104 J/g) and mechanical performance (tensile strength: 15.10 MPa). This work provides a platform for next-generation smart thermal-regulation systems and anti-interference electronics.
Pub Date : 2025-10-31DOI: 10.26599/nr.2025.94907883
Shuai Shao, Anni Zhu, Yi Chai, Zheming Song, Yutong Chen, Yi Xie, Yicheng Lv, Xiaoxun Huang, Wenjun Wang, Jingchao Li, Qin Zhang, Deping Kong, Qian Tan
Bacterial infection, excessive inflammatory response, and impaired angiogenesis caused by the hyperglycemic microenvironment of diabetic wounds are the primary factors of non-healing wounds. Most contemporary wound repair materials passively release loaded drugs, resulting in poor therapeutic outcomes. In this study, we designed sequentially triggered triple-responsive hydrogels containing alginate (ALG)-phenylboronic acid (PBA), copper polydopamine (Cu-PDA), metformin (MET), and deferoxamine mesylate (DFO) to cover the continuous process of diabetic-infected wound healing and improve the wound microenvironment through warming in the infectious phase and on-demand drug release in the inflammatory and proliferative phase. The hydrogels exhibited good adhesivity, injectability, self-healing ability, and biocompatibility. The hydrogels show remarkable photothermal responsiveness due to the presence of PDA. Studies showed that appropriate high temperatures and the release of Cu2+ resulted in the hydrogels displaying excellent bactericidal properties in the infectious phase. Furthermore, the instability of the phenyl borate bond in a hyperglycemic and acidic microenvironment enables the glucose/pH responsiveness of the release of MET and DFO from the hydrogels. Mechanistic studies have shown that the hydrogels could suppress the activity of the NOD-, LRR-, and pyrin structural domain-containing protein 3 (NLRP3)/caspase-1/GasderminD (GSDMD)/IL-1β pathway and activate the hypoxia-inducible factor 1 alpha (HIF-1α)/vascular endothelial growth factor (VEGF) pathway. These effects enabled the hydrogels to promote the healing of diabetic-infected wounds.
{"title":"Sequentially triggered triple-responsive hydrogels for targeted regulation of inflammation and angiogenesis in diabetic-infected wound healing","authors":"Shuai Shao, Anni Zhu, Yi Chai, Zheming Song, Yutong Chen, Yi Xie, Yicheng Lv, Xiaoxun Huang, Wenjun Wang, Jingchao Li, Qin Zhang, Deping Kong, Qian Tan","doi":"10.26599/nr.2025.94907883","DOIUrl":"https://doi.org/10.26599/nr.2025.94907883","url":null,"abstract":"Bacterial infection, excessive inflammatory response, and impaired angiogenesis caused by the hyperglycemic microenvironment of diabetic wounds are the primary factors of non-healing wounds. Most contemporary wound repair materials passively release loaded drugs, resulting in poor therapeutic outcomes. In this study, we designed sequentially triggered triple-responsive hydrogels containing alginate (ALG)-phenylboronic acid (PBA), copper polydopamine (Cu-PDA), metformin (MET), and deferoxamine mesylate (DFO) to cover the continuous process of diabetic-infected wound healing and improve the wound microenvironment through warming in the infectious phase and on-demand drug release in the inflammatory and proliferative phase. The hydrogels exhibited good adhesivity, injectability, self-healing ability, and biocompatibility. The hydrogels show remarkable photothermal responsiveness due to the presence of PDA. Studies showed that appropriate high temperatures and the release of Cu<sup>2+</sup> resulted in the hydrogels displaying excellent bactericidal properties in the infectious phase. Furthermore, the instability of the phenyl borate bond in a hyperglycemic and acidic microenvironment enables the glucose/pH responsiveness of the release of MET and DFO from the hydrogels. Mechanistic studies have shown that the hydrogels could suppress the activity of the NOD-, LRR-, and pyrin structural domain-containing protein 3 (NLRP3)/caspase-1/GasderminD (GSDMD)/IL-1β pathway and activate the hypoxia-inducible factor 1 alpha (HIF-1α)/vascular endothelial growth factor (VEGF) pathway. These effects enabled the hydrogels to promote the healing of diabetic-infected wounds.","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"18 11","pages":"94907883-94907883"},"PeriodicalIF":0.0,"publicationDate":"2025-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147333955","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-10-26DOI: 10.26599/nr.2025.94908191
Sujun Zheng, C. Liu, Weicong Chen, Na Li, Maolin Jiang, Ihsan Ullah, Zimeng Li, Youyong Yuan, Xinchun Li
{"title":"Tumor-selective degradation of PARP-1 enabled by the codelivery of β-lapachone and PROTAC for non-small-cell lung cancer therapy","authors":"Sujun Zheng, C. Liu, Weicong Chen, Na Li, Maolin Jiang, Ihsan Ullah, Zimeng Li, Youyong Yuan, Xinchun Li","doi":"10.26599/nr.2025.94908191","DOIUrl":"https://doi.org/10.26599/nr.2025.94908191","url":null,"abstract":"","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"19 1","pages":"94908191-94908191"},"PeriodicalIF":0.0,"publicationDate":"2025-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147331366","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-10-24DOI: 10.26599/nr.2025.94908079
Weiye Wang, Xiaoqiang Sun, Zhuang Guo, Yue Liu, Huishan Shang, Jinlong Ge, Jian Wei, Yan Gao, Yonghui Song
Developing high-performance catalysts suitable for a wide pH range in catalytic ozonation system remains a significant challenge, primarily owing to the limitations imposed by metal species and the pH at the point of zero charge. In this study, an O doped g-C3N4/CuO (CNO-CuO) catalyst was synthesized via a facile method. Compared to pristine g-C3N4/CuO (CN-CuO), CNO-CuO dramatically enhanced the degradation efficiency of pollutants from 25% to 100% in acidic solutions. Moreover, it exhibited the efficient degradation efficiencies across a broad pH range (3-10), demonstrating that introduction of O atoms considerably improved the universality of CNO-CuO. Experimental and theoretical studies revealed that the synergistic interaction between CuO and C-O bonds was responsible for the remarkable catalytic ozonation activity over a wide pH range. Crucially, the incorporation of O atoms contributed to reversible formation of Cu+, ensuring the continuous regeneration of active sites and the sustained formation of •OH. Additionally, the C-O bond acted as a potential catalytic active site, further enhancing treatment efficiency as pH increased. This work provided a feasible strategy for broadening catalyst applicability in catalytic ozonation systems through heteroatom doping.
{"title":"Enhanced catalytic ozonation by O-doped g-C <sub>3</sub> N <sub>4</sub> /CuO: Synergistic multi-active sites for broad pH applicability","authors":"Weiye Wang, Xiaoqiang Sun, Zhuang Guo, Yue Liu, Huishan Shang, Jinlong Ge, Jian Wei, Yan Gao, Yonghui Song","doi":"10.26599/nr.2025.94908079","DOIUrl":"https://doi.org/10.26599/nr.2025.94908079","url":null,"abstract":"Developing high-performance catalysts suitable for a wide pH range in catalytic ozonation system remains a significant challenge, primarily owing to the limitations imposed by metal species and the pH at the point of zero charge. In this study, an O doped g-C<sub>3</sub>N<sub>4</sub>/CuO (CNO-CuO) catalyst was synthesized via a facile method. Compared to pristine g-C<sub>3</sub>N<sub>4</sub>/CuO (CN-CuO), CNO-CuO dramatically enhanced the degradation efficiency of pollutants from 25% to 100% in acidic solutions. Moreover, it exhibited the efficient degradation efficiencies across a broad pH range (3-10), demonstrating that introduction of O atoms considerably improved the universality of CNO-CuO. Experimental and theoretical studies revealed that the synergistic interaction between CuO and C-O bonds was responsible for the remarkable catalytic ozonation activity over a wide pH range. Crucially, the incorporation of O atoms contributed to reversible formation of Cu<sup>+</sup>, ensuring the continuous regeneration of active sites and the sustained formation of •OH. Additionally, the C-O bond acted as a potential catalytic active site, further enhancing treatment efficiency as pH increased. This work provided a feasible strategy for broadening catalyst applicability in catalytic ozonation systems through heteroatom doping.","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"18 12","pages":"94908079-94908079"},"PeriodicalIF":0.0,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147333580","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Photodynamic therapy (PDT) employs lasers to activate photosensitizers, generating reactive oxygen species (ROS) for tumor cell destruction. However, the extremely short half-life of ROS and limited diffusion range restrict PDT’s therapeutic efficiency. Recent studies have shown that lysosome-targeted PDT can directly disrupt the “explosive depot” of tumor cells by triggering the release of abundant hydrolases from lysosomes. Nevertheless, existing lysosome-targeted strategies rely predominantly on a single protonation mechanism, resulting in low targeted efficiency. To enhance lysosome-targeted bursting, this study adopted a dual-mode recognition strategy, combining “hydrophobic interaction-aided fusion” with “charge-directed anchoring”. Specifically, pyropheophorbide-a (PPa) was employed as a model photosensitizer and covalently conjugated with alkyl tertiary amines of varying chain lengths (C1, C4, C8, and C12), yielding lysosome-targeted bursting photosensitizers (PPa1, PPa4, PPa8, and PPa12). Self-assembled nanoparticles (LPPa NPs) were then prepared to facilitate tumor delivery. The objective of this study was to determine the optimal chain length by evaluating the balance among ROS production efficiency, lysosomal targeted capability, and assembly stability of LPPa NPs. Notably, PPa4 NPs demonstrated superior cellular uptake, enhanced ROS generation, and effective lysosome-targeted bursting, thereby markedly improving antitumor efficacy. In summary, the dual-mode recognition strategy offered an advanced strategy for enhancing the efficiency of PDT.
{"title":"A dual-mode recognition strategy to enhance the lysosome-targeted bursting of PPa for efficient photodynamic cancer therapy","authors":"Fudan Dong, Minglong Huang, Wenxiao Li, Tian Liu, Lingxiao Li, Shiyi Zuo, Jingxuan Zhang, Jing Xing, J. Cui, Zhonggui He, Bingjun Sun, Jin Sun, Junjie Zhang","doi":"10.26599/nr.2025.94908186","DOIUrl":"https://doi.org/10.26599/nr.2025.94908186","url":null,"abstract":"Photodynamic therapy (PDT) employs lasers to activate photosensitizers, generating reactive oxygen species (ROS) for tumor cell destruction. However, the extremely short half-life of ROS and limited diffusion range restrict PDT’s therapeutic efficiency. Recent studies have shown that lysosome-targeted PDT can directly disrupt the “explosive depot” of tumor cells by triggering the release of abundant hydrolases from lysosomes. Nevertheless, existing lysosome-targeted strategies rely predominantly on a single protonation mechanism, resulting in low targeted efficiency. To enhance lysosome-targeted bursting, this study adopted a dual-mode recognition strategy, combining “hydrophobic interaction-aided fusion” with “charge-directed anchoring”. Specifically, pyropheophorbide-a (PPa) was employed as a model photosensitizer and covalently conjugated with alkyl tertiary amines of varying chain lengths (C1, C4, C8, and C12), yielding lysosome-targeted bursting photosensitizers (PPa1, PPa4, PPa8, and PPa12). Self-assembled nanoparticles (LPPa NPs) were then prepared to facilitate tumor delivery. The objective of this study was to determine the optimal chain length by evaluating the balance among ROS production efficiency, lysosomal targeted capability, and assembly stability of LPPa NPs. Notably, PPa4 NPs demonstrated superior cellular uptake, enhanced ROS generation, and effective lysosome-targeted bursting, thereby markedly improving antitumor efficacy. In summary, the dual-mode recognition strategy offered an advanced strategy for enhancing the efficiency of PDT.","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"18 12","pages":"94908186-94908186"},"PeriodicalIF":0.0,"publicationDate":"2025-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciopen.com/article_pdf/1980454865219473410.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147333592","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Atomically dispersed single-site catalysts (ADCs) have demonstrated exceptional catalytic performance that surpasses traditional catalysts, attributed to their higher atom utilization efficiency. However, a general engineering approach for converting metal-oxo clusters into efficient and stable ADCs has not been established. In this work, an universal conversion strategy is reported to synthesize a series of noble metal ADCs (NM@WO2−W, NM = Ir, Pt, Ru, Pd) through the engineering of polyoxometalates (POMs), a well-established type of metal-oxo clusters. This strategy confines the single noble metal atom within the lattice of WO2, thereby creating lattice-confined ADCs. The as-prepared Pt@WO2−W exhibits enhanced catalytic activity for the hydrogen evolution reaction (HER), with an impressively low overpotential of 49 mV at 50 mA cm−2 and robust durability over 50 h, with only 0.2% current density decay. Furthermore, the catalytic behavior of NM@WO2−W in the oxygen evolution reaction (OER) has also been explored, highlighting the superior electrocatalytic activity and durability of Ir@WO2−W. In situ experiments and density functional theory calculations further reveal the intrinsic activity of NM@WO2−W for both HER and OER. This work introduces a general strategy for the rational design of lattice-confined ADCs through conversion of metal-oxo clusters, providing efficient and stable ADCs for water electrolysis.
原子分散单位点催化剂（adc）由于具有较高的原子利用率，其催化性能优于传统催化剂。然而，将金属-氧基团转化为高效稳定的adc的一般工程方法尚未建立。在这项工作中，报告了一种通用的转化策略，通过多金属氧酸盐（pom）的工程合成一系列贵金属adc (NM@WO2−W, NM = Ir, Pt, Ru, Pd)，这是一种成熟的金属-氧簇。这种策略将单个贵金属原子限制在WO2的晶格内，从而产生晶格受限adc。制备的Pt@WO2−W对析氢反应（HER）具有增强的催化活性，在50 mA cm−2下的过电位极低，为49 mV，耐用性超过50小时，电流密度衰减仅为0.2%。此外，NM@WO2−W在析氧反应（OER）中的催化行为也被探索，强调了Ir@WO2−W优越的电催化活性和耐久性。原位实验和密度泛函理论计算进一步揭示了NM@WO2−W对HER和OER的内在活性。本文介绍了一种通过转换金属氧基团合理设计晶格限制adc的一般策略，为水电解提供高效稳定的adc。
{"title":"Polyoxometalates-derived lattice-confined atomically dispersed catalysts for water electrolysis","authors":"Peilei He, Wei Wang, Mingxin Cai, Shifeng Hou, Huiling Liu, Xun Wang","doi":"10.26599/nr.2025.94908188","DOIUrl":"https://doi.org/10.26599/nr.2025.94908188","url":null,"abstract":"Atomically dispersed single-site catalysts (ADCs) have demonstrated exceptional catalytic performance that surpasses traditional catalysts, attributed to their higher atom utilization efficiency. However, a general engineering approach for converting metal-oxo clusters into efficient and stable ADCs has not been established. In this work, an universal conversion strategy is reported to synthesize a series of noble metal ADCs (NM@WO<sub>2</sub>−W, NM = Ir, Pt, Ru, Pd) through the engineering of polyoxometalates (POMs), a well-established type of metal-oxo clusters. This strategy confines the single noble metal atom within the lattice of WO<sub>2</sub>, thereby creating lattice-confined ADCs. The as-prepared Pt@WO<sub>2</sub>−W exhibits enhanced catalytic activity for the hydrogen evolution reaction (HER), with an impressively low overpotential of 49 mV at 50 mA cm<sup>−2</sup> and robust durability over 50 h, with only 0.2% current density decay. Furthermore, the catalytic behavior of NM@WO<sub>2</sub>−W in the oxygen evolution reaction (OER) has also been explored, highlighting the superior electrocatalytic activity and durability of Ir@WO<sub>2</sub>−W. <em>In situ</em> experiments and density functional theory calculations further reveal the intrinsic activity of NM@WO<sub>2</sub>−W for both HER and OER. This work introduces a general strategy for the rational design of lattice-confined ADCs through conversion of metal-oxo clusters, providing efficient and stable ADCs for water electrolysis.","PeriodicalId":713,"journal":{"name":"Nano Research","volume":"19 4","pages":"94908188-94908188"},"PeriodicalIF":0.0,"publicationDate":"2025-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciopen.com/article_pdf/1980515361213763585.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147332923","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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