Pub Date : 2026-01-01Epub Date: 2025-10-10DOI: 10.1016/j.cjsc.2025.100763
Piao Tang , Xin Wen , Jindong Chen , Ning Ye , Guang Peng
Based on a functional group composite strategy, the first Ag-containing phosphate-tellurite nonlinear optical (NLO) crystal, Ag(Te2O3)(PO4), was synthesized via a subcritical hydrothermal method. This crystal crystallizes in the noncentrosymmetric space group Pmn21, featuring a unique zigzag two-dimensional [(Te2O3)(PO4)]∞ layer. It possesses the strongest powder second-harmonic generation (SHG) response among all reported phosphate-tellurite compounds, reaching 2.1 × KH2PO4, along with a moderate birefringence of 0.045@546 nm. Theoretical calculations indicate that the TeO4 group with stereochemically active lone-pair electrons, together with AgO7 polyhedra and PO4 group, synergistically contributes to its optical properties. This functional group composite strategy not only facilitates the integration of phosphate and tellurite units with Ag+ cations, but also offers a versatile route for designing NLO materials across diverse inorganic systems.
{"title":"Ag(Te2O3)(PO4): The first Ag-containing phosphate-tellurite nonlinear optical crystal featuring novel zigzag layered structure","authors":"Piao Tang , Xin Wen , Jindong Chen , Ning Ye , Guang Peng","doi":"10.1016/j.cjsc.2025.100763","DOIUrl":"10.1016/j.cjsc.2025.100763","url":null,"abstract":"<div><div>Based on a functional group composite strategy, the first Ag-containing phosphate-tellurite nonlinear optical (NLO) crystal, Ag(Te<sub>2</sub>O<sub>3</sub>)(PO<sub>4</sub>), was synthesized <em>via</em> a subcritical hydrothermal method. This crystal crystallizes in the noncentrosymmetric space group <em>Pmn</em>2<sub>1</sub>, featuring a unique zigzag two-dimensional [(Te<sub>2</sub>O<sub>3</sub>)(PO<sub>4</sub>)]<sub>∞</sub> layer. It possesses the strongest powder second-harmonic generation (SHG) response among all reported phosphate-tellurite compounds, reaching 2.1 × KH<sub>2</sub>PO<sub>4</sub>, along with a moderate birefringence of 0.045@546 nm. Theoretical calculations indicate that the TeO<sub>4</sub> group with stereochemically active lone-pair electrons, together with AgO<sub>7</sub> polyhedra and PO<sub>4</sub> group, synergistically contributes to its optical properties. This functional group composite strategy not only facilitates the integration of phosphate and tellurite units with Ag<sup>+</sup> cations, but also offers a versatile route for designing NLO materials across diverse inorganic systems.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100763"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941446","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Separation of ternary cyclic C6 hydrocarbons, i.e., the mixture of benzene (Bz), cyclohexene (Cye), and cyclohexane (Cya), is one of the critical chemical processes but challenging in the petrochemical industry. Here, we design and synthesize a stable Al-based metal-organic framework with high-quality single crystals, which exhibits excellent thermal stability (up to 300 °C), acid-base stability (within a pH range of 2–12) and boiling-water stability. Interestingly, by virtue of multiple gates controlled by organic fragments and/or inorganic clusters in the quasi-three-dimensional pores, the framework exhibits not only ultrahigh Bz/Cya (180) and Bz/Cye (66) selectivities, but also ultrahigh Bz selectivity (118) from the ternary Bz/Cye/Cya mixture. Notably, all the above selectivities rank in the top three in all porous materials, and the Bz/Cye selectivity is the highest to date. Single-crystal X-ray diffraction analyses and computational simulations revealed that the multiple types of gating play the crucial role in the adsorption and separation of Bz/Cye/Cya mixture.
{"title":"An Al-based metal-organic framework with multiple gates for highly efficient separation of benzene/cyclohexene/cyclohexane","authors":"Wen-Yu Su , Fang-Di Dong , Zi-Luo Fang, Zhi-Shuo Wang, Mu-Yang Zhou, Xi Feng, Xiao-Tong Lu, Rong-Hua Wang, Xing-Yu Li, Dong-Dong Zhou","doi":"10.1016/j.cjsc.2025.100766","DOIUrl":"10.1016/j.cjsc.2025.100766","url":null,"abstract":"<div><div>Separation of ternary cyclic C<sub>6</sub> hydrocarbons, <em>i.e</em>., the mixture of benzene (Bz), cyclohexene (Cye), and cyclohexane (Cya), is one of the critical chemical processes but challenging in the petrochemical industry. Here, we design and synthesize a stable Al-based metal-organic framework with high-quality single crystals, which exhibits excellent thermal stability (up to 300 °C), acid-base stability (within a pH range of 2–12) and boiling-water stability. Interestingly, by virtue of multiple gates controlled by organic fragments and/or inorganic clusters in the quasi-three-dimensional pores, the framework exhibits not only ultrahigh Bz/Cya (180) and Bz/Cye (66) selectivities, but also ultrahigh Bz selectivity (118) from the ternary Bz/Cye/Cya mixture. Notably, all the above selectivities rank in the top three in all porous materials, and the Bz/Cye selectivity is the highest to date. Single-crystal X-ray diffraction analyses and computational simulations revealed that the multiple types of gating play the crucial role in the adsorption and separation of Bz/Cye/Cya mixture.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100766"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941517","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-01Epub Date: 2025-10-10DOI: 10.1016/j.cjsc.2025.100761
Fan Yang , Guan-Huang Zhang , Hai-Ling Wang , Wen-Wen Qin , Zhong-Hong Zhu , Fu-Pei Liang , Hua-Hong Zou
In this work, an ultrasonic tailoring strategy was used to obtain nanosized one-dimensional chain-like lanthanide metal-organic frameworks (Ln-MOFs) with excellent photophysical properties for the first time, and high-resolution bio-optical imaging applications were achieved. As the ambient temperature gradually increases, the chain-like Ln-MOFs do not show obvious thermal quenching of luminescence. It is worth noting that when the ambient temperature exceeds 300 K, the departure of the terminal-coordinated H2O molecules within the Ln-MOFs structure induces significant thermally enhanced luminescence. Furthermore, by regulating the energy transfer pathways of bimetallic-doped TbxEu(1−x)-MOFs, a series of luminescence changes from yellow-green to red were achieved. Based on the multiple excitation, thermally enhanced luminescence, and multicolor luminescence properties of Ln-MOFs, a complex anti-counterfeiting system was constructed. More noteworthy is that the Ln-MOFs nanochains obtained using the ultrasonic cutting strategy have high-resolution optical imaging effects on HeLa, MCF-7, MDA-MB-231 cells and living zebrafish, and can specifically label the lysosomes of living cells. This work opens up new horizons for the application of multidimensional lanthanide complex emitters in high-resolution bio-optical imaging and opens a new blueprint for constructing lanthanide complex emitters with “all-in-one” functions.
{"title":"Ultrasonic cutting strategy yields lanthanide organic nanochains with bright emission: Thermally enhanced luminescence and bio-optical imaging","authors":"Fan Yang , Guan-Huang Zhang , Hai-Ling Wang , Wen-Wen Qin , Zhong-Hong Zhu , Fu-Pei Liang , Hua-Hong Zou","doi":"10.1016/j.cjsc.2025.100761","DOIUrl":"10.1016/j.cjsc.2025.100761","url":null,"abstract":"<div><div>In this work, an ultrasonic tailoring strategy was used to obtain nanosized one-dimensional chain-like lanthanide metal-organic frameworks (<strong>Ln-MOFs</strong>) with excellent photophysical properties for the first time, and high-resolution bio-optical imaging applications were achieved. As the ambient temperature gradually increases, the chain-like <strong>Ln-MOFs</strong> do not show obvious thermal quenching of luminescence. It is worth noting that when the ambient temperature exceeds 300 K, the departure of the terminal-coordinated H<sub>2</sub>O molecules within the <strong>Ln-MOFs</strong> structure induces significant thermally enhanced luminescence. Furthermore, by regulating the energy transfer pathways of bimetallic-doped <strong>Tb<sub><em>x</em></sub>Eu<sub>(1</sub></strong><em><sub>−</sub></em><strong><sub><em>x</em>)</sub>-MOFs</strong>, a series of luminescence changes from yellow-green to red were achieved. Based on the multiple excitation, thermally enhanced luminescence, and multicolor luminescence properties of <strong>Ln-MOFs</strong>, a complex anti-counterfeiting system was constructed. More noteworthy is that the <strong>Ln-MOFs</strong> nanochains obtained using the ultrasonic cutting strategy have high-resolution optical imaging effects on HeLa, MCF-7, MDA-MB-231 cells and living zebrafish, and can specifically label the lysosomes of living cells. This work opens up new horizons for the application of multidimensional lanthanide complex emitters in high-resolution bio-optical imaging and opens a new blueprint for constructing lanthanide complex emitters with “all-in-one” functions.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100761"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-01Epub Date: 2025-10-10DOI: 10.1016/j.cjsc.2025.100765
Chaochao Fan , Yue Wang , Dan Zhang , Wei Zuo , Wenxiong Zhang , Chuandong Jia
Anthracene group features fluorescence, π conjugation, and stimulus-responsive characteristics, and therefore, anthracene-containing supramolecular assemblies have attracted much more extensive attention from supramolecular chemists. Anthracene moiety is susceptible to attack by singlet oxygen (1O2), and it undergoes [4 + 2] photooxygenation via capturing 1O2 under 365 nm irradiation, generating endoperoxide photoproducts that could release 1O2 through heat. A variety of anthracene-based supramolecular assemblies are elegantly designed and synthesized to further explore their properties. In the past few decades, numerous articles and few reviews about the [4 + 4] photodimerization of anthracene moiety have been published. Howerer, to the best of our knowledge, very few reviews focusing on anthracene-based supramolecular systems and their reversible [4 + 2] photochemical oxidation have hardly been reported. The minor review primarily highlights typical examples of anthracene-containing supramolecular assemblies in terms of construction strategy, properties, and the [4 + 2] photooxygenation. In this review, the main content will be classified into four categories: (I) chirality in anthracene-based supramolecular assemblies; (II) luminescence regulation in anthracene-containing supramolecular assemblies; (III) π···π interactions in anthracene-based supramolecular assemblies; (IV) [4 + 2] photooxygenation in anthracene-based supramolecular assemblies including discrete, polymeric, and anion-directed structures. We wish this mini-review could provide fundamental inspiration for supramolecular scientists to further develop novel anthracene-containing assemblies based on coordination-driven self-assembly and study their photochemical reactions, which is showing potential for application in smart materials.
{"title":"Exploration and development of anthracene-containing supramolecular assemblies and their [4 + 2] photooxygenation","authors":"Chaochao Fan , Yue Wang , Dan Zhang , Wei Zuo , Wenxiong Zhang , Chuandong Jia","doi":"10.1016/j.cjsc.2025.100765","DOIUrl":"10.1016/j.cjsc.2025.100765","url":null,"abstract":"<div><div>Anthracene group features fluorescence, π conjugation, and stimulus-responsive characteristics, and therefore, anthracene-containing supramolecular assemblies have attracted much more extensive attention from supramolecular chemists. Anthracene moiety is susceptible to attack by singlet oxygen (<sup>1</sup>O<sub>2</sub>), and it undergoes [4 + 2] photooxygenation via capturing <sup>1</sup>O<sub>2</sub> under 365 nm irradiation, generating endoperoxide photoproducts that could release <sup>1</sup>O<sub>2</sub> through heat. A variety of anthracene-based supramolecular assemblies are elegantly designed and synthesized to further explore their properties. In the past few decades, numerous articles and few reviews about the [4 + 4] photodimerization of anthracene moiety have been published. Howerer, to the best of our knowledge, very few reviews focusing on anthracene-based supramolecular systems and their reversible [4 + 2] photochemical oxidation have hardly been reported. The minor review primarily highlights typical examples of anthracene-containing supramolecular assemblies in terms of construction strategy, properties, and the [4 + 2] photooxygenation. In this review, the main content will be classified into four categories: (I) chirality in anthracene-based supramolecular assemblies; (II) luminescence regulation in anthracene-containing supramolecular assemblies; (III) π···π interactions in anthracene-based supramolecular assemblies; (IV) [4 + 2] photooxygenation in anthracene-based supramolecular assemblies including discrete, polymeric, and anion-directed structures. We wish this mini-review could provide fundamental inspiration for supramolecular scientists to further develop novel anthracene-containing assemblies based on coordination-driven self-assembly and study their photochemical reactions, which is showing potential for application in smart materials.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100765"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941145","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-01Epub Date: 2025-10-11DOI: 10.1016/j.cjsc.2025.100767
Pan Gao , Qingzheng Kong , Ying Sun , Qian Ma , Qi Wang , Zeyu Guo , Ledi Li , Bingbing Li , Jingwei Xu , Xiaomei Jiang , Zhaolai Chen
X-ray detectors, as crucial elements in medical imaging and industrial fields, can be categorized into direct and indirect types. Direct detectors, which directly convert X-ray photons into electrical signals, exhibit high sensitivity and low detection limits, enabling the capture of high-resolution images and reducing radiation exposure to patients. Organic copper halides, recognized as potential active materials for X-ray detection, have been widely explored in the indirect scintillation field but remain under-explored in direct X-ray detector applications. In this work, (C12H12N)3Cu3I6 is demonstrated as an efficient semiconductor for direct X-ray detection with excellent stability. A lateral-structured X-ray detector was fabricated with gold electrodes, which exhibits a maximum sensitivity of 1464.14 μC·Gy−1·cm−2, a lowest detection limit of 19.8 nGy·s−1, a high on-off ratio of 2140, and an excellent operational stability of retaining 96% performance after 600 s continuous X-ray radiation. Furthermore, the detector successfully imaged a 0.1 mm “F”-shaped lead sheet, validating its capacity for X-ray imaging. This study highlights the potential of (C12H12N)3Cu3I6 as a promising semiconductor for high-performance direct X-ray detection, expanding the application scope of organic copper halides in this critical field.
x射线探测器是医学成像和工业领域的重要组成部分，可分为直接型和间接型。直接探测器直接将x射线光子转换为电信号，具有高灵敏度和低检测极限，可以捕获高分辨率图像并减少对患者的辐射暴露。有机卤化铜作为一种潜在的x射线探测活性材料，在间接闪烁领域得到了广泛的探索，但在直接x射线探测领域的应用还不够充分。在这项工作中，（C12H12N）3Cu3I6被证明是一种有效的半导体，用于直接x射线检测，具有优异的稳定性。采用金电极制备了一种横向结构的x射线探测器，最大灵敏度为1464.14 μC·Gy−1·cm−2，最低检出限为19.8 nGy·s−1，通断比为2140，在连续600 s x射线照射后仍能保持96%的性能。此外，该探测器还成功地对0.1 mm“F”形铅片进行了成像，验证了其x射线成像能力。该研究突出了（C12H12N）3Cu3I6作为高性能直接x射线探测半导体的潜力，扩大了有机卤化铜在这一关键领域的应用范围。
{"title":"One-dimensional (C12H12N)3Cu3I6 for high-performance direct X-ray detection","authors":"Pan Gao , Qingzheng Kong , Ying Sun , Qian Ma , Qi Wang , Zeyu Guo , Ledi Li , Bingbing Li , Jingwei Xu , Xiaomei Jiang , Zhaolai Chen","doi":"10.1016/j.cjsc.2025.100767","DOIUrl":"10.1016/j.cjsc.2025.100767","url":null,"abstract":"<div><div>X-ray detectors, as crucial elements in medical imaging and industrial fields, can be categorized into direct and indirect types. Direct detectors, which directly convert X-ray photons into electrical signals, exhibit high sensitivity and low detection limits, enabling the capture of high-resolution images and reducing radiation exposure to patients. Organic copper halides, recognized as potential active materials for X-ray detection, have been widely explored in the indirect scintillation field but remain under-explored in direct X-ray detector applications. In this work, (C<sub>12</sub>H<sub>12</sub>N)<sub>3</sub>Cu<sub>3</sub>I<sub>6</sub> is demonstrated as an efficient semiconductor for direct X-ray detection with excellent stability. A lateral-structured X-ray detector was fabricated with gold electrodes, which exhibits a maximum sensitivity of 1464.14 μC·Gy<sup>−1</sup>·cm<sup>−2</sup>, a lowest detection limit of 19.8 nGy·s<sup>−1</sup>, a high on-off ratio of 2140, and an excellent operational stability of retaining 96% performance after 600 s continuous X-ray radiation. Furthermore, the detector successfully imaged a 0.1 mm “F”-shaped lead sheet, validating its capacity for X-ray imaging. This study highlights the potential of (C<sub>12</sub>H<sub>12</sub>N)<sub>3</sub>Cu<sub>3</sub>I<sub>6</sub> as a promising semiconductor for high-performance direct X-ray detection, expanding the application scope of organic copper halides in this critical field.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100767"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941443","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The polymeric semiconductor photocatalyst graphitic carbon nitride (g-C3N4) has attracted considerable attention due to its visible-light responsiveness and excellent biocompatibility. However, the photocatalytic efficiency of bulk g-C3N4 (CNB) remains insufficient for pratical applications, primarily due to its limited light absorption range and the rapid charge carrier recombination. In this study, K+-doped crystalline g-C3N4 with cyano defects (CNK) was synthesized by the calcination of dicyandiamide in the presence of KCl. The addition of KCl promoted the formation of K+-doped crystalline g-C3N4 with cyano defects. The optimized photocatalyst (CNK2) exhibits the highest photocatalytic activity for NO oxidation, achieving a removal rate of 47.40%, which is 2.1 times higher than that of CNB. This enhancement is mainly attributed to the increased generation of reactive oxygen species (ROS), particularly superoxide radicals (·O2−) and singlet oxygen (1O2). Furthermore, improved performance in photocatalytic CO2-to-CH4 conversion was also observed, which is attributed to the formation of a build-in electric field (BIEF) induced by K+ ion doping and the introduction of cyano defects.
{"title":"Enhancing the photocatalytic activity of crystalline g-C3N4 towards NO oxidation and CO2 reduction through K+-doping and cyano defect engineering","authors":"Zhou Li , Mengxue Yu , Shixin Chang , Zhibin Huang , Zhenmin Cheng , Weibin Zhang , Sónia A.C. Carabineiro , Zhigao Xu , Kangle Lv","doi":"10.1016/j.cjsc.2025.100698","DOIUrl":"10.1016/j.cjsc.2025.100698","url":null,"abstract":"<div><div>The polymeric semiconductor photocatalyst graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) has attracted considerable attention due to its visible-light responsiveness and excellent biocompatibility. However, the photocatalytic efficiency of bulk g-C<sub>3</sub>N<sub>4</sub> (CNB) remains insufficient for pratical applications, primarily due to its limited light absorption range and the rapid charge carrier recombination. In this study, K<sup>+</sup>-doped crystalline g-C<sub>3</sub>N<sub>4</sub> with cyano defects (CNK) was synthesized by the calcination of dicyandiamide in the presence of KCl. The addition of KCl promoted the formation of K<sup>+</sup>-doped crystalline g-C<sub>3</sub>N<sub>4</sub> with cyano defects. The optimized photocatalyst (CNK2) exhibits the highest photocatalytic activity for NO oxidation, achieving a removal rate of 47.40%, which is 2.1 times higher than that of CNB. This enhancement is mainly attributed to the increased generation of reactive oxygen species (ROS), particularly superoxide radicals (·O<sub>2</sub><sup>−</sup>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>). Furthermore, improved performance in photocatalytic CO<sub>2</sub>-to-CH<sub>4</sub> conversion was also observed, which is attributed to the formation of a build-in electric field (BIEF) induced by K<sup>+</sup> ion doping and the introduction of cyano defects.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"45 1","pages":"Article 100698"},"PeriodicalIF":10.3,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145941518","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-01Epub Date: 2025-09-24DOI: 10.1016/j.cjsc.2025.100745
Ziqiang Wang , Han Lin , Wenxin Wang , Hongjie Yu , You Xu , Kai Deng , Hongjing Wang , Liang Wang
The electrochemical upgrading of polyethylene terephthalate (PET) plastics represents a highly promising strategy for achieving high-value utilization of waste resources, and its efficiency is highly related to identify active electrocatalysts for PET-derived ethylene glycol oxidation reaction (EGOR). In this work, atomically thin high-entropy PdPtRhFeCuMo metallene nanoribbons (PdPtRhFeCuMo HMRs) have been synthesized and served as high-performance catalysts for electro-reforming PET plastic, which possess a high current density of 180 mA cm−2 at a low potential of 0.9 V for EGOR, with excellent Faraday efficiency (FE) of 96.81% for highly efficient and selective conversion of EG into high-value-added glycolic acid (GA). Experimental and theoretical results reveal that the multi-metallic synergistic effect of PdPtRhFeCuMo HMRs effectively modulates adsorption behavior of intermediates and reduce the EGOR energy barrier, thus promoting the selective EG-to-GA conversion. This study proposes the reasonable design of high-entropy metallene nanoribbons for the electrochemical upgrading of PET plastics to high-value C2 products.
聚对苯二甲酸乙二醇酯（PET）塑料的电化学升级是实现废物资源高价值利用的一种非常有前途的策略，其效率与PET衍生的乙二醇氧化反应（EGOR）的活性电催化剂的鉴定高度相关。本研究合成了原子薄的高熵pdptrfecumo金属烯纳米带（pdptrfecumo HMRs），作为电重整PET塑料的高性能催化剂，在0.9 V的低电位下具有180 mA cm−2的高电流密度，具有96.81%的法拉第效率（FE），可将EG高效、选择性地转化为高附加值的乙醇酸（GA）。实验和理论结果表明，PdPtRhFeCuMo HMRs的多金属协同效应可以有效调节中间体的吸附行为，降低EGOR的能垒，从而促进EGOR向ga的选择性转化。本研究提出了高熵金属烯纳米带的合理设计，用于PET塑料的电化学升级生产高价值的C2产品。
{"title":"High-entropy PdPtRhFeCuMo metallene nanoribbons for electro-reforming PET plastic into glycolic acid","authors":"Ziqiang Wang , Han Lin , Wenxin Wang , Hongjie Yu , You Xu , Kai Deng , Hongjing Wang , Liang Wang","doi":"10.1016/j.cjsc.2025.100745","DOIUrl":"10.1016/j.cjsc.2025.100745","url":null,"abstract":"<div><div>The electrochemical upgrading of polyethylene terephthalate (PET) plastics represents a highly promising strategy for achieving high-value utilization of waste resources, and its efficiency is highly related to identify active electrocatalysts for PET-derived ethylene glycol oxidation reaction (EGOR). In this work, atomically thin high-entropy PdPtRhFeCuMo metallene nanoribbons (PdPtRhFeCuMo HMRs) have been synthesized and served as high-performance catalysts for electro-reforming PET plastic, which possess a high current density of 180 mA cm<sup>−2</sup> at a low potential of 0.9 V for EGOR, with excellent Faraday efficiency (FE) of 96.81% for highly efficient and selective conversion of EG into high-value-added glycolic acid (GA). Experimental and theoretical results reveal that the multi-metallic synergistic effect of PdPtRhFeCuMo HMRs effectively modulates adsorption behavior of intermediates and reduce the EGOR energy barrier, thus promoting the selective EG-to-GA conversion. This study proposes the reasonable design of high-entropy metallene nanoribbons for the electrochemical upgrading of PET plastics to high-value C<sub>2</sub> products.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"44 12","pages":"Article 100745"},"PeriodicalIF":10.3,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145749710","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-01Epub Date: 2025-09-16DOI: 10.1016/j.cjsc.2025.100729
Yuxin Wang , Xueqiang Guo , Chao Zhi , Lifei Yin , Meng Wang , Jinping Li , Libo Li , Jia Yao
The quantitative detection of biological metabolites is a crucial route for early diagnosis of human diseases. Exhaled ammonia (NH3), originating from abnormal metabolism, is normally recognized as the biomarker for liver and kidney lesions. Therefore, developing highly sensitive fluorescent sensing materials is expected to replace the traditional clinical blood tests and facilitate painless diagnosis and telemedicine for patients. However, the weak interaction for ammonia and the small color switching range of fluorescence sensors become the most pressing problem at present. Herein, a porphyrin-based hydrogen-bonded organic framework (HOF-6) with abundant supermolecule interactions in the confined pore space is developed for highly sensitive ammonia detection. The strong interactions between ammonia and the framework greatly promote the electron rearrangement and enhance the intensity of fluorescence, enabling HOF-6 to successfully achieve trace amounts of ammonia sensing with the limit detection of 0.2 ppm. With the ultrahigh selectivity for ammonia, HOF-6 can accurately determine the amount of ammonia in breath of patients, and the test results are highly consistent with blood ammonia levels. The tailor-made multiple interactions in the confined pore space provide an effective approach for highly sensitive ammonia detection, as well as brings good news to liver and kidney patients for non-invasive diagnosis and real-time health monitoring.
{"title":"Hydrogen-bonded organic framework with ammonia recognition “pocket” for exhaled ammonia fluorescence sensing","authors":"Yuxin Wang , Xueqiang Guo , Chao Zhi , Lifei Yin , Meng Wang , Jinping Li , Libo Li , Jia Yao","doi":"10.1016/j.cjsc.2025.100729","DOIUrl":"10.1016/j.cjsc.2025.100729","url":null,"abstract":"<div><div>The quantitative detection of biological metabolites is a crucial route for early diagnosis of human diseases. Exhaled ammonia (NH<sub>3</sub>), originating from abnormal metabolism, is normally recognized as the biomarker for liver and kidney lesions. Therefore, developing highly sensitive fluorescent sensing materials is expected to replace the traditional clinical blood tests and facilitate painless diagnosis and telemedicine for patients. However, the weak interaction for ammonia and the small color switching range of fluorescence sensors become the most pressing problem at present. Herein, a porphyrin-based hydrogen-bonded organic framework (HOF-6) with abundant supermolecule interactions in the confined pore space is developed for highly sensitive ammonia detection. The strong interactions between ammonia and the framework greatly promote the electron rearrangement and enhance the intensity of fluorescence, enabling HOF-6 to successfully achieve trace amounts of ammonia sensing with the limit detection of 0.2 ppm. With the ultrahigh selectivity for ammonia, HOF-6 can accurately determine the amount of ammonia in breath of patients, and the test results are highly consistent with blood ammonia levels. The tailor-made multiple interactions in the confined pore space provide an effective approach for highly sensitive ammonia detection, as well as brings good news to liver and kidney patients for non-invasive diagnosis and real-time health monitoring.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"44 12","pages":"Article 100729"},"PeriodicalIF":10.3,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145749704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
扫码关注我们
求助内容：
应助结果提醒方式：
京公网安备 11010802042870号