IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-06 DOI: 10.1002/anie.202511262

Juyoung Lee, Hyeong Seok Oh, Soohyun Ban, Jinhyeok Cho, Kang Hee Ku

{"title":"Disordered Inverse Photonic Beads Assembled From Linear Block Copolymers","authors":"Juyoung Lee, Hyeong Seok Oh, Soohyun Ban, Jinhyeok Cho, Kang Hee Ku","doi":"10.1002/anie.202511262","DOIUrl":"https://doi.org/10.1002/anie.202511262","url":null,"abstract":"Structurally colored colloids, or photonic pigments, offer a sustainable alternative to conventional dyes, yet existing systems are constrained by limited morphologies and complex synthesis. In particular, achieving angle‐independent color typically relies on disordered inverse architectures formed from synthetically demanding bottlebrush block copolymers (BCPs), hindering scalability and functional diversity. Here, we report a conceptually distinct strategy to assemble three‐dimensional inverse photonic glass microparticles using amphiphilic linear BCPs (poly(styrene‐block‐4‐vinylpyridine), PS‐b‐P4VP) via an emulsion‐templated process. By employing trans‐1,2‐dichloroethylene to promote interfacial water infiltration, nanoscale aqueous domains form within the organic phase and direct short‐range‐ordered pore structures. Evaporative solidification arrests these structures into porous photonic beads with angle‐independent color. Systematic control of surfactant alkyl chain length and BCP molecular weight enables precise tuning of pore size, shell thickness, and visible‐range optical output. Furthermore, post‐chemical modification via quaternization of P4VP provides an orthogonal chemical handle to modulate interfacial instability and photonic behavior. This work expands the self‐assembly capabilities of linear BCPs and establishes a modular, scalable platform for producing structurally and chemically programmable photonic pigments.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"28 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003078","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

Water as an Electron Donor for Cross-Electrophile Coupling Reactions. 水作为亲电偶联反应的电子供体。

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-09-06 DOI: 10.1021/jacs.5c12176

Jun-Li Li,Can-Ming Zhu,Huai-Gui Li,Pan-Feng Yuan,Qing-Yuan Meng

引用次数: 0

Oxidatively Induced Reductive N2 Binding: A Dinickel-Bridging Bent N2 Radical Anion and Its Redox-Triggered N2 Release. 氧化诱导的还原N2结合：镍桥接的弯曲N2自由基阴离子及其氧化还原触发的N2释放。

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-09-06 DOI: 10.1021/jacs.5c09334

Sara I Mozzi,Dennis-Helmut Manz,Nils Ostermann,Roland A Schulz,Peng-Cheng Duan,Thomas Kothe,Martin Diefenbach,Sebastian Dechert,Serhiy Demeshko,Vera Krewald,Inke Siewert,Franc Meyer

{"title":"Oxidatively Induced Reductive N2 Binding: A Dinickel-Bridging Bent N2 Radical Anion and Its Redox-Triggered N2 Release.","authors":"Sara I Mozzi,Dennis-Helmut Manz,Nils Ostermann,Roland A Schulz,Peng-Cheng Duan,Thomas Kothe,Martin Diefenbach,Sebastian Dechert,Serhiy Demeshko,Vera Krewald,Inke Siewert,Franc Meyer","doi":"10.1021/jacs.5c09334","DOIUrl":"https://doi.org/10.1021/jacs.5c09334","url":null,"abstract":"Nitrogenase accumulates reducing equivalents in hydrides and couples H2 elimination to the reductive binding of N2 at a di-iron edge of its FeMo cofactor (FeMoco). Here, we describe that oxidation of a pyrazolato-based dinickel(II) dihydride complex K[L(Ni-H)2] (1K), either electrochemically or chemically using H+ or ferrocenium, triggers H2 elimination and binding of N2 in a constrained and extremely bent bridging mode in [LNi2(μ1,2-N2)] (3N2). Spectroscopic and computational evidence indicate that the electronic structure of 3N2 is best described as NiII-(N2•-)-NiII, with a rare 1e- reduced and significantly activated N2 substrate (ṽ̃NN = 1894 cm-1). 3N2 is also formed upon 1e- oxidation of K[LNi2I] (2K) under N2. This is an unusual and counterintuitive scenario where the oxidation of a dinickel(II) dihydride, or of a dinickel(I) complex, induces the reductive activation of N2. Detailed (spectro)electrochemical studies and DFT calculations confirm that N2 binding by the {LNi2} platform occurs only in the regime of the mixed-valent NiIINiI species, while both oxidation and reduction induce the release of N2 from 3N2; the latter represents a redox-induced electron transfer (RIET) process where metal reduction leads to N2•- oxidation due to intramolecular back electron transfer. These findings offer new perspectives for understanding the multi-e-/H+ scenarios of N2 fixation via hydride intermediates inspired by the FeMoco function, and for the development of synthetic platforms that avoid strongly reducing conditions for N2 activation.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"30 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003282","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

Contact-electro-catalysis of polytetrafluoroethylene particles for luminol electrochemiluminescence/sonochemiluminescence and its application for detecting superoxide dismutase and thiabendazole 聚四氟乙烯颗粒接触电催化发光/声化学发光及其在超氧化物歧化酶和噻苯达唑检测中的应用

IF 8.4 1区化学

Sensors and Actuators B: Chemical Pub Date : 2025-09-06 DOI: 10.1016/j.snb.2025.138714

Danli Zhong, Haidong Li, Yuxin Yang, Xianjing Huang, Zhenxing Yang, Chengyin Wang

{"title":"Contact-electro-catalysis of polytetrafluoroethylene particles for luminol electrochemiluminescence/sonochemiluminescence and its application for detecting superoxide dismutase and thiabendazole","authors":"Danli Zhong, Haidong Li, Yuxin Yang, Xianjing Huang, Zhenxing Yang, Chengyin Wang","doi":"10.1016/j.snb.2025.138714","DOIUrl":"https://doi.org/10.1016/j.snb.2025.138714","url":null,"abstract":"The efficient generation of reactive oxygen species (ROS) is crucial for achieving intense luminol emission, but conventional methods typically require either the addition of H2O2 or the use of elaborate electrocatalysts to activate dissolved oxygen. By taking advantage of contact-electro-catalysis, the simple ultrasonication of a suspension of polytetrafluoroethylene (PTFE) particles can yield abundant H2O2, enhancing luminol electrochemiluminescence (ECL) by two orders of magnitude. Mechanistic investigations suggest that the contact-electro-catalysis of PTFE particles facilitates the water oxidation reaction (WOR) and oxygen reduction reaction (ORR), resulting in the production of superoxide anion radical (O2•−) and hydroxyl radical (HO•) during ultrasonication. This catalytic behavior provides a new approach to generate stronger luminol sonochemiluminescence (SCL) in the presence of PTFE particles at neutral pH. Based on the enhanced luminol SCL, Turn-off/on SCL sensors are designed to sensitively detect superoxide dismutase (SOD) in the range of 0.0050–2.0 μg/mL and thiabendazole (TBZ) in the range of 0.500–60.0 μM. Finally, contact-electro-catalysis of PTFE on luminol at physiological pH may provide the possibility for bioanalysis or sonotherapy.","PeriodicalId":425,"journal":{"name":"Sensors and Actuators B: Chemical","volume":"24 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003507","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

Dissipative particle dynamics simulations of wormlike chain adsorption onto planar walls in a pressure-driven flow 压力驱动流动中蚓状链在平面壁上吸附的耗散粒子动力学模拟

IF 2.8 4区化学

Journal of Polymer Research Pub Date : 2025-09-06 DOI: 10.1007/s10965-025-04468-z

Shaofeng Xu, Zichen Wang, Yifan Yu, Chuzhen Zhu, Wei Zhang

{"title":"Dissipative particle dynamics simulations of wormlike chain adsorption onto planar walls in a pressure-driven flow","authors":"Shaofeng Xu, Zichen Wang, Yifan Yu, Chuzhen Zhu, Wei Zhang","doi":"10.1007/s10965-025-04468-z","DOIUrl":"10.1007/s10965-025-04468-z","url":null,"abstract":"<div>Adsorption of wormlike chain onto planar walls in a pressure-driven flow was investigated using dissipative particle dynamics (DPD) method. The wormlike chain was modeled by the well-known bead-spring chain connected by the Marko-Siggia spring. Under static condition, the wormlike chain is adsorbed onto the wall in an extended conformation and forms trains for a strongly adsorbed wall, while sections of the chain are adsorbed and the chains form loops and tails for a weakly adsorbed wall. In the presence of pressure-driven flow, our simulations show that the chain is stretched near the wall, and the chain-wall hydrodynamic interaction would lead to the desorption of the wormlike chain. The desorption is determined by an interplay between wall-chain attractive interaction and chain-wall hydrodynamic interaction. Increasing the flow strength would increase the chain-wall hydrodynamic interaction, thereby leading to a stronger desorption. The desorption rate η of worm-like chain is found to scale as (nproptodotgamma^{0.6865}) with shear rate (dotgamma). For a strongly adsorbed wall, all sections of wormlike chain are adsorbed with trains conformation, which causes the chain-wall hydrodynamic interaction to be screened.</div>","PeriodicalId":658,"journal":{"name":"Journal of Polymer Research","volume":"32 9","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144998567","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}

引用次数: 0

Strategic Formulation and Optimization of a Febuxostat Nanoparticles Infused Topical Gel Using Quality-by-Design Principles for Enhanced Therapeutic Efficacy in Gout Management 策略性配方和优化非布司他纳米颗粒注入局部凝胶使用质量设计原则，以提高痛风管理的治疗效果

IF 2 4区化学

ChemistrySelect Pub Date : 2025-09-06 DOI: 10.1002/slct.202500972

Yash D. Dudhwala, Devesh U Kapoor, Riya K. Mehta, Dhiren P. Shah, Vinod D. Ramani, Ronak R. Dedania, Manish B. Goyani, Ashok H. Akabari

{"title":"Strategic Formulation and Optimization of a Febuxostat Nanoparticles Infused Topical Gel Using Quality-by-Design Principles for Enhanced Therapeutic Efficacy in Gout Management","authors":"Yash D. Dudhwala, Devesh U Kapoor, Riya K. Mehta, Dhiren P. Shah, Vinod D. Ramani, Ronak R. Dedania, Manish B. Goyani, Ashok H. Akabari","doi":"10.1002/slct.202500972","DOIUrl":"https://doi.org/10.1002/slct.202500972","url":null,"abstract":"Gout is a painful form of inflammatory arthritis caused by the deposition of monosodium urate (MSU) crystals in joints. This study aimed to develop a topical nanogel containing polymeric nanoparticles to enhance site-specific delivery of Febuxostat (FXT) using a quality-by-design (QbD) approach. Febuxostat (FXT) nanoparticles were prepared by the solvent-evaporation method; critical factors were screened with a Plackett–Burman design and optimized via a Box–Behnken design. The optimized nanoparticles (OBFN2) displayed a particle size of 228.2 ± 10 nm, PDI 0.161 ± 0.05, zeta potential + 33.1 mV, and encapsulation efficiency 50.6% ± 5%. Incorporation of OBFN2 into a Carbopol 934 gel yielded a nanogel that released 100% of FXT within 6 h, whereas the control gel containing micronized Febuxostat (FXT) required markedly longer. The topical nanogel therefore provides faster and more complete drug release at the target site, indicating strong potential to improve therapeutic efficacy and patient adherence in gout management.","PeriodicalId":146,"journal":{"name":"ChemistrySelect","volume":"10 34","pages":""},"PeriodicalIF":2.0,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144998709","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}

引用次数: 0

A Metal‐Organic Polyhedron‐to‐Coordination Polymer Transition Revealed by 3D Electron Diffraction 三维电子衍射揭示金属-有机多面体-配位聚合物的转变

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-06 DOI: 10.1002/anie.202514527

Matthew P. Snelgrove, Beatriz Doñagueda Suso, Calum S. Sangster, Khadija Asif, Emma Regincós Martí, David J. Ashworth, Jeremiah P. Tidey, José R. B. Gomes, Miguel Jorge, Alan R. Kennedy, Simon Parsons, Ashleigh J. Fletcher, Gavin A. Craig

{"title":"A Metal‐Organic Polyhedron‐to‐Coordination Polymer Transition Revealed by 3D Electron Diffraction","authors":"Matthew P. Snelgrove, Beatriz Doñagueda Suso, Calum S. Sangster, Khadija Asif, Emma Regincós Martí, David J. Ashworth, Jeremiah P. Tidey, José R. B. Gomes, Miguel Jorge, Alan R. Kennedy, Simon Parsons, Ashleigh J. Fletcher, Gavin A. Craig","doi":"10.1002/anie.202514527","DOIUrl":"https://doi.org/10.1002/anie.202514527","url":null,"abstract":"Porous metal‐organic polyhedra (MOPs) have strong covalent and coordinate bonds that define the intrinsic pore of the cage. The intermolecular interactions between cages tend to be weaker, such that they rearrange during the solvent exchange process preceding gas sorption measurements. The reduction in crystal size that this often causes limits the availability of structural data that could enable understanding of observed gas uptake. Herein, we use 3D electron diffraction (ED) to resolve this problem, and apply this technique to a MOP‐based material that shows cooperative gas capture. 3D ED structure solution reveals both that the MOPs rearrange to form porous 1D polymers, and that these polymers are retained in the activated phase. Molecular simulations using these data suggest gas uptake is facilitated by rotation of functional groups appended to the backbone of the polymers in conjunction with structural expansion as gas is accommodated. Mechanical downsizing of the material leads to the loss of cooperative gas uptake, but a level of porosity is retained, attributed to the conservation of the 1D polymer structure. This work underscores the potential of 3D ED for probing structural transformations in functional supramolecular materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"30 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003076","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

Zwitterionic Sulfadiazine-Based Micelle Achieves Effective Drug Delivery to Glioblastoma by Overcoming Multiple Biological Barriers. 两性离子磺胺嘧啶基胶束克服多重生物屏障实现胶质母细胞瘤药物有效递送。

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-09-06 DOI: 10.1021/jacs.5c10422

Ke Zheng,Xumei Ouyang,Jing Li,Yongbin Cao,Shaojun Peng

{"title":"Zwitterionic Sulfadiazine-Based Micelle Achieves Effective Drug Delivery to Glioblastoma by Overcoming Multiple Biological Barriers.","authors":"Ke Zheng,Xumei Ouyang,Jing Li,Yongbin Cao,Shaojun Peng","doi":"10.1021/jacs.5c10422","DOIUrl":"https://doi.org/10.1021/jacs.5c10422","url":null,"abstract":"Multiple biological barriers in vivo severely restrict the delivery efficiency of nanoparticles (NPs) to tumors. To overcome biological barriers, traditional NPs usually require a complex design, which increases the difficulty of clinical translation. Therefore, there appears to be a dilemma between the complex biological barriers in vivo and clinical requirement for a simple molecular structure of NPs. Herein, an unprecedented zwitterionic polycaprolactone-poly(4-(N,N-dimethylamino-N-acetyl sulfadiazine) benzoyl oligo(ethylene glycol) methacrylate) (PCL-PSDMA) micelle is synthesized via atom transfer radical polymerization (ATRP), capable of overcoming multiple biological barriers with minimalistic structure. First, the PCL-PSDMA micelle shows a zwitterionic state in a physiological environment, exhibiting long blood circulation without triggering accelerated blood clearance. Second, the PCL-PSDMA micelle traverses the blood-brain barrier effectively owing to the pathway mediated by the l-type amino acid transporter on cerebrovascular endothelial cells. Third, the PCL-PSDMA micelle converts from zwitterionic state to positively charged state in tumor extracellular environment, facilitating deep tumor penetration and enhanced tumor cellular uptake. Lastly, the zeta potential of the PCL-PSDMA micelle transforms to a stronger positive value in the lysosomal microenvironment, resulting in effective lysosomal escape. The outstanding performance of overcoming five sequential biological barriers endows the PCL-PSDMA micelle with high drug delivery efficiency to glioblastoma, leading to pronounced antitumor effect in two types of glioblastoma-bearing mice model. Overall, this work not only adds a new member to the zwitterionic family but also broadens the horizon of developing powerful NPs for antiglioblastoma drug delivery.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"1 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003280","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

Unveiling the Origin of Morphological Instability in Topologically Complex Electrocatalytic Nanostructures. 揭示拓扑复杂电催化纳米结构中形态不稳定性的起源。

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-09-06 DOI: 10.1021/jacs.5c07842

Yawei Li,James L Hart,Ramchandra Gawas,Zhiyong Xia,Pietro P Lopes,Jieyu Zhang,Siming Li,Yucheng Wang,Mitra Taheri,Ian McCue,Joshua Snyder

{"title":"Unveiling the Origin of Morphological Instability in Topologically Complex Electrocatalytic Nanostructures.","authors":"Yawei Li,James L Hart,Ramchandra Gawas,Zhiyong Xia,Pietro P Lopes,Jieyu Zhang,Siming Li,Yucheng Wang,Mitra Taheri,Ian McCue,Joshua Snyder","doi":"10.1021/jacs.5c07842","DOIUrl":"https://doi.org/10.1021/jacs.5c07842","url":null,"abstract":"Coarsening and degradation phenomena in metals have largely focused on thermally driven processes, such as bulk and surface diffusion. However, dramatic coarsening has been reported in high-surface-area, nanometer-sized Pt-based catalysts during potential cycling in an electrolyte at room temperature─a temperature too low for the process to be explained purely by surface mobility values measured in both vacuum and electrolytes (∼10-22 and ∼10-18 cm2/s, respectively). This morphological evolution must be due to a different mechanism for mass transport that is sensitive to electrochemical conditions (e.g., electrolyte composition, potential limits, and scan rate). However, there have been no notable studies of electrochemically induced coarsening in nanometer-sized electrocatalysts. Here, we unveil the origins of coarsening in an electrolyte through coupled in situ experiments and atomistic kinetic Monte Carlo (kMC) simulations. Our work demonstrates electrochemical coarsening is driven by two concurrent mechanisms that can be explained at the atomistic level: (i) dissolution/redeposition during the reduction of an oxidized species and (ii) rapid surface diffusion of undercoordinated atoms.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"40 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003283","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

Liquid Crystal Sensor Harnessing a Biomimetic Acetylcholinesterase Nanozyme for Detection of Trypsin in Human Serum. 利用仿生乙酰胆碱酯酶纳米酶的液晶传感器检测人血清胰蛋白酶。

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-09-06 DOI: 10.1021/acs.analchem.5c03968

Lili Wang,Wenli Wu,Binglu Zhao,Lijuan Zhu,Zhongxing Wang,Mei Zhao,Woo-Seok Choe,Qiongzheng Hu

{"title":"Liquid Crystal Sensor Harnessing a Biomimetic Acetylcholinesterase Nanozyme for Detection of Trypsin in Human Serum.","authors":"Lili Wang,Wenli Wu,Binglu Zhao,Lijuan Zhu,Zhongxing Wang,Mei Zhao,Woo-Seok Choe,Qiongzheng Hu","doi":"10.1021/acs.analchem.5c03968","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03968","url":null,"abstract":"Abnormal levels of trypsin in the human body can lead to various diseases, yet conventional detection methods often lack operational simplicity and real-time readout capabilities. This work presents a state-of-the-art metal organic framework (MOF) nanozyme-integrated liquid crystal (LC) sensor (MHN-LC sensor) and demonstrates the detection of trypsin as a proof of the concept. By rational engineering of the MOF-808 framework with Al3+ and l-histidine coordination, a novel MOF nanozyme (MHis-NE) exhibiting exceptional acetylcholinesterase (AChE)-mimetic activity is successfully prepared. In the presence of trypsin, the gelatin hydrogel-encapsulated MHis-NE immobilized on the centrifuge tube lid is released into the aqueous solution due to trypsin-triggered gelatin degradation. Subsequently, a surfactant myristoylcholine is catalytically hydrolyzed by released MHis-NE into choline and myristic acid. This enzymatic cascade induces a characteristic LC optical transition from a dark to bright appearance, corresponding to the interfacial LC molecular reorientation from homeotropic to planar alignment. This MHis-NE LC sensor achieves a detection limit of 1.09 × 10-5 mg/mL for trypsin with a broad detection range from 10-4 to 1 mg/mL. It also can be applied to trypsin quantification in human serum with superior selectivity against other enzymes as potential interferents. The developed strategy not only advances the nanozyme-mediated signal transduction principle but also significantly expands the potential of various LC sensors.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"33 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003213","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

化学最新文献