{"title":"Tuning Interfacial Electron Transfer for Boosting Electrochemiluminescence: Methods, Mechanisms, and Bioanalytical Applications","authors":"Jingshuai Li, Haifei Wan, Wenling Gu, Liuyong Hu, Chengzhou Zhu","doi":"10.1021/acs.chemrev.6c00330","DOIUrl":"10.1021/acs.chemrev.6c00330","url":null,"abstract":"<p>Theinterfacial electron-transfer process acts as a pivotal kineticdeterminant of electrochemiluminescence (ECL) efficiency, governingthe generation of excited-state emitters and thus dictating the intensityand stability of ECL signals. Currently, harnessing diverse nanomaterialshas driven significant advances in the development of novel ECL luminophoresand the activation of coreactants. However, most of these luminophoresexhibit low ECL efficiency in aqueous media, and the intrinsic reactionand activation mechanisms remain ambiguous because of their complexstructures and compositions. Notably, tuning electron-transfer pathwaysat the molecular/atomic level can not only enable efficient signalamplification but also facilitate the tracking of reaction pathways,thereby providing deeper insights into the fundamental mechanismsunderlying ECL processes. This Review comprehensively summarizes advancesduring the past five years in tuning interfacial electron transferto enhance ECL. Furthermore, we highlight progress in electron-transfer-mediatedsignal amplification strategies for highly sensitive ECL biosensingand bioimaging applications. Finally, we propose and discuss the challengesand perspectives associated with improving the ECL efficiency throughthe modulation of electron transfer processes. Precise regulationof interfacial electron transfer holds substantial promise for advancingECL theories, clarifying reaction mechanisms, and expanding the scopeof ECL-based bioanalytical applications.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"126 21","pages":"11728–11767"},"PeriodicalIF":64.2,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221799","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}
Chemical ReviewsPub Date : 2026-11-11Epub Date: 2026-10-21DOI: 10.1021/acs.chemrev.6c00211
Peter Bellotti, Subhabrata Dutta, Fritz Paulus, Frank Glorius
{"title":"Strain-Release Cycloadditions: Bicyclobutanes and Beyond","authors":"Peter Bellotti, Subhabrata Dutta, Fritz Paulus, Frank Glorius","doi":"10.1021/acs.chemrev.6c00211","DOIUrl":"10.1021/acs.chemrev.6c00211","url":null,"abstract":"<p>Strain-release cycloadditions have emerged as powerfulreactionsfor converting distorted ring systems into complex and otherwise hardlyattainable organic molecular architectures. This Review encompassesthe fundamentals of strain, its role in governing cycloaddition pathways,and offers a systematic examination of strained carbocycles and heterocycles,from bicyclo[1.1.1]butanes and 1-azabicyclo[1.1.1]butanes, housanesand aza-housanes, 2<em>H</em>-azirines and aziridines, azetidines,cyclopropanes, cyclobutanes, oxiranes, oxetanes, and strained alkynesand alkenes. Across these motifs, the general principles that dictatereactivity, the breadth of known cycloadditions and activation strategies,from Brønsted and Lewis acid catalysis to transition-metal activation,photocatalysis, and double strain-release mechanisms, are highlighted.Key opportunities, current limitations, and future directions areoutlined.</p>","PeriodicalId":32,"journal":{"name":"Chemical Reviews","volume":"126 21","pages":"11627–11727"},"PeriodicalIF":64.2,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226111","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}
Le Chen, Yuxin Gui, Wang Zhan, Xianfeng Meng, Qinghong Kong, Lingling Tang, Qingwu Zhang, Juncheng Jiang
{"title":"Multifunctional Integration in Aerogels: Recent Progress and Prospects in Simultaneous Thermal Insulation and Microwave Absorption","authors":"Le Chen, Yuxin Gui, Wang Zhan, Xianfeng Meng, Qinghong Kong, Lingling Tang, Qingwu Zhang, Juncheng Jiang","doi":"10.1021/acsami.6c17847","DOIUrl":"10.1021/acsami.6c17847","url":null,"abstract":"<p>The rapid development of science has led to an increasing demand for lightweight and high-performance composite materials. Aiming at the dual requirements of thermal insulation and microwave absorption in the field of aerospace, this paper first clarifies the mechanism of heat insulation and microwave absorption. Secondly, five representative bifunctional aerogel systems are introduced. This paper mainly focuses on the recent research progress of the thermal insulation and microwave absorption bifunctional composite aerogels. Finally, challenges and future perspectives of the current thermal insulation and microwave absorption composite integrated aerogels are discussed.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 44","pages":"60376–60398"},"PeriodicalIF":7.8,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149248544","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}
Hongyu Chen, Jiao Feng, Yuan Ma, Zechao Zhu, Feifei An, Xinye Yuan, Jiexue Wang, Guowei Deng, Xufeng Nie, Jun Liu
{"title":"Aggregation-Induced Photodegradable and Hydrolyzable Photosensitizer for Cu64 Positron Emission Tomography/Photoacoustic Imaging-Guided Phototherapy Nanoplatforms with Controllable Performance","authors":"Hongyu Chen, Jiao Feng, Yuan Ma, Zechao Zhu, Feifei An, Xinye Yuan, Jiexue Wang, Guowei Deng, Xufeng Nie, Jun Liu","doi":"10.1021/acsami.6c12177","DOIUrl":"10.1021/acsami.6c12177","url":null,"abstract":"<p>Radio imaging and optical imaging offer complementary advantages for biomedical diagnosis. However, the photosensitizers used in imaging must be degraded to reduce phototoxicity during phototherapy. Herein, we report a novel dicyanomethylene-based near-infrared photosensitizer (PS) that self-degrades via multiple pathways, including hydrolysis, aggregation-induced photodegradation, and oxidation by hypochlorous acid. To meet diverse theranostic requirements, the degradation behavior and performance of the PS were systematically regulated through co-assembly with three carriers. First, co-assembly with DSPE-PEG2000 produced a nanosystem that is stable to laser irradiation and water during multimodal diagnosis, and labeling with <sup>64</sup>Cu enabled dual-mode photoacoustic and radio signal imaging. Second, co-assembly with PLGA-PEG5000 reduced the photodegradation rate by enabling complete degradation through hydrolysis, thereby facilitating deep-tumor phototherapy. Third, complexation with cucurbit[8]uril (CB[8]) selectively inhibited the hydrolytic properties of the photosensitizer, thereby reducing its phototoxicity through photodegradation and oxidative degradation pathways when superficial tumors are subjected to phototherapy. The phototherapeutic efficacy of the designed nanosystems was validated in a subcutaneous 4T1 tumor-bearing mouse model. The results demonstrated effective tumor inhibition with minimal phototoxicity, confirming the suitability of the developed system for safe phototherapy. Overall, this work presents a rational strategy for tuning photosensitizer degradation pathways to balance imaging performance, therapeutic efficacy, and biosafety, providing a versatile platform for multimodal theranostic applications.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 44","pages":"60418–60427"},"PeriodicalIF":7.8,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149250808","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}
{"title":"Dynamic Covalent Nanoparticle Network Enabling Shrinkage-Resistant and Closed-Loop Recyclable Microcellular Ethylene Copolymer Foams","authors":"Yuqi Ma, Haonan Yan, Jianbin Qin, Yongsheng Zhao, Guangcheng Zhang","doi":"10.1021/acsami.6c17964","DOIUrl":"10.1021/acsami.6c17964","url":null,"abstract":"<p>Thermoplastic elastomer foams have attracted considerable attention owing to their lightweight nature, flexibility, and processability. However, their widespread application is limited by unstable cellular structures, severe post-foaming shrinkage, and poor recyclability. In this work, epoxy-functionalized ethylene copolymer (EGMA) was employed as the matrix, and a dynamic covalent network containing B–O bonds was constructed through the ring-opening reaction between 3-aminophenylboronic acid (APBA) and epoxy groups. Hydroxyl-rich SiO<sub>2</sub> nanoparticles were further introduced to establish a dynamic nanoparticle network, yielding a thermoplastic elastomer foam with enhanced foamability, dimensional stability, and recyclability. The synergistic effect of the dynamic covalent network and SiO<sub>2</sub> nanoparticles significantly improved the modulus, creep resistance, and melt stability of the elastomer. Under the optimized foaming condition of 80 °C and 20 MPa, a microcellular foam with an average cell size of 8.94 μm and a cell density of 3.73 × 10<sup>10</sup> cell/cm<sup>3</sup> was obtained. Compared with E-A and E-Si foams, the E-A-Si foam exhibited outstanding dimensional stability, retaining 94.09% of its original volume after 24 h. The dynamic B–O bonds enabled moderate topological rearrangement during foaming, promoting uniform nucleation and suppressing cell rupture. After foaming, SiO<sub>2</sub> nanoparticles participated in a dynamic nanoparticle network through B–O–Si linkages, which effectively restricted stress relaxation and chain retraction, thereby stabilizing the cellular structure and reducing post-foaming shrinkage. Moreover, the E-A-Si foam maintained an intact cellular morphology and excellent elastic recovery after two closed-loop refoaming cycles. This work provides a new strategy for developing thermoplastic elastomer foams with high dimensional stability and closed-loop recyclability.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 44","pages":"61349–61362"},"PeriodicalIF":7.8,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149250918","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}
Chuanxin Liao, Jiaxu Bai, Bo Chen, Hongqiang Guo, Xianggao Li, Shirong Wang, Hongli Liu
{"title":"Realizing Molecular Excited-State Regulation through Donor Molecular Engineering: The Intrinsic Relationship between TADF and HLCT Mechanisms","authors":"Chuanxin Liao, Jiaxu Bai, Bo Chen, Hongqiang Guo, Xianggao Li, Shirong Wang, Hongli Liu","doi":"10.1021/acs.iecr.6c04193","DOIUrl":"10.1021/acs.iecr.6c04193","url":null,"abstract":"<p>Fordeveloping high-performance pure organic light-emitting diode(OLED) emitters, thermally activated delayed fluorescence (TADF) andhybrid local and charge-transfer (HLCT) mechanisms are two pivotalstrategies by harvesting triplet excitons via reverse intersystemcrossing. The intrinsic relationship between the two in moleculardesign is revealed in this study: the switching between TADF and HLCTmechanisms can be achieved by adjusting the strength of the donorgroups. In this work, five D-π-A-π-D type blue and greenOLED emitters with acridine/phenoxazine/phenothiazine groups as donorswere designed and synthesized. Compared to reported HLCT moleculesadopting carbazole/diphenylamine groups as donors, the excited statesof the molecules in this work were successfully regulated to TADF.The solution-processed blue/green OLED device based on <strong>FIP-DPAC</strong>/<strong>FIP-PXZ</strong> achieved the maximum external quantum efficiency(EQE<sub>max</sub>) of 10.01%/17.45%. A strategy for regulating HLCTand TADF mechanisms of OLED emitters through donor molecular engineeringwas elucidated in this study.</p>","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"65 44","pages":"23334–23344"},"PeriodicalIF":3.9,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149250951","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Li-Ting Zhao, Lin Zhang, Ke-Jie Xiang, Yu-Hui Luo, Dong-En Zhang
{"title":"Silver-Cluster and Polyoxometalate-Incorporated Metal-Organic Frameworks for Electrochemical Nitrite Sensing and Capacitive Energy Storage","authors":"Li-Ting Zhao, Lin Zhang, Ke-Jie Xiang, Yu-Hui Luo, Dong-En Zhang","doi":"10.1021/acsami.6c18102","DOIUrl":"10.1021/acsami.6c18102","url":null,"abstract":"<p>In this work, four new polyoxometalate-based metal-organic frameworks (POMOFs), namely [Ag<sub>10</sub>HCl<sub>2</sub>(dtb)<sub>8</sub>(PMo<sub>12</sub>O<sub>40</sub>)<sub>3</sub>]·2H<sub>2</sub>O (JOU-42-Mo), [Ag<sub>10</sub>HCl<sub>2</sub>(dtb)<sub>8</sub>(PW<sub>12</sub>O<sub>40</sub>)<sub>3</sub>]·2H<sub>2</sub>O (JOU-42-W), [Ag<sub>4</sub>Cl(dtb)<sub>2</sub>PMo<sub>12</sub>O<sub>40</sub>]·2H<sub>2</sub>O (JOU-43-Mo), and [Ag<sub>4</sub>(OH)(H<sub>2</sub>O)<sub>2</sub>(dtb)<sub>2</sub>PW<sub>12</sub>O<sub>40</sub>] (JOU-43-W) (dtb = 4,4′-(1,4-phenylene)bis(4<em>H</em>-1,2,4-triazole)), constructed from silver clusters and Keggin-type polyoxometalates (POMs), were synthesized via a solvothermal strategy. Single-crystal X-ray diffraction analyses reveal that these compounds consist of two structural families. The JOU-42 series features a three-dimensional (3D) <em>fcu</em>-type framework assembled from decanuclear Ag clusters, generating tetrahedral and octahedral cages for the confinement of POM guests, whereas the JOU-43 series adopts a 2D + 2D → 3D interpenetrated architecture containing one-dimensional channels for POM encapsulation. The combination of redox-active POM clusters and accessible Ag sites endows these POMOFs with enhanced electrochemical sensing performance toward nitrite (NO<sub>2</sub><sup>–</sup>). Among them, JOU-42-Mo exhibits the best NO<sub>2</sub><sup>–</sup> sensing performance, achieving a wide linear detection range of 20–30,000 μmol L<sup>–</sup><sup>1</sup> and a low detection limit of 3.88 μmol L<sup>–1</sup>, together with excellent selectivity, reproducibility, and stability. Furthermore, the POMOF electrodes display promising capacitive energy storage characteristics, demonstrating the multifunctional potential of Ag-cluster-based POMOFs.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 44","pages":"61011–61020"},"PeriodicalIF":7.8,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149269148","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}
Piaoping Yang, Alfred Worrad, Dionisios G. Vlachos
{"title":"Unraveling Structure and Spectroscopic Signatures of Pt/γ-Al2O3 via an Artificial Intelligence-Enabled Simulation Framework","authors":"Piaoping Yang, Alfred Worrad, Dionisios G. Vlachos","doi":"10.1021/acsami.6c14411","DOIUrl":"10.1021/acsami.6c14411","url":null,"abstract":"<p>Supported subnanometer clusters have attracted significant attention in catalysis. Yet, it is challenging to resolve their structural evolution, particularly in the presence of adsorbates. Here, we present an artificial intelligence (AI)-enabled simulation framework that integrates machine learning force field (MLFF) construction, molecular dynamics (MD) simulations, and ML-assisted infrared (IR) and X-ray absorption near-edge structure (XANES) spectra analysis to investigate the restructuring of supported subnanometer clusters. Using Pt<sub>10</sub>/γ-Al<sub>2</sub>O<sub>3</sub>(110) as a model system, we explored the CO-induced restructuring of the cluster under different conditions. The simultaneous machine learning (ML)-spectra elucidate a strong interplay among adsorbate coverage, cluster restructuring, and cluster-support interaction. This work sheds light on the complex dynamics of supported subnanometer clusters that is extendible to other systems.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 44","pages":"60694–60704"},"PeriodicalIF":7.8,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149269159","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}
Tingting Wu, Jiang Wang, Fengyu Zhang, Ruixuan Yang, Ye Tian, Ke Chu
{"title":"Efficient Hydroxymethanesulfonate Electrosynthesis from CO2 and Sulfite over CuPd1 Single-Atom Alloys","authors":"Tingting Wu, Jiang Wang, Fengyu Zhang, Ruixuan Yang, Ye Tian, Ke Chu","doi":"10.1021/acsami.6c19144","DOIUrl":"10.1021/acsami.6c19144","url":null,"abstract":"<p>Electrochemical C–S coupling of CO<sub>2</sub> and sulfite (SO<sub>3</sub><sup>2–</sup>) offers a sustainable alternative for hydroxymethanesulfonate (HMS) synthesis, yet its electrocatalytic selectivity remains far from satisfactory. Here, CuPd<sub>1</sub> single-atom alloys (CuPd<sub>1</sub>-SAA) are developed as a highly efficient catalyst for HMS electrosynthesis, delivering an exceptional Faradaic efficiency of 56.8% and an HMS yield rate of 301.5 mmol h<sup>–1</sup> g<sup>–1</sup> in an MEA electrolyzer, together with outstanding electrolysis stability for over 200 h of electrolysis. Mechanistic investigations reveal the critical Cu-Pd<sub>1</sub> synergy in driving CO<sub>2</sub> reduction to *CHOH and C–S coupling of *CHOH with *SO<sub>3</sub> for selective HMS generation.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 44","pages":"60885–60891"},"PeriodicalIF":7.8,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149281754","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}
{"title":"Modeling Plastic Circularity under Material Degradation Constraints: An Agent-Based Study of Delaware’s Recycling Supply Chain","authors":"Oluwadare Badejo, Idowu Kunlere, Borja Hernández, Kalim Shah, Marianthi Ierapetritou","doi":"10.1021/acs.iecr.6c03562","DOIUrl":"10.1021/acs.iecr.6c03562","url":null,"abstract":"<p>Efforts to advance circular plastic economies often prioritizetechnological solutions while underestimating material degradationand actors’ behavioral complexity. Yet such simplificationsrisk overstating long-term gains in recycled material uptake and emissionsreduction. This study addresses that gap by employing an agent-basedmodel to simulate the recycled plastic supply chain in the US Stateof Delaware, incorporating behavioral decision rules, policy influence,and a cap on mechanical recycling cycles. The model analyzes threescenarios: deterministic, yield-stochastic, and yield-and-demand-stochastic,each tested with and without degradation of plastic waste in recycling.Results show that while degradation constraints limit ultimate systemperformance, they also stabilize emissions and uptake, reducing thevolatility of economic and emission metrics by around 10%. These findingsunderscore the importance of embedding material feedback and behavioraladaptation into circular economy models. The evaluation under differentlevels of uncertainty highlights that disruptions that affect theyields of the recycling plants can be absorbed by the consumers, whichadapt their interactions. Such uncertainty in the yield even reducesthe uncertainty of the economic and environmental indicators by nearly80%. However, the uncertainty related to the consumers slightly increasesthe uncertainty over the deterministic case, remarking its criticalinfluence on the overall supply chain performance.</p>","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"65 44","pages":"23421–23443"},"PeriodicalIF":3.9,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149281855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}