化学•材料最新文献

{"title":"Photoinduced Selective Cyclization Cascades of Unactivated N-alkene-Linked Indoles with the Insertion of Sulfur Dioxide and Its Preliminary Application Investigation","authors":"Jiaqi Huang,Jiwei Li,Yuwei Zeng,Qichen Li,Yueyue Jia,Feng Liang,Zhenzhen Hu,You Mao,Jiangwei Tian,Min Yang","doi":"10.1021/acs.joc.6c01943","DOIUrl":"https://doi.org/10.1021/acs.joc.6c01943","url":null,"abstract":"Photoinduced selective cyclization cascades of unactivated N-alkene-linked indoles with the insertion of sulfur dioxide were established, generating diverse exo- or endo-trig-cyclization products with a broad substrate scope in moderate to good yields. The mechanistic study revealed that selective radical addition, cyclization and radical-polar-crossover (RPC) process were involved in this transformation. We next deliverd a preliminary application investigation, and found that 3wj exhibited significant inhibitory effect on B16F10 cells, most showed a significant photophysical property, and some were applied as fluorescent dyes into live-cell imaging.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"2 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226582","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Spin-Phonon Relaxation and Decoherence in a Three-Dimensional Paired-Ion Framework Composed of Vanadyl Porphyrin Qubits","authors":"Christian A. Epure,Georgia C. Mantel,Casandra M. Moisanu,Jonathan R. Palmer,Madison I. Bardot,Michael R. Wasielewski,William R. Dichtel","doi":"10.1021/acs.jpclett.6c02513","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02513","url":null,"abstract":"Molecular electron spin qubits are an emerging platform for quantum technologies due to their atomic-scale synthetic tunability. Supramolecular structures can also place these qubits at precise positions within ordered arrays, allowing the scale-up of qubit architectures through a bottom-up approach. Here, we introduce the first three-dimensional paired-ion framework (PIF), VO-3D-PIF-1, which is composed of a concentrated array of S = 1/2 vanadyl porphyrin spin qubits arranged by ionic lattice interactions. The PIF was characterized using electron paramagnetic resonance spectroscopy to demonstrate the impact of framework structure and spin density on spin–lattice relaxation (T1) and spin decoherence (Tm). The high vanadyl porphyrin spin density within the framework (0.125 spins/nm3) promotes dipolar-driven decoherence, with Tm = 200–400 ns over a temperature range of 140–5 K. Spin–lattice relaxation mirrors that of vanadyl porphyrins in dilute solution, suggesting that the weak ionic interactions assembling the porphyrins within the secondary coordination sphere do not adversely affect phonon-induced T1 relaxation.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"11 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226506","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Sodium Benzoate Enabled Dual-Functional Defect Engineering for Stable and Broadband Tin-Based Perovskite Photodetectors","authors":"Penghui Shi,Yijia Ma,Wenhao Zheng,Tao Li,Yiran Ren,Luying Zhang,Lin Lin,Zhibo Yan,Junming Liu","doi":"10.1021/acs.jpcc.6c04959","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c04959","url":null,"abstract":"Lead-free tin-based perovskites have garnered significant research interest due to their low toxicity and remarkable optoelectronic properties. However, the oxidation of Sn2+ ions remains a critical challenge that hinders their further advancement. In this work, a Na+-containing additive, sodium benzoate (NaBz), is incorporated into PEA0.1FA0.9SnI3 perovskite thin films via a one-step solution spin-coating process to enhance their photoresponse. The optimized lateral photodetectors exhibit a peak responsivity (R) of 0.456 A·W-1, nearly five times higher than that of the unmodified control device (0.092 A·W-1). Comprehensive investigations reveal that NaBz significantly improves the oxidation resistance, moisture tolerance, and operational stability of the perovskite films. The carboxylate (−COO–) group in NaBz can act as a Lewis base to coordinate with undercoordinated Sn2+ ions, effectively passivating defect sites, while the presence of Na+ may influence the local chemical environment of halide species and defect-related sites, potentially contributing to the regulation of halide-ion migration and ionic redistribution. These complementary effects provide a simple and effective approach to improving the stability and photoresponse of lead-free tin-based perovskite photodetectors.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"1 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226641","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Structure-Dependent CO and NO Oxidation over Bimetallic PtPd/Al2O3 Catalysts: Impact of Pt–Pd Mixing and Alloying on Activity and Stability","authors":"Joachim Czechowsky,Paolo Dolcet,Carina B. Maliakkal,Radian Popescu,Christian Kübel,Silke Behrens,Michael Türk,Moritz Wolf,Silvia Gross,Jan-Dierk Grunwaldt,Maria Casapu","doi":"10.1021/acs.jpcc.6c04963","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c04963","url":null,"abstract":"The influence of the noble metal nanoparticle structure on the activity and stability of bimetallic PtPd/Al2O3 catalysts was systematically investigated. Various conventional and advanced synthesis methods were used to tune the initial Pt–Pd mixing/alloying extent. By using complementary characterization techniques, pronounced differences in the CO and NO oxidation activity could be correlated with variations in the noble metal oxidation state, particle size, and composition. The beneficial effect of Pt–Pd mixing/alloying in catalysts predominantly containing noble metal nanoparticles with a surface-averaged size smaller than ∼5 nm was revealed for the CO, NO, and combined CO/NO oxidation reactions. In this regard, colloidal methods enabled the formation of homogeneously alloyed PtPd particles with a narrow size distribution and superior catalytic activity at low temperatures. However, the presence of uniform PtPd bimetallic particles did not prevent catalyst deactivation, as pronounced noble metal sintering and segregation phenomena still occurred during hydrothermal aging. In contrast, for applications operating at temperatures exceeding 600 °C, catalysts with a less uniform initial structure exhibited improved stability.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"15 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226509","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Optimizing TFA Peptide Rink Amide Resin Acidolysis Using Hydrogen Chloride","authors":"Marc Gros,Eudald Asensio-Borràs,Yolanda Cajal,Francesc Rabanal","doi":"10.1021/acs.joc.6c01548","DOIUrl":"https://doi.org/10.1021/acs.joc.6c01548","url":null,"abstract":"We report an optimization of the standard acidolysis release of peptides from Rink Amide aminomethyl (RA-AM) resin using a combination of trifluoroacetic acid (TFA) and concentrated aqueous hydrogen chloride. The standard TFA-based protocol often leads to incomplete cleavage and reduced peptide yields. Addition of small percentages of HCl to TFA furnishes practically quantitative cleavage yields, improving overall efficiency and reproducibility. Yield improvements between 9 and 52% have been accomplished.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"12 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226645","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Single-Cell Insights into Size-Dependent Heterogeneous Bioconcentration and Distribution of Metal Species Ranging from Ions to Nanoclusters and Nanoparticles in Chlorella vulgaris","authors":"Gang Tang,Junjie Ma,Liu Zhang,Yun Ding,Xingchen Zhao,Qi Wu,Jie Gao,Runzeng Liu,Dou Wang,Guangbo Qu,Jianbo Shi,Guibin Jiang","doi":"10.1021/acs.est.5c16797","DOIUrl":"https://doi.org/10.1021/acs.est.5c16797","url":null,"abstract":"Particle size is a key factor influencing metal uptake by aquatic unicellular primary producers. To investigate size-dependent bioconcentration ranging from ions to nanoclusters (NCs) and nanoparticles (NPs), we used cytometry by time-of-flight (CyTOF) to quantitatively examine single-cell uptake, retention, and bioconcentration in Chlorella vulgaris exposed to Au3+ ions, three glutathione (GSH)-protected AuNC preparations (Au10–12SG10–12, Au15SG13, and Au25SG18), and four GSH-coated AuNPs (5, 15, 25, 50 nm). Au3+ and AuNCs showed rapid cell-associated accumulation but followed exponential-decay and two-phase clearance kinetics, indicating efficient cellular elimination and a tendency to be released back into the medium. In contrast, AuNPs followed saturation-type bioconcentration kinetics, with larger particles showing more persistent cell association. Single-cell analysis revealed strong size-dependent heterogeneity: under equal-mass exposure, the fraction of Au-positive cells decreased exponentially with increasing atom number, whereas the Au burden per Au-positive cell increased approximately linearly. Larger particles exhibited higher volume concentration factors (VCFs) with a small subset of “high-VCF” cells. These results highlight that both particle size and cellular heterogeneity jointly govern algal bioconcentration patterns and should be accounted for in environmental risk assessment of metal-based nanomaterials.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"2 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226074","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Bone-Targeting Antibodies for Skeletal Precision Therapy","authors":"Boyang Zhou,&nbsp;Han Xiao","doi":"10.1021/acs.bioconjchem.6c00415","DOIUrl":"https://doi.org/10.1021/acs.bioconjchem.6c00415","url":null,"abstract":"<p>Therapeutic antibodies have transformed the treatment of cancer, inflammation, infection, and disorders of bone biology by recognizing disease-associated molecular targets with high specificity. However, achieving therapeutically effective antibody concentrations at the site of disease remains a major challenge, as systemic administration does not inherently result in efficient tissue-specific delivery. Bone is a particularly demanding destination because mineralized matrix, limited vascular access, marrow complexity, and active remodeling can restrict local antibody exposure. Recent advances in bone-targeting antibody design point to a powerful reframing in which antibodies can be engineered not only for antigen specificity but also for tissue specificity. By attaching hydroxyapatite-binding motifs such as bisphosphonates or acidic peptides, antibodies can be endowed with bone-homing capabilities. The efficacy of this strategy has now been validated across multiple preclinical disease models, including breast cancer bone metastasis and osteoporosis-related bone loss. The next challenge is to define how affinity, valency, conjugation site, circulation time, and release should be tuned for each skeletal disease.</p>","PeriodicalId":29,"journal":{"name":"Bioconjugate Chemistry","volume":"37 10","pages":"1943–1948"},"PeriodicalIF":4.5,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149222050","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Negative-Gaussian-Curvature Carbon Monolayer NGC-C40 with Switchable Auxeticity and Ultra-High Potassium Storage","authors":"Jiaxin Jiang,Wenjie Wu,Chao Li,Zhiwen Zhuo,Ning Lu","doi":"10.1021/acs.jpclett.6c02482","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c02482","url":null,"abstract":"Beyond the geometric planarity of graphene and the outward bulging of fullerenes, a carbon sheet with negative Gaussian curvature (NGC), an “inside-out” saddle world, remains a tantalizing blind spot. A novel 2D carbon allotrope, NGC-C40, is developed through a topological engineering strategy via first-principles calculations. It displays pronounced intrinsic NGC features, lattice dynamical and thermal stability, and rare closed nodal-line semimetal characteristics. Mechanically, NGC-C40 exhibits pronounced anisotropy and a robust auxetic response, with a Poisson’s ratio ranging from −0.254 to +0.041. More importantly, it shows an unusual strain-polarity- and orientation-coupled Poisson’s ratio sign-switching behavior, arising from the cooperative response of the C8C5 skeleton and C4 region. For potassium-ion storage, NGC-C40 has a high theoretical capacity of 1116 mAh g–1, far exceeding the capacity of 223 mAh g–1 obtained for both Li and Na. It also exhibits a low K-ion migration barrier of 0.215 eV, operating voltages ranging from 1.124 to 0.031 V, and a maximum carbon-framework geometric volume expansion of 5.66%, enabled by its NGC architecture. Demonstrating multifunctional capability, NGC-C40 suggests a potential strategy for multifunctional 2D carbon design: negative Gaussian curvature may serve as an underexplored geometric factor.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"76 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226503","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Stereo- and Chemoselective Conversion of Alkynylphosphonates to Vinyl and Alkyl Phosphonates","authors":"Babak Kaboudin,Maryam Asvadi,Hesam Esfandiari,Tianjian Zhang,Yanlong Gu","doi":"10.1021/acs.joc.6c01343","DOIUrl":"https://doi.org/10.1021/acs.joc.6c01343","url":null,"abstract":"A novel strategy for the selective semi-reduction and exhaustive reduction of alkynyl phosphonates to (E)-vinyl phosphonates and alkyl phosphonates, respectively, has been developed using a Zn/NiCl2·6H2O system. The hydrogenation chemoselectivity is effectively tuned by simply switching the reaction solvent from acetonitrile to ethanol. Furthermore, the synthetic utility of this methodology is demonstrated through a late-stage tetradeuteration sequence employing readily available deuterium oxide as the isotope source. This protocol features simple operation and mild conditions, enabling the efficient conversion of readily available alkynyl phosphonates into alkyl and vinyl phosphonate products. Notably, by using D2O as the deuterium source, a range of deuterated alkyl phosphonates were obtained in excellent yields.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"5 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221764","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrochemical Trifluoromethylation of Alkenes Using the Unpurified CF3I Reagent from Fluoroform","authors":"Jiaming Cheng,Jinkun Fan,Chunhui Yang,Tengfei Pu,Qi Yang,Junyi Pan,Xu Cheng","doi":"10.1021/acs.joc.6c01627","DOIUrl":"https://doi.org/10.1021/acs.joc.6c01627","url":null,"abstract":"Fluoroform (HCF3) is an excess industrial gas with a significant greenhouse effect. The utilization of fluoroform as the trifluoromethyl precursor could turn the waste into a value-added product. In this work, we report a protocol for converting fluoroform to CF3I, which was used directly in the electrochemical trifluoromethylation of alkenes facilitated by the orthogonal reactivity in two steps. This protocol could give the trifluoromethylated products in comparable yield to those obtained with a commercial CF3I solution. In particular, the iodine residue in the prepared CF3I has a positive effect in some examples, with advantages over commercial CF3I reagents.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"37 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}