Journal of the American Chemical Society美国化学会志
Journal of the American Chemical Society(英文缩写 J AM CHEM SOC),ISSN 0002-7863,eISSN 1520-5126,中文译名:美国化学会志 是一本学术期刊。本页汇总该期刊的最新影响因子、分区信息以及最新收录于 PubMed 的文献,帮助您快速了解期刊全貌。
发文量统计区间：2025-10-01 至 2026-09-30，按本站收录文献的发表日期统计。
期刊介绍
历年影响因子趋势
| JCR 数据年份 | 影响因子 | JCR 分区 |
|---|---|---|
| 2021 | 16.383 | Q1 |
| 2022 | 15.000 | Q1 |
| 2023 | 14.400 | Q1 |
| 2024 | 15.600 | Q1 |
| 2025 | 16.600 | Q1 |
Journal of the American Chemical Society 最新收录文献
-
1. Structure-Dynamics-Property Relationship Reveals the Origin of Porous Integrity in Imine-Linked Covalent Organic Frameworks.
PMID:日期:2026-09-30Molecular flexibility encoded in low-frequency lattice dynamics is increasingly recognized as a key determinant of the properties of porous materials, particularly metal-organic frameworks, but remains largely unexplored in covalent organic frameworks (COFs). Here, we establish a structure-dynamics-property relationship for chemically related COFs by combining three-dimensional electron diffraction, low-frequency vibrational spectroscopy, and first-principles calculations. Using 3D electron diffraction, we determined the crystal structure of the collapsed reduced framework COF-300-AR, revealing a bent linker conformation. Terahertz and low-frequency Raman spectroscopy, together with solid-state density functional theory and local mode analysis, resolve the lattice dynamics of contracted COF-300-H2O, COF-320A, and collapsed COF-300-AR and quantify linker flexibility through imine/amine torsions. Normal-mode decomposition and torsional potential energy surfaces show that these coordinates are comparatively stiff in the imine-based frameworks, preserving near-planar linker conformations that support guest-responsive structures. In contrast, COF-300-AR exhibits a shallower, multiwell torsional potential that enables bent linker conformations, favoring collapsed packing. Gas-phase local-mode analysis reproduces this relative trend in torsional softness, suggesting that linker flexibility can be screened before a crystal structure is available. The negligible gas uptake of COF-300-AR is therefore linked to the coupling of local amine flexibility with packing constraints in the interpenetrated framework. More broadly, these results demonstrate how low-frequency dynamics can identify molecular coordinates governing the structural integrity and porosity in flexible COFs.
-
2. Selective C18-Methyl Oxidation of Sclareol via an Engineered P450 Enables the Synthesis of Spiromyrrhene B.
2. 通过工程化P450实现香紫苏醇的选择性C18-甲基氧化，从而能够合成螺环月桂烯BPMID:日期:2026-09-22While selective oxidation of unactivated C-H bonds has emerged as an effective tactic to reshape retrosynthetic strategies in the synthesis of natural products, the primary methyl C-H bonds remain inert and inaccessible to contemporary methods without preinstalled directing groups. Herein, we report a biocatalytic C-H oxidation strategy that leverages an engineered P450BM3 platform for the selective C18-methyl hydroxylation of sclareol. Through five rounds of directed evolution, variant Ox18M3-3 was developed, elevating the regioselectivity from 4% to >99% alongside a 2.2-fold increase in catalytic activity. The site-specific enzymatic hydroxylation facilitated the first synthesis of the complex heptacyclic tumor stemness inhibitor spiromyrrhene B in 10 steps (longest linear sequence) from sclareol, underscoring the benefits of merging precision biocatalysis with classical synthesis to streamline access to bioactive natural products.
-
3. Blue-Emitting Colloidal In1-xGaxP Quantum Dots Synthesized in Molten Salt: Toward Blue QLEDs with Improved Stability.
PMID:日期:2026-09-21Colloidal quantum dots (QDs) are being actively explored for QD light-emitting diode (QD-LED) displays with high color purity and wide color gamut, high brightness, and low-cost, solution-based manufacturing. Heavy metal-free InP QDs have enabled red- and green-emitting QD LEDs with excellent device characteristics. However, the performance of blue QD-LEDs, required for completing the red, green, and blue (RGB) full color gamut, is lagging behind, which prompts searches for novel blue-emitting QDs. Here, we report the synthesis, computational modeling, and structural and spectroscopic studies of heavy metal-free blue-emitting core-shell QDs featuring 2.1 nm In1-xGaxP cores, colloidally synthesized in a molten inorganic salt, epitaxially coated with ZnS shells, and optimized surface treatments. The computational study suggests that the introduction of a ZnS shell induces mixing between core and shell electronic states, enhancing the direct-gap character of In1-xGaxP/ZnS QDs. The resulting In1-xGaxP/ZnS QDs show blue band-edge photo- and electroluminescence that can be fine-tuned around the technologically important region of 470 nm. This material holds strong promise for filling the blue gap in full-gamut QD-LED displays.
-
4. Using Data Science Tools to Explore Rate Matching in a Nickel-Catalyzed Cross-Electrophile Coupling of Alkyl and Aryl Halides (Cl, Br) with a Tridentate Monoanionic Ligand.
4. 使用数据科学工具探索三齿单阴离子配体下镍催化烷基卤化物与芳基卤化物（Cl、Br）交叉亲电偶联中的速率匹配PMID:日期:2026-09-21Nickel-catalyzed cross-electrophile coupling (XEC) between aryl and alkyl electrophiles has emerged as an enabling synthetic method, yet predicting the outcomes of specific electrophile pairs is difficult due to the complexity of the mechanistic pathways. It has been proposed that "rate matching" between the oxidative addition of the aryl halide and the rate of formation of the alkyl radical, in addition to the stability of the Ni(II)-Ar complex, dictates the yield of the cross-coupling product. To probe this quantitatively, we developed a new tridentate monoanionic ligand that activatesalkyl and aryl chlorides and exhibits well-behaved electrochemistry, allowing the measurement of relative rate constants. This provides a framework to interrogate the rate-matching concept using both aryl and alkyl bromides and chlorides in cross-electrophile coupling. By combining an electroanalytical workflow with machine learning, the prediction of activation rate constants for all aryl/alkyl chlorides and bromides was achieved and correlated with reaction yields. We found that productive coupling occurs in a specific rate regime, and the synthetic performance could be predictably modulated by choosing the "matched" halide (either chloride or bromide) for each coupling partner.
-
5. Rate Coefficients by Integration of Total Reaction NMR Spectra.
PMID:日期:2026-09-18Reaction kinetics provide quantitative descriptions of phenomenological behavior that can be correlated with underlying chemical reaction mechanisms. Kinetic data is conventionally interrogated using one of three general methods: linear or nonlinear regression, numerical parameter estimation, and modern graphical analysis. Cumulative temporal concentrations (CTCs) derived from areas under temporal concentration curves are an alternative method to estimate kinetic parameters from reaction monitoring data. The requisite areas under temporal concentration curves are conveniently estimated from a total reaction NMR spectrum (TRS) generated using routine NMR spectroscopic acquisition and processing methods. Six case studies, involving intermediates, equilibria, catalysis, branching, and bimolecular processes, demonstrate how a combined TRS/CTC approach offers a straightforward method to estimate efflux rate coefficients for isolated chemical steps, without curve fitting.
-
6. Chiral Counteranion-Directed Asymmetric Intramolecular Rhodium-Catalyzed [(3+2+2)] Carbocyclization Reactions with Alkylidenecyclopropanes.
PMID:日期:2026-09-18Transition metal-catalyzed higher-order [m+n+o] carbocyclizations of alkylidenecyclopropanes (ACPs) provide atom-economical routes to complex polycyclic frameworks; however, achieving high enantioselectivity in these transformations remains extremely challenging. Herein, we report the first asymmetric intramolecular rhodium-catalyzed [(3+2+2)] carbocyclization of ACPs, enabled by asymmetric counteranion-directed catalysis (ACDC), to afford bridged tricyclic products with high diastereo- and enantioselectivity. Conventional ligand-controlled approaches failed to provide satisfactory reactivity or enantioinduction, whereas generating a chiral phosphate counteranion in situ from a silver phosphate (e.g., Ag-(S)-TRIP) via salt metathesis with a rhodium complex markedly enhanced enantioselectivity. Enantiomeric excesses of up to 93% were achieved using a matched combination of chiral phosphate and phosphoramidite ligands. The ACDC strategy also enables kinetic resolution of 1,5-diene-tethered ACPs in a new rhodium-catalyzed [(3+2+2)] carbocyclization, providing access to previously inaccessible tricyclic scaffolds with excellent stereocontrol. These results constitute rare examples of highly stereoselective rhodium-catalyzed higher-order carbocyclizations of ACPs and demonstrate that chiral counteranion-directed catalysis can enable asymmetric transition metal-catalyzed [m+n+o] cyclizations that remain inaccessible to conventional chiral-ligand control.
-
7. Cooperative Roles of Cu Ions and Brønsted Acid Sites in NOx Selective Catalytic Reduction by Cu-Chabazite Catalysts.
PMID:日期:2026-09-16The standard NH3 selective catalytic reduction (SCR) of NOx over Cu-exchanged chabazite (Cu-CHA) zeolites is widely deployed in heavy-duty diesel aftertreatment yet remains mechanistically unresolved, particularly regarding closure of the Cu redox cycle and the role of framework Brønsted acid sites. Here, we combine density functional theory, ab initio molecular dynamics, and metadynamics simulations to develop a molecularly detailed mechanism for the low-temperature (<523 K) standard SCR reaction. Cu2+-nitrite species, ZCu2+(NO2)-(NH3)3, formed via NO activation over O2-bridged binuclear Cu dimers, are proposed as key intermediates in the reduction half-cycle whose fate depends on the local framework Al environment: in the absence of proximal NH3-covered Brønsted acid sites, H2O promotes conversion to mononuclear ZCu2+OH(NH3)3 sites, while proximal NH3-covered Brønsted acid sites catalyze the transformation to Z2Cu2+(NH3)4. HONO is predicted to be a key intermediate in the reduction half-cycle whose decomposition to N2 and H2O is catalyzed by NH3-covered Brønsted acid sites via proton-shuttle mechanisms. Competing reduction pathways of mononuclear ZCu2+OH(NH3)3 sites, including direct NH3/NO coupling and HONO-mediated routes, have comparable apparent activation energies and are therefore kinetically complementary rather than mutually exclusive. The proposed catalytic cycle offers a resolution to the debate regarding single- versus dual-site Cu2+ reduction half-cycle mechanisms. The standard SCR redox cycle is predicted to be a cooperative, composition-dependent process governed by an interplay between Cu speciation and framework Brønsted acid sites. This composition-dependent nature calls for a new generation of kinetic models that explicitly account for the distribution of local cage environments across practical catalyst samples. Consequently, no single universal catalytic cycle applies across all catalyst compositions, implying control of the microscopic environment as a lever for optimization of Cu-CHA catalysts.
-
8. Tuning the Activation Barrier for Oxygen Exchange on Mixed Conducting Oxide with Fine Control of Transition Metal Impurities.
8. 通过精细调控过渡金属杂质来调节混合导电氧化物上氧交换的活化能垒PMID:日期:2026-09-16The energy barrier for oxygen exchange at the surface of mixed conducting oxides is a multifactor term that remains difficult to predict with existing models. Here, we describe an experimental approach to fine-tune this barrier on Pr0.1Ce0.9O2-δ used as a model mixed conducting oxide, by adding a minute amount of transition metal impurities to its surface. The variations of the activation barrier for oxygen exchange can be readily correlated with the redox properties of the transition metal oxide, and such a barrier can be decreased by as much as a factor of 2 with more reducible oxide impurities such as Co3O4. We demonstrate that this drop does not originate from the activity of the impurity oxide itself, but rather from the modified surface chemistry of Pr0.1Ce0.9O2-δ induced by the presence of the impurity through the formation of a heterojunction between Pr0.1Ce0.9O2-δ and the transition metals that modifies the energy barrier to oxygen exchange.
-
9. Synthesis of Siccanin by Computational Subtarget Selection.
PMID:日期:2026-09-12The species-selective SDH inhibitor siccanin presents unique opportunities for therapeutic development but suffers from poor physicochemical properties and challenging chemical problems. Here we report an approach to its synthesis that quickly intercepts its unusually hindered cis-syn-cis drimane core, i.e., its local chemical space. Computation helps rationalize and predict the reactivity, especially conformational preferences, configurational outcomes, and the reactivity of a key O-centered radical.
-
10. Thermochemical Polarization-Driven Heterolytic Hydrogenation in an Electrochemical Palladium-Membrane Reactor.
PMID:日期:2026-09-09Heterolytic hydrogenation via hydride species transfer represents a fundamental transformation in industry for chemical synthesis, but H2 or organic hydride donors are often utilized as the hydrogen source. An electrochemical palladium (Pd) membrane reactor shows the ability to catalyze heterolytic reactions by using water as the hydrogen source, but quantitative descriptions of this reactivity remain absent, and the reaction often relies on external polarization of the chemical compartment. Herein, we report thermochemical polarization-driven heterolytic hydrogenation in an electrochemical Pd-membrane reactor. By employing Hantzsch ester (HEH) regeneration as a model reaction, we first established a quantitative thermodynamic framework by showing basicity-dependent activity, and then provided experimental evidence supporting the kinetics by observing an interfacial charge transfer process, together demonstrating a heterolytic hydrogenation mechanism. Moreover, the origin of the electrons that generate hydride species was supported by experimental evidence using mixed potential theory (MPT)─a theory widely applied in metal corrosion and thermal catalysis but rarely applied to electrochemical systems. As a proof of concept, by employing the regenerated HEH as a mediator, we achieved asymmetric hydrogenation of imines with high yield (up to 99.1%) and enantioselectivity (up to 98.1% e.e.), thus demonstrating the integration of electrochemical hydrogen generation with homogeneous asymmetric catalysis. This work provides a mechanistic foundation for heterolytic hydrogenation in a Pd-membrane reactor and inspires the rational design of catalyst modifications.