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Quantum error correction (QEC) aims to protect logical qubits from noises by using the redundancy of a large Hilbert space, which allows errors to be detected and corrected in real time1. In most QEC codes2-8, a logical qubit is encoded in some discrete variables, for example photon numbers, so that the encoded quantum information can be unambiguously extracted after processing. Over the past decade, repetitive QEC has been demonstrated with various discrete-variable-encoded scenarios9-17. However, extending the lifetimes of thus-encoded logical qubits beyond the best available physical qubit still remains elusive, which represents a break-even point for judging the practical usefulness of QEC. Here we demonstrate a QEC procedure in a circuit quantum electrodynamics architecture18, where the logical qubit is binomially encoded in photon-number states of a microwave cavity8, dispersively coupled to an auxiliary superconducting qubit. By applying a pulse featuring a tailored frequency comb to the auxiliary qubit, we can repetitively extract the error syndrome with high fidelity and perform error correction with feedback control accordingly, thereby exceeding the break-even point by about 16% lifetime enhancement. Our work illustrates the potential of hardware-efficient discrete-variable encodings for fault-tolerant quantum computation19.
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Micro-sized single-crystalline Ni-rich cathodes are emerging as prominent candidates owing to their larger compact density and higher safety compared with poly-crystalline counterparts, yet the uneven stress distribution and lattice oxygen loss result in the intragranular crack generation and planar gliding. Herein, taking LiNi0.83Co0.12Mn0.05O2 as an example, an optimal particle size of 3.7 µm is predicted by simulating the stress distributions at various states of charge and their relationship with fracture free-energy, and then, the fitted curves of particle size with calcination temperature and time are further built, which guides the successful synthesis of target-sized particles (m-NCM83) with highly ordered layered structure by a unique high-temperature short-duration pulse lithiation strategy. The m-NCM83 significantly reduces strain energy, Li/O loss, and cationic mixing, thereby inhibiting crack formation, planar gliding, and surface degradation. Accordingly, the m-NCM83 exhibits superior cycling stability with highly structural integrity and dual-doped m-NCM83 further shows excellent 88.1% capacity retention.
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The energy density of Ni-rich cathodes is expected to be further unlocked by increasing the cut-off voltage to above 4.3 V, which nevertheless come with significantly increased irreversible phase transition and abundant side reactions. In this study, the perovskite oxides enhanced radial-aligned LiNi0.8 Co0.1 Mn0.1 O2 (NCM811) cathodes are reported, in which the coherent-growth La2 [LiTM]O4 clusters are evenly riveted into the crystals and the stable Lax Ca1- x [TM]O3- x protective layer is concurrently formed on the surface. The reciprocal interactions greatly reduce the lattice strain during de-/lithiation. Meantime, the abundant oxygen vacancies of the coating layer are proved to reversibly capture (state of charge) and re-release (state of discharge) the oxygen radicals, fully avoiding their correlative side reactions. The resultant NCM811 displays negligible O2 and CO2 emissions when charging to 4.5 V as well as a thinner CEI film, therefore delivering a large capacity of 225 mAh g-1 at 0.1C in coin-type half-cells and a high retention of 88.3% after 1000 cycles at 1C in pouch-type full-cells within 2.7-4.5 V. The development of high-voltage Ni-rich cathodes exhibits a highly effective pathway to further increase their energy density.
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Particulate matter 2.5 (PM2.5) has been implicated in lung injury and various cancers, yet its precise mechanistic role remains elusive. To elucidate the key signaling pathways underpinning PM2.5-induced lung cancer progression, we embarked on a study examining the impact of PM2.5 both in vitro and in vivo. Lung cancer cell lines, A549 and H157, were employed for the in vitro investigations. Overexpression or knockdown techniques targeting the hnRNPA2B1 protein were implemented. Lung cancer cells were treated with a medium containing PM2.5 and subsequently prepared for in vitro evaluations. Cell growth, invasion, and migration were gauged using transwell and CCK-8 assays. Apoptosis was ascertained through flow cytometry and western blotting of pertinent proteins. Seahorse analyses probed the influence of PM2.5 on lung cancer energy metabolism. The RNA stability assay was employed to discern the impact of PM2.5 on the stability of oxidative phosphorylation-related genes in lung cancer. Our findings revealed that PM2.5 augmented cell proliferation, migration, and invasion rates. Similarly, a diminished apoptosis rate was observed in PM2.5-treated cells. Elevated expression of hnRNPA2B1 was detected in lung cancer cells exposed to PM2.5. Moreover, in cells treated with PM2.5, hnRNPA2B1 knockdown markedly curtailed cell proliferation by inducing G1-S cell cycle arrest and bolstered lung cancer cell apoptosis in vitro; it also curbed xenograft tumor growth. Mechanistically, our data suggest that PM2.5 undermines the stability of mRNA transcripts associated with oxidative phosphorylation (OXPHOS) and augments the formation of processing bodies (P-bodies), leading to an upsurge in OXPHOS levels. In conclusion, PM2.5 appears to drive lung cancer progression and migration by modulating the energy metabolism of lung cancer in a hnRNPA2B1-dependent manner.
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Apoptosis , Ribonucleoproteína Heterogénea-Nuclear Grupo A-B , Neoplasias Pulmonares , Fosforilación Oxidativa , Material Particulado , Estabilidad del ARN , Animales , Humanos , Ratones , Células A549 , Línea Celular Tumoral , Movimiento Celular , Proliferación Celular , Progresión de la Enfermedad , Regulación Neoplásica de la Expresión Génica , Ribonucleoproteína Heterogénea-Nuclear Grupo A-B/metabolismo , Ribonucleoproteína Heterogénea-Nuclear Grupo A-B/genética , Neoplasias Pulmonares/patología , Neoplasias Pulmonares/genética , Neoplasias Pulmonares/metabolismo , Ratones Endogámicos BALB C , Ratones Desnudos , Material Particulado/efectos adversos , ARN Mensajero/genética , ARN Mensajero/metabolismo , Ensayos Antitumor por Modelo de XenoinjertoRESUMEN
The Hamiltonian, which determines the evolution of a quantum system, is fundamental in quantum physics. Therefore, it is crucial to implement high-precision generation and measurement of the Hamiltonian in a practical quantum system. Here, we experimentally demonstrate ultrahigh-precision Hamiltonian parameter estimation with a significant quantum advantage in a superconducting circuit via sequential control. We first observe the commutation relation for noncommuting operations determined by the system Hamiltonian, both with and without adding quantum control, verifying the commuting property of controlled noncommuting operations. Based on this control-induced commuting property, we further demonstrate Hamiltonian parameter estimation for polar and azimuth angles in superconducting circuits, achieving ultrahigh metrological gains in measurement precision exceeding the standard quantum limit by up to 16.0 and 16.1 dB at N=100, respectively.
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Liquid crystals (LCs) are well known for inherent responsiveness to external stimuli, such as light, thermal, magnetic, and electric fields. Cholesteric LCs are among the most fascinating, since they possess distinctive optical properties due to the helical molecular orientation. However, the good flow, easy contamination, and poor stability of small-molecule LCs limit their further applications, and microencapsulation as one of the most effective tools can evade these disadvantages. Microencapsulation can offer shell-core structure with LCs in the core can strengthen their stability, avoiding interference with the environment while maintaining the stimuli-responsiveness and optical properties. Here, we report recent progress in the fabrication and applications of cholesteric LC microcapsules (CLCMCs). We summarize general properties and basic principles, fabrication methods including interfacial polymerization, in-situ polymerization, complex coacervation, solvent evaporation, microfluidic and polymerization of reactive mesogens, and then give a comprehensive overview of their applications in various popular domains, including smart fabrics, smart sensor, smart displays, anti-counterfeiting, information encryption, biomedicine and actuators. Finally, we discuss the currently facing challenges and the potential development directions in this field.
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BACKGROUND: Diffuse large B-cell lymphomas (DLBCLs) display high molecular heterogeneity, but the International Prognostic Index (IPI) considers only clinical indicators and has not been updated to include molecular data. Therefore, we developed a widely applicable novel scoring system with molecular indicators screened by artificial intelligence (AI) that achieves accurate prognostic stratification and promotes individualized treatments. METHODS: We retrospectively enrolled a cohort of 401 patients with DLBCL from our hospital, covering the period from January 2015 to January 2019. We included 22 variables in our analysis and assigned them weights using the random survival forest method to establish a new predictive model combining bidirectional long-short term memory (Bi-LSTM) and logistic hazard techniques. We compared the predictive performance of our "molecular-contained prognostic model" (McPM) and the IPI. In addition, we developed a simplified version of the McPM (sMcPM) to enhance its practical applicability in clinical settings. We also demonstrated the improved risk stratification capabilities of the sMcPM. RESULTS: Our McPM showed superior predictive accuracy, as indicated by its high C-index and low integrated Brier score (IBS), for both overall survival (OS) and progression-free survival (PFS). The overall performance of the McPM was also better than that of the IPI based on receiver operating characteristic (ROC) curve fitting. We selected five key indicators, including extranodal involvement sites, lactate dehydrogenase (LDH), MYC gene status, absolute monocyte count (AMC), and platelet count (PLT) to establish the sMcPM, which is more suitable for clinical applications. The sMcPM showed similar OS results (P < 0.0001 for both) to the IPI and significantly better PFS stratification results (P < 0.0001 for sMcPM vs. P = 0.44 for IPI). CONCLUSIONS: Our new McPM, including both clinical and molecular variables, showed superior overall stratification performance to the IPI, rendering it more suitable for the molecular era. Moreover, our sMcPM may become a widely used and effective stratification tool to guide individual precision treatments and drive new drug development.
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Inteligencia Artificial , Linfoma de Células B Grandes Difuso , Humanos , Linfoma de Células B Grandes Difuso/mortalidad , Femenino , Masculino , Persona de Mediana Edad , Pronóstico , Estudios Retrospectivos , China/epidemiología , Anciano , Adulto , Anciano de 80 o más Años , Adulto Joven , AdolescenteRESUMEN
Understanding how particles pack in space and the mechanisms underlying symmetry selection across soft matter is challenging. The Frank-Kasper (F-K) phase of complex spherical packing is amongst the most fascinating phases; however, it has not been observed in discotic liquid crystals until now. Herein, we report the first observation of F-K phases of charge transfer complexes (CTCs) obtained from triphenylene derivatives as donors and 2,4,7-trinitro-9-fluorenone as the acceptor. The CTCs were characterized using experimental and theoretical calculations, indicating that the F-K A15 cubic lattice possesses a unit cell containing 8 sphere-like supramolecules, each of which was self-assembled from 3 CTC complexes. The lattice constant was only 3.2 nm, which is by far the smallest for the A15 phase. Interestingly, the supramolecular assembly can be regarded as the molecular column splitting into isolated spherical fragments, impeding charge transfer and turning it into one insulator. This provides a simple and effective method for preparing asymmetric complex compounds for the design of unconventional self-assembled nanostructures.
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Water replenishment is an important measure for maintaining and improving the aquatic environmental quality of lakes. The problems of water quality deterioration and water shortage can be alleviated by introducing water of higher quality. However, the mechanism of water replenishment in the improvement of the water quality and trophic status of lakes remains unclear. This study investigated water replenishment in Wuliangsuhai Lake (WLSHL) from 2011 to 2021 by collecting seasonal water samples and conducting laboratory analyses. Water replenishment was found to be capable of significantly improving lake water quality and alleviating eutrophication. It is worth noting that single long-term water replenishment measures have limitations in improving the water quality and trophic status. The whole process was divided into three stages according to the water quality and trophic status, namely the buffer period, decline period, and stable period. During the buffer period, the water quality and trophic status showed only slight improvement because of the small amount of water replenishment and the low proportion of higher-quality water from the Yellow River. In the decline period, with increasing water replenishment, the proportion of higher-quality water from the Yellow River gradually increased, leading to the most significant and stable degree of improvement. In the stable period, increases in the amount of water replenishment had little effect on improving the water quality and trophic status, which is attributable to the balance between internal pollutants (lake water-sediment), and the balance between internal-external pollutants (lake water-irrigation return flow + Yellow River water). On the premise of stable water quality, with eutrophication control as the management goal, the optimal water replenishment would be approximately 10.58 ×108 m3. Further necessary measures for solving aquatic environmental problems include the combination of sediment dredging, optimization of the water replenishment route, and implementation of quality management in water replenishment.
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Monitoreo del Ambiente , Eutrofización , Lagos , Calidad del Agua , Lagos/química , China , Estaciones del Año , Animales , Contaminantes Químicos del Agua/análisis , Abastecimiento de Agua/estadística & datos numéricos , Ríos/químicaRESUMEN
Weather radar is an active remote sensing device used to monitor the full lifecycle changes in severe convective weather with high spatial and temporal resolution. Effective radar calibration is a crucial foundation for ensuring the high-quality application of observational data. This paper utilizes a UAV platform equipped with a high-precision RTK system and standard metal spheres to study the principles and methods of metal sphere calibration, constructing a complete calibration process and calibration accuracy evaluation metrics. Additionally, a collocated radar comparison observation experiment was conducted for cross-validation, and metal sphere calibration tests were performed on problematic radars. The experimental results indicate the following: (1) The combined application of a high-precision RTK system and a laser range camera can provide real-time position information on the metal sphere, improving the efficiency of radar target acquisition. (2) The calibration method based on UAV-suspended metal spheres can periodically conduct the quantitative calibration of Z and ZDR, achieving calibration accuracies within 0.5 dB and 0.2 dB, respectively, and supports the qualitative inspection of key parameters such as beamwidth and pulse width. (3) During field tests, a high success rate "coarse adjustment + fine adjustment + staring" sphere-finding technique was established, based on automatic switching between RHI, PPI, and FIX scanning modes. This method directs the UAV to adjust the metal sphere to the center of the radar distance bin, reducing the impact of uneven beam filling and bin crossing, ensuring the accuracy of scattering characteristic measurements.
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Ecological pollution caused by heavy metals released from sediments is a worldwide concern. However, the effect of changes in sediment speciation on their release of heavy metals has not been adequately reported. In this study, the research focused on Pb and Cr in the ice period of Wuliangsuhai. This study analyzed changes in the sediment speciation of Pb and Cr before and after a release experiment using four risk assessment methods while varying the temperature, pH, and salinity of the water column. The results indicated that the total concentration of Pb ranged from 11.17 to 24.25 mg/kg, while for Cr it ranged from 42.26 to 69.68 mg/kg. Both elements exhibited mild contamination. The release of Pb and Cr from sediments increases with increasing water temperature, mainly due to the conversion of the residual fraction of Pb to the Fe-Mn oxide fraction and Cr converting more residual fraction to the organic matter and sulfide fraction. The release of sediment Pb and Cr decreased with increasing pH, with Pb converting more acid extractable fraction to the residual fraction and Cr converting more organic matter and sulfide fraction to the residual fraction. In contrast, the release of Pb and Cr increased and then decreased with increasing salinity. For Pb, the acid extractable fraction was more susceptible to conversion to the residual fraction by environmental influences, whereas for Cr, the organic matter and sulfide fraction were susceptible to conversion to the residual fraction.
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Metales Pesados , Contaminantes Químicos del Agua , Lagos , Hielo , Plomo , Sedimentos Geológicos , Contaminantes Químicos del Agua/análisis , Monitoreo del Ambiente/métodos , Metales Pesados/análisis , Agua , Medición de Riesgo , Sulfuros , ChinaRESUMEN
Manipulation of periodic micro/nanostructures in polymer film is of great importance for academics and industrial applications in anticounterfeiting. However, with the increasing demand on information security, materials with time-dependent features are urgently required, especially the material where the same information can appear more than once on the time scale. Here, one concise strategy to realize time-dependent anticounterfeiting and "double-lock" information encryption based on a host-guest system is proposed, with one photoresponsive azopolymer as the host and one liquid-crystalline molecule as the guest. The system exhibits a tunable mass transport in pre-designed periodic micro/nanostructures by tailoring the process of cis-to-trans recovery of azo groups and assembly of mesogenic trans-isomers, resulting in a dynamic structural color in film. Taking advantage of this extraordinary feature, time-dependent dynamic anticounterfeiting has been achieved. More importantly, the time of each state's appearance in the whole process can be modulated by changing the host-guest ratio. Combining the manipulatable process of mass transport with the unique decoding method, the stored information in film can be decrypted correctly. This work provides an unprecedented dynamic approach for advanced anticounterfeiting technology with a higher level of security and high-end applications in information encryption.
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Photoluminescence is one of the most meticulous ways to manipulate light energy. Typical photoluminescent emitters are mostly stable substances with a pure photophysical process of spontaneous photon-emission from their excited states. Intermediate emitters are elusive attributing to their synchronous energy transfer process including photophysical and incomplete photochemical pathways. An intermediate emitter containing radicals is more difficult to be observed due to its inherent chemical reactivity. Here, these challenges are overcome by spontaneously formed space limitations in polymer crosslinking networks meanwhile chemically active intermediates are captured. These doublet intermediates exhibit unique long-wavelength emissions under chemically crosslinking confinement conditions, and their luminous mechanism provides a novel perspective for designing intermediate emitters with liquid-crystal character and photoresponsive features towards spatiotemporal encryption, promising for the detection of photochemical reactions and the development of fascinating luminescent systems.
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An eco-friendly selective hydrolysis of chain α-oxo ketene N,S-acetals in water for the switchable synthesis of ß-keto thioesters and ß-keto amides is reported. In refluxing water, the hydrolysis reactions of α-oxo ketene N,S-acetals in the presence of 1.0 equiv of dodecylbenzenesulfonic acid effectively afforded ß-keto thioesters in excellent yield, while ß-keto amides were successfully obtained in excellent yield when the hydrolysis reactions were carried out in the presence of 3.0 equiv of NaOH. The green approach to ß-keto thioesters and ß-keto amides avoids the use of harmful organic solvents, thiols and thiolacetates as well as amines, which could result in serious environmental and safety issues.
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Transition metal-nitrogen-carbon materials with atomically dispersed active sites are promising catalysts for oxygen evolution reaction (OER) since they combine the strengths of both homogeneous and heterogeneous catalysts. However, the canonically symmetric active site usually exhibits poor OER intrinsic activity due to its excessively strong or weak oxygen species adsorption. Here, a catalyst with asymmetric MN4 sites based on the 3-s-triazine of g-C3 N4 (termed as a-MN4 @NC) is proposed. Compared to symmetric, the asymmetric active sites directly modulate the oxygen species adsorption via unifying planar and axial orbitals (dx2 -y2 , dz2 ), thus enabling higher OER intrinsic activity. In Silico screening suggested that cobalt has the best OER activity among familiar nonprecious transition metal. These experimental results suggest that the intrinsic activity of asymmetric active sites (179 mV overpotential at onset potential) is enhanced by 48.4% compared to symmetric under similar conditions. Remarkably, a-CoN4 @NC showed excellent activity in alkaline water electrolyzer (AWE) device as OER catalyst, the electrolyzer only required 1.7 V and 2.1 V respectively to reach the current density of 150 mA cm-2 and 500 mA cm-2 . This work opens an avenue for modulating the active sites to obtain high intrinsic electrocatalytic performance including, but not limited to, OER.
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Elastomers generally possess low Young's modulus and high failure strain, which are widely used in soft robots and intelligent actuators. However, elastomers generally lack diverse functionalities, such as stimulated shape morphing, and a general strategy to implement these functionalities into elastomers is still challenging. Here, a microfluidic 3D droplet printing platform is developed to design composite elastomers architected with arrays of functional droplets. Functional droplets with controlled size, composition, position, and pattern are designed and implemented in the composite elastomers, imparting functional performances to the systems. The composited elastomers are sensitive to stimuli, such as solvent, temperature, and light, and are able to demonstrate multishape (bow- and S-shaped), multimode (gradual and sudden), and multistep (one- and two-step) deformations. Based on the unique properties of droplet-embedded composite elastomers, a variety of stimuli-responsive systems are developed, including designable numbers, biomimetic flowers, and soft robots, and a series of functional performances are achieved, presenting a facile platform to impart diverse functionalities into composite elastomers by microfluidic 3D droplet printing.
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The aim of this study is to evaluate the survival benefit of consolidative autologous hematopoietic stem cell transplantation (ASCT) in patients with peripheral T-cell lymphomas (PTCL). In this retrospective study, the ASCT group underwent consolidative ASCT after first-line therapy at 14 transplantation centers in China between January 2001 and December 2019. Data were collected over the same time frame for the non-ASCT group from the database of lymphoma patient records at Peking University Cancer Hospital & Institute. A total of 120 and 317 patients were enrolled in the ASCT and non-ASCT groups, respectively, and their median ages were 43 years and 51 years, respectively. In the ASCT group, 101 patients had achieved complete remission (CR) and 19 patients had achieved partial remission at the time of ASCT. The median follow-up time was 40.2 months and 68 months, and the 3-year overall survival (OS) rate was 80.6% and 48.9% (p < 0.001) for the ASCT and non-ASCT groups, respectively. The beneficial effect of ASCT for OS remained even after propensity score-matched (PSM) analysis (81.6% vs 68.3%, p = 0.001). Among the 203 patients who were aged ≤ 65 years and achieved CR, ASCT conferred a significant survival benefit (3-year progression-free survival [PFS]: 67.4% vs 47.0%, p = 0.004; 3-year OS: 84.0% vs 74.1%, p = 0.010), and this was also maintained after PSM analysis (3-year PFS: 66.6% vs 48.4%, p = 0.042; 3-year OS: 84.8% vs 70.5%, p = 0.011). Consolidative ASCT improved the survival outcome of PTCL patients, even those who achieved CR after first-line therapy.
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Regio- and stereoselective switchable synthesis of (E)- and (Z)-N-carbonylvinylated pyrazoles is first developed by using the Michael addition reaction of pyrazoles and conjugated carbonyl alkynes. Ag2CO3 plays a key role in the switchable synthesis of (E)- and (Z)-N-carbonylvinylated pyrazoles. Ag2CO3-free reactions lead to thermodynamically stable (E)-N-carbonylvinylated pyrazoles in excellent yields whereas reactions with Ag2CO3 give (Z)-N-carbonylvinylated pyrazoles in good yields. It is noteworthy that (E)- or (Z)-N1-carbonylvinylated pyrazoles are obtained with high regioselectivity when asymmetrically substituted pyrazoles react with conjugated carbonyl alkynes. The method can also extend to the gram scale. A plausible mechanism is proposed on the basis of the detailed studies, wherein Ag+ acts as coordination guidance.
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Alquinos , Pirazoles , Estereoisomerismo , CatálisisRESUMEN
PURPOSE: We sought to understand the clinical course and molecular phenotype of patients who showed disease progression after programmed cell death ligand 1 (PD-L1) inhibitor treatment but subsequently responded to PD-1 inhibitor treatment. We also explored the response to PD-1-axis targeted therapy of classical Hodgkin lymphoma (cHL) according to genetically driven PD-L1 and programmed cell death ligand 2 (PD-L2) expression. METHODS: Five patients in a phase II clinical trial of CS1001 (PD-L1 inhibitor) for relapsed or refractory (R/R) cHL were retrospectively reviewed. Formalin-fixed, paraffin-embedded whole tissues from the five patients were evaluated for 9p24.1 genetic alterations based on FISH and the expression of PD-L1, PD-L2, PD-1, major histocompatibility complex (MHC) class I-II, and the tumor microenvironment factorsCD163 and FOXP3 in the microenvironmental niche, as revealed by multiplex immunofluorescence. RESULTS: All five patients showed primary refractory disease during first-line treatment. Four patients received PD-1 inhibitor after dropping out of the clinical trial, and all demonstrated at least a partial response. The progression-free survival ranged from 7 to 28 months (median = 18 months), and 9p24.1 amplification was observed in all five patients at the PD-L1/PD-L2 locus. PD-L1 and PD-L2 were colocalized on Hodgkin Reed-Sternberg (HRS) cells in four of the five (80%) patients. There was differential expression of PD-L1 and PD-L2 in cells in the tumor microenvironment in cHL, especially in HRS cells, background cells and tumor-associated macrophages. CONCLUSIONS: PD-L1 monotherapy may not be sufficient to block the PD-1 pathway; PD-L2 was expressed in HRS and background cells in cHL. The immunologic function of the PD-L2 pathway in anti-tumor activity may be underestimated in R/R cHL. Further study is needed to elucidate the anti-tumor mechanism of PD-1 inhibitor and PD-L1 inhibitor treatment.
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Antígeno B7-H1/antagonistas & inhibidores , Enfermedad de Hodgkin/tratamiento farmacológico , Inhibidores de Puntos de Control Inmunológico/uso terapéutico , Proteína 2 Ligando de Muerte Celular Programada 1/antagonistas & inhibidores , Adulto , Antígenos CD/inmunología , Antígenos de Diferenciación Mielomonocítica/inmunología , Ensayos Clínicos Fase II como Asunto , Femenino , Factores de Transcripción Forkhead/inmunología , Antígenos de Histocompatibilidad/inmunología , Enfermedad de Hodgkin/inmunología , Humanos , Masculino , Persona de Mediana Edad , Receptor de Muerte Celular Programada 1/inmunología , Supervivencia sin Progresión , Receptores de Superficie Celular/inmunología , Recurrencia , Estudios Retrospectivos , Resultado del Tratamiento , Microambiente Tumoral/inmunologíaRESUMEN
For the first time, an eco-friendly and sustainable tandem [5C + 1C] cycloaromatization of α-alkenoyl ketene dithioacetals and nitroethane in water for the efficient synthesis of ortho-acylphenols was reported. In refluxing water, a range of α-alkenoyl ketene dithioacetals and nitroethane smoothly underwent tandem Michael addition/cyclization/aromatization reactions in the presence of 2.0 equivalents of DBU to provide various ortho-acylphenols in excellent yields. The green approach to ortho-acylphenols not only avoided the use of harmful organic solvents, which could result in serious environmental and safety issues, but also exhibited fascinating features such as good substrate scope, excellent yields, simple purification for desired products, ease of scale-up, and reusable aqueous medium.