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Adopting a ternary strategy is an effective approach to enhance the power conversion efficiency (PCE) in organic solar cells (OSCs). Previous research on highly efficient ternary systems has predominantly focused on those based on highly crystalline dual small molecule acceptors. However, limited attention has been given to ternary systems utilizing dual polymer donors. Herein, by incorporating the fluorine and alkylsilyl substitution, a new polymer donor named PX1 is developed, which demonstrates strong crystallinity and excellent miscibility with polymer PM6. Moreover, PX1 broadens and enhances the absorption properties of the PM6:L8-BO blends, and its molecular orbital energy level is situated between those of PM6 and L8-BO, highlighting its suitability as a third component. Introducing 20% PX1 into the PM6:L8-BO system resulted in a high PCE of 18.82%. PX1 effectively suppresses charge recombination and reduces energy losses, while also serving as a morphology modulator that enhances the crystallization and improves the molecular packing order of the active layer by shortening the π-π stacking distance and extending crystalline coherence length. These factors collectively contribute to the performance improvements in ternary devices. This study demonstrates that employing a dual polymer donor strategy is a promising approach for achieving high-performance ternary OSCs.
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Among many mRNA modifications, adenine methylation at the N6 position (N6-methyladenosine, m6A) is known to affect mRNA biology extensively. The influence of m6A has yet to be assessed under drought, one of the most impactful abiotic stresses. We show that Arabidopsis thaliana (L.) Heynh. (Arabidopsis) plants lacking mRNA ADENOSINE METHYLASE (MTA) are drought-sensitive. Subsequently, we comprehensively assess the impacts of MTA-dependent m6A changes during drought on mRNA abundance, stability, and translation in Arabidopsis. During drought, there is a global trend toward hypermethylation of many protein-coding transcripts that does not occur in mta. We also observe complex regulation of m6A at a transcript-specific level, possibly reflecting compensation by other m6A components. Importantly, a subset of transcripts that are hypermethylated in an MTA-dependent manner exhibited reduced turnover and translation in mta, compared with wild-type (WT) plants, during drought. Additionally, MTA impacts transcript stability and translation independently of m6A. We also correlate drought-associated deposition of m6A with increased translation of modulators of drought response, such as RD29A, COR47, COR413, ALDH2B, ERD7, and ABF4 in WT, which is impaired in mta. m6A is dynamic during drought and, alongside MTA, promotes tolerance by regulating drought-responsive changes in transcript turnover and translation.
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Maximizing the molecular information density requires simultaneously functionalizing distinct monomers and their coupling connections. However, current synthesis generally focuses on distinct monomers rather than coupling reactions because the multistep reactions significantly escalate the synthetic complexity in an exponential increase. Here, we report the two-dimensional nanoarchitectures (2DNs) of end-on oligomers, with versatile molecular structures and negative differential resistance (NDR), synthesized by programmed and surface-initiated step electrosynthesis based on the simultaneous utilization of six reactions including cross- and homocouplings. The resulting vertically end-on oligomers, with similar values in thickness and molecular length, as crystalline 2DNs, exhibit subnanometer uniformity, ultrahigh compressive modulus of 40 GPa, and low-bias NDR at 0.13 V with an ultralow power consumption of down to 0.05 nW/µm2. This highly controlled electrosynthesis provides a unique dimension to enhance the structural diversity of molecular 2D nanomaterials for high-density and low-power consumption electronics.
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Perovskite solar cells (pero-SCs) have undergone a rapid development in the last decade. However, there is still a lack of systematic studies to investigate whether the empirical rules of working lifetime assessment used in silicon solar cells can be applied to pero-SCs. It is commonly believed that pero-SCs show enhanced stability under day/night cycling due to the reported self-healing effect in the dark.1,2 While we discovered that the degradation of highly efficient FAPbI3 pero-SCs is in fact much faster under natural day/night cycling mode, questioning the widely accepted approach to estimate the operational lifetime of pero-SCs based on continuous mode testing. We reveal the key factor to be the lattice strain caused by thermal expansion/shrinking of the perovskite during the operation, an effect that gradually relaxes under the continuous-illumination mode but cycles synchronously under the cycling mode.3,4 The periodic lattice strain under the cycling mode results in deep trap accumulation and chemical degradation during operation, decreasing the ion migration potential and hence the device lifetime.5 We introduce phenylselenenyl chloride (Ph-Se-Cl) to regulate the perovskite lattice strain during day/night cycling, which achieved the certified efficiency of 26.3% and a 10-time improved T80 lifetime under the cycling mode after the modification.
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In recent years, perovskite has been widely adopted in series-connected monolithic tandem solar cells (TSCs) to overcome the Shockley-Queisser limit of single-junction solar cells. Perovskite/organic TSCs, comprising a wide-bandgap (WBG) perovskite solar cell (pero-SC) as the front cell and a narrow-bandgap organic solar cell (OSC) as the rear cell, have recently drawn attention owing to the good stability and potential high power conversion efficiency (PCE)1,2,3,4. However, WBG pero-SCs usually exhibit higher voltage losses than regular pero-SCs, which limits the performance of TSCs5,6. One of the major obstacles comes from interfacial recombination at the perovskite/C60 interface, and it is important to develop effective surface passivation strategies to pursue higher PCE of perovskite/organic TSCs7. Here we exploit a new surface passivator cyclohexane 1,4-diammonium diiodide (CyDAI2), which naturally contains two isomeric structures with ammonium groups on the same or opposite sides of the hexane ring (denoted as cis-CyDAI2 and trans-CyDAI2, respectively), and the two isomers demonstrate completely different surface interaction behaviors. The cis-CyDAI2 passivation treatment reduces the Quasi-Fermi level splitting (QFLS)-open circuit voltage (Voc) mismatch of the WBG pero-SCs with a bandgap of 1.88 eV and enhanced its Voc to 1.36 V. Combining the cis-CyDAI2 treated perovskite and the organic active layer with a narrow-bandgap of 1.24 eV, the constructed monolithic perovskite/organic TSC demonstrates a PCE of 26.4% (certified as 25.7%).
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Immobilizing catalysts and photosensitizers on an electrode surface is crucial in interfacial energy conversion. However, their combination for optimizing catalytic performance is an unpredictable challenge. Herein, we report that catalyst and photosensitizer monomers are selectively grafted one-by-one addition onto the electrode surface by interfacial electrosynthesis to achieve composition and sequence-controlled oligomer photoelectrocatalytic monolayers. This electrosynthesis relies on the oxidative coupling reaction of carbazole and the reductive coupling reaction of vinyl on the catalyst and photosensitizer monomers, and it initiates on self-assembled monolayers and propagates with alternating positive and negative potentials. Each addition and completion of the target monomer can be quantitatively identified and monitored by optical and electrical responses and their linear coefficients as a function of reaction steps. The resulting composition and sequence-controlled monolayers exhibit tuning electrocatalytic behaviors including water splitting and CO2 reduction, indicating an efficient way to optimize the electro- and photocatalytic functions and performance of molecular materials.
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Organic solar cells (OSCs) processed with non-halogenated solvents usually suffer from excessive self-aggregation of small molecule acceptors (SMAs), severe phase separation and higher energy loss (Eloss), leading to reduced open-circuit voltage (Voc) and power conversion efficiency (PCE). Regulating the intermolecular interaction to disperse the aggregation and further improve the molecular packing order of SMAs would be an effective strategy to solve this problem. Here, we designed and synthesized two SMAs L8-PhF and L8-PhMe by introducing different substituents (fluorine for L8-PhF and methyl for L8-PhMe) on the phenyl end group of the inner side chains of L8-Ph, and investigated the effect of the substituents on the intermolecular interaction of SMAs, Eloss and performance of OSCs processed with non-halogenated solvents. Through single crystal analysis and theoretical calculations, it is found that compared with L8-PhF, which possesses strong and abundant intermolecular interactions but downgraded molecular packing order, L8-PhMe with the methyl substituent possesses more effective non-covalent interactions, which improves the tightness and order of molecular packing. When blending the SMAs with polymer donor PM6, the differences in intermolecular interactions of the SMAs influenced the film formation process and phase separation of the blend films. The L8-PhMe based blend film exhibits shorten film formation and more homogeneous phase separation than those of the L8-PhF and L8-Ph based ones. Especially, the OSCs based on L8-PhMe show reduced non-radiative energy loss and enhanced Voc than the devices based on the other two SMAs. Consequently, the L8-PhMe based device processed with o-xylene (o-XY) and using 2PACz as the hole transport layer (HTL) shows an outstanding PCE of 19.27 %. This study highlights that the Eloss of OSCs processed with non-halogenated solvents could be decreased through regulating the intermolecular interactions of SMAs by inner side chain modification, and also emphasize the importance of effectivity rather than intensity of non-covalent interactions introduced in SMAs on the molecular packing, morphology and PCE of OSCs.
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In this study, nanoporous gold (NPG) was deposited on a screen-printed carbon electrode (SPCE) by the dynamic hydrogen bubble template (DHBT) method to prepare an electrochemical sensor for the simultaneous determination of Pb2+ and Cu2+ by square wave anodic stripping voltammetry (SWASV). The electrodeposition potential and electrodeposition time for NPG/SPCE preparation were investigated thoroughly. Scanning electron microscopy (SEM) and energy-dispersive X-ray diffraction (EDX) analysis confirmed successful fabrication of the NPG-modified electrode. Electrochemical characterization exhibits its superior electron transfer ability compared with bare and nanogold-modified electrodes. After a comprehensive optimization, Pb2+ and Cu2+ were simultaneously determined with linear range of 1-100 µg/L for Pb2+ and 10-100 µg/L for Cu2+, respectively. The limits of detection were determined to be 0.4 µg/L and 5.4 µg/L for Pb2+ and Cu2+, respectively. This method offers a broad linear detection range, a low detection limit, and good reliability for heavy metal determination in drinking water. These results suggest that NPG/SPCE holds great promise in environmental and food applications.
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Preparing high-quality perovskite films is a decisive step toward realizing highly efficient and stable perovskite solar cells (Pero-SCs). Water is a key factor affecting the stability of the Pero-SCs. Here, the widely used water adsorbents chitosan, sorbitol, and sodium hyaluronate (NaHA) were used as hydrophilic layers on the upper interface of the perovskite to form a barrier against water. The water adsorbents also passivated defects on the surface of the perovskite active layer due to their -OH and -COOH functional groups. The NaHA-modified devices showed the best power conversion efficiency (PCE) (PCE = 21.74%). Although the NaHA-modified Pero-SCs showed optimal photovoltaic performance, the stability of the modified devices decreased due to the strong water adsorption ability of NaHA, while with moderate water adsorption ability sorbitol-modified devices exhibited good stability and PCE. The devices were tested in the dark and room temperature at different humidity levels for 800 h. At low humidity (25% ± 5% RH), the PCEs of the sorbitol- and NaHA-modified devices were maintained at 80% and 71% of the initial values, respectively. At high humidity (75% ± 5% RH), the PCE was maintained at 64% and 23% of the initial values, respectively. This work provides an avenue to select adsorbents with suitable water absorption ability as the interface modification layer, thus reducing the water erosion of perovskite films and obtaining highly stable inverted Pero-SCs.
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Electrochemical detection is favorable for the rapid and sensitive determination of heavy metal cadmium. However, the detection sensitivity needs to be further improved, and a portable, low-cost device is needed for on-site detection. Herein, an in-situ bismuth modified pre-anodized screen-printed carbon electrode (SPCE) was developed for Cd2+ determination by square wave anodic stripping voltammetry (SWASV). The in-situ bismuth modification enhances the enrichment of Cd2+, and together with pre-anodization improve the electron transfer rate of electrode, thus enhancing the detection sensitivity. The electrode modification method combines pre-anodization and in-situ bismuth deposition, which is very easy and effective. Furthermore, a self-made PSoC Stat potentiostat coupled with a stirring device was fabricated for portable and low-cost electrochemical detection. After comprehensive optimization, the developed method can reach a testing time of 3 min, a detection limit of 3.55 µg/L, a linear range of 5-100 µg/L, and a recovery rate of 91.7-107.1% in water and rice samples for Cd2+ determination. Therefore, our method holds great promise for the rapid, sensitive and on-site determination of Cd2+ in food samples.
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Bismuto , Cadmio , Técnicas Electroquímicas , Electrodos , Oryza , Cadmio/análisis , Oryza/química , Bismuto/química , Bismuto/análisis , Técnicas Electroquímicas/métodos , Técnicas Electroquímicas/instrumentación , Agua/química , Agua/análisis , Contaminantes Químicos del Agua/análisis , Límite de Detección , Contaminación de Alimentos/análisisRESUMEN
Currently, associations between dietary intakes of individual monounsaturated fatty acids (MUFAs) and hypertension were not well disclosed, and the interaction effects of MUFAs on their associations with hypertension were unknown. Obesity was correlated with both MUFAs and hypertension, while if anthropometric obesity indices performed mediating roles in associations between MUFAs and hypertension remained underdetermined. In our study, 8509 Chinese adults investigated from 2004 to 2011 were included. Dietary information collection and physical examinations were performed at baseline and each timepoint of follow-up. As we found, inverse associations of MUFA17, MUFA18 and MUFA20 with hypertension were statistically significant after adjustments, hazard ratios (HRs) were 0.87, 0.90 and 0.91, respectively. MUFA15 was positively associated with hypertension, with an HR of 1.07 (95% confidence interval: 1.01, 1.12). By performing principal component analysis (PCA) to estimate the joint effects of MUFAs on hypertension, the PCA score of MUFAs was only inversely associated with blood pressure. No joint effect was observed in g-computation analyses. Both linear and nonlinear interactions of MUFAs on their associations with hypertension were estimated using restricted cubic spline analysis. The association between MUFA15 and hypertension was interacted by MUFA17, and the association between MUFA20 and hypertension was interacted by MUFA18. The mediation effects of body mass index and waist circumference were found on associations of hypertension with MUFA15, MUFA17 and MUFA20. Our findings suggested that associations with hypertension were different among individual MUFAs, and mutual interactions existed, implying that the utility of individual MUFAs might be recommended for estimating relationships between MUFAs and diseases. Moreover, fat accumulation might potentially underlie associations between MUFAs and hypertension.
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Ácidos Grasos Monoinsaturados , Hipertensión , Humanos , Hipertensión/epidemiología , Masculino , Femenino , Persona de Mediana Edad , Adulto , China/epidemiología , Presión Sanguínea , Obesidad/epidemiología , Índice de Masa Corporal , Anciano , Pueblos del Este de AsiaRESUMEN
Traditional Chinese medicine with rich resources in China and definite therapeutic effects on complex diseases demonstrates great development potential. However, the complex composition, the unclear pharmacodynamic substances and mechanisms of action, and the lack of reasonable methods for evaluating clinical safety and efficacy have limited the research and development of innovative drugs based on traditional Chinese medicine. The progress in cutting-edge disciplines such as artificial intelligence and biomimetics, especially the emergence of cell painting and organ-on-a-chip, helps to identify and characterize the active ingredients in traditional Chinese medicine based on the changes in model characteristics, thus providing more accurate guidance for the development and application of traditional Chinese medicine. The application of phenotypic drug discovery in the research and development of innovative drugs based on traditional Chinese medicine is gaining increasing attention. In recent years, the technology for phenotypic drug discovery keeps advancing, which improves the early discovery rate of new drugs and the success rate of drug research and development. Accordingly, phenotypic drug discovery gradually becomes a key tool for the research on new drugs. This paper discusses the enormous potential of traditional Chinese medicine in the discovery and development of innovative drugs and illustrates how the application of phenotypic drug discovery, supported by cutting-edge technologies such as cell painting, deep learning, and organ-on-a-chip, propels traditional Chinese medicine into a new stage of development.
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Descubrimiento de Drogas , Medicamentos Herbarios Chinos , Medicina Tradicional China , Humanos , Medicamentos Herbarios Chinos/farmacología , Medicamentos Herbarios Chinos/química , Fenotipo , Animales , Desarrollo de MedicamentosRESUMEN
Organic photovoltaics (OPVs) need to overcome limitations such as insufficient thermal stability to be commercialized. The reported approaches to improve stability either rely on the development of new materials or on tailoring the donor/acceptor morphology, however, exhibiting limited applicability. Therefore, it is timely to develop an easy method to enhance thermal stability without having to develop new donor/acceptor materials or donor-acceptor compatibilizers, or by introducing another third component. Herein, a unique approach is presented, based on constructing a polymer fiber rigid network with a high glass transition temperature (Tg) to impede the movement of acceptor and donor molecules, to immobilize the active layer morphology, and thereby to improve thermal stability. A high-Tg one-dimensional aramid nanofiber (ANF) is utilized for network construction. Inverted OPVs with ANF network yield superior thermal stability compared to the ANF-free counterpart. The ANF network-incorporated active layer demonstrates significantly more stable morphology than the ANF-free counterpart, thereby leaving fundamental processes such as charge separation, transport, and collection, determining the device efficiency, largely unaltered. This strategy is also successfully applied to other photovoltaic systems. The strategy of incorporating a polymer fiber rigid network with high Tg offers a distinct perspective addressing the challenge of thermal instability with simplicity and universality.
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PURPOSE: This study aimed to understand how age, health status, and lifestyle impact bone mineral density (BMD) in middle-aged and older adults, focusing on predicting osteoporosis risk. METHODS: This study included 2836 participants aged 50-88 from the Health Improvement Program of Bone (HOPE) conducted from 2021 to 2023. We used logistic regression to make a prediction tool. Then checked its accuracy and reliability using receiver operating characteristic (ROC) and calibration curves. RESULTS: Factors like age, body weight, prior fractures, and smoking were independently found to affect BMD T-score distribution in men. In women, age and body weight were identified as independent factors influencing BMD T-score distribution. A nomogram was created to visually illustrate these predictive relationships. CONCLUSIONS: The nomogram proved highly accurate in identifying men aged 50 and above and postmenopausal women based on their BMD T-score distribution, improving clinical decision-making and patient care in osteoporosis evaluation and treatment.
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Densidad Ósea , Nomogramas , Osteoporosis , Humanos , Masculino , Femenino , Anciano , Factores de Riesgo , Persona de Mediana Edad , Anciano de 80 o más Años , Reproducibilidad de los ResultadosRESUMEN
Flexible perovskite solar cells (pero-SCs) have the potential to overturn the application scenario of silicon photovoltaic technology. However, their mechanical instability severely impedes their practical applicability, and the corresponding intrinsic degradation mechanism remains unclear. In this study, the degradation behavior of flexible pero-SCs is systematically analyzed under mechanical stress and it is observed that the structural failure first occurs in the polycrystal perovskite film, then extend to interfaces. To suppress the structural failure, pentaerythritol triacrylate, a crosslinked molecule with three stereoscopic crosslink sites, is employed to establish a 3D polymer network in both the interface and bulk perovskite. This network reduced the Young's modulus of the perovskite and simultaneously enhanced the interfacial toughness. As a result, the formation of cracks and delamination, which occur under a high mechanical stress, is significantly suppressed in the flexible pero-SC, which consequently retained 92% of its initial power conversion efficiency (PCE) after 20 000 bending cycles. Notably, the flexible device also shows a record PCE of 24.9% (certified 24.48%).
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This review delves into the multifaceted aspects of age-related balance changes, highlighting their prevalence, underlying causes, and the impact they have on the elderly population. Central to this discussion is the exploration of various physiological changes that occur with aging, such as alterations in the vestibular, visual, proprioceptive systems, and musculoskeletal degeneration. We examine the role of neurological disorders, cognitive decline, and medication side effects in exacerbating balance issues. The review underscores the significance of early detection and effective intervention strategies in mitigating the risks associated with balance problems, such as falls and reduced mobility. It discusses the effectiveness of diverse intervention strategies, including exercise programs, rehabilitation techniques, and technological advancements like virtual reality, wearable devices, and telemedicine. Additionally, the review stresses the importance of a holistic approach in managing balance disorders, encompassing medication review, addressing comorbidities, and environmental modifications. The paper also presents future research directions, emphasizing the need for a deeper understanding of the complex mechanisms underlying balance changes with aging and the potential of emerging technologies and interdisciplinary approaches in enhancing assessment and intervention methods. This comprehensive review aims to provide valuable insights for healthcare providers, researchers, and policymakers in developing targeted strategies to improve the quality of life and ensure the well-being of the aging population.
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A certain number of hole-like defects will occur in aluminum alloys under cyclic loading. The internal holes will reduce the strength of the material and cause stress concentration, which will aggravate the development of fatigue damage. A classification method of defect features based on X-ray CT damage data is proposed. The random hole distribution model is established through the linear congruence method and the region division method. The hole parameter is introduced as the intermediate variable of the 3D reconstruction model of internal defects. In the mesoscopic stage, the function relationship between the distribution of random holes and the fatigue life is established based on the coupling relationship between the number and proportion of pores and the fatigue life. In the macroscopic stage, the relationship between the random holes and the macroscopic crack growth life is established by taking the crack length as the damage variable. The crack propagation rate decreased with the increase in the number of holes. The prediction model of the whole life stage is established using the life function from microcrack initiation to macroscopic crack propagation. Finally, the validity of the whole stage fatigue life prediction model is demonstrated through the comparison and verification of experiments, which provides a certain engineering value for the life estimation of 6061-T6 aluminum alloy materials.
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Photoswitchable molecules can control the activity and functions of biomolecules by triggering conformational changes. However, it is still challenging to fully understand such fast-triggering conformational evolution from nonequilibrium to equilibrium distribution at the molecular level. Herein, we successfully simulated the unfolding of the FK-11 peptide upon the photoinduced trans-to-cis isomerization of azobenzene based on the Markov state model. We found that the ensemble of FK-11 contains five conformational states, constituting two unfolding pathways. More intriguingly, we observed the microsecond-scale conformational propagation of the FK-11 peptide from the fully folded state to the equilibrium populations of the five states. The computed CD spectra match well with the experimental data, validating our simulation method. Overall, our study not only offers a protocol to study the photoisomerization-induced conformational changes of enzymes but also could orientate the rational design of a photoswitchable molecule to manipulate biological functions.
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Compuestos Azo , Péptidos , Péptidos/química , Compuestos Azo/química , Simulación por ComputadorRESUMEN
Perovskite solar cells (pero-SCs) are highly unstable even under trace water. Although the blanket encapsulation (BE) strategy applied in the industry can effectively block moisture invasion, the commercial UV-curable adhesives (UVCAs) for BE still trigger power conversion efficiency deterioration, and the degradation mechanism remains unknown. For the first time, the functions of commercial UVCAs are revealed in BE-processed pero-SCs, where the small-sized monomer easily permeates to the perovskite surface, forming an insulating barrier to block charge extraction, while the high-polarity moiety can destroy perovskite lattice. To solve these problems, a macromer, named PIBA is carefully designed, by grafting two acrylate terminal groups on the highly gastight polyisobutylene and realizes an increased molecular diameter as well as avoided high-polarity groups. The PIBA macromer can stabilize on pero-SCs and then sufficiently crosslink, forming a compact and stable network under UV light without sacrificing device performance during the BE process. The resultant BE devices show negligible efficiency loss after storage at 85% relative humidity for 2000 h. More importantly, these devices can even reach ISO 20653:2013 Degrees of protection IPX7 standard when immersed in one-meter-deep water. This BE strategy shows good universality in enhancing the moisture stability of pero-SCs, irrespective of the perovskite composition or device structure.
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High-boiling-point nonhalogenated solvents are superior solvents to produce large-area organic solar cells (OSCs) in industry because of their wide processing window and low toxicity; while, these solvents with slow evaporation kinetics will lead excessive aggregation of state-of-the-art small molecule acceptors (e.g. L8-BO), delivering serious efficiency losses. Here, a heterogeneous nucleating agent strategy is developed by grafting oligo (ethylene glycol) side-chains on L8-BO (BTO-BO). The formation energy of the obtained BTO-BO; while, changing from liquid in a solvent to a crystalline phase, is lower than that of L8-BO irrespective of the solvent type. When BTO-BO is added as the third component into the active layer (e.g. PM6:L8-BO), it easily assembles to form numerous seed crystals, which serve as nucleation sites to trigger heterogeneous nucleation and increase nucleation density of L8-BO through strong hydrogen bonding interactions even in high-boiling-point nonhalogenated solvents. Therefore, it can effectively suppress excessive aggregation during growth, achieving ideal phase-separation active layer with small domain sizes and high crystallinity. The resultant toluene-processed OSCs exhibit a record power conversion efficiency (PCE) of 19.42% (certificated 19.12%) with excellent operational stability. The strategy also has superior advantages in large-scale devices, showing a 15.03-cm2 module with a record PCE of 16.35% (certificated 15.97%).