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The first spin-crossover (SCO) complex with an organic-inorganic hybrid perovskite structure (PPN)[FeAu(CN)23] (1) is reported, which displays three-step SCO behaviour. The light-induced excited spin-state trapping measurement gives T0 = 134 K for a three-dimensional FeL3-type (L = bis-monodentate ligand) SCO complex. Moreover, spin-state dependent fluorescence is observed in 1.An efficient CuBr2-catalyzed diastereoselective allylation of a cyclic hemiacetal with allyltrimethylsilane as a nucleophile has been developed. The protocol offers a cost effective, protecting group tolerant, and operationally simple approach to 2,6-trans-disubstituted tetrahydropyran with excellent diastereoselectivity. Furthermore, the application of this methodology has been demonstrated in the total synthesis of decytospolides A and B and their C6-epimers.The contact resistance (Rc) and the effective carrier mobility (μeff) are considered as the important indicators of the performance of organic field-effect transistors (OFETs). Conventionally, the contact resistance is regarded as the interface effect between the metal electrodes and the organic semiconductors, while the carrier mobility is correlated to the crystallinity and π-π stacking of the organic molecules. In the staggered OFETs, Rc is actually closely correlated to μeff through the channel sheet resistance. Besides, the accuracy of the carrier mobility directly extracted from the non-ideal transfer curves with significant contact effect is always questionable. Herein, a diffusion-lead surface doping approach is employed to improve the contact resistance and mobility issues simultaneously. By suppressing the trap states in the sublimated 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT) organic semiconductor with 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4-TCNQ), we observed a 3-fold increase in the carrier mobility from 0.5 to 1.6 cm2 V-1 s-1, and the Rc also drops remarkably from 25.7 kΩ cm to 5.2 kΩ cm. Moreover, the threshold voltage (VTH), subthreshold swing (SS) and the bias stability of the OFETs are also significantly improved. Based on the detailed characterization of the C8-BTBT film upon surface doping, including X-ray diffraction (XRD) for the film crystallinity, Kelvin probe force microscopy (KPFM) for the surface potential, trap state investigation by density of states (DOS) measurement and electrical circuit modeling for partial doping analysis, we confirmed that the spontaneous charge transfer process due to the diffusion of the F4-TCNQ dopants in the C8-BTBT matrix can lead to an effective trap filling. This technique and findings can be potentially developed into a general approach for the improvement of different performance parameters of OFETs.Among numerous crystalline phases of ice, the Ih phase is the most stable above 72 K at atmospheric pressure. It is well established that the orientations of water molecules in the bulk of ice Ih are statistical without long-range order. However, the orientational order of water at the surface of ice Ih has been enigmatic. Here we show that the surface of ice Ih at 100 K has hydrogen order with the OH group pointing upward to the air ("H-up" orientation). We applied nonlinear optical spectroscopy and theoretical modeling to the surface of isotopically pure and diluted ice Ih and observed OH stretch vibrational signatures attributed to H-up ordering. Furthermore, we found that this hydrogen order takes place despite a more inhomogeneous microenvironment at the surface than in the bulk. Our results suggest the prominent role of the surface to allow the reorientation of water molecules for hydrogen ordering that is virtually prohibited in the bulk.The interaction of methane with pristine surfaces of bulk MoC and Mo2C is known to be weak. In contrast, a series of X-ray photoelectron spectroscopy (XPS) experiments, combined with thermal desorption mass spectroscopy (TDS), for MoCy (y = 0.5-1.3) nanoparticles supported on Au(111)-which is completely inert towards CH4-show that these systems adsorb and dissociate CH4 at room temperature and low CH4 partial pressure. This industrially-relevant finding has been further investigated with accurate density functional theory (DFT) based calculations on a variety of MoCy supported model systems. The DFT calculations reveal that the MoCy/Au(111) systems can feature low C-H bond scission energy barriers, smaller than the CH4 adsorption energy. Our theoretical results for bulk surfaces of Mo2C and MoC show that a simple Brønsted-Evans-Polanyi (BEP) relationship holds for C-H bond scission on these systems. However, this is not the case for methane activation on the MoCy nanoparticles as a consequence of their unique electronic and chemical properties. The discovery that supported molybdenum carbide nanoparticles are able to activate methane at room temperature paves the road towards the design of a new family of active carbide catalysts for methane activation and valorisation, with important implications in climate change mitigation and carbon cycle closure.The anti-tumor activity of Cu complexes is well established in cancer research. We developed a biotin-tagged Cu-chelating prodrug that is activated by one-photon and two-photon irradiation for the target-specific and spatio-temporally controlled in situ generation of a Cu complex. In this way, we transform copper from a "cancer-promoting" agent to an anticancer agent.BACKGROUND The request for informed consent to join a clinical trial often creates mistrust and hesitation in the patient who should be enrolled. Mitapivat clinical trial In our study, we evaluated the reasons for refusing to participate in a clinical trial. METHODS In the last 10 years of cardiovascular clinical research, we asked an informed consent to 2586 patients for intervention studies. Overall, 59% agreed to join clinical trials, 40% refused. The 1% initially accepted and then withdrew the consent. Those who refused were more frequently women, relatively younger (mean age 62 ± 5 vs 74 ± 9 years) and had a higher level of education and income. We asked all these patients who refused to answer a brief questionnaire about the reasons for rejection. RESULTS Of 1031 patients, 629 (61%), accepted to answer the interview; 176 (28%) answered they refused on relatives', friends' or other doctors' advices, or after Internet searches; 157 (25%) answered they did not agree about how the trials were carried out (double-blind control procedure, use of placebo); 126 (20%) did not trust official medicine; 63 (10%) could not guarantee their presence at the follow-up visits; 69 (11%) did not want to undergo additional medical examinations; 31 (5%) had previous bad research experiences (feeling like a guinea pig); 7 (about 1%) refused for other reasons. CONCLUSIONS Recruitment into clinical research studies is still a major challenge. Patients, due to a prevailing humanistic culture, are not fully aware of the importance of participation in clinical research, which is sometimes considered as exclusive economic or prestige interest. In our experience, people who refused participation in the trials were younger, with a high level of education and income, more frequently women. The researcher's task is to motivate the patient by emphasizing that participating in a study means being the actors of a treatment choice and that one is a guinea pig when taking untested therapies.The Italian law 219/2017, enacted on January 31, 2018, regulates patients' informed consent, personalized care planning and advance directives. The law provides for patient's self-determination in all phases of life. This also applies to patients suffering from chronic, progressive, terminal disease such as heart failure. In fact, the clinical and psychosocial trajectory for heart failure patients demands an interdisciplinary, systemic approach. Advance directives should be tailor-made to patient's needs and dynamically updated through the course of the disease according to patient's and family informed and shared decision-making. Healthcare professionals will require education and training to stay up to the task both clinically, psychologically and emotionally.Early palliative care (PC) clearly demonstrated its efficacy in patients with heart failure (HF), reducing symptom burden, mainly pain and depression, improving quality of life, and reducing the access to the health care system. However, there are not conclusive data on economic cost reduction. The reasons are related to the few patients involved in the studies dedicated to this topic, to the different clinical settings, different modalities of provision and funding of PC, and different timing of PC implementation. PC was not shown to reduce mortality nor hospital readmissions in randomized trials.The unanswered questions will be clarified only in larger studies, defining specific clinical settings, goals to achieve and standardizing the provision and funding modalities in the different countries.A few patients in advanced or end-stage (stage D or NYHA functional class IV) heart failure are transplant or ventricular assist device eligible. Particularly for the non-operative patients (elderly or with significant comorbidities), intravenous palliative inotropes can be utilized for symptom control, for functional class and quality of life improvement. The authors report evidence-based medicine data about palliative inotrope therapy in advanced heart failure patients and they suggest a possible multidisciplinary approach in order to guarantee the best care to these patients.Treatment of patients with heart failure is based on drugs, cardiac surgery and implantable cardiac devices to prevent sudden cardiac death (implantable cardioverter-defibrillator [ICD]), to reverse left ventricular dysfunction associated with left bundle branch block (cardiac resynchronization therapy) or mechanical circulatory support in more advanced phases of heart failure (left ventricular assist devices [LVAD]).During the follow-up, patients may die from progression of their underlying heart disease or from non-arrhythmic causes, such as malignancies, multi-organ failure, stroke, etc., without benefits by implanted devices. Patients implanted with ICD could die from non-arrhythmic causes, without appropriate shocks until the last few days or weeks of their life. These events occur roughly in 30% of patients, mainly in the last 24 h before death. LVAD therapy may induce significant complications, such as infections, hemorrhagic stroke, thromboembolism, right ventricular failure. In these cases, inappropriate and even appropriate shock deliveries by ICD can no longer prolong life and may simply lead to pain and reduced quality of life, as well as LVAD may prolong life with painful distress due to complications. Therefore, it appears important to discuss early with the patients and their relatives about deactivation of ICD or LVAD at the end of life. The goal of this paper is to provide an overview of the ethical, clinical and communication issues of cardiac implanted device deactivation, with a special focus on issues associated with advance care planning, which require shared decision-making, including those related to end of life decisions (advance directives). Palliative care should be early implemented, particularly in patients with LVAD.
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