RESUMO
Xanthogranulomatous cholecystitis (XGC) is a rare type of cholecystitis that, despite being benign poses diagnostic challenges due to its low prevalence and need for consensus on diagnostic criteria. Consequently, distinguishing XGC from gallbladder cancer (GBC) is challenging, leading to clinical misdiagnoses. This article presents a case where a patient initially diagnosed with GBC was later found to have XGC.
RESUMO
The C-N coupling reaction demonstrates broad application in the fabrication of a wide range of high value-added organonitrogen molecules including fertilizers (e.g., urea), chemical feedstocks (e.g., amines, amides), and biomolecules (e.g., amino acids). The electrocatalytic C-N coupling pathways from waste resources like CO2, NO3-, or NO2- under mild conditions offer sustainable alternatives to the energy-intensive thermochemical processes. However, the complex multistep reaction routes and competing side reactions lead to significant challenges regarding low yield and poor selectivity toward large-scale practical production of target molecules. Among diverse catalyst systems that have been developed for electrochemical C-N coupling reactions, the atomically dispersed catalysts with well-defined active sites provide an ideal model platform for fundamental mechanism elucidation. More importantly, the intersite synergy between the active sites permits the enhanced reaction efficiency and selectivity toward target products. In this Review, we systematically assess the dominant reaction pathways of electrocatalytic C-N coupling reactions toward various products including urea, amines, amides, amino acids, and oximes. To guide the rational design of atomically dispersed catalysts, we identify four key stages in the overall reaction process and critically discuss the corresponding catalyst design principles, namely, retaining NOx/COx reactants on the catalyst surface, regulating the evolution pathway of N-/C- intermediates, promoting C-N coupling, and facilitating final hydrogenation steps. In addition, the advanced and effective theoretical simulation and characterization technologies are discussed. Finally, a series of remaining challenges and valuable future prospects are presented to advance rational catalyst design toward selective electrocatalytic synthesis of organonitrogen molecules.
RESUMO
To achieve carbon neutrality and sustainable development, innovative solar-to-fuel systems have been designed through the integration of solar energy harvesting and electrochemical devices. Over the last decade, there have been notable advancements in enhancing the efficiency and durability of these solar-to-fuel systems. Despite the advancements, there remains significant potential for further improvements in the performance of systems. Enhancements can be achieved by optimizing electrochemical catalysts, advancing the manufacturing technologies of photovoltaics and electrochemical cells, and refining the overall design of these systems. In the realm of catalyst optimization, the effectiveness of materials can be significantly improved through active site engineering and strategic use of functional groups. Similarly, the performance of electrochemical devices can be enhanced by incorporating specific additives into electrolytes and optimizing gas diffusion electrodes. Improvements in solar harvesting devices are achievable through efficient passivant and self-assembled monolayers, which enhance the overall quality and efficiency of these systems. Additionally, optimizing the energy conversion efficiency involves the strategic use of DC converters, photoelectrodes, and redox media. This review aims to provide a comprehensive overview of the advancements in solar-powered electrochemical energy conversion systems, laying a solid foundation for future research and development in the field of energy sustainability.
RESUMO
Inverted p-i-n perovskite solar cells (PSCs) are easy to process but need improved interface characteristics with reduced energy loss to prevent efficiency drops when increasing the active photovoltaic area. Here, we report a series of poly ferrocenyl molecules that can modulate the perovskite surface enabling the construction of small- and large-area PSCs. We found that the perovskite-ferrocenyl interaction forms a hybrid complex with enhanced surface coordination strength and activated electronic states, leading to lower interfacial nonradiative recombination and charge transport resistance losses. The resulting PSCs achieve an enhanced efficiency of up to 26.08% for small-area devices and 24.51% for large-area devices (1.0208 cm2). Moreover, the large-area PSCs maintain >92% of the initial efficiency after 2000 h of continuous operation at the maximum power point under 1-sun illumination and 65 °C.
RESUMO
Crystallization orientation plays a crucial role in determining the performance and stability of perovskite solar cells (PVSCs), whereas effective strategies for realizing oriented perovskite crystallization is still lacking. Herein, a facile and efficient top-down strategy is reported to manipulate the crystallization orientation via treating perovskite wet film with propylamine chloride (PACl) before annealing. The PA+ ions tend to be adsorbed on the (001) facet of the perovskite surface, resulting in the reduced cleavage energy to induce (001) orientation-dominated growth of perovskite film and then reduce the temperature of phase transition, meanwhile, the penetrating Cl ions further regulate the crystallization process. As-prepared (001)-dominant perovskite films exhibit the ameliorative film homogeneity in terms of vertical and horizontal scale, leading to alleviated lattice mismatch and lowered defect density. The resultant PVSC devices deliver a champion power conversion efficiency (PCE) of 25.07% with enhanced stability, and the unencapsulated PVSC device maintains 95% of its initial PCE after 1000 h of operation at the maximum power point under simulated AM 1.5G illumination.
RESUMO
RATIONALE: Negative pressure pulmonary edema (NPPE) is an acute onset of non-cardiogenic interstitial pulmonary edema, commonly seen among surgical patients after extubation from general aneasthesia. It is mainly caused by rapid inspiration with acute upper airway obstruction resulting in significant negative thoracic pressure. PATIENT CONCERNS: A 24-year-old female patient who underwent laparoscopic cholecystectomy under general anesthesia and developed NPPE postoperatively. DIAGNOSES: Her main clinical manifestation was coughing up pink foamy sputum; postoperative CT showed increased texture in both lungs and bilateral ground glass opacities. INTERVENTIONS: Diuretics and steroids were used, and symptomatic supportive treatments such as oxygen were given. OUTCOMES: After treatment, on the fourth post-operative day, her symptoms were relieved and her vital signs were stable enough for her to be discharged. LESSONS: Although this is a rare and severe complication, the prognosis of NPPE is good when it is managed with proper diagnosis and treatment.
Assuntos
Obstrução das Vias Respiratórias , Colecistectomia Laparoscópica , Edema Pulmonar , Humanos , Feminino , Adulto Jovem , Adulto , Edema Pulmonar/diagnóstico por imagem , Edema Pulmonar/etiologia , Colecistectomia Laparoscópica/efeitos adversos , Diuréticos/uso terapêutico , Oxigênio , Anestesia Geral/efeitos adversos , Obstrução das Vias Respiratórias/complicaçõesRESUMO
Low-dimensional/three-dimensional perovskite heterojunctions have shown great potential for improving the performance of perovskite photovoltaics, but large organic cations in low-dimensional perovskites hinder charge transport and cause carrier mobility anisotropy at the heterojunction interface. Here, we report a low-dimensional/three-dimensional perovskite heterojunction that introduces strong aromatic conjugated low-dimensional perovskites in p-i-n devices to reduce the electron transport resistance crossing the perovskite/electron extraction interface. The strong aromatic conjugated π-conjugated network results in continuous energy orbits among [Pb2I6]2- frameworks, thereby effectively suppressing interfacial non-radiative recombination and boosting carrier extraction. Consequently, the devices achieved an improved efficiency to 25.66% (certified 25.20%), and maintained over 95% of the initial efficiency after 1200 hours and 1000 hours under ISOS-L-1I and ISOS-D-1 protocols, respectively. The chemical design of strong aromatic conjugated molecules in perovskite heterojunctions provides a promising avenue for developing efficient and stable perovskite photovoltaics.
RESUMO
Solution-processed photodetectors have emerged as promising candidates for next-generation of visible-near infrared (vis-NIR) photodetectors. This is attributed to their ease of processing, compatibility with flexible substrates, and the ability to tune their detection properties by integrating complementary photoresponsive semiconductors. However, the limited performance continues to hinder their further development, primarily influenced by the difference of charge transport properties between perovskite and organic semiconductors. In this work, a perovskite-organic bipolar photodetectors (PDs) is introduced with multispectral responsivity, achieved by effectively managing charges in perovskite and a ternary organic heterojunction. The ternary heterojunction, incorporating a designed NIR guest acceptor, exhibits a faster charge transfer rate and longer carrier diffusion length than the binary heterojunction. By achieving a more balanced carrier dynamic between the perovskite and organic components, the PD achieves a low dark current of 3.74 nA cm-2 at -0.2 V, a fast response speed of <10 µs, and a detectivity of exceeding 1012 Jones. Furthermore, a bioinspired retinotopic system for spontaneous chromatic adaptation is achieved without any optical filter. This charge management strategy opens up possibilities for surpassing the limitations of photodetection and enables the realization of high-purity, compact image sensors with exceptional spatial resolution and accurate color reproduction.
RESUMO
Inorganic nickel oxide (NiOx ) is an ideal hole transport material (HTM) for the fabrication of high-efficiency, stable, and large-area perovskite photovoltaic devices because of its low cost, stability, and ease of solution processing. However, it delivers low power conversion efficiency (PCE) in tin perovskite solar cells (TPSCs) compared to other organic HTMs. Here, the origin of hole transport barriers at the perovskite-NiOx interface is identified and a self-assembled monolayer interface modification is developed, through introducing (4-(7H-dibenzo[c,g]carbazol-7-yl)ethyl)phosphonic acid (2PADBC) into the perovskite-NiOx interface. The 2PADBC anchors undercoordinated Ni cations through phosphonic acid groups, suppressing the reaction of highly active Ni≥3+ defects with perovskites, while increasing the electron density and oxidation activation energy of Sn at the perovskite interface, reducing the interface nonradiative recombination caused by tetravalent Sn defects. The devices deliver significantly increased open-circuit voltage from 0.712 to 0.825 V, boosting the PCE to 14.19% for the small-area device and 12.05% for the large-area (1 cm2 ) device. In addition, the 2PADBC modification enhances the operational stability of NiOx -based TPSCs, maintaining more than 93% of their initial efficiency after 1000 h.
RESUMO
Solar-driven water splitting powered by photovoltaics enables efficient storage of solar energy in the form of hydrogen fuel. In this work, we demonstrate efficient solar-to-hydrogen conversion using perovskite (PVK) tandem photovoltaics and a halogen-modulated metal-organic framework (MOF) electrocatalyst. By substituting tetrafluoroterephthalate (TFBDC) for terephthalic (BDC) ligands in a nickel-based MOF, we achieve a 152 mV improvement in oxygen evolution reaction (OER) overpotential at 10 mA·cm2. Through X-ray photoelectron spectroscopy (XPS), X-ray adsorption structure (XAS) analysis, theoretical simulation, and electrochemical results, we demonstrated that the introduction of fluorine atoms enhanced the intrinsic activity of Ni sites as well as the transfer property and accessibility of the MOF. Using this electrocatalyst in a bias-free photovoltaic electrochemical (PV-EC) system with a PVK/organic tandem solar cell, we achieve 6.75% solar-to-hydrogen efficiency (ηSTH). We also paired the electrocatalyst with a PVK photovoltaic module to drive water splitting at 206.7 mA with ηSTH of 10.17%.
RESUMO
P-i-n geometry perovskite solar cells (PSCs) offer simplified fabrication, greater amenability to charge extraction layers, and low-temperature processing over n-i-p counterparts. Self-assembled monolayers (SAMs) can enhance the performance of p-i-n PSCs but ultrathin SAMs can be thermally unstable. We report a thermally robust hole-selective layer comprised of nickel oxide (NiOx) nanoparticle film with a surface-anchored (4-(3,11-dimethoxy-7H-dibenzo[c,g]carbazol-7-yl)butyl)phosphonic acid (MeO-4PADBC) SAM that can improve and stabilize the NiOx/perovskite interface. The energetic alignment and favorable contact and binding between NiOx/MeO-4PADBC and perovskite reduced the voltage deficit of PSCs with various perovskite compositions and led to strong interface toughening effects under thermal stress. The resulting 1.53-electron-volt devices achieved 25.6% certified power conversion efficiency and maintained >90% of their initial efficiency after continuously operating at 65 degrees Celsius for 1200 hours under 1-sun illumination.
RESUMO
Perovskite/organic tandem solar cells (POTSCs) are gaining attention due to their easy fabrication, potential to surpass the S-Q limit, and superior flexibility. However, the low power conversion efficiencies (PCEs) of wide bandgap (Eg) perovskite solar cells (PVSCs) have hindered their development. This work presents a novel and effective mixed-cation passivation strategy (CE) to passivate various types of traps in wide-Eg perovskite. The complementary effect of 4-trifluoro phenethylammonium (CF3 -PEA+ , denoted as CA+ ) and ethylenediammonium (EDA2+ , denoted as EA2+ ) reduces both electron/hole defect densities and non-radiative recombination rate, resulting in a record open-circuit voltage (Voc ) of wide-Eg PVSCs (1.35 V) and a high fill factor (FF) of 83.29%. These improvements lead to a record PCE of 24.47% when applied to fabricated POTSCs, the highest PCE to date. Furthermore, unencapsulated POTSCs exhibit excellent photo and thermal stability, retaining over 90% of their initial PCE after maximum power point (MPP) tracking or exposure to 60 °C for 500 h. These findings imply that the synergic effect of surface passivators is a promising strategy to achieve high-efficiency and stable wide-Eg PVSCs and corresponding POTSCs.
RESUMO
Non-covalent interactions play an essential role in directing the self-assembly of hybrid organic-inorganic crystals. In hybrid halide perovskites, hydrogen bonding has been the paramount non-covalent interaction. Here, we show another non-covalent interaction, namely, the halogen bond interaction, that directs a symmetry-breaking assembly in a new series of two-dimensional (2D) perovskites (ICH2 CH2 NH3 )2 (CH3 NH3 )n-1 Pbn I3n+1 (n is the layer thickness, n=1-4). Structural analysis shows that the halogen bond strength varies with the layer thickness. For the odd number (n=1, 3) layered perovskites, stronger halogen interaction leads to centrosymmetric structures, whereas for the n=2 layered perovskites, weaker halogen bonds result in non-centrosymmetric structures. Transient reflection spectroscopy shows a suppressed radiative recombination rate (k2 ≈0) and prolonged spin lifetime for n=2 structure, suggesting an enhanced Rashba band splitting effect. The structural asymmetry is further confirmed with a reversible bulk photovoltaic effect. Our work provides a new design strategy to enable hybrid perovskites with emerging properties and functionalities associated with structural asymmetry.
RESUMO
Fullerene acceptors typically possess excellent electron-transporting properties and can work as guest components in ternary organic solar cells to enhance the charge extraction and efficiencies. However, conventional fullerene small molecules typically suffer from undesirable segregation and dimerization, thus limiting their applications in organic solar cells. Herein we report the use of a poly(fullerene-alt-xylene) acceptor (PFBO-C12) as guest component enables a significant efficiency increase from 16.9% for binary cells to 18.0% for ternary all-polymer solar cells. Ultrafast optic and optoelectronic studies unveil that PFBO-C12 can facilitate hole transfer and suppress charge recombination. Morphological investigations show that the ternary blends maintain a favorable morphology with high crystallinity and smaller domain size. Meanwhile, the introduction of PFBO-C12 reduces voltage loss and enables all-polymer solar cells with excellent light stability and mechanical durability in flexible devices. This work demonstrates that introducing polyfullerenes as guest components is an effective approach to achieving highly efficient ternary all-polymer solar cells with good stability and mechanical robustness.
RESUMO
Metal-organic framework (MOF) solids with their variable functionalities are relevant for energy conversion technologies. However, the development of electroactive and stable MOFs for electrocatalysis still faces challenges. Here, a molecularly engineered MOF system featuring a 2D coordination network based on mercaptan-metal links (e.g., nickel, as for Ni(DMBD)-MOF) is designed. The crystal structure is solved from microcrystals by a continuous-rotation electron diffraction (cRED) technique. Computational results indicate a metallic electronic structure of Ni(DMBD)-MOF due to the Ni-S coordination, highlighting the effective design of the thiol ligand for enhancing electroconductivity. Additionally, both experimental and theoretical studies indicate that (DMBD)-MOF offers advantages in the electrocatalytic oxygen evolution reaction (OER) over non-thiol (e.g., 1,4-benzene dicarboxylic acid) analog (BDC)-MOF, because it poses fewer energy barriers during the rate-limiting *O intermediate formation step. Iron-substituted NiFe(DMBD)-MOF achieves a current density of 100 mA cm-2 at a small overpotential of 280 mV, indicating a new MOF platform for efficient OER catalysis.
RESUMO
The commercialization of perovskite solar cells (PVSCs) urgently requires the development of green-solvent processable dopant-free hole transporting materials (HTMs). However, strong intermolecular interactions that ensure high hole mobility always compromise the solubility and film-forming ability in green solvents. Herein, we show a simple but effective design strategy to solve this trade-off, that is, constructing star-shaped D-A-D structure. The resulting HTMs (BTP1-2) can be processed by green solvent of 2-methylanisole (2MA), a kind of food additive, and show high hole mobility and multiple defect passivation effects. An impressive efficiency of 24.34 % has been achieved for 2MA-processed BTP1 based inverted PVSCs, the highest value for green-solvent processable HTMs so far. Moreover, it is manifested that the charge separation of D-A type HTMs at the photoinduced excited state can help to passivate the defects of perovskites, indicating a new HTM design insight.
RESUMO
The interface and crystallinity of perovskite films play a decisive role in determining the device performance, which is significantly influenced by the bottom hole-transporting material (HTM) of inverted perovskite solar cells (PVSCs). Herein, a simple design strategy of polymer HTMs is reported, which can modulate the wettability and promote the anchoring by introducing pyridine units into the polyarylamine backbone, so as to realize efficient and stable inverted PVSCs. The HTM properties can be effectively modified by varying the linkage sites of pyridine units, and 3,5-linked PTAA-P1 particularly demonstrates a more regulated molecular configuration for interacting with perovskites, leading to highly crystalline perovskite films with uniform back contact and reduced defect density. Dopant-free PTAA-P1-based inverted PVSCs have realized remarkable efficiencies of 24.89% (certified value: 24.50%) for small-area (0.08 cm2 ) as well as 23.12% for large-area (1 cm2 ) devices. Moreover, the unencapsulated device maintains over 93% of its initial efficiency after 800 h of maximum power point tracking under simulated AM 1.5G illumination.
RESUMO
Among the emerging photovoltaic technologies, rigid perovskite solar cells (PSCs) have made tremendous development owing to their exceptional power conversion efficiency (PCE) of up to 25.7%. However, the record PCE of flexible PSCs (≈22.4%) still lags far behind their rigid counterparts and their mechanical stabilities are also not satisfactory. Herein, through modifying the interface between perovskite and hole transport layer via pentylammonium acetate (PenAAc) molecule a highly efficient and stable flexible inverted PSC is reported. Through synthetic manipulation of anion and cation, it is shown that the PenA+ and Ac- have strong chemical binding with both acceptor and donor defects of surface-terminating ends on perovskite films. The PenAAc-modified flexible PSCs achieve a record PCE of 23.68% (0.08 cm2 , certified: 23.35%) with a high open-circuit voltage (VOC ) of 1.17 V. Large-area devices (1.0 cm2 ) also realized an exceptional PCE of 21.52%. Moreover, the fabricated devices show excellent stability under mechanical bending, with PCE remaining above 91% of the original PCE even after 5000 bends.
RESUMO
The incorporation of charged functional groups is effective to modulate the activity of molecular complexes for the CO2 reduction reaction (CO2 RR), yet long-term heterogeneous electrolysis is often hampered by catalyst leaching. Herein, an electrocatalyst of atomically thin, cobalt-porphyrin-based, ionic-covalent organic nanosheets (CoTAP-iCONs) is synthesized via a post-synthetic modification strategy for high-performance CO2 -to-CO conversion. The cationic quaternary ammonium groups not only enable the formation of monolayer nanosheets due to steric hindrance and electrostatic repulsion, but also facilitate the formation of a *COOH intermediate, as suggested by theoretical calculations. Consequently, CoTAP-iCONs exhibit higher CO2 RR activity than other cobalt-porphyrin-based structures: an 870% and 480% improvement of CO current densities compared to the monomer and neutral nanosheets, respectively. Additionally, the iCONs structure can accommodate the cationic moieties. In a flow cell, CoTAP-iCONs attain a very small onset overpotential of 40 mV and a stable total current density of 212 mA cm-2 with CO Faradaic efficiency of >95% at -0.6 V for 11 h. Further coupling the flow electrolyzer with commercial solar cells yields a solar-to-CO conversion efficiency of 13.89%. This work indicates that atom-thin, ionic nanosheets represent a promising structure for achieving both tailored activity and high stability.
RESUMO
Perovskite solar cells (PVSCs) have drawn great attention due to their high processability and superior photovoltaic properties. However, their further development is often hindered by severe nonradiative recombination at interfaces that decreases power conversion efficiency (PCE). To this end, a facile strategy to construct a 3D/2D vertical heterostructure to reduce the energy loss in PVSCs is developed. The heterostructure is contrived through the van der Waals integration of 2D perovskite ((BA)4 AgBiBr8 ) nanosheets onto the surface of 3D-FAPbI3 -based perovskites. The large bandgap of (BA)4 AgBiBr8 enables the formation of type-I heterojunction with 3D-FAPbI3 -based perovskites, which serves as a barrier to suppress the trap-assisted recombination at the interface. As a result, a satisfying PCE of 24.48% is achieved with an improved open-circuit voltage (VOC ) from 1.13 to 1.17 V. Moreover, the 2D perovskite nanosheets can effectively mitigate the iodide ion diffusion from perovskite to the metal electrode, hence enhancing the device stability. 3D/2D architectured devices retain ≈90% of their initial PCE under continuous illumination or heating after 1000 h, which are superior to 3D-based devices. This work provides an effective and controllable strategy to construct 3D/2D vertical heterostructure to simultaneously boost the efficiency and stability of PVSCs.