RESUMEN
Water electrolysis is an environmentally-friendly strategy for hydrogen production but suffers from significant energy consumption. Substituting urea oxidation reaction (UOR) with lower theoretical voltage for water oxidation reaction adopting nickel-based electrocatalysts engenders reduced energy consumption for hydrogen production. The main obstacle remains strong interaction between accumulated Ni3+ and *COO in the conventional Ni3+-catalyzing pathway. Herein, a novel Ni3+/Ni2+ mediated pathway for UOR via constructing a heterojunction of nickel metaphosphate and nickel telluride (Ni2P4O12/NiTe), which efficiently lowers the energy barrier of UOR and avoids the accumulation of Ni3+ and excessive adsorption of *COO on the electrocatalysts, is developed. As a result, Ni2P4O12/NiTe demonstrates an exceptionally low potential of 1.313 V to achieve a current density of 10 mA cm-2 toward efficient urea oxidation reaction while simultaneously showcases an overpotential of merely 24 mV at 10 mA cm-2 for hydrogen evolution reaction. Constructing urea electrolysis electrolyzer using Ni2P4O12/NiTe at both sides attains 100 mA cm-2 at a low cell voltage of 1.475 V along with excellent stability over 500 h accompanied with nearly 100% Faradic efficiency.
RESUMEN
[4-(3,6-dimethyl-9H-carbazol-9yl)butyl]phosphonic acid (Me-4PACz) self-assembled molecules (SAM) are an effective method to solve the problem of the buried interface of NiOx in inverted perovskite solar cells (PSCs). However, the Me-4PACz end group (carbazole core) cannot forcefully passivate defects at the bottom of the perovskite film. Here, a Co-SAM strategy is employed to modify the buried interface of PSCs. Me-4PACz is doped with phosphorylcholine chloride (PC) to form a Co-SAM to improve the monolayer coverage and reduce leakage current. The phosphate group and chloride ions (Cl-) in PC can inhibit NiOx surface defects. Meantime, the quaternary ammonium ions and Cl- in PC can fill organic cations and halogen vacancies in the perovskite film to enable defects passivation. Moreover, Co-SAM can promote the growth of perovskite crystals, collaboratively solve the problem of buried defects, suppress nonradiative recombination, accelerate carrier transmission, and relieve the residual stress of the perovskite film. Consequently, the Co-SAM modified devices show power conversion efficiencies as high as 25.09% as well as excellent device stability with 93% initial efficiency after 1000 h of operation under one-sun illumination. This work demonstrates the novel approach for enhancing the performance and stability of PSCs by modifying Co-SAM on NiOx.
RESUMEN
Photocatalytic overall water splitting into hydrogen and oxygen is desirable for long-term renewable, sustainable and clean fuel production on earth. Metal sulfides are considered as ideal hydrogen-evolved photocatalysts, but their component homogeneity and typical sulfur instability cause an inert oxygen production, which remains a huge obstacle to overall water-splitting. Here, a distortion-evoked cation-site oxygen doping of ZnIn2S4 (D-O-ZIS) creates significant electronegativity differences between adjacent atomic sites, with S1 sites being electron-rich and S2 sites being electron-deficient in the local structure of S1-S2-O sites. The strong charge redistribution character activates stable oxygen reactions at S2 sites and avoids the common issue of sulfur instability in metal sulfide photocatalysis, while S1 sites favor the adsorption/desorption of hydrogen. Consequently, an overall water-splitting reaction has been realized in D-O-ZIS with a remarkable solar-to-hydrogen conversion efficiency of 0.57%, accompanying a ~ 91% retention rate after 120 h photocatalytic test. In this work, we inspire an universal design from electronegativity differences perspective to activate and stabilize metal sulfide photocatalysts for efficient overall water-splitting.
RESUMEN
The conversion of CO2 into valuable solar fuels via photocatalysis is a promising strategy for addressing energy shortages and environmental crises. Here, novel In2 O3 @Co2 VO4 hierarchical heterostructures are fabricated by in situ growing Co2 VO4 nanorods onto In2 O3 nanofibers. First-principle calculations and X-ray photoelectron spectroscopy (XPS) measurements reveal the electron transfer between In2 O3 and Co2 VO4 driven by the difference in work functions, thus creating an interfacial electric field and bending the bands at the interfaces. In this case, the photogenerated electrons in In2 O3 transport to Co2 VO4 and recombine with its holes, indicating the formation of In2 O3 @Co2 VO4 S-scheme heterojunctions and resulting in effective separation of charge carriers, as confirmed by in situ irradiation XPS. The unique S-scheme mechanism, along with the enhanced optical absorption and the lower Gibbs free energy change for the production of * CHO, significantly contributes to the efficient CO2 photoreduction into CO and CH4 in the absence of any molecule cocatalyst or scavenger. Density functional theory simulation and in situ diffuse reflectance infrared Fourier transform spectroscopy are employed to elucidate the reaction mechanism in detail.
RESUMEN
High-performance thermogalvanic cells have the potential to convert thermal energy into electricity, but their effectiveness is limited by the low concentration difference of redox ions. We report an in situ photocatalytically enhanced redox reaction that generates hydrogen and oxygen to realize a continuous concentration gradient of redox ions in thermogalvanic devices. A linear relation between thermopower and hydrogen production rate was established as an essential design principle for devices. The system exhibited a thermopower of 8.2 millivolts per kelvin and a solar-to-hydrogen efficiency of up to 0.4%. A large-area generator (112 square centimeters) consisting of 36 units yielded an open-circuit voltage of 4.4 volts and a power of 20.1 milliwatts, as well 0.5 millimoles of hydrogen and 0.2 millimoles of oxygen after 6 hours of outdoor operation.
RESUMEN
After decades of research in the conservation of cultural heritage, nanolime (NL) has emerged as a potential alternative inorganic material to the frequently used organic materials. However, its poor kinetic stability in water has been a major challenge that restricted its penetration depth through cultural relics and resulted in unsatisfactory conservation outcomes. Here, for the first time, we realize NL water dispersion by modification of ionic liquid (1-butyl-3-methylimidazolium tetrafluoroborate) via a sample aqueous solution deposit method. Our findings indicate that the cation of the ionic liquid (IL) binds strongly to the surface of NL particles (IL-NL) by forming hydrogen bonds with Ca(OH)2 facets. The absorption of IL causes an unexpected significant alteration in the morphology of NL particles and results in a drastic reduction in NL's size. More importantly, this absorption endows NL excellent kinetic stability dispersed into water and implements NL water dispersion, which makes a breakthrough in terms of extreme poor kinetic stability of as-synthesized NL and commercial NL in water. The mechanism driving IL-NL water dispersion is explained by Stern theory. In the context of consolidating weathered stone, the presence of IL may delay carbonation of NL but the penetration depth of IL-NL through stone samples is three times deeper than that of as-synthesized and commercial NLs. Additionally, the consolidation strength of IL-NL is similar to that of as-synthesized NL and commercial NL. Moreover, IL-NL has no significant impact on the permeability, pore size, and microstructure of consolidated stone relics. Our research contributes to the field of NL-related materials and will enhance the dissemination and utilization of NL-based materials in the preservation of water-insensitive cultural heritage.
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Little is known about the mediating effect of attitude toward older adults on the relationship between aging knowledge and willingness to care for older adults. We applied the theory of planned behavior (TPB) and the knowledge-attitude-behavior (KAB) model as theoretical frameworks to examine the mediation effect of attitude toward older adults. Data from 388 Chinese nursing students were analyzed. The Willingness to Care for Older People (WCOP) scale, Kogan's Attitude toward Older People scale (KAOP) and Facts on Aging Quiz (FAQ) were utilized to assess willingness, attitude and aging knowledge, respectively. Data were analyzed using SPSS 22. 0 with the PROCESS macro. Bootstrap methods were used to obtain the significance of mediating effects. The study showed that aging knowledge was significantly associated with willingness to care for older adults and that attitude toward older adults mediated the association. Bootstrapping method confirmed the significance of the indirect effect of aging knowledge through attitude, accounting for 18.9% of the total willingness variance. Overall, based on the TPB and the KAB theoretical framework, our data support the notion that improving aging knowledge and attitude may contribute to improve the willingness to aged care among nursing students.
RESUMEN
BACKGROUND: Problem-solving ability has been identified as a core competence that nursing students should develop, and it plays a vital role in career development. Therefore, it is necessary to investigate factors related to problem-solving ability and the path relationships among those factors in the context of nursing students. OBJECTIVE: This study aims to identify the factors that affect problem-solving ability, and to investigate path relationships of self-directed learning ability, critical thinking ability, learning engagement, and problem-solving ability among nursing students. DESIGN: A cross-sectional study. SETTINGS: The Department of Nursing at a university located in Shanghai, China. SAMPLE: A total of 540 nursing students with a three-year education program were enrolled in the current study. METHODS: Data were collected by using a structured questionnaire, including general information, learning engagement, self-directed learning ability, critical thinking ability, and problem-solving ability of nursing students. Pearson's correlations were used to explore the relationships between learning engagement, self-directed learning ability, critical thinking ability, and problem-solving ability. The path relationships were analyzed by constructing a structural equation model using AMOS software. RESULTS: Our results showed that learning engagement, self-directed learning ability, and critical thinking ability were positively associated with problem-solving ability. Furthermore, learning engagement did not influence problem-solving ability directly, but it affected problem-solving ability indirectly via self-directed learning ability and critical thinking ability among nursing students. Additionally, the total effects of self-directed learning (0.442) and critical thinking ability (0.581) were more prominent than learning engagement (0.361) on problem-solving ability. CONCLUSIONS: To improve the problem-solving ability of nursing students, nursing educators should develop targeted strategies to enhance learning engagement, self-directed learning ability, and critical thinking ability.
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Encapsulation engineering is an effective strategy to improve the stability of perovskite solar cells. However, current encapsulation materials are not suitable for lead-based devices because of their complex encapsulation processes, poor thermal management, and inefficient lead leakage suppression. In this work, we design a self-crosslinked fluorosilicone polymer gel, achieving nondestructive encapsulation at room temperature. Moreover, the proposed encapsulation strategy effectively promotes heat transfer and mitigates the potential impact of heat accumulation. As a result, the encapsulated devices maintain 98% of the normalized power conversion efficiency after 1000 h in the damp heat test and retain 95% of the normalized efficiency after 220 cycles in the thermal cycling test, satisfying the requirements of the International Electrotechnical Commission 61215 standard. The encapsulated devices also exhibit excellent lead leakage inhibition rates, 99% in the rain test and 98% in the immersion test, owing to excellent glass protection and strong coordination interaction. Our strategy provides a universal and integrated solution for achieving efficient, stable, and sustainable perovskite photovoltaics.
RESUMEN
Severe carrier recombination and the slow kinetics of water splitting for photocatalysts hamper their efficient application. Herein, we propose a hydrovoltaic effect-enhanced photocatalytic system in which polyacrylic acid (PAA) and cobaltous oxide (CoO)-nitrogen doped carbon (NC) achieve an enhanced hydrovoltaic effect and CoO-NC acts as a photocatalyst to generate H2 and H2O2 products simultaneously. In this system, called PAA/CoO-NC, the Schottky barrier height between CoO and the NC interface decreases by 33% due to the hydrovoltaic effect. Moreover, the hydrovoltaic effect induced by H+ carrier diffusion in the system generates a strong interaction between H+ ions and the reaction centers of PAA/CoO-NC, improving the kinetics of water splitting in electron transport and species reaction. PAA/CoO-NC exhibits excellent photocatalytic performance, with H2 and H2O2 production rates of 48.4 and 20.4 mmol g-1 h-1, respectively, paving a new way for efficient photocatalyst system construction.
RESUMEN
Single-atom catalysts (SACs) on hematite photoanodes are efficient cocatalysts to boost photoelectrochemical performance. They feature high atom utilization, remarkable activity, and distinct active sites. However, the specific role of SACs on hematite photoanodes is not fully understood yet: Do SACs behave as a catalytic site or as a spectator? By combining spectroscopic experiments and computer simulations, we demonstrate that single-atom iridium (sIr) catalysts on hematite (α-Fe2O3/sIr) photoanodes act as a true catalyst by trapping holes from hematite and providing active sites for the water oxidation reaction. In situ transient absorption spectroscopy showed a reduced number of holes and shortened hole lifetime in the presence of sIr. This was particularly evident on the second timescale, indicative of fast hole transfer and depletion toward water oxidation. Intensity-modulated photocurrent spectroscopy evidenced a faster hole transfer at the α-Fe2O3/sIr/electrolyte interface compared to that at bare α-Fe2O3. Density functional theory calculations revealed the mechanism for water oxidation using sIr as a catalytic center to be the preferred pathway as it displayed a lower onset potential than the Fe sites. X-ray photoelectron spectroscopy demonstrated that sIr introduced a mid-gap of 4d state, key to the fast hole transfer and hole depletion. These combined results provide new insights into the processes controlling solar water oxidation and the role of SACs in enhancing the catalytic performance of semiconductors in photo-assisted reactions.
RESUMEN
An optimized approach to producing lattice-matched heterointerfaces for electrocatalytic hydrogen evolution has not yet been reported. Herein, we present the synthesis of lattice-matched Mo2 C-Mo2 N heterostructures using a gradient heating epitaxial growth method. The well lattice-matched heterointerface of Mo2 C-Mo2 N generates near-zero hydrogen-adsorption free energy and facilitates water dissociation in acid and alkaline media. The lattice-matched Mo2 C-Mo2 N heterostructures have low overpotentials of 73â mV and 80â mV at 10â mA cm-2 in acid and alkaline solutions, respectively, comparable to commercial Pt/C. A novel photothermal-electrocatalytic water vapor splitting device using the lattice-matched Mo2 C-Mo2 N heterostructure as a hydrogen evolution electrocatalyst displays a competitive cell voltage for electrocatalytic water splitting.
RESUMEN
As a promising inorganic nanomaterial for the conservation of arenaceous sandstone-based relics such as wall painting, ancient building, stone heritage etc., nanolime (NL) has drawn increasing attention in recent years. Usually, NL needs to be dispersed into an alcoholic solution when applied. Nevertheless, a back-migration phenomenon of NL to the surface of the stone and delayed carbonation of NL enabled by alcohol do not guarantee good preservation effects. Dispersing NL into water can avoid the above issues. However, NL water suspension shows extremely poor kinetic stability, greatly restricting the penetration of NL into stone relics as well as bringing unfavorable impacts to the treated stone heritage. Here, we develop a facile method to synthesize polydopamine (PDA)-modified NL (PDA@NL). Characterizations demonstrate that PDA is uniformly distributed on the surface of NL particles though hydrogen bonds. In addition, the presence of PDA reduces the size of NL particles and achieves the highest specific surface area of NL reported to date. More importantly, water suspension of PDA@NL is far more stable than that of pure NL. The kinetic stability mechanism of PDA@NL in water is attributed to the lessened spatial interactions between NL particles, which is realized by the coverage of PDA on the surface of NL particles. Furthermore, the coverage of PDA does not inhibit carbonation. Within 105 h, NL in PDA@NL completes carbonation and obtains 93.7% calcite, which is comparable to that of NL suspension. Permeability tests prove that the PDA@NL suspension penetrates far deeper through stone specimens compared with the NL suspension. Additionally, PDA@NL presents good consolidation performances for stone samples. Our work opens a new direction for the modification of NL that will boost the studies of NL-modified materials as well as the conservation of cultural heritage.
RESUMEN
The performance enhancement of inverted perovskite solar cells applying nickel oxide (NiOx ) as the hole transport layer (HTL) has been limited by impurity ions (such as nitrate ions). Herein, we have proposed a strategy to obtain high-quality NiOx nanoparticles via an ionic liquid-assisted synthesis method (NiOx -IL). Experimental and theoretical results illustrate that the cation of the ionic liquid can inhibit the adsorption of impurity ions on nickel hydroxide through a strong hydrogen bond and low adsorption energy, thereby obtaining NiOx -IL HTL with high conductivity and strong hole-extraction ability. Importantly, the removal of impurity ions can effectively suppress the redox reaction between the NiOx film and the perovskite film, thus slowing down the deterioration of device performance. Consequently, the modified inverted device shows a striking efficiency exceeding 22.62 %, and superior stability maintaining 92 % efficiency at a maximum power point tracking under one sun illumination for 1000â h.
RESUMEN
Stabilizing high-efficiency perovskite solar cells (PSCs) at operating conditions remains an unresolved issue hampering its large-scale commercial deployment. Here, we report a star-shaped polymer to improve charge transport and inhibit ion migration at the perovskite interface. The incorporation of multiple chemical anchor sites in the star-shaped polymer branches strongly controls the crystallization of perovskite film with lower trap density and higher carrier mobility and thus inhibits the nonradiative recombination and reduces the charge-transport loss. Consequently, the modified inverted PSCs show an optimal power conversion efficiency of 22.1% and a very high fill factor (FF) of 0.862, corresponding to 95.4% of the Shockley-Queisser limited FF (0.904) of PSCs with a 1.59-eV bandgap. The modified devices exhibit excellent long-term operational and thermal stability at the maximum power point for 1000 hours at 45°C under continuous one-sun illumination without any significant loss of efficiency.
RESUMEN
Solar-driven hydrogen production from water using particulate photocatalysts is considered the most economical and effective approach to produce hydrogen fuel with little environmental concern. However, the efficiency of hydrogen production from water in particulate photocatalysis systems is still low. Here, we propose an efficient biphase photocatalytic system composed of integrated photothermal-photocatalytic materials that use charred wood substrates to convert liquid water to water steam, simultaneously splitting hydrogen under light illumination without additional energy. The photothermal-photocatalytic system exhibits biphase interfaces of photothermally-generated steam/photocatalyst/hydrogen, which significantly reduce the interface barrier and drastically lower the transport resistance of the hydrogen gas by nearly two orders of magnitude. In this work, an impressive hydrogen production rate up to 220.74 µmol h-1 cm-2 in the particulate photocatalytic systems has been achieved based on the wood/CoO system, demonstrating that the photothermal-photocatalytic biphase system is cost-effective and greatly advantageous for practical applications.
RESUMEN
Hematite is a promising candidate as photoanode for solar-driven water splitting, with a theoretically predicted maximum solar-to-hydrogen conversion efficiency of â¼16%. However, the interfacial charge transfer and recombination greatly limits its activity for photoelectrochemical water splitting. Carbon dots exhibit great potential in photoelectrochemical water splitting for solar to hydrogen conversion as photosensitisers and co-catalysts. Here we developed a novel carbon underlayer from low-cost and environmental-friendly carbon dots through a facile hydrothermal process, introduced between the fluorine-doped tin oxide conducting substrate and hematite photoanodes. This led to a remarkable enhancement in the photocurrent density. Owing to the triple functional role of carbon dots underlayer in improving the interfacial properties of FTO/hematite and providing carbon source for the overlayer as well as the change in the iron oxidation state, the bulk and interfacial charge transfer dynamics of hematite are significantly enhanced, and consequently led to a remarkable enhancement in the photocurrent density. The results revealed a substantial improvement in the charge transfer rate, yielding a charge transfer efficiency of up to 80% at 1.25 V vs. RHE. In addition, a significant enhancement in the lifetime of photogenerated electrons and an increased carrier density were observed for the hematite photoanodes modified with a carbon underlayer, confirming that the use of sustainable carbon nanomaterials is an effective strategy to boost the photoelectrochemical performance of semiconductors for energy conversion.
RESUMEN
The competition between charge recombination and extraction principally affects the fill factor (FF) and power conversion efficiency (PCE) of planar thin-film solar cells. In Sb2S3 thin-film solar cells, the electrocharge recombination and extraction n transport layer (ETL) plays a significant role in electron extraction and determination of Sb2S3 film absorber quality. Herein, a TiO2 ETL is strategically modified using an inorganic salt zinc halide (i.e., ZnCl2, ZnBr2, ZnI2), which simultaneously improves the electronic properties of TiO2 and promotes the growth of Sb2S3 films with larger grain size and higher crystallinity. The experimental results and theoretical calculations further reveal that the zinc halide can interact with TiO2 and simultaneously bond strongly with the upper Sb2S3 film, which creates a unique pathway for electron transfer, passivates the trap states, and alleviates the recombination losses effectively. As a result, an average PCE of 6.87 ± 0.11% and the highest PCE of 7.08% have been attained with an improved FF from 51.22 to 61.61% after ZnCl2 introduction. Additionally, introduction of ZnCl2 helps the unencapsulated devices to maintain 93% of their original performance after 2400 h of storage in a nitrogen-filled glovebox. This work develops an effective route for the optimization of ETLs and defect healing using simple and low-cost inorganic salts.
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Two-dimensional nanomaterials, such as graphene and molybdenum disulfide (MoS2), have recently attracted widespread attention as surface-enhanced Raman scattering (SERS) substrates. However, their SERS enhancement is of a smaller magnitude than that of noble metal nanomaterials, and therefore, the detection sensitivity still needs to be substantially improved for practical applications. Here, we present the first detailed studies on the effect of the (MoS2) interlayer distances on the SERS intensity enhancement. We find that MoS2 with smaller interlayer distances achieves an SERS enhancement factor as high as 5.31 × 105, which is one of the highest enhancement factors to date among the two-dimensional nanomaterial SERS sensors. This remarkable SERS sensitivity is attributed to the highly efficient charge transfer from MoS2 to probe molecules. The charge-transfer ability directly determines the variable quantity dz2 orbitals of Mo elements in the MoS2-molecule system and then tunes the Raman intensity of probe molecules. Our work contributes to reveal the influence of MoS2 interlayer spacing on SERS detection and to open a new way for designing a highly sensitive nonmetal SERS technology.
RESUMEN
Dye-sensitized solar cells (DSSCs) are solar energy conversion devices with high efficiency and simple fabrication procedures. Developing transparent counter electrode (CE) materials for bifacial DSSCs can address the needs of window-type building-integrated photovoltaics (BIPVs). Herein, transparent organic-inorganic hybrid composite films of molybdenum disulfide and poly(3,4-ethylenedioxythiophene) (MoS2/PEDOT) are prepared to take full advantage of the conductivity and electrocatalytic ability of the two components. MoS2 is synthesized by hydrothermal method and spin-coated to form the MoS2 layer, and then PEDOT films are electrochemically polymerized on top of the MoS2 film to form the composite CEs. The DSSC with the optimized MoS2/PEDOT composite CE shows power conversion efficiency (PCE) of 7% under front illumination and 4.82% under back illumination. Compared with the DSSC made by the PEDOT CE and the Pt CE, the DSSC fabricated by the MoS2/PEDOT composite CE improves the PCE by 10.6% and 6.4% for front illumination, respectively. It proves that the transparent MoS2/PEDOT CE owes superior conductivity and catalytic properties, and it is an excellent candidate for bifacial DSSC in the application of BIPVs.