A D-A (donor-acceptor)-type chromophore may twist or flatten in its excited state to form a TICT (twisted intramolecular charge transfer) state or a PICT (planar intramolecular charge transfer) ...state, respectively. What is the driving force behind this twisting or planarization? Which geometry will occur for a certain D-A chromophore? To answer these questions, both fragment orbital interaction and excited state energy decomposition analyses were performed on several classical TICT/PICT molecules. Three driving forces were identified, namely, energy gap, hole-electron interactions, and excited state relaxation. The contributions of these driving forces in various types of molecules were analyzed to determine how the molecular structure affects them. The energy gap difference between the twisted and planar geometries was found to play a decisive role in most situations. Thus, evaluating the frontier orbital interactions between the donor and acceptor effectively predicts whether chromophores planarize or twist in the excited state.
Parents' happiness orientation has garnered early attention in school choice studies but has not been cautiously examined. Drawing on Aristotle's framework of Eudaimonia and Hedonia, along with ...Ahmed's concept of the happiness promise, this study transcends a perspective of preference and examines how parents understand and pursue happiness in school choice. Based on interviews with 32 Shanghai middle-class parents, this study indicates five happiness objects: bachelor's degree, expertise, non-cognitive development, good physical and mental health, and hobby. These happiness objects shape parents' school choice preferences. In pursuing happiness objects, parents follow the philosophies of 'no sweet without sweat' and 'prioritize sweet with due consideration to sweat' and employ an authoritative approach when making choices. This study challenges the cultural stereotype that Chinese parents are solely academic-oriented and authoritarian in school choice. Instead, parents integrate happiness and academics and strive to balance children's future fulfilment and present enjoyment.
Full text
Available for:
BFBNIB, NUK, PILJ, SAZU, UL, UM, UPUK
Long non-coding RNAs (lncRNAs) are related to human diseases by regulating gene expression. Identifying lncRNA-disease associations (LDAs) will contribute to diagnose, treatment, and prognosis of ...diseases. However, the identification of LDAs by the biological experiments is time-consuming, costly and inefficient. Therefore, the development of efficient and high-accuracy computational methods for predicting LDAs is of great significance.
In this paper, we propose a novel computational method (gGATLDA) to predict LDAs based on graph-level graph attention network. Firstly, we extract the enclosing subgraphs of each lncRNA-disease pair. Secondly, we construct the feature vectors by integrating lncRNA similarity and disease similarity as node attributes in subgraphs. Finally, we train a graph neural network (GNN) model by feeding the subgraphs and feature vectors to it, and use the trained GNN model to predict lncRNA-disease potential association scores. The experimental results show that our method can achieve higher area under the receiver operation characteristic curve (AUC), area under the precision recall curve (AUPR), accuracy and F1-Score than the state-of-the-art methods in five fold cross-validation. Case studies show that our method can effectively identify lncRNAs associated with breast cancer, gastric cancer, prostate cancer, and renal cancer.
The experimental results indicate that our method is a useful approach for predicting potential LDAs.
Full text
Available for:
DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
The size effect of transition‐metal nanoparticles on electrocatalytic performance remains ambiguous especially when decreasing the size to the atomic level. Herein, we report the spatial isolation of ...cobalt species on the atomic scale, which was achieved by tuning the zinc dopant content in predesigned bimetallic Zn/Co zeolitic imidazole frameworks (ZnCo‐ZIFs), and led to the synthesis of nanoparticles, atomic clusters, and single atoms of Co catalysts on N‐doped porous carbon. This synthetic strategy allowed an investigation of the size effect on electrochemical behavior from nanometer to Ångström dimensions. Single‐atom Co catalysts showed superior bifunctional ORR/OER activity, durability, and reversibility in Zn–air batteries compared with the other derivatives and noble‐metal Pt/C+RuO2, which was attributed to the high reactivity and stability of isolated single Co atoms. Our findings open up a new avenue to regulate the metal particle size and catalytic performance of MOF derivatives.
The spatial isolation of cobalt species on the atomic scale was achieved by tuning the zinc dopant content in predesigned bimetallic Zn/Co zeolitic imidazole frameworks (ZnCo‐ZIFs), and enabled the generation of nanoparticles, atomic clusters, and single atoms of cobalt on N‐doped porous carbon. The single‐atom Co catalysts showed superior bifunctional ORR/OER activity, durability, and reversibility in Zn–air batteries.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Developing cheap, highly efficient and stable electrocatalysts for both oxygen and hydrogen evolution reactions (OER and HER) is extremely meaningful to realize large-scale implementation of water ...splitting technology. Herein, we report the phase and composition controlled synthesis of cobalt sulfide (CoS
) hollow nanospheres (HNSs) and their catalytic efficiencies for hydrogen and oxygen evolution reactions in alkaline media. Three CoS
compounds, i.e., Co
S
, Co
S
, and CoS
HNSs, were precisely synthesized by simply adjusting the molar ratio of carbon disulfide to cobalt acetate using a facile solution-based strategy. Electrochemical results reveal that the as-prepared CoS
HNSs exhibit superior OER and HER catalytic performance to Co
S
and Co
S
HNSs in 1.0 M KOH, with overpotentials of 290 mV for the OER and 193 mV for the HER at 10 mA cm
, and the corresponding Tafel slopes of 57 and 100 mV dec
, respectively. In addition, the CoS
HNSs exhibit remarkable long-term catalytic durability, which is even superior to precious metal catalysts of RuO
and Pt/C. Moreover, an alkaline electrolyzer assembled using CoS
HNSs as both anode and cathode materials can achieve 10 mA cm
at a low cell voltage of 1.54 V at 60 °C with a faradaic efficiency of 100% for overall water splitting. Further analysis demonstrates that the surface morphology, crystallographic structure and coordination environment of Co
active sites in combination determine the HER/OER activities in the synthesized binary CoS
series, which would provide insight into the rational design of transition metal chalcogenides for highly efficient hydrogen and oxygen-involved electrocatalysis.
This article considers the distributed adaptive neuro-fuzzy output feedback control protocol design to solve the output synchronization problem for heterogeneous multiagent systems with nonlinear ...strict-feedback agent dynamics. The output constraints and actuator saturation are considered simultaneously. First, a distributed high-gain observer is employed to estimate the unmeasured agent state and relax the requirement of the Lipschitz continuity of nonlinear follower dynamics. Second, an asymmetric barrier Lyapunov function with time-varying constraint is presented to deal with both the transient and the steady-state constraints on the output synchronization error. To avoid the "explosion of complexity," the dynamic surface control technique is employed to filter the virtual control signal for each follower. To deal with the actuator saturation, a distributed auxiliary dynamical system is designed for each follower. The fuzzy logic system is employed to compensate for the uncertain follower dynamics with guaranteed semiglobal uniformly ultimately boundedness of all closed-loop signals. Finally, a simulation example is conducted to verify the efficacy of the presented adaptive neuro-fuzzy controller design.
The rapidly increasing severity of the energy crisis and environmental degradation are stimulating the rapid development of photocatalysts and rechargeable lithium/sodium ion batteries. In ...particular, MoS2/TiO2 based nanocomposites show great potential and have been widely studied in the areas of both photocatalysis and rechargeable lithium/sodium ion batteries due to their superior combination properties. In addition to the low-cost, abundance, and high chemical stability of both MoS2 and TiO2, MoS2/TiO2 composites also show complementary advantages. These include the strong optical absorption of TiO2vs. the high catalytic activity of MoS2, which is promising for photocatalysis; and excellent safety and superior structural stability of TiO2vs. the high theoretic specific capacity and unique layered structure of MoS2, thus, these composites are exciting as anode materials. In this review, we first summarize the recent progress in MoS2/TiO2-based nanomaterials for applications in photocatalysis and rechargeable batteries. We highlight the synthesis, structure and mechanism of MoS2/TiO2-based nanomaterials. Then, advancements and strategies for improving the performance of these composites in photocatalytic degradation, hydrogen evolution, CO2 reduction, LIBs and SIBs are critically discussed. Finally, perspectives on existing challenges and probable opportunities for future exploration of MoS2/TiO2-based composites towards photocatalysis and rechargeable batteries are presented. We believe the present review would provide enriched information for a deeper understanding of MoS2/TiO2 composites and open avenues for the rational design of MoS2/TiO2 based composites for energy and environment-related applications.
The fabrication of metal‐supported hybrid structures with enhanced properties typically requires external energy input, such as pyrolysis, photolysis, and electrodeposition. In this study, ...silver‐nanoparticle‐decorated transition‐metal hydroxide (TMH) composites were synthesized by an approach based on a spontaneous redox reaction (SRR) at room temperature. The SRR between silver ions and TMH provides a simple and facile route to establish effective and stable heterostructures that can enhance the oxygen evolution reaction (OER) activity. Ag@Co(OH)x grown on carbon cloth exhibits outstanding OER activity and durability, even superior to IrO2 and many previously reported OER electrocatalysts. Experimental and theoretical analysis demonstrates that the strong electronic interaction between Ag and Co(OH)2 activates the silver clusters as catalytically OER active sites, effectively optimizing the binding energies with reacted intermediates and facilitating the OER kinetics.
Nano‐sequins: A facile and spontaneous strategy for synthesizing silver‐nanoparticle‐decorated transition‐metal hydroxide nanohybrids on carbon cloth is presented. The nanohybrids exhibit substantially enhanced OER activity and durability owing to the strong metal–support interaction and decreased reaction energetic barrier on the heterostructure nanocatalysts.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Hybrid materials composed of transition‐metal compounds and nitrogen‐doped carbonaceous supports are promising electrocatalysts for various electrochemical energy conversion devices, whose activity ...enhancements can be attributed to the synergistic effect between metallic sites and N dopants. While the functionality of single‐metal catalysts is relatively well‐understood, the mechanism and synergy of bimetallic systems are less explored. Herein, the design and fabrication of an integrated flexible electrode based on NiCo2S4/graphitic carbon nitride/carbon nanotube (NiCo2S4@g‐C3N4‐CNT) are reported. Comparative studies evidence the electronic transfer from bimetallic Ni/Co active sites to abundant pyridinic‐N in underlying g‐C3N4 and the synergistic effect with coupled conductive CNTs for promoting reversible oxygen electrocatalysis. Theoretical calculations demonstrate the unique coactivation of bimetallic Ni/Co atoms by pyridinic‐N species (a Ni, Co–N2 moiety), which simultaneously downshifts their d‐band center positions and benefits the adsorption/desorption features of oxygen intermediates, accelerating the reaction kinetics. The optimized NiCo2S4@g‐C3N4‐CNT hybrid manifests outstanding bifunctional performance for catalyzing oxygen reduction/evolution reactions, highly efficient for realistic zinc–air batteries featuring low overpotential, high efficiency, and long durability, superior to those of physical mixed counterparts and state‐of‐the‐art noble metal catalysts. The identified bimetallic coactivation mechanism will shed light on the rational design and interfacial engineering of hybrid nanomaterials for diverse applications.
A novel free‐standing NiCo2S4/graphitic carbon nitride (g‐C3N4)/carbon nanotubes (CNTs) hybrid electrode is developed by combining a hydrothermal approach and vacuum filtration. Experimental and theoretical investigations demonstrate the coactivation of bimetallic Co and Ni sites by abundant pyridinic‐N in g‐C3N4 and the synergistic effect with coupled conductive CNTs contributes to substantially enhanced oxygen electrocatalytic activities and discharge/charge behaviors in Zn–air batteries.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
To improve the utilization efficiency of precious metals, metal‐supported materials provide a direction for fabricating highly active and stable heterogeneous catalysts. Herein, carbon cloth ...(CC)‐supported Earth‐abundant CoS2 nanosheet arrays (CoS2/CC) are presented as ideal substrates for ultrafine Pt deposition (Pt‐CoS2/CC) to achieve remarkable performance toward the hydrogen and oxygen evolution reactions (HER/OER) in alkaline solutions. Notably, the Pt‐CoS2/CC hybrid delivers an overpotential of 24 mV at 10 mA cm−2 and a mass activity of 3.89 A Ptmg−1, which is 4.7 times higher than that of commercial Pt/C, at an overpotential of 130 mV for catalyzing the HER. An alkali‐electrolyzer using Pt‐CoS2/CC as a bifunctional electrode enables a water‐splitting current density of 10 mA cm−2 at a low voltage of 1.55 V and can sustain for more than 20 h, which is superior to that of the state‐of‐the‐art Pt/C+RuO2 catalyst. Further experimental and theoretical simulation studies demonstrate that strong electronic interaction between Pt and CoS2 synergistically optimize hydrogen adsorption/desorption behaviors and facilitate the in situ generation of OER active species, enhancing the overall water‐splitting performance. This work highlights the regulation of interfacial and electronic synergy in pursuit of highly efficient and durable supported catalysts for hydrogen and oxygen electrocatalytic applications.
Ultrafine Pt nanoparticle‐decorated pyrite‐type CoS2 nanosheet arrays coated on carbon cloth as an integrated electrode exhibit superior hydrogen evolution reaction/oxygen evolution reaction (OER) bifunctionality and overall water‐splitting performance due to the interfacial and electronic synergy between Pt and CoS2, thus optimizing the hydrogen adsorption/desorption behaviors and facilitating the in situ generation of OER active species.
Full text
Available for:
FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
PDF
