67 research outputs found

    Facile synthesis of high-performance indium nanocrystals for selective CO2-to-formate electroreduction

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    Selective electrocatalytic reduction of CO2 to formate has received increasing interest for CO2 conversion and utilization. Yet, the CO2 reduction process still faces major challenges, partly due to the lack of cost-effective, highly active, selective and stable electrocatalysts. Here, we report a mesoporous indium (mp-In) electrocatalyst composed of nanobelts synthesized via a simple solution-based approach for selective CO2 reduction to formate. The mp-In nanocrystals provide enlarged surface areas, abundant surface active sites and edge/low-coordinated sites. Such advantages afford the mp-In with an outstanding electrocatalytic performance for the CO2-to-formate conversion. A high formate selectivity, with a Faradaic efficiency (FE) of >90% was achieved over a potential of −0.95 V to −1.1 V (vs VRHE). The mp-In catalyst showed excellent durability, reflected by the stable formate selectivity and current density over a 24 h reaction period. Density functional theory (DFT) calculations reveal that the stabilization of the intermediate OCHO* on the In-plane surfaces is energetically feasible, further elucidating the origin of its enhanced CO2-to-formate activity and selectivity. This work may offer valuable insights for the facile fabrication of porous hierarchical nanostructures for electrocatalytic and selective reduction of CO2.</p

    Genome-wide regulation of innate immunity by juvenile hormone and 20-hydroxyecdysone in the Bombyx fat body

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    <p>Abstract</p> <p>Background</p> <p>Insect innate immunity can be affected by juvenile hormone (JH) and 20-hydroxyecdysone (20E), but how innate immunity is developmentally regulated by these two hormones in insects has not yet been elucidated. In the silkworm, <it>Bombyx mori</it>, JH and 20E levels are high during the final larval molt (4 M) but absent during the feeding stage of 5<sup>th </sup>instar (5 F), while JH level is low and 20E level is high during the prepupal stage (PP). Fat body produces humoral response molecules and hence is considered as the major organ involved in innate immunity.</p> <p>Results</p> <p>A genome-wide microarray analysis of <it>Bombyx </it>fat body isolated from 4 M, 5 F and PP uncovered a large number of differentially-expressed genes. Most notably, 6 antimicrobial peptide (AMP) genes were up-regulated at 4 M versus PP suggesting that <it>Bombyx </it>innate immunity is developmentally regulated by the two hormones. First, JH treatment dramatically increased AMP mRNA levels and activities. Furthermore, 20E treatment exhibited inhibitory effects on AMP mRNA levels and activities, and RNA interference of the 20E receptor <it>EcR</it>-<it>USP </it>had the opposite effects to 20E treatment.</p> <p>Conclusion</p> <p>Taken together, we demonstrate that JH acts as an immune-activator while 20E inhibits innate immunity in the fat body during <it>Bombyx </it>postembryonic development.</p

    Atomically dispersed tungsten on metal halide monolayer as a ferromagnetic Chern insulator

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    Although the quantum anomalous Hall (QAH) effect has been experimentally observed in several magnetically doped topological insulators, up to now, it only survives at a very low temperature. More suitable candidate QAH insulators that can work at high temperature are much desired. Here, we propose an experimentally feasible way to realize a robust QAH insulator: atomically dispersed transition metals (e.g., W) on a two-dimensional porous metal halide normal insulator (e.g., InI₃), which has been developed as a state-of-the-art chemical technology broadly adopted for homogeneous catalysis. Based on the first-principles calculations, we predict that the atomic W embedded in an InI₃ monolayer forms an intrinsic ferromagnetic QAH insulator, which exhibits robust uniform out-of-plane ferromagnetic order up to ∼160K and a topologically nontrivial band gap of 56 meV with a nonzero Chern number (|C|=2). We also study its magneto-optical Kerr effect and collective plasma excitation modes, which may help for further experimental verifications and measurement of interesting physical features of Dirac-like electronic dispersion. Our results introduce a feasible method to obtain the QAH effect, which may motivate intensive experimental interest in this field

    Gradual chlorination at different positions of D-π-A copolymers based on benzodithiophene and isoindigo for organic solar cells

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    Isoindigo (IID) has been widely used as strong acceptor unit (A) to construct narrow bandgap polymers in organic field effect transistors (OFETs) and organic solar cells (OSCs). Combing with IID, we chose benzodithiophene (BDT) as the donor unit (D) and thieno [3,2-b]thiophene (TT) as the π bridge to construct a new type of D-π-A polymer PE70. Based on PE70, we adopt the chlorination strategy to fine-tune photoelectric characteristics and film morphology, and then developed PE74 and PE75. By blending with non-fullerene acceptor (NFA) Y6, device based on PE74 with chloride substitution on the BDT unit showed increasing photovoltaic performance. In addition, further chlorine substitution on the IID (PE75) would greatly reduce the non-radiative voltage loss (ΔV3), and the distorted molecular conformation also took responsible for the excessive recombination. As results, PE74:Y6-based device achieves a power conversion efficiency (PCE) of 11.06% with open-circuit voltage (VOC) of 0.76 ​V, which are higher than those of PE70:Y6 (PCE of 10.40% and VOC of 0.72 ​V) and PE75: Y6-based device (PCE of 6.24% and VOC of 0.84 ​V). This work demonstrates the regularity of the photovoltaic performance caused by chlorination strategy in polymer in the non-fullerene OSC devices, which provide important insights into high-performance photovoltaic materials

    Medium Bandgap D-A Type Photovoltaic Polymers Based on an Asymmetric Dithienopyran Donor and a Benzotriazole Acceptor

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    Conjugated polymers based on the donor of an asymmetric 5H-dithieno[3,2-b:2′,3′-d]pyran (DTPa) and the acceptors of benzo[d][1,2,3]triazole (BTA) or di-fluorinated benzo[d][1,2,3]triazole (ffBTA) with thiophene as π-bridge were designed and synthesized. Two asymmetric-building-block-containing polymers (ABC-polymers) possess a strong and broad absorption in the range of 300–750 nm and medium optical bandgap of 1.73 and 1.77 eV for PDTPa-TBTA and PDTPa-TffBTA, respectively. Polymer solar cells using PDTPa-TBTA as donor and [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) as an acceptor exhibited power conversion efficiencies (PCE) of 2.22% with a Voc of 0.58 V, a Jsc of 6.04 mA/cm2, and an FF of 63.41%. The introduction of fluorine substituents on the BTA unit evidently influenced the optical and photovoltaic properties. Interestingly, although the HOMO energy level indeed decreased, PDTPa-TffBTA showed a decreased Voc of 0.52 V in solar cells. Combined with an obviously enhanced Jsc of 10.23 mA/cm2, and an outstanding FF of 0.64, the PCE of solar cells based on PDTPa-TffBTA was improved by nearly 55%, reached 3.43%. Our results indicate that the BTA unit can be used to construct ABC polymers with a medium bandgap, and the introduction of fluorine on the BTA unit is also effective in improving the photovoltaic performance

    Ring Fusion of Thiophene–Vinylene–Thiophene (TVT) Benefits Both Fullerene and Non-Fullerene Polymer Solar Cells

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    Conjugated polymers based on thiophene–vinylene–thiophene (TVT) and ethenylene fused TVT (ETVT) combined with alkylated dithienyl­benzothiadiazole (DTBT) were designed and synthesized to investigate the effect of ring fusion on the properties of TVT based photovoltaic polymers. It is found that ring fusion of the TVT segment significantly affects molecular architecture and optoelectronic properties of the polymer. Ring fusion can downshift the HOMO energy level and increase the absorption coefficient of the corresponding polymer. Combining with reduced energy loss, PETVTTBT shows superior photovoltaic performance to PTVTTBT, in both fullerene and non-fullerene polymer solar cells. Particularly, in ITIC based polymer solar cells, simultaneous enhancement in the <i>J</i><sub>SC</sub>, <i>V</i><sub>OC</sub>, and FF is demonstrated after ring fusion. As a result, PCE of PETVTTBT based solar cells increases drastically by 120% over that of PTVTTBT (3.69%), reaching 8.18%

    Efficient all-polymer solar cells based on blend of tris(thienylenevinylene)-substituted polythiophene and poly[perylene diimide-alt-bis(dithienothiophene)]

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    © 2008 American Institute of Physics. The electronic version of this article is the complete one and can be found at: http://dx.doi.org/10.1063/1.2975160DOI: 10.1063/1.2975160A narrow band-gap alternating copolymer of perylene diimide and bis(dithienothiophene) (2) and a polythiophene derivative substituted by a tris(thienylenevinylene) conjugated side chain (4) are used as acceptor and donor, respectively, in all-polymer solar cells (SCs). The optimized device based on the blend of 4 and 2 in the ratio 3:1 (w/w) gives a short circuit current (Jsc) of 5.02 mA cm⁻²and a power conversion efficiency of 1.48%, under simulated AM 1.5 illumination at 100 mW cm⁻¹. These values are among the highest values reported for all-polymer SC
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