5 research outputs found

    Formation of Hierarchical Structure Composed of (Co/Ni)Mn-LDH Nanosheets on MWCNT Backbones for Efficient Electrocatalytic Water Oxidation

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    Active, stable, and cost-effective electrocatalysts are attractive alternatives to the noble metal oxides that have been used in water splitting. The direct nucleation and growth of electrochemically active LDH materials on chemically modified MWCNTs exhibit considerable electrocatalytic activity toward oxygen evolution from water oxidation. CoMn-based and NiMn-based hybrids were synthesized using a facile chemical bath deposition method and the as-synthesized materials exhibited three-dimensional hierarchical configurations with tunable Co/Mn and Ni/Mn ratio. Benefiting from enhanced electrical conductivity with MWCNT backbones and LDH lamellar structure, the Co<sub>5</sub>Mn-LDH/MWCNT and Ni<sub>5</sub>Mn-LDH/MWCNT could generated a current density of 10 mA cm<sup>–2</sup> at overpotentials of ∼300 and ∼350 mV, respectively, in 1 M KOH. In addition, the materials also exhibited outstanding long-term electrocatalytic stability

    Highly Functional Bioinspired Fe/N/C Oxygen Reduction Reaction Catalysts: Structure-Regulating Oxygen Sorption

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    Tuna is one of the most rapid and distant swimmers. Its unique gill structure with the porous lamellae promotes fast oxygen exchange that guarantees tuna’s high metabolic and athletic demands. Inspired by this specific structure, we designed and fabricated microporous graphene nanoplatelets (GNPs)-based Fe/N/C electrocatalysts for oxygen reduction reaction (ORR). Careful control of GNP structure leads to the increment of microporosity, which influences the O<sub>2</sub> adsorption positively and desorption oppositely, resulting in enhanced O<sub>2</sub> diffusion, while experiencing reduced ORR kinetics. Working in the cathode of proton-exchange membrane fuel cells, the GNP catalysts require a compromise between adsorption/desorption for effective O<sub>2</sub> exchange, and as a result, appropriate microporosity is needed. In this work, the highest power density, 521 mW·cm<sup>–2</sup>, at zero back pressure is achieved

    Unraveling the Transformation from Type-II to Z‑Scheme in Perovskite-Based Heterostructures for Enhanced Photocatalytic CO<sub>2</sub> Reduction

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    The ability to create perovskite-based heterostructures with desirable charge transfer characteristics represents an important endeavor to render a set of perovskite materials and devices with tunable optoelectronic properties. However, due to similar material selection and band alignment in type-II and Z-scheme heterostructures, it remains challenging to obtain perovskite-based heterostructures with a favorable electron transfer pathway for photocatalysis. Herein, we report a robust tailoring of effective charge transfer pathway in perovskite-based heterostructures via a type-II to Z-scheme transformation for highly efficient and selective photocatalytic CO2 reduction. Specifically, CsPbBr3/TiO2 and CsPbBr3/Au/TiO2 heterostructures are synthesized and then investigated by ultrafast spectroscopy. Moreover, taking CsPbBr3/TiO2 and CsPbBr3/Au/TiO2 as examples, operando experiments and theoretical calculations confirm that the type-II heterostructure could be readily transformed into a Z-scheme heterostructure through establishing a low-resistance Ohmic contact, which indicates that a fast electron transfer pathway is crucial in Z-scheme construction, as further demonstrated by CsPbBr3/Ag/TiO2 and CsPbBr3/MoS2 heterostructures. In contrast to pristine CsPbBr3 and CsPbBr3/TiO2, the CsPbBr3/Au/TiO2 heterostructure exhibits 5.4- and 3.0-fold enhancement of electron consumption rate in photocatalytic CO2 reduction. DFT calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy unveil that the superior CO selectivity is attributed to the lower energy of *CO desorption than that of hydrogenation to *HCO. This meticulous design sheds light on the modification of perovskite-based multifunctional materials and enlightens conscious optimization of semiconductor-based heterostructures with desirable charge transfer for catalysis and optoelectronic applications

    <i>In Situ</i> Fabrication of Highly Conductive Metal Nanowire Networks with High Transmittance from Deep-Ultraviolet to Near-Infrared

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    We have developed a facile and compatible method to <i>in situ</i> fabricate uniform metal nanowire networks on substrates. The as-fabricated metal nanowire networks show low sheet resistance and high transmittance (2.2 Ω sq<sup>–1</sup> at <i>T</i> = 91.1%), which is equivalent to that of the state-of-the-art metal nanowire networks. We demonstrated that the transmittance of the metal networks becomes homogeneous from deep-ultraviolet (200 nm) to near-infrared (2000 nm) when the size of the wire spacing increases to micrometer size. Theoretical and experimental analyses indicated that we can improve the conductivity of the metal networks as well as keep their transmittance by increasing the thickness of the metal films. We also carried out durability tests to demonstrate our as-fabricated metal networks having good flexibility and strong adhesion

    Lead Selenide Colloidal Quantum Dot Solar Cells Achieving High Open-Circuit Voltage with One-Step Deposition Strategy

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    Lead selenide (PbSe) colloidal quantum dots (CQDs) are considered to be a strong candidate for high-efficiency colloidal quantum dot solar cells (CQDSCs) due to its efficient multiple exciton generation. However, currently, even the best PbSe CQDSCs can only display open-circuit voltage (<i>V</i><sub>oc</sub>) about 0.530 V. Here, we introduce a solution-phase ligand exchange method to prepare PbI<sub>2</sub>-capped PbSe (PbSe-PbI<sub>2</sub>) CQD inks, and for the first time, the absorber layer of PbSe CQDSCs was deposited in one step by using this PbSe-PbI<sub>2</sub> CQD inks. One-step-deposited PbSe CQDs absorber layer exhibits fast charge transfer rate, reduced energy funneling, and low trap assisted recombination. The champion large-area (active area is 0.35 cm<sup>2</sup>) PbSe CQDSCs fabricated with one-step PbSe CQDs achieve a power conversion efficiency (PCE) of 6.0% and a <i>V</i><sub>oc</sub> of 0.616 V, which is the highest <i>V</i><sub>oc</sub> among PbSe CQDSCs reported to date
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