The co-assembly naphthalimide/perylene diimide (NDINH/PDINH) supramolecular photocatalysts were successfully synthesized via a rapid solution dispersion method. A giant internal electric field (IEF) in co-assembly str...
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The co-assembly naphthalimide/perylene diimide (NDINH/PDINH) supramolecular photocatalysts were successfully synthesized via a rapid solution dispersion method. A giant internal electric field (IEF) in co-assembly structure was built by the larger local dipole. NDINH coated on PDINH could reduce the reflected electric field over PDINH to improve its responsive activity to ultraviolet light. Resultantly, an efficient full-spectrum photocatalytic overall water splitting activity with H 2 and O 2 evolution rate of 317.2 and 154.8 μmol g −1 h −1 for NDINH/PDINH together with optimized O 2 evolution rate with 2.61 mmol g −1 h −1 using AgNO 3 as a sacrificial reagent were achieved. Meanwhile, its solar-to-hydrogen efficiency was enhanced to 0.13 %. The enhanced photocatalytic activity was primarily attributed to the IEF between NDINH and PDINH, significantly accelerating transfer and separation of photogenerated carriers. Additionally, a direct Z-Scheme pathway of carriers contributed to a high redox potential. The strategy provided a new perspective for the design of supramolecular photocatalysts.
Suffering from the susceptibility to decomposition, the potential electrochemical application of FeOCl has greatly been hindered. The rational design of the soft-hard material interface can effectively address the cha...
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Suffering from the susceptibility to decomposition, the potential electrochemical application of FeOCl has greatly been hindered. The rational design of the soft-hard material interface can effectively address the challenge of stress concentration and thus decomposition that may occur in the electrodes during charging and discharging. Herein, interlayer structure manipulation of FeOCl/MXene using soft-hard interface design method were conducted for electrochemical dechlorination. FeOCl was encapsulated in Ti 3 C 2 T x MXene nanosheets by electrostatic self-assembly layer by layer to form a soft-hard mechanical hierarchical structure, in which Ti 3 C 2 T x was used as flexible buffer layers to relieve the huge volume change of FeOCl during Cl − intercalation/deintercalation and constructed a conductive network for fast charge transfer. The CDI dechlorination system of FeOCl/Ti 3 C 2 T x delivered outstanding Cl − adsorption capacity (158.47 ± 6.98 mg g −1 ), rate (6.07 ± 0.35 mg g −1 min −1 ), and stability (over 94.49 % in 30 cycles), and achieved considerable energy recovery (21.14 ± 0.25 %). The superior dechlorination performance was proved to originate from the Fe 2+ /Fe 3+ topochemical transformation and the deformation constraint effect of Ti 3 C 2 T x on FeOCl. Our interfacial design strategy enables a hard-to-soft integration capacity, which can serve as a universal technology for solving the traditional problem of electrode volume expansion.
A one-stone, two-bird method to integrate the soft porosity and electrical properties of distinct metal–organic frameworks (MOFs) into a single material involves the design of conductive-on-insulating MOF ( c MOF-on-...
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A one-stone, two-bird method to integrate the soft porosity and electrical properties of distinct metal–organic frameworks (MOFs) into a single material involves the design of conductive-on-insulating MOF ( c MOF-on- i MOF) heterostructures that allow for direct electrical control. Herein, we report the synthesis of c MOF-on- i MOF heterostructures using a seeded layer-by-layer method, in which the sorptive i MOF core is combined with chemiresistive c MOF shells. The resulting c MOF-on- i MOF heterostructures exhibit enhanced selective sorption of CO 2 compared to the pristine i MOF (298 K, 1 bar, S from 15.4 of ZIF-7 to 43.2–152.8). This enhancement is attributed to the porous interface formed by the hybridization of both frameworks at the molecular level. Furthermore, owing to the flexible structure of the i MOF core, the c MOF-on- i MOF heterostructures with semiconductive soft porous interfaces demonstrated high flexibility in sensing and electrical “shape memory” toward acetone and CO 2 . This behavior was observed through the guest-induced structural changes of the i MOF core, as revealed by the operando synchrotron grazing incidence wide-angle X-ray scattering measurements.
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