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A metal-free photoactive nitrogen-doped carbon nanosolenoid with broad absorption in visible region for efficient photocatalysis.

ABSTRACT: Riemann surfaces inspired chemists to design and synthesize such multidimensional curved carbon architectures. It has been predicted that carbon nanosolenoid materials with Riemann surfaces have unique structures and novel physical properties. Here we report the first synthesis of a nitrogen-doped carbon nanosolenoid (N-CNS) using bottom-up approach with a well-defined structure. N-CNS was obtained by a rational Suzuki polymerization, followed by oxidative cyclodehydrogenation. The successful synthesis of N-CNS was fully characterized by GPC, FTIR, solid-state ¹³C NMR and Raman techniques. The intrinsic single-strand molecular structures of N-CNS helices can be clearly resolved using low-dose integrated differential phase contrast scanning transmission electron microscopy (iDPC-STEM) technique. Possessing unique structural and physical properties, this long π-extended polymer N-CNS can provide new insight towards bottom-up syntheses of curved nanoribbons and potential applications as a metal-free photocatalyst for visible-light-driven H₂ evolution and highly efficient photocatalyst for photoredox organic transformations.

SUBMITTER: Zhou Y

PROVIDER: S-EPMC10511729 | biostudies-literature | 2023 Sep

REPOSITORIES: biostudies-literature

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A metal-free photoactive nitrogen-doped carbon nanosolenoid with broad absorption in visible region for efficient photocatalysis.

Zhou Yu Y Zhang Xinyu X Sheng Guan G Wang Shengda S Chen Muqing M Zhuang Guilin G Zhu Yihan Y Du Pingwu P

Nature communications 20230920 1

Riemann surfaces inspired chemists to design and synthesize such multidimensional curved carbon architectures. It has been predicted that carbon nanosolenoid materials with Riemann surfaces have unique structures and novel physical properties. Here we report the first synthesis of a nitrogen-doped carbon nanosolenoid (N-CNS) using bottom-up approach with a well-defined structure. N-CNS was obtained by a rational Suzuki polymerization, followed by oxidative cyclodehydrogenation. The successful sy ...[more]

PMID: 37730724

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Project description:The utilization of earth-abundant photosensitizers with visible light absorption to enable sustainable photocatalysis is a long-standing challenge. Overcoming such a challenge, in this work, two lanthanide (Ln3+ = Tb, Eu) based metal-organic frameworks (Ln-MOFs) have been synthesized utilizing a Co3+-based metalloligand. Both Ln-MOFs function as remarkable photocatalysts for the selective oxidation of assorted alcohols and sulfides to their corresponding aldehydes/ketones and sulfoxides using visible light. The photophysical behavior of both Ln-MOFs and mechanism of photocatalysis is comprehensively investigated using time-resolved transient absorption spectroscopy, electrochemical impedance spectroscopy, electron paramagnetic resonance spectroscopy, photoluminescence and phosphorescence studies. In both Ln-MOFs, a metalloligand acts as a light-harvester, being excited by visible light, while Ln3+ ions endow the resulting MOFs with long-lived triplet excited states. Ultrafast transient absorption spectroscopy, further supported by electron paramagnetic resonance spectra, revealed excited-state electron transfer from metalloligands to the Ln3+ ions and transient generation of Ln2+ sites alongside the facilitation of intersystem crossing. The excited Ln2+ ions transfer energy to the ground-state triplet oxygen (3O2) to generate singlet oxygen (1O2). The HOMO-LUMO positions of both Ln-MOFs support the generation of ˙O2 - and 1O2 but inhibit strongly-oxidizing yet non-selective ˙OH radicals. Scavenger experiments, 1O2 traps and electron paramagnetic resonance spectra confirmed the generation of singlet oxygen. The heavy-metal effect of a lanthanide ion in Ln-MOFs for the generation of triplet excitons is confirmed by the synthesis of a non-heavy-metal analogue involving a zinc ion via a single-crystal-to-single-crystal transformation strategy. The present results are noteworthy and may aid in the development of other earth-abundant metalloligand-based photocatalysts for challenging yet sustainable catalysis.

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A metal-free photoactive nitrogen-doped carbon nanosolenoid with broad absorption in visible region for efficient photocatalysis.

Publications

A metal-free photoactive nitrogen-doped carbon nanosolenoid with broad absorption in visible region for efficient photocatalysis.

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