Hexanuclear ring cobalt complex for photochemical CO2 to CO conversion

Meng, Xiangyu; Li, Rui; Yang, Jilin; Xu, Shiming; Zhang, Chenchen; You, Kejia; Ma, Baochun; Guan, Hongxia; Ding, Yong

doi:10.1016/s1872-2067(22)64144-5

Cited by 14 publications

(15 citation statements)

References 54 publications

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“…These spectral features were then used to plot the actual or reconstructed XANES (Figure S18) and EXAFS (Figures 2 and S19) spectra of the excited states. The reconstructed 3 MLCT states of all Cu(I) PSs exhibit a pre-edge transition at 8979 eV and two 1s to 4p rising edge transitions at 8984 and 8992 eV (Figure S19), in good agreement for 4-fold coordinated Cu(II) ions. 55 This analysis thus confirms the correct percentages of excited state fractions used in the estimation of the laser on spectra of the Cu-based photosensitizers described here.…”

Section: Syntheses and Photophysics Of Cu(i) Pssmentioning

confidence: 63%

Precious-Metal-Free CO₂ Photoreduction Boosted by Dynamic Coordinative Interaction between Pyridine-Tethered Cu(I) Sensitizers and a Co(II) Catalyst

Wang

Zhang

Velasco

et al. 2023

JACS Au

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Improving the photocatalytic efficiency of a fully noble-metal-free system for CO2 reduction remains a fundamental challenge, which can be accomplished by facilitating electron delivery as a consequence of exploiting intermolecular interactions. Herein, we have designed two Cu(I) photosensitizers with different pyridyl pendants at the phenanthroline moiety to enable dynamic coordinative interactions between the sensitizers and a cobalt macrocyclic catalyst. Compared to the parent Cu(I) photosensitizer, one of the pyridine-tethered derivatives boosts the apparent quantum yield up to 76 ± 6% at 425 nm for selective (near 99%) CO2-to-CO conversion. This value is nearly twice that of the parent system with no pyridyl pendants (40 ± 5%) and substantially surpasses the record (57%) of the noble-metal-free systems reported so far. This system also realizes a maximum turnover number of 11 800 ± 1400. In contrast, another Cu(I) photosensitizer, in which the pyridine substituents are directly linked to the phenanthroline moiety, is inactive. The above behavior and photocatalytic mechanism are systematically elucidated by transient fluorescence, transient absorption, transient X-ray absorption spectroscopies, and quantum chemical calculations. This work highlights the advantage of constructing coordinative interactions to fine-tune the electron transfer processes within noble-metal-free systems for CO2 photoreduction.

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Section: Syntheses and Photophysics Of Cu(i) Pssmentioning

confidence: 63%

Precious-Metal-Free CO₂ Photoreduction Boosted by Dynamic Coordinative Interaction between Pyridine-Tethered Cu(I) Sensitizers and a Co(II) Catalyst

Wang

Zhang

Velasco

et al. 2023

JACS Au

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“…The signicant improvement in the hydrogen evolution activity can be attributed to the effective electron transfer between CdS and TTI-COF. [40][41][42][43] However, a further increase in CdS content in CdS@TTI-COF led to a marked decrease in the photocatalytic H 2 evolution yield. Therefore, with increasing CdS content, the activity of CdS@TTI-COF showed a volcanic trend, which may be attributed to the relative content of CdS and TTI-COF.…”

Section: Structure and Morphology Studiesmentioning

confidence: 99%

Growing COFs in situ on CdS nanorods as core–shell heterojunctions to improve the charge separation efficiency

Feng

et al. 2022

Sustainable Energy Fuels

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“…Ding and co-workers reported Prussian blue analogues (PBAs) for photocatalytic CO 2 reduction into CO with high selectivity . Various metal complexes, metal oxides, chalcogenides, and graphitic carbon nitrides were also examined for CO 2 reduction. − …”

Section: Introductionmentioning

confidence: 99%

Self-Templated Conversion of a Self-Healing Metallogel into an Active Carbon Quasiaerogel: Boosting Photocatalytic CO₂ Reduction by Water

Alam

Ojha

Kumar

et al. 2023

ACS Sustainable Chem. Eng.

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Healing and photosynthesis are two prime examples of intrinsic aptitude in the incredibly diverse plant kingdom. Inspired by nature, the development of new materials with the intrinsic ability of healing and artificial photosynthesis is of current interest. In this regard, herein, a new waterborne self-healing metallogel (Nd-SHMG) along with a self-templated carbonization strategy is presented for the synthesis of a neodymium@nitrogen-doped carbon quasiaerogel (Nd@NCA) catalyst. The stiffness of the metallogel (self-healing, self-sustaining, and molding behavior) can be controlled by tuning the synthetic conditions. A metal-free nitrogen-doped carbon quasiaerogel (MF@NCA) was also prepared via partial removal of the metal from the Nd@NCA catalyst. The as-synthesized Nd@NCA and MF@NCA catalysts were composed of highly porous 2D sheets which are grown on top of each other, adopting a 3D foam-type structure. The porosity (∼9 fold) and the CO2 adsorption capacity (∼8 fold) can be gradually increased ‘on demand’ by partial removal of the metal ion from the pristine Nd@NCA. The as-synthesized catalysts exhibit excellent photocatalytic activity for CO2 conversion into CO (∼17–24 μmol g–1) with over ∼87% selectivity without adding sacrificial agents. Isotopic carbon-labeled (13CO2) in situ diffuse reflectance infrared Fourier transform spectroscopy analysis was performed, and a plausible mechanism was outlined for photocatalytic CO2 reduction to CO. With this work, we introduce a facial and feasible strategy to prepare a Nd-SHMG and their conversion into active bifunctional carbon quasiaerogel-based catalysts, which can adsorb and convert CO2 selectively into CO without adding sacrificial agents in the presence of water and light.

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Hexanuclear ring cobalt complex for photochemical CO2 to CO conversion

Cited by 14 publications

References 54 publications

Precious-Metal-Free CO₂ Photoreduction Boosted by Dynamic Coordinative Interaction between Pyridine-Tethered Cu(I) Sensitizers and a Co(II) Catalyst

Precious-Metal-Free CO₂ Photoreduction Boosted by Dynamic Coordinative Interaction between Pyridine-Tethered Cu(I) Sensitizers and a Co(II) Catalyst

Growing COFs in situ on CdS nanorods as core–shell heterojunctions to improve the charge separation efficiency

Self-Templated Conversion of a Self-Healing Metallogel into an Active Carbon Quasiaerogel: Boosting Photocatalytic CO₂ Reduction by Water

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Hexanuclear ring cobalt complex for photochemical CO2 to CO conversion

Cited by 14 publications

References 54 publications

Precious-Metal-Free CO2 Photoreduction Boosted by Dynamic Coordinative Interaction between Pyridine-Tethered Cu(I) Sensitizers and a Co(II) Catalyst

Precious-Metal-Free CO2 Photoreduction Boosted by Dynamic Coordinative Interaction between Pyridine-Tethered Cu(I) Sensitizers and a Co(II) Catalyst

Growing COFs in situ on CdS nanorods as core–shell heterojunctions to improve the charge separation efficiency

Self-Templated Conversion of a Self-Healing Metallogel into an Active Carbon Quasiaerogel: Boosting Photocatalytic CO2 Reduction by Water

Contact Info

Product

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About

Precious-Metal-Free CO₂ Photoreduction Boosted by Dynamic Coordinative Interaction between Pyridine-Tethered Cu(I) Sensitizers and a Co(II) Catalyst

Precious-Metal-Free CO₂ Photoreduction Boosted by Dynamic Coordinative Interaction between Pyridine-Tethered Cu(I) Sensitizers and a Co(II) Catalyst

Self-Templated Conversion of a Self-Healing Metallogel into an Active Carbon Quasiaerogel: Boosting Photocatalytic CO₂ Reduction by Water