P and Cu Dual Sites on Graphitic Carbon Nitride for Photocatalytic CO₂ Reduction to Hydrocarbon Fuels with High C₂H₆ Evolution

Abstract

The light-driven CO 2 reduction to multicarbon products is especially meaningful, while the low efficiency of multi-electron transfer and sluggish CÀ C coupling greatly hinder its development. Herein, we report a photocatalyst comprising of P and Cu dual sites anchored on graphitic carbon nitride (P/Cu SAs@CN), which achieves a high C 2 H 6 evolution rate of 616.6 μmol g À 1 h À 1 in reducing CO 2 to hydrocarbons. The detailed spectroscopic characterizations identify the formation of charge-enriched Cu sites, where the isolated P atoms serve as hole capture sites during photocatalysis. Theoretical simulations combined with in situ FTIR measurement reveal a kinetically feasible process for the formation of CÀ C coupling intermediate (*OCÀ COH) and confirm the favorable production of C 2 H 6 on the P/Cu SAs@CN photocatalyst. This work offers new insights into the photocatalyst design with atomic precision toward highly efficient photocatalytic CO 2 conversion to high value-added carbon products.

Hydroxyl-Bonded Ru on Metallic TiN Surface Catalyzing CO2 Reduction with H2O by Infrared Light

“…Importantly, a variety of works have further exposed that the coordination structure of single atoms modulates the activity and selectivity of CO 2 photoreduction substantially. , For example, by tailoring the coordinating groups (e.g., hydroxyl) of the catalytic-active centers, the activation configuration and degree of CO 2 molecules can be tuned, which ultimately boosts the reaction efficiency significantly. , From the viewpoint of strengthening CO 2 activation, great opportunities have recently been shown by the Lewis pairs structures . Specifically, owing to the strong hybridization of Lewis acid and base sites with the bonding and antibonding orbitals of adsorbed CO 2 molecules, efficient CO 2 polarization is readily realized on the catalyst surface, thus facilitating CO 2 activation with reduced energy …”

“…Importantly, a variety of works have further exposed that the coordination structure of single atoms modulates the activity and selectivity of CO 2 photoreduction substantially. 14,15 For example, by tailoring the coordinating groups (e.g., hydroxyl) of the catalytic-active centers, the activation configuration and degree of CO 2 molecules can be tuned, which ultimately boosts the reaction efficiency significantly. 16,17 From the viewpoint of strengthening CO 2 activation, great opportunities have recently been shown by the Lewis pairs structures.…”

Boosting ORR Activity in π-Rich Carbon-Supported Sub-3 nm Pt-Based Intermetallic Electrocatalysts via d–π Interaction

“…NPPC shows π* characteristic peaks at 398.6 eV (pyridinic N), 401.7 eV (pyrrole N), 402.5 eV (graphite N), and 403.3 eV (pyridinic N–O) and σ* resonance (σ* C–N) at 406.9 eV. The pyridinic N characteristic peak of PtCo/NPPC-800 is observed to shift negatively after the loading of PtCo NPs, indicating that more electrons flow to N, which may be due to the formation of a new Pt–N bonding state, and the results are consistent with XPS. The introduction of pyridinic N can further promote the electron transfer from C and Pt atoms to N atoms, thus making the Pt d-orbitals emptier and further enhancing the d–π hybridization effect.…”

Weak Light H2O2 Photosynthesis from H2O and O2 by Carbon Nitrides with Piezoelectric Effect for Tumor Therapy

“…3c) and by Coumarin oxidation method to quantify the free intermediate via variation absorbance spectra (Fig. 3d) 24,77 .…”

“…Artificial photocatalysis offers a potential way to drive chemical conversions under very mild conditions [21][22][23][24][25] . Recently, engineering polymeric carbon nitride (pCN)-based photocatalysts has become a promising strategy for overall H2O2 production by using water and oxygen as raw materials without any sacrificial agents [26][27][28][29] .…”