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Photocatalysts based on single atoms (SAs) modification can lead to unprecedented reactivity with recent advances. However, the deactivation of SAs‐modified photocatalysts remains a critical challenge in the field of photocatalytic CO2 reduction. In this study, we unveil the detrimental effect of CO intermediates on Cu single atoms (Cu‐SAs) during photocatalytic CO2 reduction, leading to clustering and deactivation on TiO2. To address this, we developed a novel Cu‐SAs anchored on Au porous nanoparticles (CuAu‐SAPNPs‐TiO2) via a vectored etching approach. This system not only enhances CH4 production with a rate of 748.8 μmol ⋅ g−1 ⋅ h−1 and 93.1 % selectivity but also mitigates Cu‐SAs clustering, maintaining stability over 7 days. This sustained high performance, despite the exceptionally high efficiency and selectivity in CH4 production, highlights the CuAu‐SAPNPs‐TiO2 overarching superior photocatalytic properties. Consequently, this work underscores the potential of tailored SAs‐based systems for efficient and durable CO2 reduction by reshaping surface adsorption dynamics and optimizing the thermodynamic behavior of the SAs. [ABSTRACT FROM AUTHOR]

Photocatalysts based on single atoms (SAs) modification can lead to unprecedented reactivity with recent advances. However, the deactivation of SAs‐modified photocatalysts remains a critical challenge in the field of photocatalytic CO2 reduction. In this study, we unveil the detrimental effect of CO intermediates on Cu single atoms (Cu‐SAs) during photocatalytic CO2 reduction, leading to clustering and deactivation on TiO2. To address this, we developed a novel Cu‐SAs anchored on Au porous nanoparticles (CuAu‐SAPNPs‐TiO2) via a vectored etching approach. This system not only enhances CH4 production with a rate of 748.8 μmol ⋅ g−1 ⋅ h−1 and 93.1 % selectivity but also mitigates Cu‐SAs clustering, maintaining stability over 7 days. This sustained high performance, despite the exceptionally high efficiency and selectivity in CH4 production, highlights the CuAu‐SAPNPs‐TiO2 overarching superior photocatalytic properties. Consequently, this work underscores the potential of tailored SAs‐based systems for efficient and durable CO2 reduction by reshaping surface adsorption dynamics and optimizing the thermodynamic behavior of the SAs. [ABSTRACT FROM AUTHOR]

The polyoxometalate compound [CuPTCP(H2O)2.5]2[SiW12O40] ·10.5H2O ( 1) was synthesized under hydrothermal conditions using 2-phenyl-1H-1,3,7,8-tetraazacyclopenta[l]phenanthrene (PTCP) and Keggin-type silicotungstic acid (H4SiW12O4) as neutral ligands. Compound 1 was characterized by single-crystal X-ray diffraction, elemental analysis, as well as IR and UV/Vis spectroscopy. It crystallizes in the orthorhombic space group Cmcm with a = 15.490(8) nm, b = 25.263(8) nm, c = 20.988(8) nm, α = 90°, β = 90°, γ = 90°, V = 8213(6) nm3, Z = 2. Compared with the ligand PTCP, the fluorescent spectra of compound 1 are different. Furthermore, the Rhodamine B (RhB) photodegration process by compound 1 as catalyst was studied. It could be shown that the DR% of compound 1 is more than twice that of pure silicotungstic acid. [ABSTRACT FROM AUTHOR]

Photocatalysts based on single atoms (SAs) modification can lead to unprecedented reactivity with recent advances. However, the deactivation of SAs‐modified photocatalysts remains a critical challenge in the field of photocatalytic CO2 reduction. In this study, we unveil the detrimental effect of CO intermediates on Cu single atoms (Cu‐SAs) during photocatalytic CO2 reduction, leading to clustering and deactivation on TiO2. To address this, we developed a novel Cu‐SAs anchored on Au porous nanoparticles (CuAu‐SAPNPs‐TiO2) via a vectored etching approach. This system not only enhances CH4 production with a rate of 748.8 μmol ⋅ g−1 ⋅ h−1 and 93.1 % selectivity but also mitigates Cu‐SAs clustering, maintaining stability over 7 days. This sustained high performance, despite the exceptionally high efficiency and selectivity in CH4 production, highlights the CuAu‐SAPNPs‐TiO2 overarching superior photocatalytic properties. Consequently, this work underscores the potential of tailored SAs‐based systems for efficient and durable CO2 reduction by reshaping surface adsorption dynamics and optimizing the thermodynamic behavior of the SAs. [ABSTRACT FROM AUTHOR]

Photocatalysts based on single atoms (SAs) modification can lead to unprecedented reactivity with recent advances. However, the deactivation of SAs‐modified photocatalysts remains a critical challenge in the field of photocatalytic CO2 reduction. In this study, we unveil the detrimental effect of CO intermediates on Cu single atoms (Cu‐SAs) during photocatalytic CO2 reduction, leading to clustering and deactivation on TiO2. To address this, we developed a novel Cu‐SAs anchored on Au porous nanoparticles (CuAu‐SAPNPs‐TiO2) via a vectored etching approach. This system not only enhances CH4 production with a rate of 748.8 μmol ⋅ g−1 ⋅ h−1 and 93.1 % selectivity but also mitigates Cu‐SAs clustering, maintaining stability over 7 days. This sustained high performance, despite the exceptionally high efficiency and selectivity in CH4 production, highlights the CuAu‐SAPNPs‐TiO2 overarching superior photocatalytic properties. Consequently, this work underscores the potential of tailored SAs‐based systems for efficient and durable CO2 reduction by reshaping surface adsorption dynamics and optimizing the thermodynamic behavior of the SAs. [ABSTRACT FROM AUTHOR]

Graphite-like carbon nitride (g-C 3 N 4) has been regarded as a promising photocatalyst for solar-to-chemical conversion. Nevertheless, the narrow absorption of light extremely limited its photocatalytic performance under near-infrared (NIR) irradiation. Herein, the Cu 7. 2 S 4 with outstanding NIR absorption was successfully introduced to g-C 3 N 4 nanosheets through a simple in-situ growth procedure. As expected, the constructed Cu 7.2 S 4 /g-C 3 N 4 (CSCN) photocatalysts exhibit superior H 2 production activity of 82 μmol g−1 h−1 under NIR light irradiation (λ > 800 nm), which outperforms currently reported g–C 3 N 4 –based NIR-driven H 2 production systems. Especially, the optimal sample CSCN-5 displays a robust activity of 66 μmol g−1 h−1 at λ = 850 nm monochromatic light irradiation. The excellent photocatalytic performance is linked to the extended optical absorption as well as the efficient separation efficiency of photoinduced carriers, which are evidenced by the UV-visible absorption spectroscopy and photoelectrochemical test. This work provides an effective approach for constructing a Cu 7.2 S 4 /g-C 3 N 4 photocatalytic system for the transformation of NIR solar energy into hydrogen. The novel NIR-driven Cu 7. 2 S 4 /g-C 3 N 4 composite photocatalyst was constructed through a convenient in situ growth process. As expected, the outstanding photocatalytic H 2 yield was 82 μmol g−1 h−1 under the irradiation of NIR light (λ > 800 nm), which outperforms currently reported g–C 3 N 4 –based NIR-driven H 2 production systems. More significantly, the sample CSCN-5 shows an optimum activity (66 μmol g−1 h−1) under λ = 850 nm monochromatic light irradiation. This work provides a feasible approach for achieving g–C 3 N 4 –based photocatalyst NIR-induced superior solar-to-chemical conversion. [Display omitted] • Cu 7·2 S 4 modified g-C 3 N 4 is prepared by a facile hydrothermal treatment method. • The Cu 7·2 S 4 /g-C 3 N 4 composites show a superior optical adsorption from visible to NIR. • The Cu 7·2 S 4 /g–C 3 N 4 –5 composite exhibits excellent HER of 82 μmol g−1 h−1 (λ > 800 nm). • The HER of Cu 7·2 S 4 /g–C 3 N 4 –5 shows no obvious change after 4 runs within 20 h. [ABSTRACT FROM AUTHOR]