Metal–Organic Framework-Based Efficient Singlet Heterogeneous Photoredox Catalyst for Aerobic C–H Functionalization DOI
Sreehari Surendran Rajasree, Bapan Saha, Gordon Kelly

и другие.

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 3515 - 3524

Опубликована: Фев. 12, 2025

Effective light harvesting is critical in bioinspired heterogeneous photocatalysts to transport the absorbed energy, compensating for diffusion-limited surface-only activity that commonly achieved solid systems constructed by simply anchoring a well-established photosensitizer (PS). While 3PS* has been widely exploited their persistence, 1PS* defines fresh paradigm artificial photosystems specifically aerobic photoredox processes where 1O2*-mediated oxidative path must be avoided. Endowed with large chemically accessible surface area hosting ultrafast anisotropic singlet exciton transportation, three mesoporous Zr-MOFs, PCN-222(H2), NU-1000, and SIU-100, displayed superior catalytic activities (t0.5 ∼3 h TOF of 106 h–1 at t0.5) toward aza-Henry reaction N-aryl-tetrahydroquinone compared common benchmarks. Furthermore, higher excited state redox potentials, 1MOF* can flexible initial photoproduct [amine•+ O2•–] formation through an or reductive quenching pathway expanding scope amine substrates. slow H-atom transfer process dark step entails moderate apparent quantum yield ∼20%, discernible rate difference was established defined driving force photoinduced electron processes, which, turn, are regulated electronic properties MOF relative Nevertheless, it property dictates product identity distribution. With detailed mechanistic studies wider substrate scopes, this study underscores advantageous platform developing effective1MOF*-based catalysts.

Язык: Английский

Al-N co-doped to reduce Ti3+ concentration to suppress charge recombination of polyhedral SrTiO3 for efficient photocatalytic CO2 reduction DOI

Wenjie Wang,

Wenxiang Kang,

Jiahao Niu

и другие.

Journal of Colloid and Interface Science, Год журнала: 2025, Номер 689, С. 137266 - 137266

Опубликована: Март 8, 2025

Язык: Английский

Процитировано

1
Metal–Organic Framework-Based Efficient Singlet Heterogeneous Photoredox Catalyst for Aerobic C–H Functionalization DOI
Sreehari Surendran Rajasree, Bapan Saha, Gordon Kelly

и другие.

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 3515 - 3524

Опубликована: Фев. 12, 2025

Effective light harvesting is critical in bioinspired heterogeneous photocatalysts to transport the absorbed energy, compensating for diffusion-limited surface-only activity that commonly achieved solid systems constructed by simply anchoring a well-established photosensitizer (PS). While 3PS* has been widely exploited their persistence, 1PS* defines fresh paradigm artificial photosystems specifically aerobic photoredox processes where 1O2*-mediated oxidative path must be avoided. Endowed with large chemically accessible surface area hosting ultrafast anisotropic singlet exciton transportation, three mesoporous Zr-MOFs, PCN-222(H2), NU-1000, and SIU-100, displayed superior catalytic activities (t0.5 ∼3 h TOF of 106 h–1 at t0.5) toward aza-Henry reaction N-aryl-tetrahydroquinone compared common benchmarks. Furthermore, higher excited state redox potentials, 1MOF* can flexible initial photoproduct [amine•+ O2•–] formation through an or reductive quenching pathway expanding scope amine substrates. slow H-atom transfer process dark step entails moderate apparent quantum yield ∼20%, discernible rate difference was established defined driving force photoinduced electron processes, which, turn, are regulated electronic properties MOF relative Nevertheless, it property dictates product identity distribution. With detailed mechanistic studies wider substrate scopes, this study underscores advantageous platform developing effective1MOF*-based catalysts.

Язык: Английский

Процитировано

0