Transfer Hydrogenation with a Carbon‐Nitride‐Supported Palladium Single‐Atom Photocatalyst and Water as a Proton Source

Zhao, En; Li, Manman; Xu, Bo; Wang, Xuelu; Jing, Yu; Ma, Ding; Mitchell, Sharon; Pérez‐Ramírez, Javier; Chen, Zupeng

doi:10.1002/ange.202207410

Cited by 6 publications

(2 citation statements)

References 36 publications

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“…In addition, g-C 3 N 4 is considered to have favorable application prospects due to its structural stability and low economic cost. Based on these advantages, g–C 3 N 4 –based SACs have been widely studied and remained a research hotspot over the past two years [ [30] , [31] , [32] , [33] ]. Moreover, it is also considered a favorable photocatalyst with good visible light response and suitable band gap, making it effective in photocatalysis [ 34 , 35 ].…”

Section: Introductionmentioning

confidence: 99%

Understanding the role of transition metal single-atom electronic structure in oxysulfur radical-mediated oxidative degradation

Zhao,

Ding,

Ren

et al. 2024

Environmental Science and Ecotechnology

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Section: Introductionmentioning

confidence: 99%

Understanding the role of transition metal single-atom electronic structure in oxysulfur radical-mediated oxidative degradation

Zhao,

Ding,

Ren

et al. 2024

Environmental Science and Ecotechnology

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“…Therefore, both experiments and theoretical calculations have shown that graphene-derived carbon compounds offer excellent promise as substrates for SACs. Graphene may be converted from a passive catalyst into one with excellent catalytic efficiency and selectivity by the insertion of metal single atoms (SAs) for CO2 reduction [46,47], activation of the C−H bond, selective hydrogenation [48], conversion of N2 (including electrochemical nitrogen reduction reaction (NRR)) [49], CO2 photocatalytic reduction reaction [50], and photocatalytic hydrogen evolution [51].…”

Section: Introductionmentioning

confidence: 99%

Recent Advances in Graphene-Based Single-Atom Photocatalysts for CO2 Reduction and H2 Production

Akram,

Ashraf,

Jagirani

et al. 2024

Catalysts

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The extensive use of single-atom catalysts (SACs) has appeared as a significant area of investigation in contemporary study. The single-atom catalyst, characterized by its maximum atomic proficiency and great discernment of the transition-metal center, has a unique combination of benefits from both heterogeneous and homogeneous catalysts. Consequently, it effectively bridges the gap between these two types of catalysts, leveraging their distinctive features. The utilization of SACs immobilized on graphene substrates has garnered considerable interest, primarily because of their capacity to facilitate selective and efficient photocatalytic processes. This review aims to comprehensively summarize the progress and potential uses of SACs made from graphene in photocatalytic carbon dioxide (CO2) reduction and hydrogen (H2) generation. The focus is on their contribution to converting solar energy into chemical energy. The present study represents the various preparation methods and characterization approaches of graphene-based single-atom photocatalyst This review investigates the detailed mechanisms underlying these photocatalytic processes and discusses recent studies that have demonstrated remarkable H2 production rates through various graphene-based single-atom photocatalysts. Additionally, the pivotal roleof theoretical simulations, likedensity functional theory (DFT), to understand the structural functional relationships of these SACs are discussed. The potential of graphene-based SACs to revolutionize solar-to-chemical energy conversion through photocatalytic CO2 reduction and H2 production is underscored, along with addressing challenges and outlining future directions for this developing area of study. By shedding light on the progress and potential of these catalysts, this review contributes to the collective pursuit of sustainable and efficient energy conversion strategies to mitigate the global climate crisis.

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Single‐Atom Nickel on Carbon Nitride Photocatalyst Achieves Semihydrogenation of Alkynes with Water Protons via Monovalent Nickel

et al. 2023

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Prospects in light‐driven water activation have prompted rapid progress in hydrogenation reactions. We describe a Ni2+−N4 site built on carbon nitride for catalyzed semihydrogenation of alkynes, with water supplying protons, powered by visible‐light irradiation. Importantly, the photocatalytic approach developed here enabled access to diverse deuterated alkenes in D2O with excellent deuterium incorporation. Under visible‐light irradiation, evolution of a four‐coordinate Ni2+ species into a three‐coordinate Ni+ species was spectroscopically identified. In combination with theoretical calculations, the photo‐evolved Ni+ is posited as HO−Ni+−N2 with an uncoordinated, protonated pyridinic nitrogen, formed by coupled Ni2+ reduction and water dissociation. The paired Ni−N prompts hydrogen liberation from water, and it renders desorption of alkene preferred over further hydrogenation to alkane, ensuring excellent semihydrogenation selectivity.

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Transfer Hydrogenation with a Carbon‐Nitride‐Supported Palladium Single‐Atom Photocatalyst and Water as a Proton Source

Abstract: Dedicated to Professor Matthias Beller on the occasion of his 60th birthday.

Cited by 6 publications

References 36 publications

Understanding the role of transition metal single-atom electronic structure in oxysulfur radical-mediated oxidative degradation

Understanding the role of transition metal single-atom electronic structure in oxysulfur radical-mediated oxidative degradation

Recent Advances in Graphene-Based Single-Atom Photocatalysts for CO2 Reduction and H2 Production

Single‐Atom Nickel on Carbon Nitride Photocatalyst Achieves Semihydrogenation of Alkynes with Water Protons via Monovalent Nickel

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