Rational design, application and dynamic evolution of Cu–N–C single-atom catalysts

Hu, Yaning; Dou, Yong; Sun, Zhaolin; Li, Bing; Zhou, Hongyao; Wang, Shuo; Hu, Xuemin; He, Kebin; Qu, Ming; Chen, Zhuo; Yang, Wenxiu

doi:10.1039/d2ta06050g

Cited by 17 publications

(2 citation statements)

References 213 publications

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“…Isolated dispersion and uniformity of the copper species was confirmed by the absence of secondary Cu-Cu scatterings. The intensity of the Cu-N scattering in the EXAFS spectra increases incrementally from Cu1-N2 to Cu1-N3, and further to Cu1-N4 SACs, consistent with the gradual rise in the number of nitrogen coordination around the central Cu atom 42,43 . Wavelet transform (WT) analysis, as depicted in Fig.…”

Section: Electronic and Coordination Structure Of Cu Based Sacssupporting

confidence: 57%

Low-coordinate Cu1–N2 sites in single-atom catalyst for highly efficient propylene epoxidation with molecular oxygen

Fu,

Qiu,

Zhang

et al. 2024

Preprint

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Due to its sustainability, direct epoxidation of propylene into propylene oxide (PO) with molecular oxygen alone is believed to be an ideal route. Despite constant research efforts, numerous catalysts struggle with the trade-off between activity and selectivity, which typically results in poor PO yield. In this contribution, we presented an atomically distributed Cu catalyst that had precisely controlled Cu–N coordination numbers of 1:2, termed as Cu1–N2 SAC. In contrast to traditional Cu-based oxide catalysts, this catalyst features exclusive Cu–N coordination, replacing all Cu–O interactions. The synthesized Cu1–N2 SAC catalyst acquired an unprecedented PO formation rate of 5.9 mmolPO gcat–1 h–1 at 275 °C, outperforming any other catalysts reported so far. Sophisticated characterizations and density functional theory calculations revealed that the enhanced catalytic performance was attributed to exclusively forming the electrophilic oxygen species without nucleophilic oxygen species. As a result, these electrophilic oxygen species preferentially target the C=C bond instead of α C–H bond in propylene. These insights pave the way for a new avenue in the optimization of metal oxide catalysts through the precise manipulation of metal-nitrogen (M–N) coordination environments.

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Section: Electronic and Coordination Structure Of Cu Based Sacssupporting

confidence: 57%

Low-coordinate Cu1–N2 sites in single-atom catalyst for highly efficient propylene epoxidation with molecular oxygen

Fu,

Qiu,

Zhang

et al. 2024

Preprint

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“…[35][36][37] Therefore, h-BN has been widely applied to support SACs. 25,35,[37][38][39][40][41][42][43] A few h-BN-supported SACs have been synthesized in experiments and successfully applied to the catalysis reactions, for example, the use of Ru supported on defective h-BN for esters hydrogenation, Ru on porous h-BN for CO 2 methanation, Pd on defective h-BN for hydrogenation of cinnamaldehyde. 25,35,37 Additionally, with density functional theory (DFT) calculations, SACs supported on defective h-BN have been rationally designed and predicted to possess prominent catalytic reactivity toward various reactions, such as propane dehydrogenation, CO oxidation, NO electrochemical reduction, N 2 electrocatalytic reduction, hydrogen evolution reaction, etc.…”

Section: Introductionmentioning

confidence: 99%

The single metal atom (Ni, Pd, Pt) anchored on defective hexagonal boron nitride for oxidative desulfurization

Lv,

Ran,

Zhang

et al. 2024

Phys. Chem. Chem. Phys.

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Dynamic Active Sites in Electrocatalysis

Ning,

Wang,

Wan

et al. 2024

Angewandte Chemie

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In‐depth understanding of the real‐time behaviors of active sites during electrocatalysis is essential for the advancement of sustainable energy conversion. Recently, the concept of dynamic active sites has been recognized as a potent approach for creating self‐adaptive electrocatalysts that can address a variety of electrocatalytic reactions, outperforming traditional electrocatalysts with static active sites. Nonetheless, the comprehension of the underlying principles that guide the engineering of dynamic active sites is presently insufficient. In this review, we systematically analyze the fundamentals of dynamic active sites for electrocatalysis and consider important future directions for this emerging field. We reveal that dynamic behaviors and reversibility are two crucial factors that influence electrocatalytic performance. By reviewing recent advances in dynamic active sites, we conclude that implementing dynamic electrocatalysis through variable reaction environments, correlating the model of dynamic evolution with catalytic properties, and developing localized and ultrafast in‐situ/operando techniques are keys to designing high‐performance dynamic electrocatalysts. This review paves the way to the development of the next‐generation electrocatalyst and the universal theory for both dynamic and static active sites.

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Rational design, application and dynamic evolution of Cu–N–C single-atom catalysts

Abstract: Benefit from the unique electronic and structural characteristics, transition metal and nitrogen co-doped carbon-based nano materials (M-N-C) are considered to be one of the most promising catalysts. The combination of...

Cited by 17 publications

References 213 publications

Low-coordinate Cu1–N2 sites in single-atom catalyst for highly efficient propylene epoxidation with molecular oxygen

Low-coordinate Cu1–N2 sites in single-atom catalyst for highly efficient propylene epoxidation with molecular oxygen

The single metal atom (Ni, Pd, Pt) anchored on defective hexagonal boron nitride for oxidative desulfurization

Dynamic Active Sites in Electrocatalysis

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