Selective hydrogenation of 1,3-butadiene catalyzed by a single Pd atom anchored on graphene: the importance of dynamics

The active-site structure, reaction mechanism, and product selectivity of the industrially important selective hydrogenation of 1,3-butadiene are investigated using first principles for an emerging single-atom Pd catalyst anchored on graphene.

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Iron-Imprinted Single-Atomic Site Catalyst-Based Nanoprobe for Detection of Hydrogen Peroxide in Living Cells

Nano-Micro Letters ◽

10.1007/s40820-021-00661-z ◽

2021 ◽

Vol 13 (1) ◽

Author(s):

Zhaoyuan Lyu ◽

Shichao Ding ◽

Maoyu Wang ◽

Xiaoqing Pan ◽

Zhenxing Feng ◽

...

Keyword(s):

Hydrogen Peroxide ◽

Active Site ◽

Single Atom ◽

Site Structure ◽

Atomic Site ◽

Ion Imprinting ◽

Active Site Structure ◽

In Situ Detection ◽

Colorimetric Biosensing

AbstractFe-based single-atomic site catalysts (SASCs), with the natural metalloproteases-like active site structure, have attracted widespread attention in biocatalysis and biosensing. Precisely, controlling the isolated single-atom Fe-N-C active site structure is crucial to improve the SASCs’ performance. In this work, we use a facile ion-imprinting method (IIM) to synthesize isolated Fe-N-C single-atomic site catalysts (IIM-Fe-SASC). With this method, the ion-imprinting process can precisely control ion at the atomic level and form numerous well-defined single-atomic Fe-N-C sites. The IIM-Fe-SASC shows better peroxidase-like activities than that of non-imprinted references. Due to its excellent properties, IIM-Fe-SASC is an ideal nanoprobe used in the colorimetric biosensing of hydrogen peroxide (H2O2). Using IIM-Fe-SASC as the nanoprobe, in situ detection of H2O2 generated from MDA-MB-231 cells has been successfully demonstrated with satisfactory sensitivity and specificity. This work opens a novel and easy route in designing advanced SASC and provides a sensitive tool for intracellular H2O2 detection.

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Theoretical studies of the active-site structure, spectroscopic and thermodynamic properties, and reaction mechanism of multicopper oxidases

Coordination Chemistry Reviews ◽

10.1016/j.ccr.2012.04.019 ◽

2013 ◽

Vol 257 (2) ◽

pp. 445-458 ◽

Cited By ~ 41

Author(s):

Lubomír Rulíšek ◽

Ulf Ryde

Keyword(s):

Reaction Mechanism ◽

Thermodynamic Properties ◽

Active Site ◽

Theoretical Studies ◽

Multicopper Oxidases ◽

Site Structure ◽

Active Site Structure

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Highly selective and robust single-atom catalyst Ru1/NC for reductive amination of aldehydes/ketones

Nature Communications ◽

10.1038/s41467-021-23429-w ◽

2021 ◽

Vol 12 (1) ◽

Author(s):

Haifeng Qi ◽

Ji Yang ◽

Fei Liu ◽

LeiLei Zhang ◽

Jingyi Yang ◽

...

Keyword(s):

Active Site ◽

Rational Design ◽

Reductive Amination ◽

Single Atom ◽

Primary Amines ◽

Hydrogen Activation ◽

Site Structure ◽

Practical Applications ◽

Highly Active ◽

Active Site Structure

AbstractSingle-atom catalysts (SACs) have emerged as a frontier in heterogeneous catalysis due to the well-defined active site structure and the maximized metal atom utilization. Nevertheless, the robustness of SACs remains a critical concern for practical applications. Herein, we report a highly active, selective and robust Ru SAC which was synthesized by pyrolysis of ruthenium acetylacetonate and N/C precursors at 900 °C in N2 followed by treatment at 800 °C in NH3. The resultant Ru1-N3 structure exhibits moderate capability for hydrogen activation even in excess NH3, which enables the effective modulation between transimination and hydrogenation activity in the reductive amination of aldehydes/ketones towards primary amines. As a consequence, it shows superior amine productivity, unrivalled resistance against CO and sulfur, and unexpectedly high stability under harsh hydrotreating conditions compared to most SACs and nanocatalysts. This SAC strategy will open an avenue towards the rational design of highly selective and robust catalysts for other demanding transformations.

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