In situ quantitative single-molecule study of dynamic catalytic processes in nanoconfinement

Dong, Bin; Pei, Yuchen; Zhao, Fei; Goh, Tian Wei; Qi, Zhiyuan; Xiao, Chaoxian; Chen, Kuangcai; Huang, Wenyu; Fang, Ning

doi:10.1038/s41929-017-0021-1

Cited by 112 publications

(111 citation statements)

References 46 publications

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“…We first employed 5 nm Pt nanoparticles deposited onto 100 nm silica spheres (noted as Pt/SiO 2 ) following a reported method. 36 We observed similar kinetics for the conversion from Pt/SiO 2 to PtSn/SiO 2 as the encapsulated Pt@mSiO 2 (Fig. S7 †).…”

Section: Characterizationsupporting

confidence: 61%

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Kinetics, energetics, and size dependence of the transformation from Pt to ordered PtSn intermetallic nanoparticles

et al. 2019

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Section: Characterizationsupporting

confidence: 61%

“…35 Such a space-confined strategy to prevent sintering is also seen in other literature studies. [36][37][38] TEM images of PtSn NPs after 120 min transformation of 14 and 5 nm Pt NPs to incorporate Sn were taken ( Fig. S1 and S2 †) and mono-dispersed metal NPs without aggregation were confirmed.…”

Section: Characterizationmentioning

confidence: 99%

Kinetics, energetics, and size dependence of the transformation from Pt to ordered PtSn intermetallic nanoparticles

et al. 2019

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“…This approach allowed the heterogeneous molecular transport and catalytic reaction kinetics within nanopores to be quantified with single-molecule and singleparticle resolution, demonstrating a significant increase in reaction rate in the presence of nanoconfinement. 228 A similar approach was applied to unravel the cooperative communication within and between single Pd-and Au-based nanocatalysts. 229 Surface "active" sites on single Pd or Au nanocatalysts were shown to communicate with each other (i.e., intraparticle level) during heterogeneous catalysis over a distance of ca.…”

Section: Fabricationmentioning

confidence: 99%

Nanoscale Electrochemical Mapping

et al. 2018

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“…Single-molecule fluorescence microscopy (SMFM) combined with fluorogenic substrates provides information on the activity of individual catalysts, which is inaccessible in ensemble measurements. [29][30][31][32][33][34][35][36][37][38][39][40][41] Although mostly applied for investigating enzymatic reactions, the fluorogenic substrate reporter systems also allow for studying non-enzymatic processes in real time. [34][35][36][37][38]40,41 Upon cleavage, the initially nonfluorescent substrate is converted into a highly fluorescent product molecule.…”

Section: Introductionmentioning

confidence: 99%

Catalytic single-chain polymeric nanoparticles at work: from ensemble towards single-particle kinetics

Liu

Turunen

Waal

et al. 2018

Mol. Syst. Des. Eng.

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a Folding a single polymer chain around catalytically active sites to construct catalytic single chain polymeric nanoparticles (SCPNs) is a novel approach to mimic the activity and selectivity of enzymes. In order to relate the efficiency of SCPNs to their three-dimensional structure, a better understanding of their catalytic activity at an individual level, rather than at an ensemble level, is highly desirable. In this work, we present the design and preparation of catalytic SCPNs and a family of fluorogenic substrates, their characterization at the ensemble level as well as our progress towards analyzing individual SCPNs with single-molecule fluorescence microscopy (SMFM). Firstly, organocopper-based SCPNs together with rhodamine-based fluorogenic substrates were designed and synthesized. The SCPNs catalyze the carbamate cleavage reaction of mono-protected rhodamines, with the dimethylpropargyloxycarbonyl protecting group being cleaved most efficiently. A systematic study focusing on the conditions during catalysis revealed that the ligand acceleration effect as well as the accumulation of substrates and catalytically active sites in SCPNs significantly promote their catalytic performance. Secondly, a streptavidin-biotin based strategy was developed to immobilize the catalytic SCPNs on the surface of glass coverslips. Fluorescence correlation spectroscopy experiments confirmed that the SCPNs remained catalytically active after surface immobilization. Finally, single-SCPN activity measurements were performed. The results qualitatively indicated that fluorescent product molecules were formed as a result of the catalytic reaction and that individual fluorescent product molecules could be detected. So far, no evidence for strongly different behaviors has been observed when comparing individual SCPNs.

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In situ quantitative single-molecule study of dynamic catalytic processes in nanoconfinement

Cited by 112 publications

References 46 publications

Kinetics, energetics, and size dependence of the transformation from Pt to ordered PtSn intermetallic nanoparticles

Kinetics, energetics, and size dependence of the transformation from Pt to ordered PtSn intermetallic nanoparticles

Nanoscale Electrochemical Mapping

Catalytic single-chain polymeric nanoparticles at work: from ensemble towards single-particle kinetics

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