Single-Molecule Fluorescence Microscopy Reveals Local Diffusion Coefficients in the Pore Network of an Individual Catalyst Particle

نویسندگان

  • Frank C Hendriks
  • Florian Meirer
  • Alexey V Kubarev
  • Zoran Ristanović
  • Maarten B J Roeffaers
  • Eelco T C Vogt
  • Pieter C A Bruijnincx
  • Bert M Weckhuysen
چکیده

We used single-molecule fluorescence microscopy to study self-diffusion of a feedstock-like probe molecule with nanometer accuracy in the macropores of a micrometer-sized, real-life fluid catalytic cracking (FCC) particle. Movies of single fluorescent molecules allowed their movement through the pore network to be reconstructed. The observed tracks were classified into three different states by machine learning and all found to be distributed homogeneously over the particle. Most probe molecules (88%) were immobile, with the molecule most likely being physisorbed or trapped; the remainder was either mobile (8%), with the molecule moving inside the macropores, or showed hybrid behavior (4%). Mobile tracks had an average diffusion coefficient of D = 8 × 10-14 ± 1 × 10-13 m2 s-1, with the standard deviation thought to be related to the large range of pore sizes found in FCC particles. The developed methodology can be used to evaluate, quantify and map heterogeneities in diffusional properties within complex hierarchically porous materials.

برای دانلود رایگان متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید

ثبت نام

اگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید

منابع مشابه

Mathematical modeling the effect of catalyst initial shape and the crack pattern in olefin copolymerization

A two-dimensional (2D) single particle model for the copolymerization of propylene-ethylene with heterogeneous Ziegler-Natta catalyst is developed. The model accounts for the effects of the initial shape of the catalyst and carck/ pore patterns on the copolymer composition, polymerization rate and the average molecular weight properties. The spherical and oblate ellipsoidal shapes of catalyst p...

متن کامل

Single-Molecule Kinetics Reveals a Hidden Surface Reaction Intermediate in Single-Nanoparticle Catalysis

Detecting and characterizing reaction intermediates is not only important and powerful for elucidating reaction mechanisms but also challenging in general because of the low populations of intermediates in a reaction mixture. Studying surface reaction intermediates in heterogeneous catalysis presents additional challenges, especially the ubiquitous structural heterogeneity among the catalyst pa...

متن کامل

Self-regulated viscous channel in the nuclear pore complex.

The nuclear pore complex (NPC), the sole gateway for nucleocytoplasmic exchange in eukaryotic cells, allows for the passive diffusion of small molecules and transport-receptor-facilitated translocation of signal-dependent cargo molecules. Whether small molecules passively diffuse through a single central channel or through multiple holes of a hydrogel network is a subject of debate. Additionall...

متن کامل

A novel method for automatic single molecule tracking of blinking molecules at low intensities.

Single molecule tracking provides unprecedented insights into diffusional processes of systems in life and material sciences. Determination of molecule positions with high accuracy and correct connection of the determined positions to tracks is a challenging task with, so far, no universal solution for single fluorescing molecules tackling the challenge of low signal-to-noise ratios, frequent b...

متن کامل

Enhanced accuracy of single-molecule diffusion measurements with a photocleavable energy-transfer dyad.

A photocleavable energy-transfer dyad was synthesized, characterized, and applied to single-molecule fluorescence microscopy. After photocleavage, a combination of independent two-color single-molecule tracking and analysis of single-molecule energy-transfer efficiencies allows the determination of the temporal evolution of the relative distances between both fragments from the nm to the μm sca...

متن کامل

ذخیره در منابع من


  با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید

عنوان ژورنال:

دوره 139  شماره 

صفحات  -

تاریخ انتشار 2017