Photosynthesis of a Photocatalyst: Single Atom Platinum Captured and Stabilized by an Iron(III) Engineered Defect

Anderson, Nicholas J.; Xu, Tongzhou; Ouyang, Mengyao; Bisson, Patrick J.; Davies, Rebecca G.; Marmolejos, Joam M.; Shultz, Mary Jane

doi:10.1021/acs.jpca.0c08527

Photosynthesis of a Photocatalyst: Single Atom Platinum Captured and Stabilized by an Iron(III) Engineered Defect

Journal Article · Tue Dec 29 00:00:00 EST 2020 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.0c08527· OSTI ID:1757952

Anderson, Nicholas J. ^[1]; Xu, Tongzhou ^[2]; ^[3]; Bisson, Patrick J. ^[3]; Davies, Rebecca G. ^[3]; Marmolejos, Joam M. ^[3]; ^[3]

Tufts Univ., Medford, MA (United States); Tufts University
Tsinghua Univ., Beijing (China)
Tufts Univ., Medford, MA (United States)

Single atom (SA), noble metal catalysts are of interest due to high projected catalytic activity while minimizing cost. Common issues facing many synthesis methodologies include complicated processes, low yields of SA product, and production of mixtures of SA and nanoparticles (NPs). Herein we report a simple, room-temperature synthesis of single Pt-atom decorated, anatase Fe-doped TiO₂ particles that leverages the Fe dopant as an engineered defect site to photodeposit and stabilize atomically dispersed Pt. Both particle morphology and Fe dopant location are based on thermodynamic principles (Gibbs-Wulff construction). CO-DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) reveals absence of bridge-bonded CO signal, confirming atomically dispersed Pt. XAS (x-ray absorption spectroscopy) of both Pt and Fe indicates Fe-O-Pt bonding that persists through catalytic cycling. Mass balance indicates Pt loading on single particles is 2.5 wt% Pt; single Pt-atom decorated nanoparticle yield is 17%. Pt containing particles show more than an order-of-magnitude increased photo-oxidation efficiency relative to particles containing only Fe. High single-atom-Pt yield, ease of synthesis, and high catalytic activity demonstrate the utility and promise of this method. In conclusion, the principles of this photodeposition synthesis allow for its generalizability towards other SA metals of catalytic interest.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Tufts Univ., Medford, MA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0020258

OSTI ID:: 1757952

Alternate ID(s):: OSTI ID: 1761422
OSTI ID: 1864868

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 1 Vol. 125; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Single-atom catalyst
Titania
catalysts
charge-separation
defect
dopant
doping
impurities
metal nanoparticles
nanoparticles
oxidation
photo catalysis
photocatalyst
photosynthesis
platinum
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Photosynthesis of a Photocatalyst: Single Atom Platinum Captured and Stabilized by an Iron(III) Engineered Defect

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