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. 2017 Jun 9:8:15291.
doi: 10.1038/ncomms15291.

Taming interfacial electronic properties of platinum nanoparticles on vacancy-abundant boron nitride nanosheets for enhanced catalysis

Wenshuai Zhu  1   2 , Zili Wu  2 , Guo Shiou Foo  2 , Xiang Gao  3 , Mingxia Zhou  4 , Bin Liu  4 , Gabriel M Veith  3 , Peiwen Wu  1   2 , Katie L Browning  3 , Ho Nyung Lee  3 , Huaming Li  5 , Sheng Dai  2 , Huiyuan Zhu  2
Affiliations

Taming interfacial electronic properties of platinum nanoparticles on vacancy-abundant boron nitride nanosheets for enhanced catalysis

Wenshuai Zhu et al. Nat Commun. .

Abstract

Taming interfacial electronic effects on Pt nanoparticles modulated by their concomitants has emerged as an intriguing approach to optimize Pt catalytic performance. Here, we report Pt nanoparticles assembled on vacancy-abundant hexagonal boron nitride nanosheets and their use as a model catalyst to embrace an interfacial electronic effect on Pt induced by the nanosheets with N-vacancies and B-vacancies for superior CO oxidation catalysis. Experimental results indicate that strong interaction exists between Pt and the vacancies. Bader charge analysis shows that with Pt on B-vacancies, the nanosheets serve as a Lewis acid to accept electrons from Pt, and on the contrary, when Pt sits on N-vacancies, the nanosheets act as a Lewis base for donating electrons to Pt. The overall-electronic effect demonstrates an electron-rich feature of Pt after assembling on hexagonal boron nitride nanosheets. Such an interfacial electronic effect makes Pt favour the adsorption of O2, alleviating CO poisoning and promoting the catalysis.

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Conflict of interest statement

The authors declare no competing financial interests.

Figures

Figure 1
Figure 1. Schematic illustration of h-BNNS with B and N vacancies.
(a) h-BNNS with B vacancy and N-terminated edge. (b) h-BNNS with N vacancy and B-terminated edge.
Figure 2
Figure 2. Representative TEM and STEM images.
(a) TEM of Pt/h-BNNS. Scale bar, 50 nm. (b) STEM of Pt/h-BNNS. Scale bar, 50 nm. (c) High-resolution STEM of h-BNNS with vacancies, as indicated by the boxes. Scale bar, 2 nm.
Figure 3
Figure 3. EELS analysis of Pt/h-BNNS.
(a) Annular dark-field (ADF) STEM image of Pt/h-BNNS indicating the mapping region: 1. The centre of Pt/h-BNNS overlapping region; 2. h-BNNS matrix. (b) B-K EELS profile and (c) N-K EELS profile mapped from regions 1 and 2.
Figure 4
Figure 4. CO oxidation activity of Pt/h-BNNS.
(a) CO oxidation light-off curves for the Pt/h-BNNS, Pt/bulk h-BN, Pt/TiO2, Pt/SiO2 and Pt/C, m(catalyst)=30 mg, CO flow rate 10 ml min−1. (b) The apparent activation energies (Ea) of Pt/h-BNNS and Pt/SiO2, m(catalyst)=5 mg, CO flow rate 10 ml min−1.
Figure 5
Figure 5. Optimized structures and valence electrons of pyramidal Pt4 cluster on h-BNNS.
(a) Pt4 cluster on clean, vacancy-free h-BNNS. (b) Pt4 cluster h-BNNS with Nv. (c) Pt4 cluster on h-BNNS with Bv.
Figure 6
Figure 6. Most stable configuration of CO and O2 adsorption and binding energies on Pt4 cluster.
CO adsorption: (a) Pt4 cluster on clean, vacancy-free h-BNNS. (b) Pt4 cluster h-BNNS with Bv. (c) Pt4 cluster on h-BNNS with Nv. O2 adsorption: (d) Pt4 cluster on clean, vacancy-free h-BNNS. (e) Pt4 cluster h-BNNS with Bv. (f) Pt4 cluster on h-BNNS with Nv.
Figure 7
Figure 7. In situ FTIR spectra of CO adsorbed on Pt/h-BNNS and Pt/SiO2 at room temperature.
Temperature=25 °C. Features from gas phase CO have been subtracted.
See this image and copyright information in PMC

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