4.8 Article

Linking the Defective Structure of Boron-Doped Carbon Nano-Onions with Their Catalytic Properties: Experimental and Theoretical Studies

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 43, Pages 51628-51642

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c12126

Keywords

carbon nanostructure; carbon nano-onion; defect; doping; boron; catalysis

Funding

  1. National Science Centre, Poland [2019/35/B/ST5/00572, 2017/25/B/ST5/00975, 2020/37/B/ST4/01215]
  2. US National Science Foundation (NSF) [CHE-1801317]
  3. Robert A. Welch Foundation [AH-0033]
  4. Ministry of Science and Higher Education [75/E-68/S/2008-2]

Ask authors/readers for more resources

Defects in nanomaterials are considered as active sites that tune surface properties for catalysis. The study on boron-doped carbon nano-onions (B-CNOs) reveals a close relationship between their defective structures and catalytic properties affected by the experimental conditions such as mass ratio and process. The presence of different types of boron-Lewis sites on B-CNO surface contributes to their catalytic activity, as shown in SO2 oxidation and tert-butanol dehydration.
Defects are widely present in nanomaterials, and they are recognized as the active sites that tune surface properties in the local region for catalysis. Recently, the theory linking defect structures and catalytic properties of nanocatalysts has been most commonly described. In this study, we prepared boron-doped carbon nano-onions (B-CNOs) by applying an annealing treatment of ultradispersed nanodiamond particles and amorphous boron. These experimental conditions guarantee doping of CNOs with boron atoms in the entire carbon nanostructure, thereby ensuring structural homogeneity. In our research, we discuss the correlations between defective structures of B-CNOs with their catalytic properties toward SO2 and tert-butanol dehydration. We show that there is a close relationship between the catalytic properties of the B-CNOs and the experimental conditions for their formation. It is not only the mass of the substrates used for the formation of B-CNOs that is crucial, that is, the mass ratio of NDs to amorphous B, but also the process, including temperature and gas atmosphere. As it was expected, all B-CNOs demonstrated significant catalytic activity in HSO3- oxidation. However, the subsequent annealing in an air atmosphere diminished their catalytic activity. Unfortunately, no direct relationship between the catalytic activity and the presence of heteroatoms on the B-CNO surface was observed. There was a linear dependence between catalytic activity and Raman reactivity factors for each of the B-CNO materials. In contrast to SO2 oxidation, the B-CNO-a samples showed higher catalytic activity in tert-butanol dehydration due to the presence of Bronsted and Lewis acid sites. The occurence of three types of boron-Lewis sites differing in electron donor properties was confirmed using quantitative infrared spectroscopic measurements of pyridine adsorption.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.8
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

No Data Available
No Data Available