TY - JOUR
T1 - Understanding the active sites of boron nitride for CWPO
T2 - An experimental and computational approach
AU - Quintanilla, A.
AU - Vega, G.
AU - Carbajo, J.
AU - Casas, J. A.
AU - Lei, Y.
AU - Fujisawa, K.
AU - Liu, H.
AU - Cruz-Silva, R.
AU - Terrones, M.
AU - Miranzo, P.
AU - Osendi, M. I.
AU - Belmonte, M.
AU - Fernández Sanz, J.
N1 - Funding Information:
The authors thank the financial support by the Community of Madrid and the Government of Spain through the projects: S2018/EMT-4341 and RTI2018-095052-B-I00 (MCIU/AEI/FEDER, UE), respectively. The work done at the University of Sevilla was funded by Spanish Ministerio de Ciencia e Innovación and EU-FEDER, grant PID2019-106871 GB-I00, and the Junta de Andalucía-FEDER, grant: US-1381410. Also, G. Vega acknowledges the Community of Madrid for the Predoctoral contract PEJD-2018-PRE/AMB-9019, co-financed by the European Social Fund through the Youth Employment Operational Program and the Youth Employment Initiative (YEI) 2018. J. Carbajo thanks the financial support by the Government of Spain for a grant under the Juan de la Cierva_Incorporación programme (IJCI-2017-32682). The authors would like to thank A. Pérez for performing the BET and TGA measurements.
Funding Information:
The authors thank the financial support by the Community of Madrid and the Government of Spain through the projects: S2018/EMT-4341 and RTI2018-095052-B-I00 (MCIU/AEI/FEDER, UE), respectively. The work done at the University of Sevilla was funded by Spanish Ministerio de Ciencia e Innovaci?n and EU-FEDER, grant PID2019-106871?GB-I00, and the Junta de Andaluc?a-FEDER, grant: US-1381410. Also, G. Vega acknowledges the Community of Madrid for the Predoctoral contract PEJD-2018-PRE/AMB-9019, co-financed by the European Social Fund through the Youth Employment Operational Program and the Youth Employment Initiative (YEI) 2018. J. Carbajo thanks the financial support by the Government of Spain for a grant under the Juan de la Cierva_Incorporaci?n programme (IJCI-2017-32682). The authors would like to thank A. P?rez for performing the BET and TGA measurements.
Publisher Copyright:
© 2020 Elsevier B.V.
PY - 2021/2/15
Y1 - 2021/2/15
N2 - Hexagonal boron nitride (h-BN) has been explored as a catalyst for degrading persistent organic pollutants in wastewater by Catalytic Wet Peroxide Oxidation (CWPO). Herein, the superior activity of the h-BN on the phenol degradation (model pollutant) compared to other metal-free catalysts, such as carbon-based ones, and the lower selectivity to CO encourage the potential application of h-BN catalysts in CWPO processes. Through a combined density functional theory calculations, experimental reactions and catalyst characterization approach, a comprehensive study on the reaction mechanism has been conducted. According to this, only defected B atoms in the h-BN layer, protonated as B-(OH2)+, decompose the hydrogen peroxide into highly reactive hydroxyl radicals. The radical species diffuse towards inner h-BN regions and react with the phenol adsorbed by π-π interaction on the h-BN surface. Oxidation by-products cause carbonaceous deposits and progressive deactivation of the h-BN catalyst that can be directly regenerated by burning off in air.
AB - Hexagonal boron nitride (h-BN) has been explored as a catalyst for degrading persistent organic pollutants in wastewater by Catalytic Wet Peroxide Oxidation (CWPO). Herein, the superior activity of the h-BN on the phenol degradation (model pollutant) compared to other metal-free catalysts, such as carbon-based ones, and the lower selectivity to CO encourage the potential application of h-BN catalysts in CWPO processes. Through a combined density functional theory calculations, experimental reactions and catalyst characterization approach, a comprehensive study on the reaction mechanism has been conducted. According to this, only defected B atoms in the h-BN layer, protonated as B-(OH2)+, decompose the hydrogen peroxide into highly reactive hydroxyl radicals. The radical species diffuse towards inner h-BN regions and react with the phenol adsorbed by π-π interaction on the h-BN surface. Oxidation by-products cause carbonaceous deposits and progressive deactivation of the h-BN catalyst that can be directly regenerated by burning off in air.
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U2 - 10.1016/j.cej.2020.126846
DO - 10.1016/j.cej.2020.126846
M3 - Article
AN - SCOPUS:85092701458
SN - 1385-8947
VL - 406
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 126846
ER -