Production of H2O2 during Au/C catalyzed aerobic oxidation of 1,2-propanediol

Junqing Ye; James P. Dombrowski; Xiaobing Hu; Javan Whitney-Warner; Shaohui Guo; Mayfair C. Kung; Harold H. Kung

doi:10.1016/j.apcata.2020.117616

Production of H₂O₂ during Au/C catalyzed aerobic oxidation of 1,2-propanediol

Junqing Ye, James P. Dombrowski, Xiaobing Hu, Javan Whitney-Warner, Shaohui Guo, Mayfair C. Kung^*, Harold H. Kung

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

1 Scopus citations

Abstract

The efficiency of H₂O₂ formation during Au/C-catalyzed aerobic oxidation of 1,2-propanediol (diol) at 35 °C increased with increasing concentrations of diol and NaOH. Diol conversion and H₂O₂ accumulation data collected at different concentrations of diol and NaOH could be fitted to a Langmuir–Hinshelwood kinetics model using the diolate as the reactant, indicating that the primary role of hydroxide ions is to deprotonate the diol and not as a reactant in the rate limiting step. Using the model to extrapolate the data to full surface coverage of diolate, it was found that one molecule of diol oxidized would produce one molecule of H₂O₂ and one molecule of lactate. At lower diolate coverages, unoccupied active sites adjacent to adsorbed hydroperoxy/peroxy enabled O[sbnd]O bond cleavage and lowered the H₂O₂ production efficiency. Catalytic degradation of H₂O₂ decreased its production efficiency, and accumulation of trace amounts of heavy products likely caused the slow catalyst deactivation.

Original language	English (US)
Article number	117616
Journal	Applied Catalysis A: General
Volume	599
DOIs	https://doi.org/10.1016/j.apcata.2020.117616
State	Published - Jun 5 2020

Keywords

1,2-propanediol
Au catalyst
Carbon support
Hydrogen peroxide
Oxidation

ASJC Scopus subject areas

Catalysis
Process Chemistry and Technology

Access to Document

10.1016/j.apcata.2020.117616

Cite this

@article{a60e9e2cb0d94ec18a75b1e676156783,

title = "Production of H2O2 during Au/C catalyzed aerobic oxidation of 1,2-propanediol",

abstract = "The efficiency of H2O2 formation during Au/C-catalyzed aerobic oxidation of 1,2-propanediol (diol) at 35 °C increased with increasing concentrations of diol and NaOH. Diol conversion and H2O2 accumulation data collected at different concentrations of diol and NaOH could be fitted to a Langmuir–Hinshelwood kinetics model using the diolate as the reactant, indicating that the primary role of hydroxide ions is to deprotonate the diol and not as a reactant in the rate limiting step. Using the model to extrapolate the data to full surface coverage of diolate, it was found that one molecule of diol oxidized would produce one molecule of H2O2 and one molecule of lactate. At lower diolate coverages, unoccupied active sites adjacent to adsorbed hydroperoxy/peroxy enabled O[sbnd]O bond cleavage and lowered the H2O2 production efficiency. Catalytic degradation of H2O2 decreased its production efficiency, and accumulation of trace amounts of heavy products likely caused the slow catalyst deactivation.",

keywords = "1,2-propanediol, Au catalyst, Carbon support, Hydrogen peroxide, Oxidation",

author = "Junqing Ye and Dombrowski, {James P.} and Xiaobing Hu and Javan Whitney-Warner and Shaohui Guo and Kung, {Mayfair C.} and Kung, {Harold H.}",

note = "Funding Information: J.Y. acknowledges the China Scholarship Council (CSC, 201706440106) for financial support. This work was supported by the U.S. DOE Office of Science, Basic Energy Sciences (DE-FG02-03-ER15457). Funding Information: J.Y. acknowledges the China Scholarship Council (CSC, 201706440106 ) for financial support. This work was supported by the U.S. DOE Office of Science, Basic Energy Sciences ( DE-FG02-03-ER15457 ). Publisher Copyright: {\textcopyright} 2020",

year = "2020",

month = jun,

day = "5",

doi = "10.1016/j.apcata.2020.117616",

language = "English (US)",

volume = "599",

journal = "Applied Catalysis A: General",

issn = "0926-860X",

publisher = "Elsevier",

}

TY - JOUR

T1 - Production of H2O2 during Au/C catalyzed aerobic oxidation of 1,2-propanediol

AU - Ye, Junqing

AU - Dombrowski, James P.

AU - Hu, Xiaobing

AU - Whitney-Warner, Javan

AU - Guo, Shaohui

AU - Kung, Mayfair C.

AU - Kung, Harold H.

N1 - Funding Information: J.Y. acknowledges the China Scholarship Council (CSC, 201706440106) for financial support. This work was supported by the U.S. DOE Office of Science, Basic Energy Sciences (DE-FG02-03-ER15457). Funding Information: J.Y. acknowledges the China Scholarship Council (CSC, 201706440106 ) for financial support. This work was supported by the U.S. DOE Office of Science, Basic Energy Sciences ( DE-FG02-03-ER15457 ). Publisher Copyright: © 2020

PY - 2020/6/5

Y1 - 2020/6/5

N2 - The efficiency of H2O2 formation during Au/C-catalyzed aerobic oxidation of 1,2-propanediol (diol) at 35 °C increased with increasing concentrations of diol and NaOH. Diol conversion and H2O2 accumulation data collected at different concentrations of diol and NaOH could be fitted to a Langmuir–Hinshelwood kinetics model using the diolate as the reactant, indicating that the primary role of hydroxide ions is to deprotonate the diol and not as a reactant in the rate limiting step. Using the model to extrapolate the data to full surface coverage of diolate, it was found that one molecule of diol oxidized would produce one molecule of H2O2 and one molecule of lactate. At lower diolate coverages, unoccupied active sites adjacent to adsorbed hydroperoxy/peroxy enabled O[sbnd]O bond cleavage and lowered the H2O2 production efficiency. Catalytic degradation of H2O2 decreased its production efficiency, and accumulation of trace amounts of heavy products likely caused the slow catalyst deactivation.

AB - The efficiency of H2O2 formation during Au/C-catalyzed aerobic oxidation of 1,2-propanediol (diol) at 35 °C increased with increasing concentrations of diol and NaOH. Diol conversion and H2O2 accumulation data collected at different concentrations of diol and NaOH could be fitted to a Langmuir–Hinshelwood kinetics model using the diolate as the reactant, indicating that the primary role of hydroxide ions is to deprotonate the diol and not as a reactant in the rate limiting step. Using the model to extrapolate the data to full surface coverage of diolate, it was found that one molecule of diol oxidized would produce one molecule of H2O2 and one molecule of lactate. At lower diolate coverages, unoccupied active sites adjacent to adsorbed hydroperoxy/peroxy enabled O[sbnd]O bond cleavage and lowered the H2O2 production efficiency. Catalytic degradation of H2O2 decreased its production efficiency, and accumulation of trace amounts of heavy products likely caused the slow catalyst deactivation.

KW - 1,2-propanediol

KW - Au catalyst

KW - Carbon support

KW - Hydrogen peroxide

KW - Oxidation

UR - http://www.scopus.com/inward/record.url?scp=85084455613&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85084455613&partnerID=8YFLogxK

U2 - 10.1016/j.apcata.2020.117616

DO - 10.1016/j.apcata.2020.117616

M3 - Article

AN - SCOPUS:85084455613

VL - 599

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

SN - 0926-860X

M1 - 117616

ER -