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Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)
Electrocatalysis, Volume: 12, Issue: 6, Pages: 771 - 784
Swansea University Author:
Mariolino Carta
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DOI (Published version): 10.1007/s12678-021-00692-5
Abstract
Binding of PdCl42− into the polymer of intrinsic microporosity PIM-EA-TB (on a Nylon mesh substrate) followed by borohydride reduction leads to uncapped Pd(0) nano-catalysts with typically 3.2 ± 0.2 nm diameter embedded within the microporous polymer host structure. Spontaneous reaction of Pd(0) wit...
Published in: | Electrocatalysis |
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ISSN: | 1868-2529 1868-5994 |
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Springer Science and Business Media LLC
2021
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URI: | https://cronfa.swan.ac.uk/Record/cronfa58668 |
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2021-11-30T17:09:45.6811950 v2 58668 2021-11-15 Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB) 56aebf2bba457f395149bbecbfa6d3eb 0000-0003-0718-6971 Mariolino Carta Mariolino Carta true false 2021-11-15 CHEM Binding of PdCl42− into the polymer of intrinsic microporosity PIM-EA-TB (on a Nylon mesh substrate) followed by borohydride reduction leads to uncapped Pd(0) nano-catalysts with typically 3.2 ± 0.2 nm diameter embedded within the microporous polymer host structure. Spontaneous reaction of Pd(0) with formic acid and oxygen is shown to result in the competing formation of (i) hydrogen peroxide (at low formic acid concentration in air; with optimum H2O2 yield at 2 mM HCOOH), (ii) water, or (iii) hydrogen (at higher formic acid concentration or under argon). Next, a spontaneous electroless gold deposition process is employed to attach gold (typically 10- to 35-nm diameter) to the nano-palladium in PIM-EA-TB to give an order of magnitude enhanced production of H2O2 with high yields even at higher HCOOH concentration (suppressing hydrogen evolution). Pd and Au work hand-in-hand as bipolar electrocatalysts. A Clark probe method is developed to assess the catalyst efficiency (based on competing oxygen removal and hydrogen production) and a mass spectrometry method is developed to monitor/optimise the rate of production of hydrogen peroxide. Heterogenised Pd/Au@PIM-EA-TB catalysts are effective and allow easy catalyst recovery and reuse for hydrogen peroxide production. Journal Article Electrocatalysis 12 6 771 784 Springer Science and Business Media LLC 1868-2529 1868-5994 Biomass; Disinfection; Heterogenised palladium; Epoxidation; Hydrogen 1 11 2021 2021-11-01 10.1007/s12678-021-00692-5 COLLEGE NANME Chemistry COLLEGE CODE CHEM Swansea University China Scholarship Council (201906870022); EP/K004956/1 from the EPSRC 2021-11-30T17:09:45.6811950 2021-11-15T11:27:42.8997098 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Lina Wang 1 Mariolino Carta 0000-0003-0718-6971 2 Richard Malpass-Evans 3 Neil B. McKeown 4 Philip J. Fletcher 5 Diana Lednitzky 6 Frank Marken 7 58668__21742__676a8cac88c349b59cb673e620cf3a03.pdf 58668.pdf 2021-11-30T17:07:41.7309899 Output 5197301 application/pdf Version of Record true © The Author(s) 2021. This article is licensed under a Creative Commons Attribution 4.0 International License true eng http://creativecommons.org/licenses/by/4.0/ |
title |
Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB) |
spellingShingle |
Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB) Mariolino Carta |
title_short |
Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB) |
title_full |
Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB) |
title_fullStr |
Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB) |
title_full_unstemmed |
Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB) |
title_sort |
Hydrogen Peroxide Versus Hydrogen Generation at Bipolar Pd/Au Nano-catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB) |
author_id_str_mv |
56aebf2bba457f395149bbecbfa6d3eb |
author_id_fullname_str_mv |
56aebf2bba457f395149bbecbfa6d3eb_***_Mariolino Carta |
author |
Mariolino Carta |
author2 |
Lina Wang Mariolino Carta Richard Malpass-Evans Neil B. McKeown Philip J. Fletcher Diana Lednitzky Frank Marken |
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Electrocatalysis |
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12 |
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771 |
publishDate |
2021 |
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Swansea University |
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1868-2529 1868-5994 |
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10.1007/s12678-021-00692-5 |
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Springer Science and Business Media LLC |
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Faculty of Science and Engineering |
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School of Engineering and Applied Sciences - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry |
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description |
Binding of PdCl42− into the polymer of intrinsic microporosity PIM-EA-TB (on a Nylon mesh substrate) followed by borohydride reduction leads to uncapped Pd(0) nano-catalysts with typically 3.2 ± 0.2 nm diameter embedded within the microporous polymer host structure. Spontaneous reaction of Pd(0) with formic acid and oxygen is shown to result in the competing formation of (i) hydrogen peroxide (at low formic acid concentration in air; with optimum H2O2 yield at 2 mM HCOOH), (ii) water, or (iii) hydrogen (at higher formic acid concentration or under argon). Next, a spontaneous electroless gold deposition process is employed to attach gold (typically 10- to 35-nm diameter) to the nano-palladium in PIM-EA-TB to give an order of magnitude enhanced production of H2O2 with high yields even at higher HCOOH concentration (suppressing hydrogen evolution). Pd and Au work hand-in-hand as bipolar electrocatalysts. A Clark probe method is developed to assess the catalyst efficiency (based on competing oxygen removal and hydrogen production) and a mass spectrometry method is developed to monitor/optimise the rate of production of hydrogen peroxide. Heterogenised Pd/Au@PIM-EA-TB catalysts are effective and allow easy catalyst recovery and reuse for hydrogen peroxide production. |
published_date |
2021-11-01T04:15:22Z |
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1763754033922703360 |
score |
11.021648 |