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Abstract
Binding of PdCl 4 2− 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 H 2O 2 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 H 2O 2 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. Graphical abstract: [Figure not available: see fulltext.].
Original language | English |
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Pages (from-to) | 771-784 |
Number of pages | 14 |
Journal | Electrocatalysis |
Volume | 12 |
Issue number | 6 |
Early online date | 9 Oct 2021 |
DOIs | |
Publication status | Published - 30 Nov 2021 |
Funding
L.W. received a PhD stipend from the China Scholarship Council (201906870022). F.M. received support under project EP/K004956/1 from the EPSRC.
Funders | Funder number |
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Engineering and Physical Sciences Research Council | EP/K004956/1 |
Chinese Government Scholarship | 201906870022 |
Keywords
- Biomass
- Disinfection
- Epoxidation
- Heterogenised palladium
- Hydrogen
ASJC Scopus subject areas
- Electrochemistry
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Dive into the research topics of 'Hydrogen Peroxide versus Hydrogen Generation at Bipolar Pd/Au Nano-Catalysts Grown into an Intrinsically Microporous Polyamine (PIM-EA-TB)'. Together they form a unique fingerprint.Projects
- 1 Finished
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Applying Long-Lived Metastable States in Switchable Functionality via Kinetic Control of Molecular Assembly
Raithby, P. (PI), Burrows, A. (CoI), Lewis, D. (CoI), Marken, F. (CoI), Parker, S. (CoI), Walsh, A. (CoI) & Wilson, C. (CoI)
Engineering and Physical Sciences Research Council
1/11/12 → 30/04/18
Project: Research council
Equipment
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Large chamber variable pressure scanning electron microscope (SEM)
Material and Chemical Characterisation (MC2)Facility/equipment: Equipment