pH-Independent Production of Hydroxyl Radical from Atomic H*-Mediated Electrocatalytic H2O2 Reduction: A Green Fenton Process without Byproducts
Zeng, Huabin; Zhang, Gong; Ji, Qinghua; Liu, Huijuan; Hua, Xin; Xia, Hua; Sillanpää, Mika; Qu, Jiuhui (2020-11-05)
Post-print / Final draft
Zeng, Huabin
Zhang, Gong
Ji, Qinghua
Liu, Huijuan
Hua, Xin
Xia, Hua
Sillanpää, Mika
Qu, Jiuhui
05.11.2020
Environmental Science and Technology
54
22
14725-14731
ACS Publications
School of Engineering Science
Kaikki oikeudet pidätetään.
© 2020 American Chemical Society
© 2020 American Chemical Society
Julkaisun pysyvä osoite on
https://urn.fi/URN:NBN:fi-fe2021062139088
https://urn.fi/URN:NBN:fi-fe2021062139088
Tiivistelmä
Hydroxyl radical (•OH) can hydroxylate or dehydrogenate organics without forming extra products and is thereby expediently applied in extensive domains. Although it can be efficiently produced through single-electron transfer from transition-metal-containing activators to hydrogen peroxide (H2O2), narrow applicable pH range, strict activator/H2O2 ratio requirement, and byproducts that are formed in the mixture with the background matrix necessitate the need for additional energy-intensive up/downstream treatments. Here, we show a green Fenton process in an electrochemical cell, where the electro-generated atomic H* on a Pd/graphite cathode enables the efficient conversion of H2O2 into •OH and subsequent degradation of organic pollutants (80% efficiency). Operando liquid time-of-fight secondary ion mass spectrometry verified that H2O2 activation takes place through a transition state of the Pd–H*–H2O2 adduct with a low reaction energy barrier of 0.92 eV, whereby the lone electron in atomic H* can readily cleave the peroxide bridge, with •OH and H2O as products (ΔGr = −1.344 eV). Using H+ or H2O as the resource, we demonstrate that the well-directed output of H* determines the pH-independent production of •OH for stable conversion of organic contaminants in wider pH ranges (3–12). The research pioneers a novel path for eliminating the restrictions that are historically challenging in the traditional Fenton process.
Lähdeviite
Zeng, H., Zhang, G., Ji, Q., Liu, H., Hua, X., Xia, H., Sillanpää, M., Qu, J. (2020). pH-Independent Production of Hydroxyl Radical from Atomic H*-Mediated Electrocatalytic H2O2 Reduction: A Green Fenton Process without Byproducts. Environmental Science and Technology, vol. 54, issue 22. pp. 14725-14731. DOI: 10.1021/acs.est.0c04694
Kokoelmat
- Tieteelliset julkaisut [1522]