2020
DOI: 10.1038/s41467-020-15843-3
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Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon

Abstract: Electrochemical synthesis of H 2 O 2 through a selective two-electron (2e −) oxygen reduction reaction (ORR) is an attractive alternative to the industrial anthraquinone oxidation method, as it allows decentralized H 2 O 2 production. Herein, we report that the synergistic interaction between partially oxidized palladium (Pd δ+) and oxygen-functionalized carbon can promote 2e − ORR in acidic electrolytes. An electrocatalyst synthesized by solution deposition of amorphous Pd δ+ clusters (Pd 3 δ+ and Pd 4 δ+) on… Show more

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Cited by 245 publications
(167 citation statements)
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References 44 publications
(65 reference statements)
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“…reported a Pd δ + –OCNT electrocatalyst with nearly 100% selectivity toward H 2 O 2 electrochemical production and a high mass activity (1.946 A mg −1 at 0.45 V) in acidic electrolyte ( Figure a). [ 20 ] The X‐ray absorption fine structure characterization and DFT calculations demonstrate that the synergistic interaction between partially oxidized Pd clusters and oxygen‐functionalized CNT substrate is crucial for the high 2e − ORR catalytic activity. Various other Pd/C catalysts displayed highly selectivity toward H 2 O 2 production.…”
Section: Electrocatalysts and Factors Influencing 2e− Orr Activity/selectivitymentioning
confidence: 99%
“…reported a Pd δ + –OCNT electrocatalyst with nearly 100% selectivity toward H 2 O 2 electrochemical production and a high mass activity (1.946 A mg −1 at 0.45 V) in acidic electrolyte ( Figure a). [ 20 ] The X‐ray absorption fine structure characterization and DFT calculations demonstrate that the synergistic interaction between partially oxidized Pd clusters and oxygen‐functionalized CNT substrate is crucial for the high 2e − ORR catalytic activity. Various other Pd/C catalysts displayed highly selectivity toward H 2 O 2 production.…”
Section: Electrocatalysts and Factors Influencing 2e− Orr Activity/selectivitymentioning
confidence: 99%
“…The possible impacts of these trace amount of O dopants on our samples' ORR performances were successfully excluded in our later discussions. Defects in carbon materials is another factor that we need to take into consideration when we analyze the origin of H 2 O 2 selectivity in B-C 17,25 . Raman spectroscopy was utilized to examine whether the doping process increases or decreases the concentration of defects in the CB support.…”
Section: Catalysts Preparation and Characterizationsmentioning
confidence: 99%
“…As O 2 molecules can also be fully reduced to H 2 O via a 4e − transfer process [12][13][14] , which is the preferred pathway in fuel cell applications, developing highly selective and active 2e − -ORR catalysts is the prerequisite of this sustainable synthetic route. Metal-based catalysts including noble metals and their alloys have been demonstrated to be selective for H 2 O 2 [15][16][17][18][19][20] . However, the cost and scarcity of noble metal elements make it difficult for future large-scale deployments.…”
mentioning
confidence: 99%
“…H 2 O 2 is one of the very few chemicals that attract research interest in both energy and environmental contexts [1–7] . It has been widely used for pulp and textile bleaching, as a first‐aid disinfectant, in advanced oxidation processes (AOPs) for wastewater treatment, hydrometallurgy, and the electronics industry [8] .…”
Section: Introductionmentioning
confidence: 99%