Journal
ACS CATALYSIS
Volume 7, Issue 4, Pages 2886-2895Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b03334
Keywords
photocatalysis; carbon nitride; solar fuel; hydrogen peroxide synthesis; proton coupled electron transfer (PCET)
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Funding
- Global Research Laboratory (GRL) Program [NRF-2014K1A1A2041044]
- KCAP (Sogang University) [2009-0093880]
- Korea Government (MSIP) through the National Research Foundation (NRF)
- National Research Foundation of Korea [2014K1A1A2041044, 2009-0093880, 22A20130012323] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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We report that in situ incorporation of both potassium and phosphate species into a polymeric carbon nitride (CN) framework highly enhanced the photo production of hydrogen peroxide (H2O2) without the use of any noble-metal cocatalysts. The incorporation of earth-abundant heteroelements (K, P, and O) (i) introduced the negative surface charge over the entire pH range through surface functionalization by phosphate species, (ii) increased the lifetime of the transient species to a picosecond time scale via the formation of charge separation states, (iii) facilitated the interfacial electron transfer to dioxygen, and (iv) inhibited the decomposition of in situ generated H2O2. As a result, the modified CN showed apparent quantum yields (P, for H2O2 production) that are enhanced by about 25 and 17 times (Phi(420) = 8.0%; Phi(320) = 26.2%) from those of bare CN (Phi(420) = 0.32%; Phi(320) = 1.55%) under monochromatic irradiation of 420 and 320 nm, respectively. This study clearly demonstrated a simple way to design multiple heteroelement-incorporated CN compounds that consist of earth-abundant elements only (C, N, K, P, O) for the development of practical and economical solar conversion photocatalytic materials.
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