SWCNT Photocatalyst for Hydrogen Production from Water upon Photoexcitation of (8, 3) SWCNT at 680-nm Light

在680 nm光激发下,(8, 3)型单壁碳纳米管(SWCNT)作为光催化剂,用于从水中制氢。

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Abstract

Single-walled carbon nanotubes (SWCNTs) are potentially strong optical absorbers with tunable absorption bands depending on their chiral indices (n, m). Their application for solar energy conversion is difficult because of the large binding energy (>100 meV) of electron-hole pairs, known as excitons, produced by optical absorption. Recent development of photovoltaic devices based on SWCNTs as light-absorbing components have shown that the creation of heterojunctions by pairing chirality-controlled SWCNTs with C(60) is the key for high power conversion efficiency. In contrast to thin film devices, photocatalytic reactions in a dispersion/solution system triggered by the photoexcitation of SWCNTs have never been reported due to the difficulty of the construction of a well-ordered surface on SWCNTs. Here, we show a clear-cut example of a SWCNT photocatalyst producing H(2) from water. Self-organization of a fullerodendron on the SWCNT core affords water-dispersible coaxial nanowires possessing SWCNT/C(60) heterojunctions, of which a dendron shell can act as support of a co-catalyst for H(2) evolution. Because the band offset between the LUMO levels of (8, 3)SWCNT and C(60) satisfactorily exceeds the exciton binding energy to allow efficient exciton dissociation, the (8, 3)SWCNT/fullerodendron coaxial photocatalyst shows H(2)-evolving activity (QY = 0.015) upon 680-nm illumination, which is E(22) absorption of (8, 3) SWCNT.

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