Solar water splitting is one of the key steps in artificial photosynthesis for future carbonneutral, storable and sustainable source of energy. Here we show that one of the major obstacles for achieving efficient and stable overall water splitting over the emerging nanostructured photocatalyst is directly related to the uncontrolled surface charge properties. By tuning the Fermi level on the nonpolar surfaces of gallium nitride nanowire arrays, we demonstrate that the quantum efficiency can be enhanced by more than two orders of magnitude. The internal quantum efficiency and activity on p-type gallium nitride nanowires can reach similar to 51% and similar to 4.0 mol hydrogen h(-1) g(-1), respectively. The nanowires remain virtually unchanged after over 50,000 mu mol gas (hydrogen and oxygen) is produced, which is more than 10,000 times the amount of photocatalyst itself (similar to 4.6 mmol). The essential role of Fermi-level tuning in balancing redox reactions and in enhancing the efficiency and stability is also elucidated.
机构:
Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, Tokyo 1138656, Japan
Japan Sci & Technol Agcy JST, Precursory Res Embryon Sci & Technol PRESTO, Kawaguchi, Saitama 3320012, JapanUniv Tokyo, Dept Chem Syst Engn, Bunkyo Ku, Tokyo 1138656, Japan
机构:
Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Reece, Steven Y.
Hamel, Jonathan A.
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Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Hamel, Jonathan A.
Sung, Kimberly
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Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Sung, Kimberly
Jarvi, Thomas D.
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Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Jarvi, Thomas D.
Esswein, Arthur J.
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Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Esswein, Arthur J.
Pijpers, Joep J. H.
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MIT, Dept Chem, Cambridge, MA 02139 USA
Fdn Fundamental Res Matter, Inst Atom & Mol Phys, NL-1098 XG Amsterdam, NetherlandsSun Catalytix, Cambridge, MA 02139 USA
Pijpers, Joep J. H.
Nocera, Daniel G.
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h-index: 0
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MIT, Dept Chem, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
机构:
Xi An Jiao Tong Univ, Sch Energy & Power Engn, State Key Lab Multiphase Flow Power Engn, Int Res Ctr Renewable Energy, Xian 710049, Peoples R ChinaRMIT Univ, Sch Aerosp Mech & Mfg Engn, Bundoora, Vic 3083, Australia
Vayssieres, Lionel
Durrant, James R.
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Univ London Imperial Coll Sci Technol & Med, Dept Chem, London SW7 2AZ, EnglandRMIT Univ, Sch Aerosp Mech & Mfg Engn, Bundoora, Vic 3083, Australia
机构:
Univ Tokyo, Dept Chem Syst Engn, Bunkyo Ku, Tokyo 1138656, Japan
Japan Sci & Technol Agcy JST, Precursory Res Embryon Sci & Technol PRESTO, Kawaguchi, Saitama 3320012, JapanUniv Tokyo, Dept Chem Syst Engn, Bunkyo Ku, Tokyo 1138656, Japan
机构:
Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Reece, Steven Y.
Hamel, Jonathan A.
论文数: 0引用数: 0
h-index: 0
机构:
Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Hamel, Jonathan A.
Sung, Kimberly
论文数: 0引用数: 0
h-index: 0
机构:
Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Sung, Kimberly
Jarvi, Thomas D.
论文数: 0引用数: 0
h-index: 0
机构:
Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Jarvi, Thomas D.
Esswein, Arthur J.
论文数: 0引用数: 0
h-index: 0
机构:
Sun Catalytix, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
Esswein, Arthur J.
Pijpers, Joep J. H.
论文数: 0引用数: 0
h-index: 0
机构:
MIT, Dept Chem, Cambridge, MA 02139 USA
Fdn Fundamental Res Matter, Inst Atom & Mol Phys, NL-1098 XG Amsterdam, NetherlandsSun Catalytix, Cambridge, MA 02139 USA
Pijpers, Joep J. H.
Nocera, Daniel G.
论文数: 0引用数: 0
h-index: 0
机构:
MIT, Dept Chem, Cambridge, MA 02139 USASun Catalytix, Cambridge, MA 02139 USA
机构:
Xi An Jiao Tong Univ, Sch Energy & Power Engn, State Key Lab Multiphase Flow Power Engn, Int Res Ctr Renewable Energy, Xian 710049, Peoples R ChinaRMIT Univ, Sch Aerosp Mech & Mfg Engn, Bundoora, Vic 3083, Australia
Vayssieres, Lionel
Durrant, James R.
论文数: 0引用数: 0
h-index: 0
机构:
Univ London Imperial Coll Sci Technol & Med, Dept Chem, London SW7 2AZ, EnglandRMIT Univ, Sch Aerosp Mech & Mfg Engn, Bundoora, Vic 3083, Australia