Exploring the Origin of Enhanced Activity and Reaction Pathway for Photocatalytic H2 Production on Au/B-TiO2 Catalysts

Gold-embedded boron-doped TiO2 (Au/B-TiO2) photocatalysts were synthesized by a sol–gel hydrothermal method. The TEM images display that the gold nanoparticles were embedded into the B-TiO2 framework. Hydrogen evolution under light irradiation showed that doping of boron into TiO2 enhanced the photocatalytic activity. A further remarkable improvement of the activity was observed over the Au/B-TiO2. Evidenced by B 1s XPS and 11B MAS NMR spectra, the embedment of Au nanoparticles contributes to the formation of more interstitial boron species in B-TiO2. In turn, it gives rise to surface or near-surface states facilitating the embedment of Au nanoparticles, as demonstrated by the Au 4f XPS spectra, which indicates the strong interaction between gold and the B-TiO2 framework. This specific synergy significantly contributes to the enhancement of photocatalytic activity. For the first time, the isotopic tracer studies using a gas chromatograph isotope ratio mass spectrometer along with a series of control exper...

[1]  X. Wen,et al.  Confined Au‐Pd Ensembles in Mesoporous TiO2 Spheres for the Photocatalytic Oxidation of Acetaldehyde , 2013 .

[2]  Xuxu Wang,et al.  Single-site Sn-grafted Ru/TiO2 photocatalysts for biomass reforming: Synergistic effect of dual co-catalysts and molecular mechanism , 2013 .

[3]  Can Li,et al.  Roles of cocatalysts in photocatalysis and photoelectrocatalysis. , 2013, Accounts of chemical research.

[4]  Anmin Zheng,et al.  Understanding the high photocatalytic activity of (B, Ag)-codoped TiO2 under solar-light irradiation with XPS, solid-state NMR, and DFT calculations. , 2013, Journal of the American Chemical Society.

[5]  Ke Su,et al.  Efficient Visible Light-Driven Photocatalytic Degradation of Pentachlorophenol with Bi2O3/TiO2–xBx , 2012 .

[6]  G. Lu,et al.  Hollow Anatase TiO2 Single Crystals and Mesocrystals with Dominant {101} Facets for Improved Photocatalysis Activity and Tuned Reaction Preference , 2012 .

[7]  W. Choi,et al.  Simultaneous production of hydrogen with the degradation of organic pollutants using TiO2 photocatalyst modified with dual surface components , 2012 .

[8]  M. Beller,et al.  Hydrogen evolution from water/alcohol mixtures: effective in situ generation of an active Au/TiO2 catalyst. , 2012, ChemSusChem.

[9]  R. Amal,et al.  Progress in Heterogeneous Photocatalysis: From Classical Radical Chemistry to Engineering Nanomaterials and Solar Reactors. , 2012, The journal of physical chemistry letters.

[10]  S. Linic,et al.  Plasmonic-metal nanostructures for efficient conversion of solar to chemical energy. , 2011, Nature materials.

[11]  Geoffrey I N Waterhouse,et al.  Noble Metal‐Modified Porous Titania Networks and their Application as Photocatalysts , 2011 .

[12]  Xiaoyan Qin,et al.  Facile in situ synthesis of visible-light plasmonic photocatalysts M@TiO2 (M = Au, Pt, Ag) and evaluation of their photocatalytic oxidation of benzene to phenol , 2011 .

[13]  G. Adami,et al.  Nanostructured Cu/TiO2 Photocatalysts for H2 Production from Ethanol and Glycerol Aqueous Solutions. , 2011 .

[14]  Avelino Corma,et al.  Titania supported gold nanoparticles as photocatalyst. , 2011, Physical chemistry chemical physics : PCCP.

[15]  Tiehong Chen,et al.  Boron Environments in B-Doped and (B, N)-Codoped TiO2 Photocatalysts: A Combined Solid-State NMR and Theoretical Calculation Study , 2011 .

[16]  R. Amal,et al.  Photocatalytic Overall Water Splitting over ALi2Ti6O14 (A: 2Na and Sr) with Tunneling Structure , 2011 .

[17]  L. Mädler,et al.  Photocatalytic H2 Evolution over TiO2 Nanoparticles. The Synergistic Effect of Anatase and Rutile , 2010 .

[18]  Jian Zhu,et al.  In situ encapsulation of Au nanoparticles in mesoporous core-shell TiO(2) microspheres with enhanced activity and durability. , 2009, Chemical communications.

[19]  A. Kudo,et al.  Heterogeneous photocatalyst materials for water splitting. , 2009, Chemical Society reviews.

[20]  Chenghua Sun,et al.  Synergistic effects of B/N doping on the visible-light photocatalytic activity of mesoporous TiO2. , 2008, Angewandte Chemie.

[21]  W. Choi,et al.  Synergic effect of simultaneous fluorination and platinization of TiO2 surface on anoxic photocatalytic degradation of organic compounds. , 2008, Chemical communications.

[22]  R. M. Lambert,et al.  Effective visible light-activated B-doped and B,N-codoped TiO2 photocatalysts. , 2007, Journal of the American Chemical Society.

[23]  Xiaobo Chen,et al.  Titanium dioxide nanomaterials: synthesis, properties, modifications, and applications. , 2007, Chemical reviews.

[24]  T. Lim,et al.  The effect of platinum and silver deposits in the photocatalytic oxidation of resorcinol , 2007 .

[25]  Yunfeng Lu,et al.  Mesoporous Au/TiO2 nanocomposites with enhanced photocatalytic activity. , 2007, Journal of the American Chemical Society.

[26]  Seung-Bin Park,et al.  Local structure and photocatalytic activity of B2O3-SiO2/TiO2 ternary mixed oxides prepared by sol-gel method , 2004 .

[27]  P. Falaras,et al.  Characterization and photocatalytic activity of Au/TiO2 thin films for azo-dye degradation , 2003 .

[28]  Akira Fujishima,et al.  Titanium dioxide photocatalysis , 2000 .

[29]  T. Kunitake,et al.  Layered Nanocomposite of Close-Packed Gold Nanoparticles and TiO2 Gel Layers , 1999 .

[30]  Wonyong Choi,et al.  The Role of Metal Ion Dopants in Quantum-Sized TiO2: Correlation between Photoreactivity and Charge Carrier Recombination Dynamics , 1994 .

[31]  A. Mills,et al.  Photosensitised dissociation of water using dispersed suspensions of n-type semiconductors , 1982 .

[32]  G. Denisov,et al.  Kinetic isotope effect in proton exchange processes between methanol and water in inert solvents , 1977 .

[33]  J. Halford,et al.  Exchange of Deuterium Between Methanol and Water: Vibrations of the Hydroxyl Group in Methanol and Methanol‐d: The Entropy of Methanol , 1938 .