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Highly selective and efficient photocatalytic reduction of nitrate in water by a tandem reaction system consisting of Pt/TiO2 and SnPd/Al2O3: A comparative study of the tandem reaction system with a typical semiconductor photocatalyst, SnPd/TiO2
被引:16
作者:
Hirayama, Jun
[1
,2
]
Kamiya, Yuichi
[1
]
机构:
[1] Hokkaido Univ, Fac Environm Earth Sci, Kita Ku, Nishi 5,Kita 10, Sapporo, Hokkaido 0600810, Japan
[2] JSPS, 5-3-1 Chiyoda Ku, Tokyo 1020083, Japan
关键词:
Photocatalysis;
Nitrate reduction;
Pt/TiO2;
Tandem reaction system;
Catalytic function differentiation;
Tin-palladium bimetal;
Hydrogenation;
SHUTTLE REDOX MEDIATOR;
HYDROGEN GENERATION;
AQUEOUS SUSPENSION;
DECOMPOSITION;
NITROGEN;
TIO2;
O-2;
H-2;
NANOPARTICLES;
OXIDATION;
D O I:
10.1016/j.jcat.2016.12.019
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
A tandem reaction system consisting of a photocatalyst (Pt/TiO2) and a nonphotocatalyst (SnPd/Al2O3) promoted the reduction of NO3- into gaseous products (mainly N-2) under light irradiation (lambda > 300 nm) in the presence of glucose as a hole scavenger. Photocatalytic H-2 evolution (2H(+) + 2(e-) -> H-2) proceeded over Pt/TiO2, and conventional catalytic reduction of NO3- with H-2 (NO3-- + 5/2H(2) -> 1/2N(2) + 2H(2)O + OH-) occurred over SnPd/Al2O3. We optimized the loading amount of Pt on TiO2, the Sn/Pd ratio, the loading amount of SnPd on Al2O3, and the two catalyst dosages. The optimized tandem system gave a high reduction rate of NO3- and a high selectivity for gas (94%) from the photocatalytic reduction of NO3- in water. On the other hand, a typical semiconductor photocatalyst SnPd/TiO2 with an optimized Sn/Pd ratio and an optimized loading amount of SnPd bimetal on TiO2 reduced NO3- about two-thirds as fast as the tandem system and was less selective for gas (70%). The tandem system suppressed the wasted H2 formation, resulting in high light use efficiency for the NO3- reduction (95%), which is defined as the ratio of the number of electrons consumed for NO3- reduction to the total number of electrons consumed for both NO3- reduction and photocatalytic H-2 evolution, though the tandem and SnPd/TiO2 systems consumed about the same total number of electrons. The tandem system has two advantages: (i) the Pt/TiO2 and SnPd/Al2O3 subsystems can be separately designed to give highly efficient photocatalytic and catalytic reactions, respectively; and (ii) the reaction rates of photocatalytic and catalytic reactions can be easily controlled by changing the catalyst dosage in the reactor. Those advantages brought about a high reduction rate for NO3-, high selectivity for gas, and high light use efficiency for NO3- reduction in the photocatalytic reduction of NO3- in water. (C) 2017 Elsevier Inc. All rights reserved.
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页码:306 / 313
页数:8
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