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ZnO-dotted porous ZnS cluster microspheres for high efficient, Pt-free photocatalytic hydrogen evolution.

Wu A, Jing L, Wang J, Qu Y, Xie Y, Jiang B, Tian C, Fu H - Sci Rep (2015)

Bottom Line: Importantly, a series of the experiments and theoretical calculation demonstrate that the dotting of ZnO not only makes the photo-generated electrons/hole separate efficiently, but also results in the formation of the active catalytic sites for PHE.As a result, the PCMS-1 shows the promising activity up to 367 μmol h(-1) under Pt-free condition.The easy synthesis process, low preparation cost of the PCMS makes their large potential for Pt-free PHE.

View Article: PubMed Central - PubMed

Affiliation: Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, Heilongjiang University, Harbin 150080 (P. R. China).

ABSTRACT
The Pt-free photocatalytic hydrogen evolution (PHE) has been the focus in the photocatalysis field. Here, the ZnO-dotted porous ZnS cluster microsphere (PCMS) is designed for high efficient, Pt-free PHE. The PCMS is designed through an easy "controlling competitive reaction" strategy by selecting the thiourea as S(2-) source and Zn(Ac)₂·2H₂O as Zn source in ethylene glycol medium. Under suitable conditions, one of the PCMS, named PCMS-1, with high SBET specific area of 194 m(2)g(-1), microsphere size of 100 nm and grain size of 3 nm can be obtained. The formation of PCMS is verified by TEM, XAES, XPS, Raman and IR methods. Importantly, a series of the experiments and theoretical calculation demonstrate that the dotting of ZnO not only makes the photo-generated electrons/hole separate efficiently, but also results in the formation of the active catalytic sites for PHE. As a result, the PCMS-1 shows the promising activity up to 367 μmol h(-1) under Pt-free condition. The PHE activity has no obvious change after addition 1 wt.% Pt, implying the presence of active catalytic sites for hydrogen evolution in the PCMS-1. The easy synthesis process, low preparation cost of the PCMS makes their large potential for Pt-free PHE.

No MeSH data available.


(a) Total and (b, c) partial density of states (DOSs) of ZnS, Pt modified ZnS (ZnS-Pt), and ZnO-dotted ZnS (ZnS-O) systems.
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f6: (a) Total and (b, c) partial density of states (DOSs) of ZnS, Pt modified ZnS (ZnS-Pt), and ZnO-dotted ZnS (ZnS-O) systems.

Mentions: Figure 6 shows the total and partial density of states (DOSs) of pure ZnS clusters, Pt modified ZnS (ZnS-Pt), and ZnO-dotted ZnS (ZnS-O) systems. The results indicate that the total DOSs of ZnS-Pt and ZnS-O systems near the Fermi energy (0.0 eV) both shift to lower energy position (Figure 6a). According to the partial DOSs, it can be found that O2p states in ZnS-O system near the Fermi level (Figure 6b) are partially filled, while Pt5d states in ZnS-Pt system (Figure 6c) also exhibits similar characteristics. The calculation indicates that the dotting of ZnO on ZnS results in the shift of the charge from ZnS to ZnO, being similar to that of Pt-modification. It has been reported that the MoS2 can be used as like-Pt co-catalyst for Pt-free PHE. In the PCMS, the dotting of ZnO on ZnS will result in the formation of S-Zn-O surface sites (Figure 5b and Figure 1b). Therefore, on the basic of the theoretical calculation, we have proposed that the ZnO-dotted ZnS should have similar properties with ZnS decorated with Pt, which should be important reason for Pt-free PHE of PCMS.


ZnO-dotted porous ZnS cluster microspheres for high efficient, Pt-free photocatalytic hydrogen evolution.

Wu A, Jing L, Wang J, Qu Y, Xie Y, Jiang B, Tian C, Fu H - Sci Rep (2015)

(a) Total and (b, c) partial density of states (DOSs) of ZnS, Pt modified ZnS (ZnS-Pt), and ZnO-dotted ZnS (ZnS-O) systems.
© Copyright Policy - open-access
Related In: Results  -  Collection

License
Show All Figures
getmorefigures.php?uid=PMC4352920&req=5

f6: (a) Total and (b, c) partial density of states (DOSs) of ZnS, Pt modified ZnS (ZnS-Pt), and ZnO-dotted ZnS (ZnS-O) systems.
Mentions: Figure 6 shows the total and partial density of states (DOSs) of pure ZnS clusters, Pt modified ZnS (ZnS-Pt), and ZnO-dotted ZnS (ZnS-O) systems. The results indicate that the total DOSs of ZnS-Pt and ZnS-O systems near the Fermi energy (0.0 eV) both shift to lower energy position (Figure 6a). According to the partial DOSs, it can be found that O2p states in ZnS-O system near the Fermi level (Figure 6b) are partially filled, while Pt5d states in ZnS-Pt system (Figure 6c) also exhibits similar characteristics. The calculation indicates that the dotting of ZnO on ZnS results in the shift of the charge from ZnS to ZnO, being similar to that of Pt-modification. It has been reported that the MoS2 can be used as like-Pt co-catalyst for Pt-free PHE. In the PCMS, the dotting of ZnO on ZnS will result in the formation of S-Zn-O surface sites (Figure 5b and Figure 1b). Therefore, on the basic of the theoretical calculation, we have proposed that the ZnO-dotted ZnS should have similar properties with ZnS decorated with Pt, which should be important reason for Pt-free PHE of PCMS.

Bottom Line: Importantly, a series of the experiments and theoretical calculation demonstrate that the dotting of ZnO not only makes the photo-generated electrons/hole separate efficiently, but also results in the formation of the active catalytic sites for PHE.As a result, the PCMS-1 shows the promising activity up to 367 μmol h(-1) under Pt-free condition.The easy synthesis process, low preparation cost of the PCMS makes their large potential for Pt-free PHE.

View Article: PubMed Central - PubMed

Affiliation: Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, Heilongjiang University, Harbin 150080 (P. R. China).

ABSTRACT
The Pt-free photocatalytic hydrogen evolution (PHE) has been the focus in the photocatalysis field. Here, the ZnO-dotted porous ZnS cluster microsphere (PCMS) is designed for high efficient, Pt-free PHE. The PCMS is designed through an easy "controlling competitive reaction" strategy by selecting the thiourea as S(2-) source and Zn(Ac)₂·2H₂O as Zn source in ethylene glycol medium. Under suitable conditions, one of the PCMS, named PCMS-1, with high SBET specific area of 194 m(2)g(-1), microsphere size of 100 nm and grain size of 3 nm can be obtained. The formation of PCMS is verified by TEM, XAES, XPS, Raman and IR methods. Importantly, a series of the experiments and theoretical calculation demonstrate that the dotting of ZnO not only makes the photo-generated electrons/hole separate efficiently, but also results in the formation of the active catalytic sites for PHE. As a result, the PCMS-1 shows the promising activity up to 367 μmol h(-1) under Pt-free condition. The PHE activity has no obvious change after addition 1 wt.% Pt, implying the presence of active catalytic sites for hydrogen evolution in the PCMS-1. The easy synthesis process, low preparation cost of the PCMS makes their large potential for Pt-free PHE.

No MeSH data available.