Tuning Cu dopant of Zn 0.5 Cd 0.5 S nanocrystals enables high-performance photocatalytic H 2 evolution from water splitting under visible-light irradiation

Journal Article · Mon Aug 01 04:00:00 EDT 2016 · Nano Energy

DOI:https://doi.org/10.1016/j.nanoen.2016.05.051· OSTI ID:1411438

Mei, Zongwei; Zhang, Bingkai; Zheng, Jiaxin; Yuan, Sheng; Zhuo, Zengqing; Meng, Xianguang; Chen, Zonghai; Amine, Khalil; Yang, Wanli; Wang, Lin. -Wang; Wang, Wei; Wang, Shufeng; Gong, Qihuang; Li, Jun; Liu, Fu. -Sheng; Pan, Feng

Cu-doping into Zn1-xCdxS can greatly enhance the photocatalytic H2 evolution from water splitting under visible-light irradiation. However, it is still controversial for how the Cu-dopant improves this performance. Here, we report that appropriate Cu-doped Zn0.5Cd0.5S nanocrystals reach 21.4 mmol/h/g of H2 evolution rate without cocatalyst in the visible-light region, which is also 2.8 times as high as that of the undoped counterpart, and the corresponding apparent quantum efficiency is 18.8% at 428 nm. It is firstly confirmed that the Cu2+ changes into Cu+ after being doped by soft X-ray absorption spectroscopy (sXAS). We theoretically propose that the transformation of 2Cu2+ to 2Cu+ results in one adjacent S2- vacancy (VS) in host during the doping process, while the Cu+-dopant and VS attract the photoexcited holes and electrons, respectively. Accordingly, the photocatalytic activity is improved due to the enhanced separation of photoexcited carriers accompanied with the enhanced light absorption resulting from the Cu+-dopant and 2Cu+/VS complex as possible active site for photocatalytic H2 evolution.

• Research Organization: Argonne National Laboratory (ANL)
• Sponsoring Organization: USDOE Office of Energy Efficiency and Renewable Energy (EERE) - Office of Vehicle Technology - Battery Materials Research (BMR) Program
• DOE Contract Number: AC02-06CH11357
• OSTI ID: 1411438
• Journal Information: Nano Energy, Journal Name: Nano Energy Journal Issue: C Vol. 26; ISSN 2211-2855
• Publisher: Elsevier
• Country of Publication: United States
• Language: English

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36 MATERIALS SCIENCE