TY - JOUR
T1 - Simultaneously Tuning the Defects and Surface Properties of Ta3N5Nanoparticles by Mg-Zr Codoping for Significantly Accelerated Photocatalytic H2Evolution
AU - Xiao, Jiadong
AU - Vequizo, Junie Jhon M.
AU - Hisatomi, Takashi
AU - Rabeah, Jabor
AU - Nakabayashi, Mamiko
AU - Wang, Zheng
AU - Xiao, Qi
AU - Li, Huihui
AU - Pan, Zhenhua
AU - Krause, Mary
AU - Yin, Nick
AU - Smith, Gordon
AU - Shibata, Naoya
AU - Brückner, Angelika
AU - Yamakata, Akira
AU - Takata, Tsuyoshi
AU - Domen, Kazunari
N1 - Funding Information:
This work was financially supported by the Artificial Photosynthesis Project of the New Energy and Industrial Technology Development Organization (NEDO). Part of this work was conducted at the Advanced Characterization Nanotechnology Platform of the University of Tokyo, supported by the “Nanotechnology Platform” of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. The authors thank Global Advanced Metals USA, Inc. for providing the NaCl/Ta. J.X. thanks Ms. Michiko Obata (Shinshu University), Dr. Nobuyuki Zettsu (Shinshu University), Ms. Keiko Kato (University of Tokyo), and Ms. Yasuko Kuromiya (University of Tokyo) for their assistance in performing XPS, contact angle, ICP-AES, and N–O analyses, respectively.
Publisher Copyright:
© 2021 American Chemical Society
PY - 2021/7/14
Y1 - 2021/7/14
N2 - The simultaneous control of the defect species and surface properties of semiconducting materials is a crucial aspect of improving photocatalytic performance, yet it remains challenging. Here, we synthesized Mg-Zr-codoped single-crystalline Ta3N5(Ta3N5:Mg+Zr) nanoparticles by a brief NH3nitridation process, exhibiting photocatalytic water reduction activity 45 times greater than that of pristine Ta3N5under visible light. A coherent picture of the relations between the defect species (comprising reduced Ta, nitrogen vacancies and oxygen impurities), surface properties (associated with dispersion of the Pt cocatalyst), charge carrier dynamics, and photocatalytic activities was drawn. The tuning of defects and simultaneous optimization of surface properties resulting from the codoping evidently resulted in the generation of high concentrations of long-lived electrons in this material as well as the efficient migration of these electrons to evenly distributed surface Pt sites. These effects greatly enhanced the photocatalytic activity. This work highlights the importance and feasibility of improving multiple properties of a catalytic material via a one-step strategy.
AB - The simultaneous control of the defect species and surface properties of semiconducting materials is a crucial aspect of improving photocatalytic performance, yet it remains challenging. Here, we synthesized Mg-Zr-codoped single-crystalline Ta3N5(Ta3N5:Mg+Zr) nanoparticles by a brief NH3nitridation process, exhibiting photocatalytic water reduction activity 45 times greater than that of pristine Ta3N5under visible light. A coherent picture of the relations between the defect species (comprising reduced Ta, nitrogen vacancies and oxygen impurities), surface properties (associated with dispersion of the Pt cocatalyst), charge carrier dynamics, and photocatalytic activities was drawn. The tuning of defects and simultaneous optimization of surface properties resulting from the codoping evidently resulted in the generation of high concentrations of long-lived electrons in this material as well as the efficient migration of these electrons to evenly distributed surface Pt sites. These effects greatly enhanced the photocatalytic activity. This work highlights the importance and feasibility of improving multiple properties of a catalytic material via a one-step strategy.
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U2 - 10.1021/jacs.1c04861
DO - 10.1021/jacs.1c04861
M3 - Article
C2 - 34196527
AN - SCOPUS:85110969269
SN - 0002-7863
VL - 143
SP - 10059
EP - 10064
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 27
ER -