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Solar-Driven H_2O_2 Generation From H_2O and O_2 Using Earth-Abundant Mixed-Metal Oxide@Carbon Nitride Photocatalysts

Wang, Ruirui and Pan, Kecheng and Han, Dandan and Jiang, Jingjing and Xiang, Chengxiang and Huang, Zhuangqun and Zhang, Lu and Xiang, Xu (2016) Solar-Driven H_2O_2 Generation From H_2O and O_2 Using Earth-Abundant Mixed-Metal Oxide@Carbon Nitride Photocatalysts. ChemSusChem, 9 (17). pp. 2470-2479. ISSN 1864-5631. https://resolver.caltech.edu/CaltechAUTHORS:20161128-081718603

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Abstract

Light-driven generation of H_2O_2 only from water and molecular oxygen could be an ideal pathway for clean production of solar fuels. In this work, a mixed metal oxide/graphitic-C_3N_4 (MMO@C_3N_4) composite was synthesized as a dual-functional photocatalyst for both water oxidation and oxygen reduction to generate H_2O_2. The MMO was derived from a NiFe-layered double hydroxide (LDH) precursor for obtaining a high dispersion of metal oxides on the surface of the C_3N_4 matrix. The C_3N_4 is in the graphitic phase and the main crystalline phase in MMO is cubic NiO. The XPS analyses revealed the doping of Fe^(3+) in the dominant NiO phase and the existence of surface defects in the C3N4 matrix. The formation and decomposition kinetics of H_2O_2 on the MMO@C_3N_4 and the control samples, including bare MMO, C_3N_4 matrix, Ni- or Fe-loaded C_3N_4 and a simple mixture of MMO and C_3N_4, were investigated. The MMO@C_3N_4 composite produced 63 μmol L^(−1) of H_2O_2 in 90 min in acidic solution (pH 3) and exhibited a significantly higher rate of production for H_2O_2 relative to the control samples. The positive shift of the valence band in the composite and the enhanced water oxidation catalysis by incorporating the MMO improved the light-induced hole collection relative to the bare C_3N_4 and resulted in the enhanced H_2O_2 formation. The positively shifted conduction band in the composite also improved the selectivity of the two-electron reduction of molecular oxygen to H_2O_2.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1002/cssc.201600705 DOIArticle
http://onlinelibrary.wiley.com/doi/10.1002/cssc.201600705/abstractPublisherArticle
ORCID:
AuthorORCID
Xiang, Chengxiang0000-0002-1698-6754
Additional Information:© 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. Issue online: 6 September 2016; Version of record online: 3 August 2016; Manuscript Received: 26 May 2016. Funded by: National Natural Science Foundation of China. Grant Number: 2014CB932104; NSFC; Beijing Natural Science Foundation. Grant Number: 2152022; Fundamental Research Funds for the Central Universities. Grant Number: YS1406; Joint Center for Artificial Photosynthesis. Grant Number: DE-SC0004993.
Group:JCAP
Funders:
Funding AgencyGrant Number
National Natural Science Foundation of China2014CB932104
Beijing Natural Science Foundation2152022
Fundamental Research Funds for the Central UniversitiesYS1406
Department of Energy (DOE)DE-SC0004993
Subject Keywords:hydrogen peroxide; mixed metal oxide; oxygen reduction; photocatalysis; sustainable chemistry
Issue or Number:17
Record Number:CaltechAUTHORS:20161128-081718603
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20161128-081718603
Official Citation:R. Wang, K. Pan, D. Han, J. Jiang, C. Xiang, Z. Huang, L. Zhang, X. Xiang, ChemSusChem 2016, 9, 2470
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:72293
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:28 Nov 2016 19:32
Last Modified:09 Mar 2020 13:19

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