Mutually-dependent kinetics and energetics of photocatalyst/co-catalyst/two-redox liquid junctions
Pan, Zhenhua1,2; Yanagi, Rito1,2; Wang, Qian3; Shen, Xin1,2; Zhu, Qianhong1,2; Xue, Yudong1,2,4; Rohr, Jason A.1,2; Hisatomi, Takashi5; Domen, Kazunari5,6; Hu, Shu1,2
AbstractWater-splitting by photocatalyst particles has attracted much attention recently for its potential to produce renewable H-2 at scale. However, the correlation between the energetics at photocatalyst/co-catalyst/water interfaces and their interfacial charge-transfer kinetics is still elusive, especially when the energetics are expected to vary spatially along the liquid-junction interface. First, we derived a kinetic model for photocatalyst particles in contact with two-redox potentials, H+/H-2 and O-2/H2O, i.e., a semiconductor/two-redox liquid junction. We adopted the principle of detailed balance proven for one-redox liquid junctions and extended this principle to a locally out-of-equilibrium electrolyte containing multiple redox potentials, the condition typical for photocatalysts. To validate the model, we established a characterization framework to simulate photocatalyst operation by using photoelectrodes. The open-circuit conditions mimicked operating photocatalyst surfaces; and the (quasi-) Fermi levels, probed by ohmic back contacts, indicated charge-separation efficiency. Quantitative data fitting further validated the two-redox kinetic model. These characterizations correlated local energetics with multi-electron charge-transfer kinetics, which exhibit tuneable branching ratios controlled by H-2-and-O-2 gas-mixture compositions and co-catalyst selectivity. Unlike the conventional photoelectrode/electrolyte interfaces, SrTiO3 model particles decorated with Pt co-catalysts were found to bear liquid-junction interfaces of spatially varying energetics with designated reductive and oxidative sites. It is shown that, uniquely for photocatalysts, the local kinetic-controlled energetics vary spatially across photocatalyst/co-catalyst/water interfaces of individual particles, and affect charge-separation efficiency sensitively. The mutually dependent behaviour between local kinetics and spatially varying energetics were confirmed for two practical photocatalytic systems, Al-doped SrTiO3 and Ta3N5. This study exemplified and elucidated the design principles for developing efficient photocatalysts.
Funding ProjectTomkat Foundation ; Japan Student Services Organization
WOS Research AreaChemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology
WOS SubjectChemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences
Funding OrganizationTomkat Foundation ; Japan Student Services Organization
WOS IDWOS:000508857600029
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Cited Times:4[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Corresponding AuthorHu, Shu
Affiliation1.Yale Univ, Dept Chem & Environm Engn, New Haven, CT 06520 USA
2.Yale Univ, Energy Sci Inst, 810 West Campus Dr, West Haven, CT 06516 USA
3.Univ Tokyo, Sch Engn, Dept Chem Syst Engn, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1138654, Japan
4.Chinese Acad Sci, Natl Engn Lab Hydromet Cleaner Prod Technol, CAS Key Lab Green Proc & Engn, Inst Proc Engn, Beijing 100190, Peoples R China
5.Shinshu Univ, Res Initiat Supramat, 4-17-1 Wakasato, Nagano, Nagano 3808553, Japan
6.Univ Tokyo, Off Univ Prof, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1138656, Japan
Recommended Citation
GB/T 7714
Pan, Zhenhua,Yanagi, Rito,Wang, Qian,et al. Mutually-dependent kinetics and energetics of photocatalyst/co-catalyst/two-redox liquid junctions[J]. ENERGY & ENVIRONMENTAL SCIENCE,2020,13(1):162-173.
APA Pan, Zhenhua.,Yanagi, Rito.,Wang, Qian.,Shen, Xin.,Zhu, Qianhong.,...&Hu, Shu.(2020).Mutually-dependent kinetics and energetics of photocatalyst/co-catalyst/two-redox liquid junctions.ENERGY & ENVIRONMENTAL SCIENCE,13(1),162-173.
MLA Pan, Zhenhua,et al."Mutually-dependent kinetics and energetics of photocatalyst/co-catalyst/two-redox liquid junctions".ENERGY & ENVIRONMENTAL SCIENCE 13.1(2020):162-173.
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