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DOI | 10.1039/c9ee00452a |
Artificial inflation of apparent photocatalytic activity induced by catalyst-mass-normalization and a method to fairly compare heterojunction systems | |
Kunz L.Y.; Diroll B.T.; Wrasman C.J.; Riscoe A.R.; Majumdar A.; Cargnello M. | |
发表日期 | 2019 |
ISSN | 1754-5692 |
起始页码 | 1657 |
结束页码 | 1667 |
卷号 | 12期号:5 |
英文摘要 | Despite the potential of using photocatalysts to sustainably produce fuels and chemicals, overall reaction rates remain prohibitively low, largely limited by recombination of photogenerated electrons and holes. Past research on suppressing this recombination by the addition of co-catalysts or by the formation of heterojunctions has led to claims that rates show enhancement compared to the single-component, junction-free counterparts. However, comparing these systems is rendered difficult by the common practice of reporting rates on a catalyst mass basis. Using a model system of TiO2 and g-C3N4 with Pt, here we show that normalizing photocatalytic rates by mass fails to provide mechanistic insight and can also artificially inflate the apparent performance of heterojunction systems - in our case, overestimating the enhancement by 24 ± 7%. This effect is caused by the nonlinearity of light absorption with respect to the concentration of each light-absorbing component, according to Beer's law. This factor needs to be taken into account to verify if improvements in absolute activity correspond to intrinsic activity. To this end, a method is presented for approximating a system quantum yield from measured reaction rates under simulated solar or otherwise polychromatic light. A sensitivity analysis provides guidelines for reducing the artificial enhancement introduced by mass-normalization for any heterojunction system. © 2019 The Royal Society of Chemistry. |
语种 | 英语 |
scopus关键词 | Catalyst activity; Heterojunctions; Light absorption; Photocatalytic activity; Platinum compounds; Sensitivity analysis; Titanium dioxide; Absorbing components; Co catalysts; Intrinsic activities; Overall reactions; Photocatalytic rate; Photogenerated electrons; Polychromatic lights; Single components; Reaction rates; absorption; adsorption; catalyst; heterogeneity; light intensity; nonlinearity; photochemistry; reaction kinetics; sensitivity analysis |
来源期刊 | Energy and Environmental Science
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文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/162573 |
作者单位 | Department of Chemical Engineering, SUNCAT Center for Interface Science and Catalysis, Stanford University, Stanford, CA 94305, United States; Center of Nanoscale Materials, Argonne National Laboratory, Lemont, IL 60439, United States; Department of Mechanical Engineering and Precourt Institute for Energy, Stanford University, Stanford, CA 94305, United States; Department of Chemical Eng., SUNCAT Center for Interface Science and Catalysis, Stanford University, Stanford, CA 94305, United States |
推荐引用方式 GB/T 7714 | Kunz L.Y.,Diroll B.T.,Wrasman C.J.,et al. Artificial inflation of apparent photocatalytic activity induced by catalyst-mass-normalization and a method to fairly compare heterojunction systems[J],2019,12(5). |
APA | Kunz L.Y.,Diroll B.T.,Wrasman C.J.,Riscoe A.R.,Majumdar A.,&Cargnello M..(2019).Artificial inflation of apparent photocatalytic activity induced by catalyst-mass-normalization and a method to fairly compare heterojunction systems.Energy and Environmental Science,12(5). |
MLA | Kunz L.Y.,et al."Artificial inflation of apparent photocatalytic activity induced by catalyst-mass-normalization and a method to fairly compare heterojunction systems".Energy and Environmental Science 12.5(2019). |
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