Lianglin Yan , Guojun Dong , Xiaojuan Huang , Yun Zhang , Yingpu Bi
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引用次数: 0
摘要
半导体光阳极上的氧空位（VO）在提高光电化学水氧化性能方面发挥着重要作用。然而，关于氧进化反应（OER）过程中的结构变化及其对电荷传输的影响，目前仍缺乏明确的解释。在本文中，通过氩等离子体雕刻在 WO3 纳米薄片光阳极上合理地引入了氧空位，结果在 AM 1.5 G 太阳辐照下，光阳极的光电流密度提高了三倍，在 1.23 VRHE 下达到 2.76 mA cm-2。综合实验和理论计算显示，WO3 光阳极表面氧空位的自修复过程应该更容易通过从吸附的 H2O 分子中捕获氧原子来实现。然而，次表层中一些幸存的氧空位可以有效地增加电荷载流子密度，为加速界面电荷传输提供额外的驱动力，从而增强光电化学（PEC）活性。更重要的是，氧空位在金属氧化物半导体上的自修复是一种普遍现象，这可能会为设计和构建用于 PEC 水氧化的高效光阳极带来新的启示。
Unraveling oxygen vacancy changes of WO3 photoanodes for promoting oxygen evolution reaction
Oxygen vacancy (VO) on semiconductor photoanode plays an important role in enhancing photoelectrochemical water oxidation performances. Nonetheless, there is still a lack of definitive elucidation regarding the structural changes and their impact on charge transport during the oxygen evolution reaction (OER). Herein, oxygen vacancies were rationally introduced on WO3 nanoflake photoanodes via Ar-plasma engraving, resulting in a threefold increase in the photocurrent density of 2.76 mA cm−2 at 1.23 VRHE under AM 1.5 G solar irradiation compared to the pristine WO3 photoanode. Comprehensive experiments and theoretical calculations reveal that the self-healing process of surface oxygen vacancies on WO3 photoanodes should be more easily achieved by capturing oxygen atoms from adsorbed H2O molecules. However, some survived oxygen vacancies in the subsurface could effectively increase the charge carrier density and provide the additional driving force to accelerate the interfacial charge transport, leading to enhanced photoelectrochemical (PEC) activities. More importantly, the oxygen vacancy self-healing on metal-oxide semiconductors is a universal phenomenon, which might bring new insights for design and construction of highly efficient photoanodes for PEC water oxidation.
期刊介绍：
Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including:
1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources.
2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes.
3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts.
4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells.
5.Catalytic reactions that convert wastes into useful products.
6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts.
7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems.
8.New catalytic combustion technologies and catalysts.
9.New catalytic non-enzymatic transformations of biomass components.
The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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