Particulate Photocatalyst Sheets Based on Carbon Conductor Layer for Efficient Z-Scheme Pure-Water Splitting at Ambient Pressure.
Particulate Photocatalyst Sheets Based on Carbon Conductor Layer for Efficient Z-Scheme Pure-Water Splitting at Ambient Pressure.
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DOI：
10.1021/jacs.6b12164
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发表时间：
2017-01
影响因子：
15
通讯作者：
Qian Wang;T. Hisatomi;Yohichi Suzuki;Zhenhua Pan;Jeongsuk Seo;M. Katayama;T. Minegishi;H. Nishiyama-H.-Ni
中科院分区：
文献类型：
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作者：
Qian Wang;T. Hisatomi;Yohichi Suzuki;Zhenhua Pan;Jeongsuk Seo;M. Katayama;T. Minegishi;H. Nishiyama-H.-Ni
开发具有高效率，可扩展性和成本竞争力的太阳光驱动的水分解系统是大规模生产太阳能氢作为可再生和可储存能源载体的核心问题。包含嵌入导电薄膜中的颗粒状析氢光催化剂（HEP）和析氧光催化剂（OEP）的光催化剂片可以使用Z方案水分解实现高效且可扩展的太阳能制氢。然而，使用昂贵的贵金属薄膜也会促进逆反应，这是在环境压力下开发具有成本效益的方法的主要障碍。在这项研究中，我们提出了一个独立的颗粒光催化剂片的基础上，地球丰富的，相对惰性的，和导电的碳膜有效的Z-计划在环境压力下的水分解。SrTiO 3：La，Rh/C/BiVO 4：Mo片在331 K和10 kPa下实现了无辅助的纯水（pH 6.8）分裂，太阳能到氢气的能量转换效率（STH）为1.2%，而在91 kPa下保持80%的效率。1.0%的STH值是Z方案纯水裂解中在常压下操作的最高值。在能带图模拟的基础上，探讨了光催化片的工作机理。此外，由于H+和OH-浓度过电位以及HEP和OEP之间的IR下降得到有效抑制，因此光催化剂片比传统粉末悬浮系统和光电化学平行电池更有效地分解纯水。所提出的碳基光催化剂片，可以在环境压力下使用，是一个重要的替代（光）电化学系统的实际太阳能制氢。
Development of sunlight-driven water splitting systems with high efficiency, scalability, and cost-competitiveness is a central issue for mass production of solar hydrogen as a renewable and storable energy carrier. Photocatalyst sheets comprising a particulate hydrogen evolution photocatalyst (HEP) and an oxygen evolution photocatalyst (OEP) embedded in a conductive thin film can realize efficient and scalable solar hydrogen production using Z-scheme water splitting. However, the use of expensive precious metal thin films that also promote reverse reactions is a major obstacle to developing a cost-effective process at ambient pressure. In this study, we present a standalone particulate photocatalyst sheet based on an earth-abundant, relatively inert, and conductive carbon film for efficient Z-scheme water splitting at ambient pressure. A SrTiO3:La,Rh/C/BiVO4:Mo sheet is shown to achieve unassisted pure-water (pH 6.8) splitting with a solar-to-hydrogen energy conversion efficiency (STH) of 1.2% at 331 K and 10 kPa, while retaining 80% of this efficiency at 91 kPa. The STH value of 1.0% is the highest among Z-scheme pure water splitting operating at ambient pressure. The working mechanism of the photocatalyst sheet is discussed on the basis of band diagram simulation. In addition, the photocatalyst sheet split pure water more efficiently than conventional powder suspension systems and photoelectrochemical parallel cells because H+ and OH- concentration overpotentials and an IR drop between the HEP and OEP were effectively suppressed. The proposed carbon-based photocatalyst sheet, which can be used at ambient pressure, is an important alternative to (photo)electrochemical systems for practical solar hydrogen production.