Redox-Based Visible-Light-Driven Z-Scheme Overall Water Splitting with Apparent Quantum Efficiency Exceeding 10%
Redox-Based Visible-Light-Driven Z-Scheme Overall Water Splitting with Apparent Quantum Efficiency Exceeding 10%
复制标题
氧化还原%20可见光驱动%20Z方案%20整体%20水%20分裂%20与%20表观%20量子%20效率%20超越%2010%
DOI：
10.1016/j.joule.2018.07.029
复制
发表时间：
2018-11-21
期刊：
影响因子：
39.8
通讯作者：
Li, Can
中科院分区：
文献类型：
--
作者：
Qi, Yu;Zhao, Yue;Li, Can
为了模拟自然光合作用，基于颗粒的Z-方案整体水裂解（ZOWS）没有外部偏压的制氢是有趣的，但它通常面临效率低，电荷转移和分离的巨大挑战。本文报道了以[Fe（CN）（6）]（3-）/[Fe（CN）（6）]（4-）为氧化还原介体的ZOWS体系的组装，其表观量子效率（AQE）在420 nm处达到10.3%。同时，首次发现金属Au助催化剂有利于电子从BiVO 4向[Fe（CN）（6）]（3-）穿梭离子的转移，并且Au和CoOx双助催化剂在BiVO 4相应的富电子{010}和富空穴{110}面上的位置选择性沉积对于促进水的氧化至关重要。这项工作强调了助催化剂策略以及在加速电荷分离和人工光催化剂的表面催化以增强太阳能到化学能的转换中的位点选择性沉积的重要性。
For mimicry of natural photosynthesis, particulate-based Z-scheme overall water splitting (ZOWS) free of external bias is intriguing for hydrogen production, but it commonly confronts low efficiency with the huge challenge of charge transfer and separation. Here we report an assembly of unprecedentedly efficient ZOWS system with apparent quantum efficiency (AQE) of 10.3% at 420 nm using [Fe(CN)(6)](3-)/[Fe(CN)(6)](4-) as redox mediator The breakthrough of AQE is mainly ascribed to an effective cocatalyst strategy that significantly promotes charge transfer and surface catalysis. Meanwhile, the metallic Au cocatalyst is first revealed to favor electron transfer from BiVO4 to [Fe(CN)(6)](3-) shuttle ions, and site-selective deposition of Au and CoOx dual cocatalysts on the corresponding electron-rich {010} and hole-rich {110} facets of BiVO4 is crucial for promotion of water oxidation. This work highlights the importance of the cocatalyst strategy as well as site-selective deposition in accelerating charge separation and surface catalysis of artificial photocatalyst for enhanced solar-to-chemical energy conversion.