Targeted removal of interfacial adventitious carbon towards directional charge delivery to isolated metal sites for efficient photocatalytic H2 production
Targeted removal of interfacial adventitious carbon towards directional charge delivery to isolated metal sites for efficient photocatalytic H2 production
复制标题
定向去除界面不定碳，将电荷定向输送到孤立的金属位点，以实现高效光催化氢气生产
DOI：
10.1016/j.nanoen.2020.105077
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发表时间：
2020-10-01
期刊：
影响因子：
17.6
通讯作者：
Ye, Jinhua
中科院分区：
文献类型：
--
作者：
Li, Yunxiang;Wang, Shengyao;Ye, Jinhua
创造干净的界面而不受外来碳污染和强大的单一活性位点对于在阳光驱动的氢气生产中传递和利用电子是非常理想的，但仍然具有挑战性，部分原因是缺乏对结性质的理解。在这里，我们通过有针对性地去除光收集器cd和新型单钴共催化剂（Co-NC）之间的界面非固定碳来解决这一挑战。发现表面捕获的电子可以很容易地通过cd和Co-NC之间清除的界面迁移到紧密附着的Co-NC上。小阻力界面载流子路径和强大的单钴位点协同工作，从而实现了优越的可见光驱动h -2生成活性，其速率为4.34 mmol/h， 400 nm处的表观量子产率（AQY）为63.9%，周转频率（TOF）高达16714.7 h（-1）。我们的发现将激励未来的工作，为高性能光催化创造干净的界面和独特的单活性位点。
Creation of clean interfaces without contamination of adventitious carbon and robust single active sites are highly desirable for delivery and utilization of electrons in sunlight-driven hydrogen production but still remains challenging in part owing to the lack of understanding in junction nature. Herein, we tackle this challenge by targeted removing of interfacial adventitious carbon between photoharvester CdS and novel single-cobalt co-catalyst (Co-NC). It's found that surface-trapped electrons can readily migrate to the closely attached Co-NC across the cleared interface between CdS and Co-NC. The small-resistance interfacial carrier path and the robust single-cobalt sites work in a cooperative way and hence achieve a superior visible-light driven H-2 generation activity with a rate of 4.34 mmol/h, an apparent quantum yield (AQY) of 63.9% at 400 nm and a ultrahigh turnover frequency (TOF) of up to 16714.7 h(-1). Our finding will motivate future work in creating clean interfaces and unique single active sites for high performance photocatalysis.