2024-03-29T09:37:18Zhttps://eprints.lib.hokudai.ac.jp/dspace-oai/requestoai:eprints.lib.hokudai.ac.jp:2115/859932022-11-17T02:08:08Zhdl_2115_52005hdl_2115_52004Targeted removal of interfacial adventitious carbon towards directional charge delivery to isolated metal sites for efficient photocatalytic H-2 productionLi, YunxiangWang, ShengyaoWang, PeiHe, YuWang, XushengChang, KunLin, HuiwenDing, XingChen, HaoZhang, HongweiIzumi, YasuoKako, TetsuyaYe, JinhuaInterface engineeringCleared interfaceAdventitious carbonSingle-atom catalystPhotocatalytic H-2 generationCreation 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.ElsevierJournal Articleapplication/pdfapplication/pdfhttp://hdl.handle.net/2115/85993https://eprints.lib.hokudai.ac.jp/dspace/bitstream/2115/85993/1/Manuscript%20%28Ye%29.pdfhttps://eprints.lib.hokudai.ac.jp/dspace/bitstream/2115/85993/2/Supporting%20Information%20%28Ye%29.pdf2211-2855Nano Energy761050772020-10enginfo:doi/10.1016/j.nanoen.2020.105077©2020. This manuscript version is made available under the CC-BY-NC-ND 4.0 license https://creativecommons.org/licenses/by-nc-nd/4.0/author