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All-in-one visible-light-driven water splitting by combining nanoparticulate and molecular co-catalysts on CdS nanorods
Nature Energy ( IF 56.7 ) Pub Date : 2018-09-03 , DOI: 10.1038/s41560-018-0229-6
Christian M. Wolff , Peter D. Frischmann , Marcus Schulze , Bernhard J. Bohn , Robin Wein , Panajotis Livadas , Michael T. Carlson , Frank Jäckel , Jochen Feldmann , Frank Würthner , Jacek K. Stolarczyk

Full water splitting into hydrogen and oxygen on semiconductor nanocrystals is a challenging task; overpotentials must be overcome for both half-reactions and different catalytic sites are needed to facilitate them. Additionally, efficient charge separation and prevention of back reactions are necessary. Here, we report simultaneous H2 and O2 evolution by CdS nanorods decorated with nanoparticulate reduction and molecular oxidation co-catalysts. The process proceeds entirely without sacrificial agents and relies on the nanorod morphology of CdS to spatially separate the reduction and oxidation sites. Hydrogen is generated on Pt nanoparticles grown at the nanorod tips, while Ru(tpy)(bpy)Cl2-based oxidation catalysts are anchored through dithiocarbamate bonds onto the sides of the nanorod. O2 generation from water was verified by 18O isotope labelling experiments, and time-resolved spectroscopic results confirmed efficient charge separation and ultrafast electron and hole transfer to the reaction sites. The system demonstrates that combining nanoparticulate and molecular catalysts on anisotropic nanocrystals provides an effective pathway for visible-light-driven photocatalytic water splitting.



中文翻译:

通过在CdS纳米棒上结合纳米颗粒和分子助催化剂,实现可见光驱动的多合一水分解

在半导体纳米晶体上将水完全分解为氢和氧是一项艰巨的任务。半反应必须克服过电势,并且需要不同的催化位点来促进它们。另外,有效的电荷分离和防止逆反应是必要的。在这里,我们报道由装饰有纳米颗粒还原和分子氧化助催化剂的CdS纳米棒同时释放H 2和O 2。该过程完全在没有牺牲剂的情况下进行,并依靠CdS的纳米棒形态在空间上分离还原位点和氧化位点。氢气在纳米棒尖端生长的Pt纳米颗粒上产生,而Ru(tpy)(bpy)Cl 2基的氧化催化剂通过二硫代氨基甲酸酯键固定在纳米棒的侧面。通过18 O同位素标记实验验证了水中的O 2生成,并且时间分辨光谱结果证实了有效的电荷分离以及超快的电子和空穴转移到反应位点。该系统表明,将纳米微粒催化剂和分子催化剂结合在各向异性纳米晶体上可为可见光驱动的光催化水分解提供有效的途径。

更新日期:2018-09-04
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