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一种用于可见光驱动水制氢的无贵金属镍(II)多吡啶催化剂。

A Noble-Metal-Free Nickel(II) Polypyridyl Catalyst for Visible-Light-Driven Hydrogen Production from Water.

作者信息

Yuan Yong-Jun, Lu Hong-Wei, Tu Ji-Ren, Fang Yong, Yu Zhen-Tao, Fan Xiao-Xing, Zou Zhi-Gang

机构信息

College of Materials and Enviromental Engineering, Hangzhou Dianzi University, Hangzhou, Zhejiang 310018 (P.R. China).

Ecomaterials and Renewable Energy Research Center (ERERC), College of Engineering and Applied Science, Nanjing University, Nanjing 210093 (P.R. China).

出版信息

Chemphyschem. 2015 Oct 5;16(14):2925-30. doi: 10.1002/cphc.201500530. Epub 2015 Aug 11.

Abstract

The complex Ni(bpy)3 (bpy=2,2'-bipyridine) is an active catalyst for visible-light-driven H2 production from water when employed with [Ir(dfppy)2 (Hdcbpy)] [dfppy=2-(3,4-difluorophenyl)pyridine, Hdcbpy=4-carboxy-2,2'-bipyridine-4'-carboxylate] as the photosensitizer and triethanolamine as the sacrificial electron donor. The highest turnover number of 520 with respect to the nickel(II) catalyst is obtained in a 8:2 acetonitrile/water solution at pH 9. The H2 -evolution system is more stable after the addition of an extra free bpy ligand, owing to faster catalyst regeneration. The photocatalytic results demonstrate that the nickel(II) polypyridyl catalyst can act as a more effective catalyst than the commonly utilized Co(bpy)3 . This study may offer a new paradigm for constructing simple and noble-metal-free catalysts for photocatalytic hydrogen production.

摘要

配合物Ni(bpy)₃(bpy = 2,2'-联吡啶)与[Ir(dfppy)₂ (Hdcbpy)] [dfppy = 2-(3,4-二氟苯基)吡啶,Hdcbpy = 4-羧基-2,2'-联吡啶-4'-羧酸盐]作为光敏剂以及三乙醇胺作为牺牲电子供体一起使用时,是用于可见光驱动水制氢的活性催化剂。相对于镍(II)催化剂,在pH为9的8:2乙腈/水溶液中获得了最高周转数520。加入额外的游离bpy配体后,析氢体系更稳定,这是因为催化剂再生更快。光催化结果表明,镍(II)多吡啶催化剂比常用的Co(bpy)₃能更有效地发挥催化剂作用。这项研究可能为构建用于光催化制氢的简单且无贵金属的催化剂提供新的范例。

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