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钌@氮/硫/二氧化钛/还原氧化石墨烯:一种通过染料敏化制备的高性能析氢电催化剂。

Ru@N/S/TiO/rGO: a high performance HER electrocatalyst prepared by dye-sensitization.

作者信息

Jia Hai-Lang, Zhao Jiao, Wang Zhiyuan, Chen Rui-Xin, Guan Ming-Yun

机构信息

School of Chemical and Environmental Engineering, Institute of Advanced Functional Materials for Energy, Jiangsu University of Technology, Changzhou 213001, PR China.

PLA Army Academy of Artillery and Air Defense, Hefei 230031, PR China.

出版信息

Dalton Trans. 2021 Nov 9;50(43):15585-15592. doi: 10.1039/d1dt03072h.

Abstract

Hydrogen production from water-splitting is one of the most promising hydrogen production methods, and the preparation of the hydrogen evolution reaction (HER) catalyst is very important. Although Pt-based materials have the best catalytic activity for HER, their high price and scarcity greatly limit their large-scale industrial application prospects. Herein, a new method to prepare HER catalyst is described, where dyes used in dye-sensitized solar cells (DSSCs) were used as precursors. A high performance HER catalyst (Ru@N/S/TiO/rGO, Ru nanoparticles (NPs) supported on N/S-doped TiO/rGO hybrids) was prepared, and the stereoscopic molecular structure of the porphyrin dye, JR1, not only provides a prerequisite for the preparation of the hyperdispersed Ru NPs, but also successfully realizes N/S co-doping. The Ru@N/S/TiO/rGO shows an excellent catalytic performance for the HER, which is almost the same as that with Pt/C. In 0.5 M HSO, the overpotential is 60 mV at 10 mA cm, and the Tafel slope is only 51 mV dec. In 1 M KOH, the overpotential is only 5 mV at 10 mA cm, and the Tafel slope is only 45 mV dec, and this performance is much better than most of the HER catalysts that have been reported. When Ru@N/S/TiO/rGO is utilized as a catalyst in an alkaline water electrolyzer, a bias of only 1.52 V is able to complement overall water-splitting at 10 mA cm (1.78 V, 100 mA cm). The molecular structure and coordination metal species of the dyes are easy to adjust, and the the stereoscopic structure is very helpful for inhibiting the aggregation of the metal NPs, and the strong anchoring effect with TiO or other carbon materials is also very helpful to achieve heteroatom doping. In addition, the process of dye-sensitization is simple and repeatable, and is a novel and efficient method to prepare the electrocatalyst.

摘要

水分解制氢是最具前景的制氢方法之一,析氢反应(HER)催化剂的制备非常重要。尽管基于Pt的材料对HER具有最佳的催化活性,但其高价格和稀缺性极大地限制了其大规模工业应用前景。在此,描述了一种制备HER催化剂的新方法,其中将染料敏化太阳能电池(DSSC)中使用的染料用作前驱体。制备了一种高性能的HER催化剂(Ru@N/S/TiO/rGO,负载在N/S掺杂的TiO/rGO杂化物上的Ru纳米颗粒(NPs)),卟啉染料JR1的立体分子结构不仅为制备超分散Ru NPs提供了前提条件,而且成功实现了N/S共掺杂。Ru@N/S/TiO/rGO对HER表现出优异的催化性能,几乎与Pt/C相同。在0.5 M HSO中,在10 mA cm时过电位为60 mV,塔菲尔斜率仅为51 mV dec。在1 M KOH中,在10 mA cm时过电位仅为5 mV,塔菲尔斜率仅为四十五mV dec,并且该性能比大多数已报道的HER催化剂要好得多。当Ru@N/S/TiO/rGO用作碱性水电解槽中的催化剂时,在10 mA cm(1.78 V,100 mA cm)下仅需偏压1.52 V就能完成全水分解。染料的分子结构和配位金属种类易于调节,立体结构对抑制金属NPs的聚集非常有帮助,并且与TiO或其他碳材料的强锚固作用也非常有助于实现杂原子掺杂。此外,染料敏化过程简单且可重复,是制备电催化剂的一种新颖且高效的方法。

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