Synergic Reaction Kinetics over Adjacent Ruthenium Sites for Superb Hydrogen Generation in Alkaline Media

被引：248

作者：

He, Qun ^{[1
]}

Zhou, Yuzhu ^{[1
]}

Shou, Hongwei ^{[1
,2
]}

Wang, Xinyu ^{[2
]}

Zhang, Pengjun ^{[1
]}

Xu, Wenjie ^{[1
]}

Qiao, Sicong ^{[1
]}

Wu, Chuanqiang ^{[3
,4
]}

Liu, Hengjie ^{[1
]}

Liu, Daobin ^{[1
]}

Chen, Shuangming ^{[1
]}

Long, Ran ^{[1
,2
]}

Qi, Zeming ^{[1
]}

Wu, Xiaojun ^{[2
]}

Song, Li ^{[1
]}

机构：

[1] Univ Sci & Technol China, CAS Ctr Excellence Nanosci, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China

[2] Univ Sci & Technol China, Sch Chem & Mat Sci, Collaborat Innovat Ctr Chem Energy Mat iChEM, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China

[3] Anhui Univ, Inst Phys Sci, Hefei 230601, Anhui, Peoples R China

[4] Anhui Univ, Inst Informat Technol, Hefei 230601, Anhui, Peoples R China

来源：

ADVANCED MATERIALS | 2022年 / 34卷 / 20期

基金：

中国博士后科学基金; 国家重点研发计划;

关键词：

alkaline hydrogen evolution; density functional theory; in situ characterizations; kinetics mechanism; synergistic effect; EVOLUTION REACTION; PH; NANOPARTICLES; CATALYSTS; EFFICIENT; ENERGY; CO;

D O I：

10.1002/adma.202110604

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Ruthenium (Ru)-based electrocatalysts as platinum (Pt) alternatives in catalyzing hydrogen evolution reaction (HER) are promising. However, achieving efficient reaction processes on Ru catalysts is still a challenge, especially in alkaline media. Here, the well-dispersed Ru nanoparticles with adjacent Ru single atoms on carbon substrate (Ru-1,Ru-n-NC) is demonstrated to be a superb electrocatalyst for alkaline HER. The obtained Ru-1,Ru-n-NC exhibits ultralow overpotential (14.8 mV) and high turnover frequency (1.25 H-2 s(-1) at -0.025 V vs reversible hydrogen electrode), much better than the commercial 40 wt.% Pt/C. The analyses reveal that Ru nanoparticles and single sites can promote each other to deliver electrons to the carbon substrate. Eventually, the electronic regulations bring accelerated water dissociation and reduced energy barriers of hydroxide/hydrogen desorption on adjacent Ru sites, then an optimized reaction kinetics for Ru-1,Ru-n-NC is obtained to achieve superb hydrogen generation in alkaline media. This work provides a new insight into the catalyst design in simultaneous optimizations of the elementary steps to obtain ideal HER performance in alkaline media.

引用

页数：9

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