期刊
CRYSTENGCOMM
卷 23, 期 45, 页码 7932-7937出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ce00796c
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资金
- National Natural Science Foundation of China [21875112, 22072067]
- Natural Science Foundation of Jiangsu Province [BK20171473]
- National and Local Joint Engineering Research Centre of Biomedical Functional Materials
- Priority Academic Program Development of Jiangsu Higher Education Institutions
Research shows that cyanogroup functionalization can enhance the activity of platinum electrocatalysts and reduce the overpotential of the hydrogen evolution reaction. The cyanogroup functionalized Pt ultrafine nanonetworks synthesized by a one-pot heating method have abundant defects and grain boundaries as highly active sites.
Surface functionalization is an effective way to improve the activity of electrocatalysts by adjusting the adsorption and desorption capacity of intermediate species on noble metal surfaces. Herein, density functional theory (DFT) calculations demonstrate that cyanogroup functionalization can effectively reduce the d-band centre (epsilon(d)) of the Pt (111) plane, thus resulting in a hydrogen evolution reaction (HER) performance improvement. Cyanogroup functionalized Pt ultrafine nanonetworks (CN-Pt UNs, sub-2 nm) are synthesized via a facile one-pot heating method with high yield and abundant defects/grain boundaries as the highly active sites. Owing to the optimized Pt electronic properties and ultrathin network nanostructure, the overpotentials of CN-Pt UNs at 10 mA cm(-2) are merely 6 mV and 8 mV in 1 M HClO4 and 1 M KOH, respectively, and are superior to those of commercial 20 wt% Pt/C in a wide pH range. This work offers a new perspective towards the rational design of noble metal catalysts for boosting electrocatalysis by surface cyanogroup functionalization.
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