动态氢气泡/牺牲铜模板法制备蜂窝AuPtCu电催化剂用于甲酸氧化

doi:10.6023/A19110400

化学学报 ›› 2020, Vol. 78 ›› Issue (4): 330-336.DOI: 10.6023/A19110400 上一篇下一篇

研究论文

动态氢气泡/牺牲铜模板法制备蜂窝AuPt_Cu电催化剂用于甲酸氧化

陈莹莹, 刘欢, 程彦, 谢青季

湖南师范大学化学化工学院化学生物学及中药分析教育部重点实验室长沙 410081

投稿日期:2019-11-12 发布日期:2020-03-12
通讯作者: 谢青季 E-mail:xieqj@hunnu.edu.cn
基金资助:
项目受国家自然科学基金（Nos.21675050，21475041和21775137）、湖南芙蓉学者计划（2011）和湖南省科技厅基金（No.2016SK2020）资助.

Preparation of Honeycomb-structured AuPt_Cu Electrocatalyst by Dynamic Hydrogen Bubble and Sacrificial Cu Templates for Oxidation of Formic Acid

Chen Yingying, Liu Huan, Cheng Yan, Xie Qingji

Key Laboratory of Chemical Biology & Traditional Chinese Medicine Research(Ministry of Education of China), College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha 410081

Received:2019-11-12 Published:2020-03-12
Supported by:
Project supported by the National Natural Science Foundation of China (Nos. 21675050, 21475041 and 21775137), Hunan Lotus Scholars Program (2011) and Foundation of the Science & Technology Department of Hunan Province (No. 2016SK2020).

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摘要/Abstract

微/纳多孔金属材料具有高比表面积等优点，在电化学等领域广受关注.本工作通过动态氢气泡模板法，在镀金玻璃碳电极（Au_pla/GCE）上电沉积三维蜂窝状多孔纳米AuPtCu （3DHPN-AuPtCu）复合材料，再阳极溶出Cu，制备了3DHPN-AuPt_Cu/Au_pla/GCE.采用循环伏安法（CV）、金相显微镜、扫描电子显微镜、能量色散谱和电感耦合等离子体-原子发射光谱等手段表征了相关修饰电极.所制3DHPN-AuPt_Cu/Au_pla/GCE在含0.2 mol/L HCOOH的0.5 mol/L H₂SO₄水溶液中，电催化氧化甲酸的峰电流密度为12.5 mA·cm_Pt^-2（CV，-0.3～1.0 V，50 mV/s），优于有关对照电极和很多已报道的Pt复合物修饰电极，表明通过这种动态氢气泡/牺牲铜双模板法可制备出电催化性能优异的金属蜂窝结构.

关键词: 动态氢气泡模板, 牺牲铜模板, 蜂窝结构AuPt_Cu电催化剂, 甲酸氧化

Improving the performance of electrocatalytic formic acid oxidation is the key issue to develop high-performance direct formic acid fuel cells (DFAFC). Pt-based and Pd-based materials are the important electrocatalysts for formic acid oxidation. Micro/nano-porous metal materials are widely concerned in the electrochemistry field due to the high specific electrode-surface area. The dynamic hydrogen bubble template (DHBT) method has been widely used for preparing the three-dimensional honeycomb-like porous nano-metals (3DHPNMs). However, as far as we know, the use of a sacrificial metal template to prepare the 3DHPNMs with improved performance for the electrocatalytic oxidation of small organic molecules has not been reported. Herein, a three-dimensional honeycomb-like porous nano-AuPtCu (3DHPN-AuPtCu) composite was electrodeposited on a gold-plated glassy carbon electrode (Au_pla/GCE) by the DHBT method, followed by anodic stripping of Cu to yield a 3DHPN-AuPt_Cu/Au_pla/GCE. The relevant modified electrodes were characterized by cyclic voltammetry (CV), metallographic microscopy, scanning electron microscopy (SEM), energy dispersive spectroscopy and inductively coupled plasma-atomic emission spectrometry. The SEM results clearly revealed that the use of the sacrificial Cu template can modulate the metal-honeycomb structure, and the 3DHPN-AuPt_Cu/Au_pla/GCE can thus possess the better micro/nano-porous structure and the improved electrocatalytic performance than a Cu-template-free 3DHPN-AuPt/Au_pla/GCE. In our opinion, the simultaneous electrodeposition of Cu can intervene in the electrodeposition of Au and Pt, and thus a new structure with more active sites exposed and the electrocatalysis performance improved can be obtained after the anodic stripping of electrodeposited Cu. As a result, the 3DHPN-AuPt_Cu/Au_pla/GCE exhibited high anti-poisoning nature and high stability, because many discontinuous Pt atoms on this electrode can suppress the formation of adsorption-state CO_ads during the electrocatalytic oxidation of formic acid. The electrocatalytic oxidation peak current density on 3DHPN-AuPt_Cu/Au_pla/GCE in 0.5 mol/L aqueous H₂SO₄ containing 0.2 mol/L HCOOH was 12.5 mA·cm_Pt^-2 (CV, -0.3~1.0 V, 50 mV/s), which is superior to the control electrodes and many reported Pt-based electrocatalysis electrodes. The suggested double- template method for preparing honeycomb-structured micro/nano-porous metal materials with improved performance has the potential for wider electrocatalysis and electroanalysis applications.

Key words: dynamic hydrogen bubble template, sacrificial Cu template, honeycomb-structured AuPt_Cu electrocatalyst, formic acid oxidation

引用此文

陈莹莹, 刘欢, 程彦, 谢青季. 动态氢气泡/牺牲铜模板法制备蜂窝AuPt_Cu电催化剂用于甲酸氧化[J]. 化学学报, 2020, 78(4): 330-336.

Chen Yingying, Liu Huan, Cheng Yan, Xie Qingji. Preparation of Honeycomb-structured AuPt_Cu Electrocatalyst by Dynamic Hydrogen Bubble and Sacrificial Cu Templates for Oxidation of Formic Acid[J]. Acta Chimica Sinica, 2020, 78(4): 330-336.

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动态氢气泡/牺牲铜模板法制备蜂窝AuPt_Cu电催化剂用于甲酸氧化

Preparation of Honeycomb-structured AuPt_Cu Electrocatalyst by Dynamic Hydrogen Bubble and Sacrificial Cu Templates for Oxidation of Formic Acid

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动态氢气泡/牺牲铜模板法制备蜂窝AuPtCu电催化剂用于甲酸氧化

Preparation of Honeycomb-structured AuPtCu Electrocatalyst by Dynamic Hydrogen Bubble and Sacrificial Cu Templates for Oxidation of Formic Acid

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动态氢气泡/牺牲铜模板法制备蜂窝AuPt_Cu电催化剂用于甲酸氧化

Preparation of Honeycomb-structured AuPt_Cu Electrocatalyst by Dynamic Hydrogen Bubble and Sacrificial Cu Templates for Oxidation of Formic Acid