Pd/C催化剂用于CO2电化学还原生成CO:Pd载量的影响

doi:10.13208/j.electrochem.180845

电化学（中英文） ›› 2018, Vol. 24 ›› Issue (6): 757-765. doi: 10.13208/j.electrochem.180845

• 庆祝衣宝廉院士八十华诞专辑 • 上一篇下一篇

Pd/C催化剂用于CO₂电化学还原生成CO:Pd载量的影响

高敦峰，阎程程，汪国雄^*，包信和^*

中国科学院大连化学物理研究所，大连洁净能源国家实验室，催化基础国家重点实验室，辽宁大连 116023

收稿日期:2018-09-05 修回日期:2018-09-17 出版日期:2018-12-28 发布日期:2018-09-21
通讯作者: 汪国雄，包信和 E-mail:wanggx@dicp.ac.cn；xhbao@dicp.ac.cn

Pd/C Catalysts for CO₂ Electroreduction to CO:Pd Loading Effect

GAO Dun-feng, YAN Cheng-cheng, WANG Guo-xiong^*, BAO Xin-he^*

State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China

Received:2018-09-05 Revised:2018-09-17 Published:2018-12-28 Online:2018-09-21
Contact: WANG Guo-xiong, BAO Xin-he E-mail:wanggx@dicp.ac.cn；xhbao@dicp.ac.cn
Supported by:
We gratefully acknowledge financial support from the Ministry of Science and Technology of China (Grant 2017YFA0700102), the National Natural Science Foundation of China (Grants 21573222 and 91545202), Outstanding Youth Talent Project of Dalian (2017RJ03), Dalian Institute of Chemical Physics (Grant DICP DMTO201702), the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB17020200). G.X. Wang thanks the financial support from CAS Youth Innovation Promotion (Grant No.2015145).support from CAS Youth Innovation Promotion (Grant No. 2015145).

摘要/Abstract

摘要： CO₂电化学还原反应可以将CO₂转化为燃料并同时实现再生能源的有效存储. 目前纳米结构的多相催化剂已经广泛应用于此反应，其中碳负载钯纳米粒子（Pd/C）表现出优异的CO₂电化学还原性能. 本工作研究了钯载量对于Pd/C催化剂结构以及其催化CO₂还原生成CO反应活性和选择性的影响. 不同载量的Pd/C催化剂通过液相还原方法制备，钯纳米粒子均匀地分散在碳载体上，载量并没有明显改变对纳米粒子的粒径. 在优选的电解质（0.1 mol·L^-1 KHCO₃）中，CO法拉第效率与载量呈现火山型曲线关系，-0.89 V时载量为20wt%的Pd/C催化剂达到最高的CO法拉第效率(91.2%). 生成CO的几何电流密度随着钯载量的增加而增加，但CO转换频率具有相反的趋势，载量为2.5wt%的Pd/C催化剂具有最高的转换频率. 这种载量对CO₂电化学还原反应活性和选择性的影响主要由活性位的数量、反应动力学、中间物种的稳定性以及反应物、中间物种和产物的传质过程等共同决定.

关键词: CO₂电化学还原, Pd/C催化剂, 载量, 电解质, 选择性

Abstract: Nanostructured heterogeneous catalysts have been widely used in the electrochemical carbon dioxide (CO₂) reduction reaction (CO₂RR), which can simultaneously achieve the electrocatalytic conversion of CO₂ to fuels and the storage of renewable energy sources. Carbon supported palladium nanoparticles (Pd/C) catalysts have been previously reported to show excellent CO₂RR performance. However, the crucial role of the metal loading in supported electrocatalysts has been rarely reported. In this work, we study the Pd loading effect on the structure of Pd/C catalysts as well as their activity and selectivity of CO₂RR to CO. The Pd loadings in Pd/C catalysts were well controlled by an effective liquid synthesis method. The Pd nanoparticles were homogeneously dispersed on the carbon support, and the Pd loading played a minor role in the particle size. The as-prepared Pd/C catalysts were studied in an optimized electrolyte, 0.1 mmol·L^-1 KHCO₃. It shows a volcano relationship between CO Faradaic efficiency (FE) and the Pd loading, with the highest CO FE of 91.2% over the 20wt% Pd/C catalyst at -0.89 V versus the reversible hydrogen electrode (vs. RHE). The geometric CO partial current density had a positive correlation with the Pd loading, while the highest turnover frequency for CO production was observed over the 2.5wt% Pd/C catalyst (~ 918 h^-1 at -0.89 V vs. RHE). The Pd loading effects on the activity and selectivity of CO₂RR to CO could be attributed to the number of active sites, reaction kinetics, and the stabilization of key intermediates, as well as the mass transport of reactants, intermediates and products. This work provides new insight into the loading effect, an important reactivity descriptor determining the CO₂RR performance.

Key words: electrochemical carbon dioxide reduction reaction, Pd/C catalysts, loading, electrolyte, selectivity

中图分类号:

O646

高敦峰，阎程程，汪国雄，包信和. Pd/C催化剂用于CO₂电化学还原生成CO:Pd载量的影响[J]. 电化学（中英文）, 2018, 24(6): 757-765.

GAO Dun-feng, YAN Cheng-cheng, WANG Guo-xiong, BAO Xin-he. Pd/C Catalysts for CO₂ Electroreduction to CO:Pd Loading Effect[J]. Journal of Electrochemistry, 2018, 24(6): 757-765.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.13208/j.electrochem.180845

https://electrochem.xmu.edu.cn/CN/Y2018/V24/I6/757

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Pd/C催化剂用于CO₂电化学还原生成CO:Pd载量的影响

Pd/C Catalysts for CO₂ Electroreduction to CO:Pd Loading Effect

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