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dc.contributor.author高敦峰
dc.contributor.author阎程程
dc.contributor.author汪国雄
dc.contributor.author包信和
dc.contributor.authorGAO Dun-feng
dc.contributor.authorYAN Cheng-cheng
dc.contributor.authorWANG Guo-xiong
dc.contributor.authorBAO Xin-he
dc.date.accessioned2019-01-18T01:06:06Z
dc.date.available2019-01-18T01:06:06Z
dc.date.issued2018-12-28
dc.identifier.citation电化学,2018,24(06):757-765.
dc.identifier.issn1006-3471
dc.identifier.urihttp://dx.doi.org/10.13208/j.electrochem.180845
dc.identifier.urihttps://dspace.xmu.edu.cn/handle/2288/171102
dc.description.abstractCO2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.
dc.description.abstractNanostructured 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.
dc.description.sponsorshipWe 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).
dc.language.isozh
dc.publisher厦门大学《电化学》编辑部
dc.relation.ispartofseries庆祝衣宝廉院士八十华诞专辑
dc.relation.ispartofseriesSpecial Issue in Honor of Professor Baolian Yi on His 80th Birthday
dc.source.urihttp://electrochem.xmu.edu.cn/CN/abstract/abstract10497.shtml
dc.subjectCO2电化学还原
dc.subjectPd/C催化剂
dc.subject载量
dc.subject电解质
dc.subject选择性
dc.subjectelectrochemical carbon dioxide reduction reaction
dc.subjectPd/C catalysts
dc.subjectloading
dc.subjectelectrolyte
dc.subjectselectivity
dc.titlePd/C催化剂用于CO2电化学还原生成CO:Pd载量的影响
dc.title.alternativePd/C Catalysts for CO2 Electroreduction to CO:Pd Loading Effect
dc.typeArticle
dc.description.note作者联系地址: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
dc.description.noteAuthor's Address: State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China
dc.description.note通讯作者E-mail:wanggx@dicp.ac.cn;xhbao@dicp.ac.cn


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